Sustainability 13 09604 v2

sustainability
Review
A Systematic Review of the Most Recent Concepts in Smart
Windows Technologies with a Focus on Electrochromics
Marcin Brzezicki
Faculty of Architecture, Wroclaw University of Science and Technology, Prusa 53/55, 50-317 Wroclaw, Poland;
marcin.brzezicki@pwr.edu.pl; Tel.: +48-71-320-63-10
Abstract: In the context of sustainability and in the face of ambitious goals towards the reduction of
CO2 emission, the modification of transparency in architecture becomes an important tool of energy
flow management into the building. Windows that dim to stop the energy transfer reduce the cooling
load in the building. Recently, however, the latest achievements in the development of electrochromic
materials allowed us to integrate some additional—previously unknown—functionalities into EC de-
vices. The purpose of this paper is to provide a systematic review of recent technological innovations
in the field of smart windows and present the possibilities of recently established functionalities. This
review article outlines recent general progress in electrochromic but concentrates on multicolour and
neutral black electrochromism, spectrally selective systems, electrochromic energy storage windows,
hybrid EC/TC systems, OLED lighting integrated with the EC device, and EC devices powered by
solar cells. The review was based on the most recent publication from the years 2015–2020 recorded
in the databases WoS and Scopus.
Keywords: smart glass; smart window; electrochromic

Citation: Brzezicki, M. A Systematic

Review of the Most Recent Concepts
in Smart Windows Technologies with 1. Introduction
a Focus on Electrochromics. Humans need daylight to live a healthy life. Vitamin D is synthesised only in the
Sustainability 2021, 13, 9604. https://
presence of sunlight. The physiological diurnal cycle of rest and activity is also governed by
doi.org/10.3390/su13179604
the day/night cycle. The provision of an adequate amount of daylight indoors is, therefore,
a matter of health and well-being. Daylight is allowed through openings into buildings.
Academic Editors: Sivanand
Windows provide the illumination of rooms where people live. However, a positive impact
Somasundaram and Swapnil Dubey
of contemporary windows in the building is appreciable “as long as they do not cause glare,
thermal discomfort, or a loss of privacy” (Hellinga [1]). Together with the visible part of the
Received: 10 July 2021
Accepted: 23 August 2021
daylight spectrum, heat (an infrared portion of the spectrum) is also transmitted through
Published: 26 August 2021
glazing into the rooms, resulting in internal temperature build-up. Mechanical removal of
excessive heat from a room involves high energy consumption and high environmental
Publisher’s Note: MDPI stays neutral
costs, such as carbon footprint and exhaustion of non-renewable materials. Buildings
with regard to jurisdictional claims in
are, therefore, of special concern as they are responsible for 30–40% of the world’s energy
published maps and institutional affil- consumption. Cooling, especially, has grown strongly in importance in recent years.
iations. Indeed, more energy is required to cool buildings than to heat them [2]. Therefore, in
light of the ongoing climate change and global warming, technologies designed to reduce
energy demand in the warm season of the year are receiving particular attention because
of their significance in achieving the 17 sustainable development goals defined by United
Copyright: © 2021 by the author.
Nations [3], with particular attention to goal 11 (sustainable cities and communities) and
Licensee MDPI, Basel, Switzerland.
goal 9 (fostering innovation). Any technology that prevents heat build-up in a building
This article is an open access article
translates into energy savings and reduction of CO2 emissions. In addition, heat loss might
distributed under the terms and contribute significantly to the overall energy balance. Window frames—as an important
conditions of the Creative Commons element of the system—are modelled to evaluate the thermal transmittance to reduce the
Attribution (CC BY) license (https:// energy requirement of the whole building [4].
creativecommons.org/licenses/by/ The term “smart window” was coined by Granqvist in 1985 [5]. From the early 1980s,
4.0/). smart glazing has been a rapidly developing innovative technology that is aimed to help
Sustainability 2021, 13, 9604. https://doi.org/10.3390/su13179604 https://www.mdpi.com/journal/sustainability

Sustainability 2021, 13, 9604 2 of 25
manage energy transfer through the building’s envelope, evading unnecessary “cooling
and heating of indoor air” [6]. The use of smart glass, which helps to regulate the amount
of light (and heat) entering a building, is one of the possible ways to reduce energy con-
sumption in buildings while maintaining an appropriate level of comfort for users. Smart
glass greatly influences the building envelope performance in (i) thermal management,
(ii) daylight harvesting and regulation, (iii) reduction of glare, (iv) maintenance of views,
(v) power capture, and finally (vi) activating the envelope as information display [7]. Some
technologies are currently available on the market, although—in light of the many short-
comings of the existing solutions—smart glass is the subject of ongoing “intensive research
aimed at improving the technology and its widespread use” [8].
1.1. Method and Eligibility Criteria

The data for the review were acquired from international scientific databases (WoS
and Scopus—last search 28 January 2021), and the manufacturers’ websites (e.g., https:
//www.saint-gobain-glass.com/products/priva-lite (accessed on 20 August 2021), and
other open channels (Google Scholar). The reports analysed were published in English.
Candidate search terms (“keywords”) were identified by examining the words in the titles
and abstracts of the studies included in the previous reviews of smart glass technologies
(see Section 1.3. for the detailed description). The search strategy was validated by cross-
testing on different databases whether it produces similar results (WoS and Scopus), and
the results of this test were positively evaluated. Search strategy for all databases included
the papers that featured keywords “smart glass”, “smart window” and—after the first
refinement was made—also “electrochromic” keyword.
The review was carried out by a single researcher (M.B.). The inclusion algorithm (the
procedure to decide which reports were included in the review) consisted of three steps:
(i) whether the technology can “dim-on-demand”, (ii) whether the technology is re-
versible, and (iii) the reported technology reached the stage of a small-scale working
prototype (big enough to measure the optical transmittance). Certain studies were ineli-
gible to be included in the review as the outcomes were out of the scope of the interest,
e.g., because the results were not scalable or the technology did not reach the stage of the
working prototype.
Study selection was a multi-stage process in which potentially eligible studies were
first identified from screening titles and abstracts. The researcher (M.B.) reviewed titles
and abstracts of the 1850 records (published in the years 2015–2020) and, after duplicates
removal, 1092 records were screened, from which 145 full-text documents were reviewed,
and finally, 105 (each cited) papers were included in the review. Later, a cross-check of the
citations was performed, however, no extra articles that fulfilled inclusion criteria were
found in these searches (a flow diagram is available see Supplementary Materials). Because
of time constraints, only approx. 30% of the titles and abstracts were dually screened; for
the rest, a single screening was used. A recent study in epidemiology showed that single
abstract screening misses up to 13% of relevant studies [9]. Nevertheless, the author is
confident that this methodological limitation would not change the overall conclusions
of this review in engineering, as the most recent smart window technologies are well
represented in the analysed reports.
Data extraction from the studies was based on the data given by the authors; a small
spreadsheet was designed to collect and compare extracted data. The detailed information
about the metric is given in Section 2, General Classification and Metrics.
Given the complexity of the report being investigated, the attempt was made to
categorise the included reports/papers along four dimensions: (1) passive vs. active tech-
nologies, (2) the stimulus that is used to activate the dimming behaviour, and (3) technology
scale (micro-, nano-scale). Some of the reports included technologies that had multiple
components (e.g., diming on the demand with photovoltaic effect). These reports were
categorised according to the main component (the component that the primary authors
emphasised, e.g., by stating the keywords).
Results of individual studies were presented in the form of tables, comparing the
different results achieved by individual teams of researchers. No statistical synthesis was
conducted. The risk of missing or including unclear information from the reported studies
is limited, as information concerning a single smart window technology is derived from
at least a few sources. This fact increases the credibility of information and reduces the
risk of bias. The risk of bias is also reduced by the fact that all analysed reports were
peer-reviewed publications. The risk of bias due to missing results is marginal, as the
results come from numerous sources included in the paper.
Below-described solutions were studied and systematised to compare the most recent
concepts and possible areas of future development in the years 2015–2020.
The main/core scientific method that was used is a desk study; no automation tools
were used. The main tool used was a PC with an internet connection.
1.2. Rationale behind the Presented Review and Objectives

The current review was considered necessary as previous reviews were either focused
on the other area (perspective) or outdated, e.g., reported in the year 2016—previous
reviews are discussed in the detail in Section 1.4.
The presented review examines the results of the most recent research and extracts the
technologies that are the most promising in the context of the use in sustainable solutions
in architecture and building engineering. The objectives of the review were to give a bird’s
eye view on novel active smart glass technologies (active meaning = dimming on demand)
with the focus on electrochromic devices (further addressed as ECDs) which appeared in
the years 2015–2020 and were published.
This review aims to present the most recent concepts in active smart glazing that
present possible—i.e., available in the future—functionalities, without deeply diving into
the issues of material engineering. It is hoped that the materials that are currently in
the stage of development would finally result in commercially available products in the
building industry.
1.3. Originality of the Paper

The purpose of this paper is to give an overview of the most recent solutions in smart
glass, with special attention being given to the phenomenon of electrochromism and its use
in technical devices. The original aim is to report on the cutting-edge laboratory solutions,
which might outline the potential areas of future development. The original approach
presented is concentrated on the comparison of the parameters of the devices, mainly
visual and NIR modulation. Optical metrics are especially important when it comes to
practical application in building engineering and in architecture, from which the author
of the paper derives. Metrics are used to show the performance of different solutions
that are responsible for reducing the carbon footprint and thus contribute to sustainable
development (e.g., NIR modulation that reduces the temperature build-up in the room).
The original method of the presentation of the data in the presented paper derives
from the simplified presentation of data that was pioneered by Ke et al. [10] but has been
improved. Modulation data (solar, vis and NIR) presented in the paper could be easily
compared and are more accessible for a wider audience. Due to the space limitations in the
paper, all available parameters related to all the metrics are presented in Supplementary
Materials, as well.
A review-type paper has its own rules. As in the case of similar works, in this study,
WoS and Scopus databases were used to retrieve the most recent publications related to
featured keywords: “smart glass”, “smart window”, and also “electrochromic”. Despite
the strict definition of what a review-type paper is, some innovations can be distinguished
in the presented work. These are: (i) the use of the PRISMA protocol to process the data
(PRISMA flow chart and PRISMA 2020 Checklist are available as Supplementary Materials);
(ii) the use of the objective evaluation of presented technologies based on the parameters
given by the authors; and (iii) the recognition of the relationship between results of the
laboratory experiments and potential future application of presented technologies. Further,

by comparing research results, technologies, and types of innovation, a simplified typology
of technologies and featured systems could be established. The results of the review could
also be used to find points at which emerging technologies (TRL Proof-of-Concept) and
final products (TRL System Adequacy Validated) might overlap in future. The paper
also offers a more accurate understanding of how the different research groups can be
cross-fertilised to strive for innovation.
1.4. Previous Research, State of the Art

The issues of smart glass were recently (2015–2020) extensively studied, mainly in the
area of material science, nano-chemistry, and energy simulation. In total, almost 2000 research
papers were published on the topic in the years 2015–2020, some of which were review
papers. The extensive review of the energy-saving potential of commercially available
solutions based on the manufacturer’s data was given in 2019 by Tällberg et al. [11] fea-
turing also building energy simulation of the active smart windows. A review of active
dynamic windows for buildings was also provided by Casini [12,13], with particular
attention given to the main active chromogenic technologies on the market. Ongoing
advances in the area of ECD and materials, its modes of operation in different categories
alongside existing difficulties, and suggestions to improve performance are summed up
by Rai et al. [14]. Ge et al. [15] have provided a less general and more detailed review
of one-dimensional TiO2 nanostructured materials for environmental and energy appli-
cations. A most recent review of micro shutters for switchable glass was provided by
Lamontagne et al. [16]. An interesting lecture summarising the most recent EC technologies
was published by Kraft [17] while Granqvist et al. [18], in their review, concentrated on the
device longevity and lifetime prediction of EC solutions. In 2019, Aburas et al. provided
a review on thermochromic smart window technologies for building applications [19].
Recent reviews were provided by Ke et al. [10] and Wang et al. [20], while Park et al.
have concentrated on the improvement in the energy performance of building envelopes
incorporating electrochromic windows [21]. In 2021, Feng et al. provided the most re-
cent critical review of fenestration/window system design methods for high-performance
buildings [22]. (See Table 1.)
Table 1. Previously conducted review research on the topic.
No. Team Year Focus

1 Tällberg et al. 2019 energy saving potential of adaptive and controllable smart windows
2 Casini 2018 active dynamic windows for buildings
3 Rai et al. 2020 recent advances in electrochromic devices
4 Ge et al. 2016 a review of one-dimensional TiO2 nanostructured materials
5 Lamontagne et al. 2019 review of micro shutters for switchable glass
6 Kraft 2019 general issues of electrochromism
7 Granqvist et al. 2019 advances in electrochromic coating technology
8 Aburas 2019 thermochromic smart window technologies for building application
9 Ke at al 2019 perspectives on the future of electrochromic
10 Wang et al. 2015 review of switchable materials used in smart windows
energy performance of building envelope incorporating
11 Park et al. 2019
electrochromic windows
a critical review of fenestration/window system design methods for
12 Feng et al. 2021
high-performance buildings
2. General Classification and Metrics

In general, the term “smart glazing” or “smart window” refers to various technological
solutions that change light transmission through the material (usually glass). Optical
transparency can be altered qualitatively or quantitatively. A qualitative change is made
when a transparent glass pane turns into a translucent one (the amount of light does
not significantly change, while the light becomes scattered). A quantitative change is
made when the amount of light changes, e.g., the transparent panel is dimmed and
blocks the portion of incoming radiation (so-called: coloured/darkened state vs. bleached
state). Qualitative technologies are used when privacy is required, while quantitative ones
are used to protecting buildings from overheating and users from glare. Although the
techniques used to achieve such effects have evolved, they generally fall into one of the two
categories mentioned above [8]. The layers of smart materials are usually incorporated into
the standard insulating glass unit on the surface No. 2, which means the internal surface of
the external pane.
The objective of this work is also to provide the readers with information about the
smart window properties. However, it has to be stressed, that the information about the
characteristics is difficult to systematise, as the researchers are using different metrics, e.g.,
the team of Mori [23] is measuring the difference in the increase in in-room temperature
when the micro blinds are on and off, without any reports considering optical properties.
Metrics
Smart windows, in general, might be characterised by several solar radiation glazing
factors, including visible solar transmittance, solar transmittance, ultraviolet solar trans-
mittance solar material protection factor, solar skin protection factor, external visible solar
reflectance, internal visible solar reflectance, solar reflectance, solar absorbance, emissiv-
ity, solar factor, and colour rendering factor. All these factors are exhaustively discussed
by Tällberg et al. [11], based on Jelle [24], who provides a mathematical and physical
background for all the measures.
Comparison of these solar quantities for different scientific teams is difficult, as differ-
ent teams concentrated on different metrics, usually the one that illustrated the result of
their research in the most appropriate way.
The term “smart window” is used to describe the whole range of different technolo-
gies that can either (i) self-regulate the passage of solar radiation (thermochromic and
photochromic) or (ii) regulate the transparency by the application of an external voltage.
This change is achieved either by regulation of the absorbance or the reflectance, as ad-
dressed in detail by Jelle [24]. Jelle also presents two figures, illustrating the difference
between the change in transmittance by a movable reflectance edge and the change in
transmittance by a movable absorbance edge. Moreover, technologies exist that feature
combined regulation of both absorbance and reflectance. An exemplary diagram—in
a different graphic form—is given in Figure 1 for the illustration.
Nguyen et al. state that “most of ( . . . ) smart window research focuses only on
modulation within the visible range of the solar radiation ( . . . ) However, since nearly 50%
of solar energy comes from IR radiation” [25], dynamic modulation of IR radiation should
be also included in the review. To quantify and compare solar characteristics of different
glass materials (or the same material in a different energy state), the three most popular
metrics are used: (i) solar radiation transmittance Tsol or (ii) visible (luminous) transmittance
Tvis and (iii) near-infrared transmittance TNIR . Visible (luminous) transmittance is usually
measured at 550–660 nm, while TNIR is usually given for the range of 1000–1600 nm.
Many authors also describe the change in light-transmitting properties by describing the
“modulation”. The modulation level is calculated by subtracting the radiation glazing
factors for the same smart window at the “high and low potentials” [24], e.g., according to
the formulas below:
∆Tsol = Tsol(bleached) − Tsol(coloured) (1)
∆Tvis = Tvis(bleached) − Tvis(coloured) (2)
∆TNIR = TNIR(bleached) − TNIR(coloured) (3)

For the sake of simplicity, the modulation will be used thought the paper to char-
acterise the presented solutions and technologies, however, three different values of the
modulation will be given of ∆Tsol , ∆Tvis , and ∆TNIR (Equations (1) and (3)) as given by the
different authors in their papers. However, it must be stated that the authors also provide
Sustainability 2021, 13, x FOR PEER REVIEW 6 of 26
other metrics, depending on the characteristics of ECD measured. All detailed metrics that
were available in the original papers are given in the Supplementary Materials.
Figure1.1.Diagram
Figure Diagramillustrating
illustratingthe
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transmittance in in smart
smart glass
glass device
device by by
the the regulation
regulation of
of absorbance.
absorbance. Diagram
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by the author
author modelled
modelled on the
on the graphs
graphs by Jelle
by Jelle [24].[24].
3. Results—Passive
Nguyen et al. state Technologies
that “most of (…) smart window research focuses only on modu-
lation
The within the visible range
light transmission of the solar
modulation through radiation (…) However,
smart windows can besince nearly
achieved by50%
many of
solar energy
different comes from
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best examples T or (ii) visible
ofsolpassive (luminous)
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tance Tvis andcoatings (glass that dims
(iii) near-infrared under theTinfluence
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of 1000–1600
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The modulationare usuallylevelsimpler”
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subtracting the passive technologies
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the “high and low reporting
potentials” that vanadium dioxide
[24], e.g., according
(VO
to the) seems to
2 formulas below: be a promising alternative for developing thermochromic glazings since
its “critical” temperature at which the temperature-dependent properties are changed is
at approx. 68 ◦ C, not very far from ΔTthesol = Tsol(bleached) − Tsol(coloured)
usual room temperature [26]. The development (1)
of thermochromic—based mainlyΔT onvis vanadium
= Tvis(bleached) −dioxide
Tvis(coloured)(VO2 )—has led to the design (2)
of spectrally selective smart windows which are capable of shielding ∆TNIR = 96.2% of
the NIR irradiation and transparency ΔTNIR =modulation
TNIR(bleached) − TofNIR(coloured)
∆Tvis = 32.9% [27]. In this device, (3)
Lee etFor al. have usedoftungsten
the sake simplicity, oxide
the(WO 3 )-based will
modulation EC and vanadium
be used thought oxide
the (VO
paper 2 )-based TC
to charac-
integrated into a single device. Another interesting thermal-based
terise the presented solutions and technologies, however, three different values of the technology is presented
by La et al. inwill
modulation a device
be given thatofcan
ΔTcontrol both the transmittance of solar radiance with the
sol, ΔTvis, and ΔTNIR (Equations (1) and (3)) as given by the
use of thermally
different authorsresponsive material
in their papers. [28]. The
However, teambe
it must isstated
using thatthe layer of polyampholyte
the authors also provide
hydrogel
other (PAH),
metrics, which
depending is exposing
on the the phase
characteristics transition
of ECD in temperatures
measured. All between
detailed 25 and
metrics that
55 ◦ C (transparency to opacity). In a device, a layer of PAH is heated by an array of electric
were available in the original papers are given in the Supplementary Materials.
heaters made of printed elastomeric composite.
Photochromic windows
3. Results—Passive are also actively researched, with the most recent significant
Technologies
results. In 2019, Timmermans et al. [29] reported dual responsive smart widow regu-
lated The
bothlight transmission
by specific modulation
wavelengths of lightthrough smart windows
and electrical triggers. canThebe achieved by many
optical response
different technologies. These can be divided into passive
was due to the content of diarylethene dye incorporated in liquid crystals. Enhanced and active technologies. Passive
technologies are thosephotochromic
colouration/bleaching in which the performance
change in thewas statusalsoofreported
a window (e.g.,bydimming)
in 2019 the team of re-
sults from an external stimulus that could not be influenced (e.g., surrounding parame-
ters) without any external regulation. The best examples of passive technologies are glass
with photochromic coatings (glass that dims under the influence of sunlight) or thermo-
chromic coatings (glass that dims under the influence of heat). Some authors—e.g., Park
et al.—claim that “passive (technology) is typically more suitable for building application
Li et al. [30]. The device was based on tungsten trioxide (WO3 ) that constituted a composite
matrix with polyurethane (PU) and polyvinyl pyrrolidone (PVP).
Photo- and thermochromic smart windows are promising technologies, but unfortu-
nately, they do not actively influence the transmission modulation of smart windows. For
example, the photochromic glass will be dimmed on a sunny winter day when the green-
house effect is desired, especially in passive buildings. Similarly, the thermochromic glass
will be dimmed on warm days, even if we want to keep the light transmission unchanged,
for the reason of, e.g., keeping the proper level of daylight in the room.
An important element of passive technologies is also Phase Change Materials, which
react to heat by changing the state from solid (light-scattering) to liquid (light-transmitting).
It is important to remember that PCM offers control over the quality of light but is not
possible to control on-demand. It was also recently reported by Chou et al. that a passive
smart window was proposed with the use of thermotropic hydrogel containing graphene
oxide, which changes the state from opaque to transparent under the influence of so-
lar radiation. In this solution, the hydrogel can effectively convert the “photoenergy
of sunlight into thermal energy and cause the smart glass to reach an opaque state ow-
ing to the increased temperature of the hydrogel heated by solar light” [31]. In 2019,
Kim et al. [32] recently presented a device featuring a phase transition of the thermosensi-
tive hydrogel that exhibited optical transition from transparent to opaque state. The phase
of the gel was controlled by the film of nanopatterned silver, which effectively generated
the heat by the Joule-heating mechanism. Table 2 features the schematic illustrating all the
described technologies:
Table 2. Typological diagram illustrating the described technologies. Diagram by the author.
Type Stimulus Technology Featured Systems

Heat—Thermochromic
Passive technologies: Light—Photochromic
Heat—Phase Change Materials
Gas—Gasochromic
Fluid—Optofluidic glass
Microsystems
Microwrinkled Nanometric Films
Polymer dispersed liquid crystal
Suspended particle devices (SPD)
Multicolour EC
Active technologies:
Electrical current: Neutral black electrochromism
Spectrally selective systems
NIR/VIS
Electrochromic: Electrochromic energy storage
window
Hybrid EC/TC solutions
EC devices powered by solar cells
Nanostructures
4. Results—Active Technologies
Active solutions are implemented using several groups of different technologies. They
can be divided into several groups, depending on the stimulus that causes the transmission
modulation of the smart window.
4.1. Gas
Gasochromic windows (GC) can change their transmittance in the presence of gas—
usually diluted hydrogen with some addition of argon—that induces the reduction reaction
of the gasochromic layer, resulting in colouring. Two main substances are used: (1) a layer
of tungsten trioxide (WO3 ) covered by a very thin layer of silver or (2) magnesium yttrium
(Mg-Y) alloy. In the first technology, Wittwer et al. produced porous, columnar film of WO3
by sputtering, and used a low concentration of H2 to change the colour of gasochromic film.
The reverse reaction is obtained with the use of O2 , which bleaches the film to the original
transparent state [33]. In the second technology, Liang et al. produced a device with a WO3
layer, which—after being exposed to diluted H2 at room temperature—is hydrogenated,
which leads to the blue tinting in approx. 5 s (coloured state). The dehydrogenation
process is initiated by the use of diluted O2 , which leads to an increase in transmittance
(bleaching) [34]. Additionally, magnesium yttrium (Mg-Y) alloys could be also used in the
manufacturing of switchable mirrors. The energy efficiency of the latter technology in the
building is currently discussed as the gasochromic Mg-Y layer does effectively block the
heat, but the corresponding lower solar transmittance reduces daylight availability and the
energy consumption for artificial lighting increases.
4.2. Fluid
Optofluidic glass is based on the principle of refractive index matching. The optoflu-
idic window features two layers of transparent material (one of which is roughened/pattered
from the inside) and an air cavity between. A roughened surface causes the light rays
to reflect and scatter, reducing the light transmittance. When the fluid of specific refrac-
tive index matching with the index of the material with roughened/patterned surface is
introduced into the cavity, light transmittance is increased. Optofluidic smart windows
suffer from many potential maintenance problems, including leakage and the influence of
the potential low air temperature (below the freezing point of the liquid), but recently, 3D
printing technology allowed for an evident step forward allowing for the manufacture of
sealed modules using VeroClear photopolymer. In [35], the team of Wolfe et al. present a
novel optofluidic smart glass prototype capable of modulating visible light transmittance
(∆Tvis ) from 8% to 85% using air (reflective state), water (diffuse transmittance state), and
methyl salicylate for specular transmittance. The refractive index of methyl salicylate and
photopolymer VeroClear are matched.
Recently, Heiz et al. [36] also presented smart glass that is based on the magneto-
active liquid (magnetite nanoparticles in monopropylene glycol) circulating in the cavi-
ties/channels parallel to the surface of the glass. The magneto-active liquid is loaded with
magnetic nanoparticles, the density of which can be controlled through remote switch-
ing in a magnetic particle collector-suspender device in which permanent magnets or
electromagnets are used to draw the magnetic nanoparticles from the liquid.
4.3. Electrical Current

Smart windows that are controlled by electrical current include a large group of
solutions that will be addressed below. Their common feature is that the change in the state
of the window requires the flow of electrons (charged ions)—they are electrically activated.
This brief review is given below follows the scale of the technology (from macro, through
micro- to nano-solutions).
4.3.1. MEMS-Based Microsystems

In general, micro-blinds made of curling electrodes actuated by electrostatic forces
belong to the category of microelectromechanical systems [16]. Microelectromechanical
systems (MEMS) include microscopic devices, particularly those with moving parts. Micro-
blinds are composed of a trapezoid- or rectangle-shaped curling micro-thin metal blinds on
a transparent conductive oxide (TCO). In the absence of voltage, the blinds are curled and
light passes through. Once the voltage is applied, the difference of potential is created and
the electrostatic force stretches the micro blinds so that light is blocked. Most micro shutters
are based on standard microelectronic fabrication processes (e.g., e-beam evaporation,
magnetron sputtering, optical lithography). The main advantages of micro shutters are fast
(virtually instant) switching time, neutral colouration of the transmitted light, low power
consumption, and stability for UV and temperature. Few institutions currently work on
the development of the micro-blinds including the University of Kassel, Germany [37];
Institut National d’Optique, Canada; and University of Tokyo, Japan [23].
Another type of MEMS is micromirror arrays. Each unit consists of the mirror, the
hinge, and the steering mechanism. Micromirror glass is composed of millions of electro-
statically actuatable micromirrors that can guide and control light dynamically (typical
dimensions are 150 × 400 mm2 ). Those systems are used to guide the daylight within
the façade, not to block it. Due to the size of the individual mirror, the system is imper-
ceptible for the human eye. The main advantage of the system reported by Hillmer et al.
is that the light is reflected, not absorbed, and has low energy consumption, as low as
0.2 mW/m2 [38].
4.3.2. Microwrinkled Nanometric Films

As was already mentioned above, the roughness of the transparent surface scatters
the light. This phenomenon was exploited in the electrically controlled smart glass de-
vice that is using transparent soft media with electrically tuneable surface roughness for
transparent-to-translucent switching. The system in a “wrinkled” state scatters the light,
while in a “stretched” state becomes transparent. The media used as a membrane in the
system is a TiO2 nanometric thin film that is sandwiched between transparent conductive
polymers. This system survives 1000 cycles and has a strikingly low power consumption of
0.83 W/m2 [39].
4.3.3. PDLC (Polymer Dispersed Liquid Crystal)

A smart window based on the Polymer Dispersed Liquid Crystals (PDLCs) features
liquid crystal dispersions in a polymer matrix (simply, microdroplets of liquid crystals
encapsulated in a polymer), sandwiched between two transparent conducting electrodes.
They scatter light in their OFF state because the molecules liquid crystals are randomly ar-
ranged, but become transparent when the voltage is applied in their ON state (when
the crystals are ordered) [40]. To remain transparent, PDLC smart windows require
the continuous application of an electric field, with an average power consumption of
20 W/m2 as stated by Lampert in [41]. LC molecules embedded in the polymer matrix can
be oriented on the demand, thus the transmission could be gradually regulated, as in [42].
This technology is widely used in privacy windows and projection displays because of the
fast switching speeds. One of the most widely known commercially available products on
the market is Privalite by Saint-Gobain [43].
The latest PDLC technology includes the use of membranes containing liquid crystals
with the parameters of an opaque OFF state with a TOFF = 0.5%, and a transparent ON state
with a TON = 65% (difficult to translate to ∆Tvis as the haze is described) when the system
is switched on, as presented by De Filpo et al [44]. Liquid crystals and polymers with
other additives and other forms are also studied. Kim et al. solved the dye contamination
problems by encapsulating the dye in monodispersed capsules. Using this technology,
a fabricated “dye-doped PDLC had a contrast ratio of >120 at 600 nm” [45]. Although
PDLC systems are mainly used for privacy purposes, they can also achieve energy savings.
Alghamdi et al. recently reported that a system comprising of sensors with an Arduino
to control the percentage PDLC glass transparency produced 39% in energy savings com-
pared to the standard systems in a hot climate [46]. Sol et al. recently reported a smart
window featuring liquid crystalline luminescent solar concentrator that allows switching
the window between three states: “coloured” for increased light absorption, “light” for
transparency (5% of haze), and “scattering” for diffuse transmission of light (66% of haze).
In the LSC system, luminescent molecules embedded in a polymer absorb light and reemit
downshifted spectrum that is channelled by total internal reflection to the edge of the
device, where it is collected by PV cells [47].
4.3.4. SPD Windows

Suspended particle devices (SPD) smart windows work on a similar principle to PDLC,
but instead of liquid crystal, they use a suspension of fine, strongly absorbing particles.
In the OFF state, the particles are randomly arranged and block the passage of the light.
When the voltage is applied in the ON state, the particles align to let the light through. SPD
device requires approx. 5 watts per m2 to remain transparent, as reported by Schwarz [48].
Light transmission values range from about 64–80% in the clear state to 0.5–12% in the
dark state [49] as reported by Ghosh. However, it must be noted that due to the number
of technological problems, stability, and particle settings, the development of suspended
particle devices has been recently slowed. International scientific databases show only less
than 10 reports submitted in the years 2015–2020.
The overview of the presented technologies is summarised in Table 3.
Table 3. The comparison of the performance of non-electrochromic devices, including the technologies, where the data
are available.
No. Team Year Type ∆Tsol ∆Tvis Remarks

1 Wittwer et al. 2004 Active gasochromic 71% 72% Switching from transparent
2 Liang et al. 2019 Active gasochromic 42% n/a to mirror state
3 Wolfe et al. 2018 Optofluidic n/a 77% Clear to foggy

Magneto-Active Magnetic particles
4 Heiz et al. 2017 95% n/a
Liquid in liquid
Micromirrors. The team only
measured a temperature
5 Hillmer et al. 2018 Microelectromechanical n/a n/a
build-up
in the room.
6 Mori et al. 2016 Electrostatic n/a 17% Micro blinds
Microwrinkled
7 Shrestha et al. 2018 n/a 79.2% haze
TiO2 Films
8 Lampert 1998 PDLC n/a 40% haze
9 Lampert 2004 PDLC 60% 57% haze Transparent to
10 Murray et al. 2016 PDLC n/a 25–29% haze translucent switching
11 De Filpo et al. 2019 PDLC n/a 64% haze

12 Sol et al. 2017 PDLC n/a 61% haze
13 Ghosh 2017 SPD 46% n/a
4.3.5. ECDs
Electrochromic windows are—according to the survey performed by the author—
the leading branch in smart window applications, constituting the majority of search
results in international science databases in the years 2015–2020. The technology has been
known since the 1960s, when S.K. Deb published important work on the characterisation
of molybdenum and tungsten oxide thin films [50]. He had originally observed that some
types of metal oxides can change the colour to blue (and brown) due to the reduction
reaction and become uncoloured again due to the oxidation reaction.
Electrochromic devices (ECDs), in general, are used for applications ranging from
commercialised smart window glasses, goggles, and auto-dimming rear-view mirrors [51].
Recent achievements in electrochromic smart windows technology call for a review study
of the most recent concepts that are used to obtain hitherto impossible results, and are
studied in detail in the following section.
5. Electrochromic Devices
5.1. Switching Mechanism
Electrochromism is a reversible chemical phenomenon, where the electrochromic
material changes its colour when the voltage is applied. As Kraft writes, the substances,
“which change from an uncoloured oxidised state to a coloured reduced state by electro-
chemical reduction are called cathodic electrochromic, whereas compounds which change
from an uncoloured reduced to a coloured oxidised state are called anodic electrochromic
compounds” [17]. EC windows operate on the principle of the reversible electrochemical
intercalation of positive ions (e.g., H+ , Li+ , Na+ ) accompanying the insertion of charge
balancing electrons into the multivalent transition metal oxides (e.g., WO3 , NiO, IrO, MoO3 ,
V2 O5 ) [27]. The basic chemical reaction featuring the most popular cathodic electrochromic
compound WO3 transforming from transparent to blue is given below:
MxWO3 WO3 + xe− + xM+ x ≤ 0.3 (4)
while nickel oxide (NiO) can be coloured anodically to a brown colour in a reaction of
LiNiO NiO + Li+ + e− (5)
However, other transition metal oxides such as Co3 O4 , MoO3 , V2 O5 , TiO2 also exhibit
electrochromic properties [52,53]. Prussian blue (iron ferrocyanide)—originally reported
by Mortimer [54]—also currently is studied as a material presenting some electrochromic
behaviour [55]. Recently, polystyrene sulfonate (PEDOT:PSS) were researched as exhibiting
electrochromic properties, as well as presented by Singh [51].
5.2. Electrochromic Device Architecture

Electrochromic devices typically consist of five thin layers that are located (sand-
wiched) between two panes of glass or flexible polyester foil: two external layers of
transparent conductive films (usually indium tin oxide, ITO) and the counter electrode
(Ni-oxide-based film), electrolyte, and electrochromic electrode in between (W-oxide-based
film). The counter electrode is used for ion storage, the electrolyte for conducting ions, and
the electrochromic electrode for attracting ions. When the electrical current is applied, the
ions stored in the counter electrode (bleached state) migrate through the electrolyte to the
electrochromic electrode, resulting in the colouration (coloured state). The mobile ions
should be small. Hydrogen protons (H+ ) or lithium (Li+ ) ions are commonly used [18]. EC
device can be considered as an electrical battery in which the optical absorption is related to
its charge; therefore, the crucial component of an ECD is an electrolyte, which can be liquid,
gel, or solid, as addressed by Cannavale et al. [56]. The most popular ECD architecture is
pictured in Figure 2.
5.3. Simulated Energy Performance

Visible light transmission in commercially available electrochromic windows can vary
from 3.5% to 62% depending on their operating state [35]. This difference in transmittance
translates into energy savings in the building. Picollo et al. report that ECD is effective in
reducing heat loads in a cooling dominated climate during the summer season (optimal
when the cooling demand is dominant over the heating/lighting demand) [57], while
Cannavale et al. report overall yearly energy savings as high as 40 kW h/m2 /yr in the
hottest climates, assuming clear glazing as a benchmark [58]. Park et al. report a reduction
of 8.43% in energy consumption, relative to the reference model when EC device is used,
and in a different paper, a reduction of about 11,207 kWh/yr (of 8.89%) for heating/cooling
and lighting energy [21]. Generally, Park et al. report the effectiveness of EC technologies
particularly in office buildings for which the cooling energy consumption ratio is high.
Javad and Navid in 2018 showed a 50% temperature difference reduction between the floor
and ceiling, which is achievable with the use of EC windows [59].
Sustainability 2021, 13, x FOR PEER REVIEW 12 of 26
Figure2.
Figure 2. The
The most
most popular
popular ECD
ECD architecture.
architecture. Diagram
Diagram by
bythe
theauthor.
author.
5.4.
5.3. Most Recent
Simulated Concepts
Energy in EC Smart Windows
Performance
As is said above, EC technologies
Visible light transmission suffer from
in commercially many electrochromic
available problems that are currently
windows can
being addressed
vary from by62%
3.5% to many research teams
depending tackling
on their the challenges
operating state [35]. of thedifference
This EC windows. The
in trans-
concepts
mittanceoftranslates
the most into
recent solutions
energy are briefly
savings in thediscussed
building. below
Picolloand adequately
et al. compared
report that ECD is
in the tables and the Supplementary Materials.
effective in reducing heat loads in a cooling dominated climate during the summer season
(optimal when the cooling demand is dominant over the heating/lighting demand) [57],
5.4.1. Multicolour EC Solutions
while Cannavale et al. report overall yearly energy savings as high as 40 kW h/m2/yr in
Multicolour
the hottest solutions
climates, assumingare possible thanksas
clear glazing to athe co-existence
benchmark of Park
[58]. electrochromic
et al. report materi-
a re-
als with different redox potentials. This allows for colour change
duction of 8.43% in energy consumption, relative to the reference model when EC device that is different from the
blueish-transparent cycle that is known from tungsten trioxide (WO
is used, and in a different paper, a reduction of about 11,207 kWh/yr (of 8.89%) for heat- 3 ). Lee et al. [60] re-
cently reported a multicolour EC device using Co(OH) 2 /Ni(OH) 2 nanofilms.
ing/cooling and lighting energy [21]. Generally, Park et al. report the effectiveness of EC The nano-thin
double layers of Co(OH)2 and Ni(OH)2 were produced using two-step minute electrode-
technologies particularly in office buildings for which the cooling energy consumption
positions. The co-existence of electrochromic materials with different redox potentials
ratio is high. Javad and Navid in 2018 showed a 50% temperature difference reduction
allowed for the multicolour change (at −0.2, 0.2, and 0.5 V potentials) among yellow, green,
between the floor and ceiling, which is achievable with the use of EC windows [59].
and brown, and those changes were entirely reversible. Some combined polymers with
precisely tailored energy gaps have expanded the colour palette/gamut for electrochromic
5.4. Most Recent Concepts in EC Smart Windows
devices. The team of Liu et al. [61] reported an EC device capable of changing from
brown, Asdark
is said above,purple,
brown, EC technologies
to blue using sufferfreestanding
from many problems
copolymer that are currently being
P(PVK-co-EDOT) as
an electrochromic colouring layer. In the laboratory scale, when potentials were The
addressed by many research teams tackling the challenges of the EC windows. con-
applied
cepts of −
between the
0.9most
V andrecent
+0.5 V, solutions
the device arepresented
briefly discussed below and
an electrochromic adequately
behaviour with compared
a colour
in the tables and the Supplementary Materials.
reversibly changing from blue to purple. Electrochromic conducting polymers based on
the PEDOT structure offer different colours that could be switched electrochemically [62],
5.4.1.
as Multicolour
reported EC Solutions
by Argun et al. The transitions from transparent to magenta, or from blue
throughMulticolour
green to solutions
yellow are arepossible
possiblewiththanksthetoapplication
the co-existence of −0.1 Vmate-
of electrochromic
of potentials and
rialsV.
+0.9 with
Thedifferent
authors redox potentials.
also present This allows
a summary for colour
of different change
colours thatare
that is possible
different with
from
the
the use of the different polymers,
blueish-transparent cycle thatwith an even
is known fromgreater colour
tungsten palette:(WO
trioxide yellow-green-blue,
3). Lee et al. [60]
or blue-magenta-grey.
recently Futsch etEC
reported a multicolour al.device
[63] report
usingthe electrochromic
Co(OH) device thatThe
2/Ni(OH)2 nanofilms. is using
nano-
vanadium
thin double oxide (Vof
layers O
2 5 ) deposited
Co(OH) 2 and as a
Ni(OH)micrometric
2 were thick
produced film.
usingDepending
two-step on the
minute content
electro-
(different
depositions.weight
The percentages
co-existenceofofVelectrochromic
2 O5 and polymer ink PEDOT),
materials material changes
with different colours
redox potentials
from blue to green and orange, depending on the voltage applied
allowed for the multicolour change (at −0.2, 0.2, and 0.5 V potentials) among yellow, green,( − 1.0 V and +1.5 V).
The
and characteristic
brown, and thosefeature of vanadium
changes oxide is
were entirely the existence
reversible. Someofcombined
several oxidation
polymersstateswith
that offer tailored
precisely the possibility
energy of gapscreating multicolour
have expanded theEC windows/displays.
colour palette/gamut forThe papers on
electrochromic
the electrochromic properties of V2 O5 were recently published by Chu et al. [64] and
Mjejri et al. [65].
The main area of the application of multicolour EC windows is seen in architecture as
a decoration and possible information display.
5.4.2. Neutral Black Electrochromism

Neutral black electrochromism is a Holy Grail of EC devices. A neutral EC device
is supposed to absorb all the visible radiation ranging in 400–750 nm in the same degree,
and therefore, work as a grey filter. A typical EC device (e.g., based on WO3 ) is working
as a spectrally selective filter altering the colour of the light that is passing through the
device. It is usually filtering out specific wavelength ranges. An extensive review of
the colour rendering properties of different types of switchable glazing was provided by
Aste et al. [66]. Jarosz et al. claim, that black electrochromic devices “grant control over the
visible light intensity, indiscriminately of wavelength” [67].
One of the possible solutions to obtain neutral colouration is subtractive colour mixing,
usually by setting up a series of different filters that absorb or reflect different complemen-
tary wavelength ranges, and, in this way, finally providing the neutral colouration. As
it was originally reported by Passerini et al. [68] in 1990, the combination of cathodically
blue-colouring electrochromic such as WO3 and the nickel oxide that is an anodically
brown-colouring substance might produce an EC device that is changing the colouration
from transparent to neutral grey.
However, subtractive colour mixing is regarded as a difficult method in colour creation;
therefore, a few other concepts have been tested. These include (i) chemical copolymeri-
sation (different parts of copolymer absorbing defend wavelength ranges), (ii) physical
blending (by straightforward mixing of two polymers), (iii) stacking the polymers one
on the other, and finally, (iv) by using three-electrode devices, where each electrochromic
layer is controlled separately as addressed by the team of Jarosz et al. [67]. Li et al. have
reported the neutral EC device based on copolymers, PTTBTPh0.35 and PTTBTTh0.30
that have showed high colour neutrality with CIE 1976 coordinates (L = 37.23; a = −1.59;
b = 0.32), when the difference of potentials of −0.4 and +0.8 V was applied [69].
Alesanco et al. [70] recently reported a device that uses asymmetric viologens (ECDs
based on a single 1-alkyl-10 -aryl asymmetric viologen) with the simplest device architec-
ture (glass/TCO/EC gel/TCO/glass) that exhibited colourless electrochromism with the
parameters of Tbleached ≈ 77%, and ∆Tvis = 60%.
5.4.3. Spectrally Selective Systems

Electrochromic materials alter the visible radiation ranging in 400–750 nm (VIS) but
also are capable of reducing NIR (near-infrared, approx. 1000–1500 nm) transmission
through the window. As NIR transmission is associated with the heat load filtering,
NIR allows for increased thermal comfort while simultaneously decreasing the energy
expenditure on cooling. The solutions that are the most intensively sought include those
that allow for independent filtering NIR and visible radiation with the use of mainly
plasmonic EC materials. Plasmonic nanoparticles are particles whose electron density
can couple with electromagnetic radiation of wavelengths that are far larger than the size
of the particle, and therefore can exhibit spectrally selective behaviour, as reported by
Wu et al. [71].
The system usually works in the four states that are named bright (allowing only
the VIS transmittance), warm (VIS + NIR transmitted), cool (only VIS transmitted), and
dark (VIS blocked, NIR transmitted). Those states are cycled depending on the voltage
applied (usually in the range of −0.5 to +1.2 V, or −3.0 to +3.0). The advances in the field
of spectrally selective EC systems were reported by many researchers. Yilmaz et al. [72]
have used nanocrystalline ITO (indium-tin-oxide) with high optical contrast of polyaniline
(PANI). Laboratory-scale sandwich EC devices were fabricated “using the PANI/ITO
nanocomposite film as the active working electrode and a mesoporous CeO2 film (thickness
∼350 nm) as the counter electrode”. The synergistic features of PANI/ITO make possible
the implementation of a four-state tuneable electrochromic system that permits selectively
regulating optical transmittance in the visible and near-infrared range. They achieved
an outstanding result of ∆TNIR = 80%. Another system featuring hybrid multi-layered
inverse opal (IO) nanostructure composed of tin (SnO2 ), titanium (TiO2 ), and tungsten
(WO3 ) oxides developed by Nguyen et al. [73] was reported in 2019 to modulate up to
63.6% NIR radiation at the wavelength of 1200 nm. Inverse opal (IO) nanostructures are
three-dimensionally ordered microporous materials formed through the infiltration of an
artificial opal with a material precursor. Earlier in 2019, the same team have reported an IO
structure that shows modulation of 70% visible light transparency and 62% NIR blockage
at 1200 nm [25]. Other teams use different materials. Transparent amorphous indium
zinc oxide (a-IZO) was used by the team of Nunes et al. [74], who reported a selective
device that was able to work in two, not four, modes: semi-bright warm mode (VIS + NIR
transmitted) and dark cold mode (VIS and NIR blocked) at the modulation ∆Tvis = 50% at
550 nm and ∆TNIR = 60% at 1000 nm.
Other teams used the different idea of using two electrodes operating in different
spectral ranges, one which selectively operates in the NIR and NIR + VIS regimes (usually
WO3 ), and the second which selectively operates in the VIS regime only. The team of
Cao et al. [75] used Ta (tantalum) doped titanium oxide (TiO2 ). The synthesis produces
Ta-doped TiO2 NCs as a highly uniform colloidal solution, which is a promising electrode
for smart electrochromic windows. The laboratory-scale device exhibited the modulation of
∆Tvis = 86.3% at 550 nm and ∆TNIR = 81.4% at 1600 nm. In May of 2018, the team of Barawi
et al. [76] developed a system featuring four states: fully transparent, VIS blocking, NIR
blocking, and VIS and NIR blocking. The device was based on vanadium enriched TiO2 .
It exploits the peculiar spectro-electrochemical features of colloidal nanocrystals, which
exhibit a distinctive electrochromic response at visible wavelengths upon the application
of a small cathodic potential. The laboratory-scale device showed a performance of approx.
30% modulation in 550 nm and 70% in 1200 nm. Wu et al. [71] recently reported a device
which is capable of shielding 96.2% of the NIR irradiation from 800 to 2500 nm while
permitting the acceptable amount of visible light ∆Tvis = 33%, using caesium tungsten
bronze (Csx WO3 ). The effect of the optical switching is a direct result of the phase transition
of PAM–PNIPAM hydrogel, which in turn is induced by the photothermal effect of Csx WO3
under sunlight irradiation. (See Table 4.)
Table 4. The comparison of the performance of spectrally selective systems, including the technologies, where the data are
available. * Different data for different samples were given.
No. Team Year Type/Technology ∆Tvis /∆TNIR Remarks

Cool/Warm/Dark
1 Yilmaz et al. 2020 nanocrystalline ITO 44%/77%
states
2 Nguyen et al. 2019 (SnO2 ), (TiO2 ), (WO3 ) 21%/64% Vis/NIR
3 Nguyen et al. 2019 opal (IO) nanostructures 12%/57% * Vis/NIR
4 Nunes et al. 2019 a-IZO 45%/57% NIR at 1000 nm
5 Cao et al. 2018 Ta (tantalum) doped titanium oxide (TiO2 ) 86%/81% NIR at 1600 nm
6 Barawi et al. 2018 vanadium enriched TiO2 30%/70% NIR at 1500 nm
7 Wu et al. 2018 caesium tungsten bronze (Csx WO3 ) 33%/96.2% NIR at 800 to 2500 nm
5.4.4. Electrochromic Energy Storage Window (EESD)

Standard EC devices (windows) operate by consuming electrical energy to stimulate
the chemical reaction of reduction or oxidation with negligible energy storage ability. By
the analogy of standard EC window to the battery—with the use of proper materials—
the device shows the electrical phenomenon of pseudocapacitance, which is the storage
of electricity in an electrochemical capacitor. The energy is stored by electron charge

transfer between electrode and electrolyte. Recently, electrochromic energy storage win-
dows (EESWs) that integrate functions of energy storage and electrochromism are seen as
a novel alternative to many existing solutions in the fields of self-powered displays and
energy-efficient smart windows. Recently, colour-tuneable (nonemissive-red-yellow-green)
self-powered EESW is reported by Zhai et al. [77], which is using the phenomenon of
utilising Prussian blue (PB) as a controller of the fluorescent component of CdSe quantum
dots. Many electrochromic-luminescent windows in different technologies were reported
in the review by Kim et al. in 2019 [78].
In EESW, chemical reactions allow the device to collect the energy during the colouring
phase (charge), e.g., during the day and discharge while bleaching. The energy stored in the
ECCs could be used during the night for powering, e.g., the LED lighting, but could be also
used to switch their optical modulation. The materials used in the class of electrochromic
devices are mainly WO3 , MnO2 , and NiO, but the possibilities are wider. This type of EC
device does not require external voltage to trigger the bleaching process, as the stored
energy could be used to perform this task, as previously proved by Nguyen [73].
Electrochromic energy storage windows (EESW) have recently become the focus of
many research projects that produced different results. In 2019, Cao et al. [79] reported
a dual-band electrochromic energy storage window capable of independent control of the
NIR and visible light at the dynamic range of VIS and NIR light modulation (89.1% at
550 nm and 81.4% at 1600 nm). The device is simultaneously capable of a high charge-
storage capacity of 466.5 mAh m−2 at 150 mA m−2 of current density. The technology
used was Ta-doped TiO2 nanocrystals used for the working electrode (WE). In the year
2020, Wang et al. [55] presented an EESW based on Prussian blue that presented an
energy storage ability of average output voltage of 1.24 V and an aerial capacity of
78.9 mAh m−2 . In this case, a battery-type Prussian blue (PB, Fe4 III [FeII (CN)6 ]3 )/Zn EC win-
dow was demonstrated with the remarkable transmittance modulation of
∆Tvis = 84.9% at 633 nm. In 2018, Kim et al. [80] reported the electrochromic capaci-
tive windows (ECCs) with high transparency (>72%) with the use of blue (PR-Br) and red
(Th-OR) EC polymers combined in a single device. Thin polyaniline (25 nm thick PANI)
film was used as a capacitive layer. The energy stored in the blue ECCs could be transferred
to charge the red ECC or to light a LED. The laboratory-scale device that performed with
the power density of 58.8 kW kg−1 .
EESW is exhibiting typical problems for all EC devices. Practically all reported EESW
devices are blue or green in the coloured state and are not completely transparent in
the bleached state. In 2019, Xie et al. [81] demonstrated EESW with transparent-to-dark
electrochromic with the use of Mo-doped tungsten oxide (WO3 ) and nanoflake MnO2 film
electrode, which exhibited an aerial capacitance of 19.1 mF cm− 2 and presented the optical
modulations of over ∆Tvis = 60% in all visible bands (420–800 nm). In the same paper,
Xie et al. presented the comparison of EESW materials, stating that the best performance
is currently achieved with the use of WO3 /WO3 electrodes that demonstrate the areal
capacitance of 22.0 mF cm− 2 . In 2018, Wang et al. [82] reported mesoporous WO3 film
on FTO glass via a facile dip-coating sol-gel method. Mesoporous WO3 film exhibited
advantages including high transparency, good adhesion, and high porosity. The device
in the laboratory scale showed noticeable electrochromic energy storage with a specific
capacity of 75.3 mAh g−1 . In May 2020, Pan et al. [83] demonstrated a device using
novel NiO/PB composite hexagon nanosheets that exhibited a high areal capacitance of
11.50 mF cm−2 . NiO/PB composite nanosheet electrode exhibited higher exchanged charge
density, larger optical modulation, and better cyclic stability. An additional advantage of
the presented solution was the large optical modulation ∆Tvis = 67.6% at 630 nm, and the
fact that the process of charging/discharging can be repeated for at least 4000 cycles with
little decay. For a comparison of the results, see Table 5.
Table 5. The comparison of the performance of electrochromic energy storage windows, including the technologies, where
the data are available.
Energy Storage
No. Team Year Type/Technology ∆Tvis/ ∆TNIR
(W, mAh, Areal Capacitance)
1 Sheng et al. 2019 Ta-doped TiO2 nanocrystals 89%/81% 466.5 mAh m−2
2 Wang et al. 2020 Prussian blue 84.9%/n/a 78.9 mAh m−2
3 Kim et al. 2018 blue and a red colour ECP n/a 58.8 kW kg−1
4 Xie et al. 2019 Mo-doped WO3 60%/n/a 19.1 mF cm−2
5 Wang et al. 2018 mesoporous WO3 75.6%/n/a 75.3 mAh g−1
6 Pan et al. 2020 NiO/PB composite nanosheets 67.6%/n/a 11.50 mF cm−2
5.4.5. Hybrid EC/TC Solutions

Electrochromic devices (EC) can be integrated with thermochromic (TC) devices into
a single apparatus. The most frequently used method employs ultra-thin layers of tungsten
trioxide (WO3 ) for EC performance and vanadium oxide for VO2 -based thermochromic
cells. Such a hybrid device can control optical and solar energy transmission independently
as a response to electric current and the change in temperature. The biggest advantage is
that this technology allows for selective modulation of VIS and NIR wavelength ranges. In
2019, the team of Lee et al. [27] reported the EC/TC system that integrated two technologies
into one all-solid-state device using a solid electrolyte (tantalum oxide Ta2 O5 ). TC layer
VO2 was deposited directly on the ITO positive electrode. The device exhibited four states.
With the applied voltage (−2V), colour changed from transparent to deep blue due to
the EC reaction. Then, the coloured device was heated (80 ◦ C) and the device became
even darker because of the additional TC behaviour further decreasing the transmission.
Then, the voltage was inverted (+2V), and the transmittance was increased (as of the
EC phenomenon). Finally, the device was cooled and returned to its original state. The
∆Tvis between transmittances in the bleached and coloured state was decreased by approx.
30% due to the synergic effect of EC and TC layers (e.g., from Tbleached = 73.57% in room
temperature to Tcoloured = 8.33% in 80 ◦ C). For a comparison of the results, see Table 6 and
Supplementary Materials.
Table 6. The performance of Hybrid EC/TC solutions including the technologies, where the data are
available.
No. Team Year Type/Technology ∆Tsol /∆Tvis Remarks

45%/45% at 20◦
1 Lee et al. 2019 tantalum oxide Ta2 O5
36%/34% at 80◦
5.4.6. EC + OLED Lighting

Sold state electrochromic cell could be also coupled with a solid-state organic light-
emitting diode (OLED) producing the device capable of regulating the transparency and
simultaneously providing artificial light. This type of device was demonstrated for the
first time by the team of Lu et al. in 2018 with the use of PEDOT polymer for tuning
the light-emitting direction. The colour of the glass changes from pale blue to dark blue
upon the application of an external voltage. Therefore, “the utilization of this coloration or
discolouration of the glass substrate can adjust the light-emitting direction of OLED” [84].
When the EC component of the device is switched to semi-transparent mode, the device
exhibits a “graceful spatial impression”; when the glass is switched to a highly opaque
mode, “top emission with a significantly enhanced luminance efficiency” is visible. Fur-
thermore, in 2018, Cossari et al. [85] presented the device named ECOLED capable of
tuning the transmittance (EC phenomenon) and producing light by electroluminescence,
simultaneously or independently. The architecture of the device was based on 300 nm thick
WO3 layers and showed blue tinting via reduction of W6+ sites to W5+ . ECOLED device is
possible to be applied in many fields: in EC smart windows, EC mirror, and technologies
of transparent displays. The OLED component exhibits luminance above the minimum
values required for display and lighting applications, which are 300 cd m−2 and above
800 cd m−2 , respectively. The technology also allows for the simultaneous control of light
transmittance and artificial lighting achieving an optical contrast of ∆Tvis = 57% at 650 nm
and high colouration efficiency. For a comparison of the results, see Table 7.
Table 7. The performance of EC + OLED lighting solutions including the technologies, where the data are available.

switch between two semi-transparent states,
≈45% ≈70% absorption,
1 Lu et al. 2018 PEDOT polymer 25%/n/a
light emitting
35.0 and 7.5 cdA−1
2 Cossari et al. 2018 57%/n/a luminance from 300 cd m−2 to 800 cd m−2
5.4.7. EC Devices Powered by Solar Cells (DSSC-EC)

An EC device could be combined with dye-sensitised solar cell (DSSC), resulting
in the device named DSSC-EC. DSSCs are solar cells of low construction cost belonging
to the group of thin-film solar cells. The first dye-sensitised solar cell coupled with an
electrochromic layer (EC-DSSC) was reported by Bechinger et al. [86] in 1996. The DSSC-EC
devices were gradually improved. Wu et al. [87] report the device manufactured with
the use of PProDOT-Et2 that plays two roles, namely, as the electrochromic thin layer for
electrochromic action and the counter electrode for dye-sensitised solar cell (DSSC). Under
the light illumination, the photoactive layer of a dye-adsorbed TiO2 is sensitised initially
and produces electrons that cannot migrate to the electrochromic layer, as the circuit is open.
When the circuit is closed, electrons generated from the dye-sensitised TiO2 can migrate
through the gel electrolyte, and the device is darkened. In this case, the transmittance
can be changed reversibly from TVIS(bleached) = 46% to TVIS(coloured) = 15% at 590 nm, which
is triggered without any external voltage. In 2019, Costa et al. [88] reported a system
that is self-powered and changes colour spontaneously when illuminated. The device
exploits the architecture of dye, TiO2 , and WO3 as an electrochromic layer in the different
configurations. The performance of the device changes according to the location of the thin
layer of WO3. When the WO3 is deposited on the working electrode, the device exhibits
the best colour contrast; when it is applied on photoanode (anode of the photoelectric cell),
the electricity conversion efficiency of ca. 7% was obtained in the closed-circuit conditions.
5.5. Application of Nanostructures in EC Device Design

Nanostructured electrochromic materials are used in electrochromic devices to achieve
increased colouration efficiency, faster-switching speed, and longer cycling lifetime [78].
The mechanism behind the increased efficacy is that a nanostructure has a large specific
surface area and high aspect ratio that allows for the better penetration of the electrolyte
and to improve the ion diffusion [15].
It must be said that electrochromic devices based on bulk WO3 usually demonstrate
a slower switching time. To overcome this drawback, one-dimensional (1D) nanostructured
materials, such as nanowires and nanotubes, have been used and tested by different teams
since the beginning of the 20th century, as covered in the review from the year 2010
by Wang et al. [89]. Recently, many tungsten oxide (WO3 ) nanostructures including
nanowires [90,91], nanotubes [92], nanobelts [93], nanorods [94,95], and spindle-shaped
WO3 [96] have been synthesised.
In the year 2012, TiO2 nanowires were proved to demonstrate enhanced optical
transparency in the visible range by Chen et al. [97] and Tokudome et al. [98]. Regarding
reports from the years 2015–2020, in 2017, Lu et al. [99] presented a device using the
arrays of tungsten oxide nanorods with a diameter of 22 nm and length of 240 nm. This
architecture provided high surface area, uniform thickness, and good adhesion to the
substrate. The produced EC device demonstrated optical modulation of ∆Tvis = 41.2%, at
632.8 nm under the voltage of 0.1 V for 10 s.
In 2018, the team of Najafi-Ashtiani et al. [100] demonstrated an EC device featuring
synthesised Ag nanorods that are covered by tungsten oxide (WO3 ) shells. The device ex-
hibited a significant optical modulation of 36.81% at 633 nm, and a relatively fast switching
time of 5.7 s.
In 2019, the team of Shi et al. [101] presented a hybrid device comprising hybrid
nanorods are composed of WO3 nanocores wrapped by thin amorphous PEDOT nanoshells.
Wrapped WO3 nanocores present EC behaviour of a much shorter response time of approx.
3.7 s. than bare WO3 nanocores. The dynamic analysis presented by the team of Shi et al.
suggests a synergistic effect between the WO3 nanocore and the PEDOT nanoshell. As a
result, the colour depth and optical contrast of the hybrid nanorods can be modulated by
adjusting the applied voltage and the deposition of the PEDOT nanoshell.
Consequently, in 2020, the team of Shi et al. [102] presented a bilayer hybrid WO3
nanoarray device composed of crystalline WO3 nanobowls. The hybrid device exhibits
very good electrochromic performance in both visible and NIR wavelength ranges of
colour contrast, ∆Tvis = 93.9% at 633 nm and ∆TNIR = 89.6% at 1500 nm, respectively.
The nanobowls are produced with the use of polystyrene (PS) spheres template with a
diameter of 500 nm. The WO3 layer was deposited on the spheres and then the spheres
were removed by solving them in a solvent. The resulting surface was comprised of the
nanobowls of WO3 .
Mesoporous material is a material containing pores with diameters between 2 and
50 nm, according to IUPAC nomenclature. Mesoporous WO3 film usually exhibits im-
proved optical modulation performance. Optical modulation up to 71% at the wavelength
of 633 nm was presented by Wang et al. in a previously cited report [82]. The mesoporous
structure exhibits a noticeable electrochromic energy storage performance with a large
optical modulation up to 75.6% at 633 nm. For a comparison of the results, see Table 8.
Table 8. The performance of EC with the use of nanostructures including the technologies, where the data are available.

1 Lu et al. 2016 tungsten oxide nanorods 41%/n/a at 632.8 nm
80%/n/a only WO3
WO3 /PEDOT core/shell
2 Shi et al. 2018 26%/n/a only PEDOT
hybrid nanorod arrays
72%/n/a WO3 and PEDOT
3 Najafi-Ashtiani et al. 2018 Ag nanorods 37%/n/a range 32–37%
areal capacitance
4 Shi et al. 2020 WO3 nanoarray 94%/90%
47.4 mF/cm2
capacity of
5 Wang et al. 2018 mesoporous WO3 75.6%/n/a
75.3 mA h g−1
6. Discussion—Main Challenges
The most recent examples of ECD are presented in the paper also for some speculation
considering the most important areas of future application. Most of them are currently in
the development phase at the stage of working on a small-size prototype. In most cases,
the prototypes are only a few square centimetres of surface area, and the manufacturing
technology is available only on a laboratory scale. It must also be clearly stated that no
unified standard of the results presentations is valid/present, and therefore, different teams
use different metrics. This might limit the accuracy of the evidence and results included in
the review. Although it is needed to exercise caution in interpreting these presented data
because of the limited number of reviewed papers (105), these findings nonetheless appear
to be largely in line with systematic reviews by other researchers [12,13].
Nevertheless, the future application could be briefly discussed as the aspect of the
technology that should be focused on, to bring a wider range of opportunities.
The optical performance of electrochromic smart windows should be improved, es-
pecially for large-scale commercial applications. The main issues are low optical contrast
and long response time, as addressed by Zhang et al. [103]. Wider customer acceptance
for electrochromic systems is prevented by the still-to-be-solved drawbacks of the EC
systems, despite the long-time research, development, patents, and start-ups [18]. The
main disadvantage of electrochromic materials is the fact that they are unable to produce
neutral colouration, and the neutral grey electrochromism is in the development stage.
Electrochromic devices based on the tungsten trioxide (WO3 ) switch from deep blue to
transparent, while the nickel oxide (NiO) switches from transparent to brown. This colour
filtering is generally considered as a disadvantage, as the light filtered through the smart
glass influences the colour perception in the room [104]. In addition, blue light is consid-
ered to be a dangerous part of the visible spectrum because of the generation of reactive
oxygen species in the retina [105].
Another disadvantage of current EC technologies is the long switching time. This
also should be improved to earn more customer acceptance of the technology. Small
samples of electrochromic materials in the conditions of laboratory experiment present fast
coloured/bleached transitions that could be measured in seconds. However, window-size
(approx. 2.5 sq. m), commercially available solutions take much more time to switch
(up to 20 min) due to the increased resistance of the system and a greater amount of
electrical charge that must be transmitted through electrical contacts and electrolyte [26].
This has been considered both as an advantage—a desirable feature that permits the eye to
light-adapt [106]—but also as an evident disadvantage, preventing quick reaction, e.g., to
moving clouds in the sky. ECD smart windows also lack long-term cyclic stability [107]
and feature low optical contrast [61].
Another drawback of the currently available commercial solution is the high capital
cost, averaging 540–1080 USD/m2 [35].
7. Conclusions
The presented review systematically summarises the recent progress on prototype
smart windows solutions that are currently in the stage of research and examines the
quantitative parameters of smart window devices. The previous section focused on the
main challenges that the technology is facing, although the conducted review allows the
following conclusions to be formulated. The key findings are summarised by the following
categories:
7.1. Smart Windows

• The smart window is a mature technology that has been studied for many years in
many variations. The proof of this is the industrial application of the selected technolo-
gies and the presence of brands (e.g., View, Sage, Gesimat, Gentex, ChromoGenics);
• Smart windows have not achieved significant market penetration due to the factors
discussed in the previous paragraph;
• Smart windows must also switch deeply and quickly enough to mitigate glare and
prevent user discomfort, or they will not gain user acceptance;
• In the case of so-called privacy windows, the haze effect must be considered when
discussing the transparency/translucency (high) and energy-saving performance
(relatively low);
• The review shows that the widespread adoption of smart window technology calls for
better performance and cost competitiveness.
7.2. Electrochromics
• Many ECD technologies are currently at the stage of research and development as
multicolour, neutral black, spectrally selective, energy storage, and generation;
• Hybrid technologies are of special attention, e.g., smart glass joining in one device
the PV and ECD (self-powering smart windows), or ECD and OLED light-emitting
diodes or ECD and TC technologies;
• Hybrid devices usually expose lower either VIS or NIR performance while presenting
other functionalities;
• Within the review, the best visual performance was presented with the use of
two technologies: ECD featuring Ta (tantalum) doped titanium oxide (TiO2 ) with the
modulation ∆Tvis of 86.3% [75], and WO3 nanoarray with the impressive modulation
∆Tvis of 93.9% [102];
• Dual-band (NIR/VIS) technologies are promising in the context of energy flow man-
agement. In this category, the best performance was achieved by a device which is
capable of shielding 96.2% of the NIR irradiation from 800 to 2500 nm [71];
• The application of nano-technologies seems to be opening a wealth of new opportuni-
ties presenting the best performance;
• The observed tendency is that the complexity of ECDs is growing, especially the
number of layers, the architecture of nano-structures, and manufacturing technology
(deposition sequence).
The results provide important insight into the determination of the most promising
technologies. The present review also demonstrates the need to standardise the metrics
that are used to make it easier and faster to benchmark different technologies. Although
the most common metric reported by the authors was luminous/visual transmittance Tvis ,
the used metrics do not always reflect the most important parameters within the described
category. Moreover, the relationship between the performance and adopted technology
could be recognised in the paper.
7.3. Limitations of the Study

Limitations of the review study usually result from the insufficient number of included
publications. To counteract possible bias, PRISMA protocols were used in the writing of
this paper, but this potential limitation should nevertheless be explicitly mentioned. The
limitations are due to (i) different metrics used by different authors (e.g., only modulation
values were given without the Tcoloured and Tbleached values); (ii) values of Tcoloured and
Tbleached were not explicitly stated in papers and had to be retrieved from the graphs; and
(iii) the small size of laboratory samples (possibly not replicable results on a larger scale).
Despite the constraints, the study, the method, and the results are original and valuable
contributions to the review of the most recent electrochromic technologies.
7.4. Future Application

Despite the challenges that ECD technology is currently facing, there are also oppor-
tunities strongly connected with ECD application in the built environment. Dual-band
electrochromic materials would finally allow for the regulation of daylight and heat flow
into buildings. Both spectral ranges (VIS and NIR) are particularly interesting. In future
practice, the separate, independent regulation of VIS and NIR radiation would be very
beneficial for passive homes. ECD in the coloured state is used to optimise a building’s
energy performance in the summer by reducing the heat load; this results from the fact
that energy savings with the use of ECD are “due to a lower cooling demand” [10]. Es-
pecially, coupled EC/TC devices might show additional benefits here. However, it must
be remembered that NIR radiation fulfils an important function in the building’s energy
balance in winter, as the greenhouse effect is used in the winter season to raise the internal
temperature. A device that can independently screen both wavelength ranges would be
beneficial for the overall building’s energy balance. The use of ECD shows benefits not
only in the energy context but also in the reduction of the carbon footprint of new and
existing office buildings [108].
Multicolour ECD solutions might be also used to regulate internal rooms’ lighting
atmosphere and compensate for the natural daylight. Multicolour ECD might be used as a
large-scale transparent display. Simultaneously, neutral black electrochromism is widely
sought after as the most correct solution for light dimming in work and living spaces,
preventing glare and thermal discomfort without impairing the glazing’s primary function
of direct eye contact with the surrounding [106].
8. Summary
Buildings account for 40% of total energy consumption in the European Union and
even more in other countries whose energy-saving policies are not so up to date. To help
bring about a carbon-neutral future, it is thus necessary to reduce the consumption of
energy from non-renewable sources and decrease the energy demand through energy-
saving, environmentally friendly technologies. In this perspective, ECD, which can regulate
the flow of energy during the day and provide artificial lighting during the night, might
reduce the demand for separate lighting systems and reduce the demand for energy
for cooling. Currently existing and still developing ECD technologies open up a very
wide range of possibilities for their use in construction. This is the reason why broad
research is necessary, and hopefully, it will finally be able to identify technologies that have
the potential of scaling, which seems to be one of the most important challenges of the
ECD technology.
Supplementary Materials: The following are available online at https://www.mdpi.com/article/

10.3390/su13179604/s1, Table 9: All the systems described in the paper in a tabularise form, with the
data where available. Figure. X Prisma checklist, Figure. X Prisma flow diagram.
Funding: The financial support of this study that was provided through a grant entitled: “New
trends in architecture of transparent facades—formal experiments, technological innovations”, ref.
no. 2014/15/B/ST8/00191 by the National Science Centre, Poland. The APC was funded by Wroclaw
University of Science and Technology.
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Data Availability Statement: Prisma checklist is available at https://drive.google.com/file/d/
1erEaqla-gXLLsYf3alorAmPcU4MIorII/view?usp=sharing (accessed on 20 August 2021), Prisma
flow diagram is available at: https://drive.google.com/file/d/1L5pnUIrEqxkVXTp5UDEEUsEWf6
4iKEFg/view?usp=sharing (accessed on 20 August 2021).
Conflicts of Interest: The author declares no conflict of interest.
Nomenclature
TC thermochromic DSSC dye-sensitised solar cell

EC electrochromic OLED organic light-emitting diode
GC gasochromic MEMS microelectromechanical systems
TC thermochromic EESW electrochromic energy storage windows
ECD electrochromic device PDLC polymer dispersed liquid crystal
Tvis /Tlum visible transmittance SPD suspended particle devices
conducting polymer based on
Tsol solar transmittance PEDOT
3,4-ethylene dioxythiophene
near-infrared
TNIR UV ultraviolet
transmittance
∆Tvis visual modulation TRL technology readiness level
∆Tsol solar modulation
∆TNIR near-infrared modulation
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 Keywords: smart glass; smart window; electrochromic

Citation: Brzezicki, M. A Systematic

Sustainability 2021, 13, 9604. https://doi.org/10.3390/su13179604 https://www.mdpi.com/journal/sustainability

1.1. Method and Eligibility Criteria

1.2. Rationale behind the Presented Review and Objectives

1.3. Originality of the Paper

laboratory experiments and potential future application of presented technologies. Further,

1.4. Previous Research, State of the Art

Table 1. Previously conducted review research on the topic.

No. Team Year Focus

2. General Classification and Metrics

∆TNIR = TNIR(bleached) − TNIR(coloured) (3)

Type Stimulus Technology Featured Systems

4.3. Electrical Current

4.3.1. MEMS-Based Microsystems

4.3.2. Microwrinkled Nanometric Films

4.3.3. PDLC (Polymer Dispersed Liquid Crystal)

4.3.4. SPD Windows

No. Team Year Type ∆Tsol ∆Tvis Remarks

3 Wolfe et al. 2018 Optofluidic n/a 77% Clear to foggy

11 De Filpo et al. 2019 PDLC n/a 64% haze

MxWO3  WO3 + xe− + xM+ x ≤ 0.3 (4)

LiNiO  NiO + Li+ + e− (5)

5.2. Electrochromic Device Architecture

5.3. Simulated Energy Performance

5.4.2. Neutral Black Electrochromism

5.4.3. Spectrally Selective Systems

No. Team Year Type/Technology ∆Tvis /∆TNIR Remarks

5.4.4. Electrochromic Energy Storage Window (EESD)

of electricity in an electrochemical capacitor. The energy is stored by electron charge

5.4.5. Hybrid EC/TC Solutions

No. Team Year Type/Technology ∆Tsol /∆Tvis Remarks

5.4.6. EC + OLED Lighting

No. Team Year Type/Technology ∆Tvis /∆TNIR Remarks

5.4.7. EC Devices Powered by Solar Cells (DSSC-EC)

5.5. Application of Nanostructures in EC Device Design

No. Team Year Type/Technology ∆Tvis /∆TNIR Remarks

7.1. Smart Windows

7.3. Limitations of the Study

7.4. Future Application

Supplementary Materials: The following are available online at https://www.mdpi.com/article/

TC thermochromic DSSC dye-sensitised solar cell

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Keywords: smart glass; smart window; electrochromic

MxWO3 WO3 + xe− + xM+ x ≤ 0.3 (4)

LiNiO NiO + Li+ + e− (5)