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Novel temperature-sensitive label based on thermochromic ink for hot food

packaging and serving applications

Article in Journal of Thermal Analysis and Calorimetry · April 2023

DOI: 10.1007/s10973-023-12147-8

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Journal of Thermal Analysis and Calorimetry
https://doi.org/10.1007/s10973-023-12147-8

Novel temperature‑sensitive label based on thermochromic ink for hot

food packaging and serving applications
Jitendra Kumar1 · Konala Akhila1 · Pardeep Kumar1 · Ram Kumar Deshmukh1 · Kirtiraj K. Gaikwad1

Received: 23 August 2022 / Accepted: 22 March 2023

© Akadémiai Kiadó, Budapest, Hungary 2023

Abstract
Changes in the lifestyle of the millennials have started a revolution in the food industry. They started preferring to have
effortless ready-to-eat or cook meals (RTE) or fast-food chains and restaurants, and at the same time, they expect the food
to be served hot. Nonetheless, it is impossible to know whether the desired temperature has been maintained in the RTE
pouches or delivered food. Employing thermochromic materials as temperature indicators on the packaging can commu-
nicate the temperature of food inside. This work proposes a thermochromic coating composed of silver tetraiodomercurate
(STIM) and cellulose acetate in the form of a coated label as a temperature indicator. From the thermochromism property of
STIM, it was observed that the phase transition occurs at temperatures between 323 and 333 K. Colorimetric analysis of the
labels revealed that the color changes from yellow to orange to red, indicating normal temperature and higher temperatures,
respectively. Microstructural analysis of the label via FESEM reveals a uniform coating formation with traces of STIM
agglomerates. Rub resistance and adhesion tests proved that the solid particles have good adhesion with the substrate and
no scuffing traces. Hence, silver tetraiodomercurate-based thermochromic pigment can be used as a temperature indicator
label for hot beverages, ready-to-cook retort pouches, and hot-served food delivered through apps for better communication
of products’ temperature.

Keywords Thermochromic ink · Intelligent packaging · Food · Distribution · Temperature indicator

Introduction purchasing, the importance of packaging is increasing nowa-

days [8]. Incorporating smart materials like freshness indi-
Food products need the utmost care of all packed goods cators, thermochromic inks, and sensors into conventional
because food is a prime necessity for survival making food packaging can serve the purpose [9]. Food quality is dra-
product packaging indispensable Deshmukh et al. [1], [2]. matically affected by external factors like temperature, light,
Smart packaging techniques can be used to achieve food pro- and moisture [10]. Packaging is well known to be exposed
tection goals and better communicate real-time monitoring to varying temperatures during storage and transportation
of food inside the package [3]. Smart packaging is broadly despite its suggested storage temperature. Hence monitor-
classified as active packaging and intelligent packaging. ing the temperature throughout its shelf life is essential [11].
Intelligent packaging techniques are used to communicate There is a massive potential for thermochromic that may be
any alteration in the quality of food inside the packet and used to make printing inks and coatings to apply as a tem-
display an alert of the potential problem within the pack- perature indicator in packaging.
aging [4–6]. Intelligent packaging is all about incorporat- Thermochromism is a physical process of the irreversible
ing modern technology into traditional packaging and thus or reversible color change in a compound when exposed to
modifying the conventional packaging to meet the end-users heat [12]. Within a defined broad temperature range, these
needs [7]. Because of the growing popularity of self-service inks can undergo a reversible color change; they can become
colorless or change from one color to another. Examples of
* Kirtiraj K. Gaikwad thermochromics include liquid crystals, leuco dyes, vana-
kirtiraj.gaikwad@pt.iitr.ac.in dium dioxide, and heavy metal tetraiodo mercurates. So far
in the literature, this thermochromic has been used as print-
1
Department of Paper Technology, Indian Institute ing inks. A single liquid crystal called halide perovskite has
of Technology Roorkee, Roorkee 247667, India

13
Vol.:(0123456789)
 J. Kumar et al.

been used to develop a reversible thermochromic compound Preparation of thermochromic pigment

that is colorless at 298 K and changes its color to orange at
333 K and black at 393 K [13]. An enzyme-activated dye The thermochromic pigment was prepared using a simple
was proposed to act as a time–temperature indicator in pack- precipitation reaction. Initially, the silver nitrate solution
aging. Food's freshness is indicated using the kinetic release was prepared by dissolving 7.8 g of silver nitrate in 100 mL
of time when exposed to temperatures from 277 to 310 K distilled water. 60 mL of Nessler’s reagent was measured
[14]. There were several studies based on time–temperature and kept for stirring at 323 K. Once it reached the desired
indicators, but studies on only temperature indicators were temperature, 50 mL of the prepared silver nitrate solution
seldom seen in the literature. was added while mixing. After 30 min of continuous stir-
The silver tetraiodomercurate or silver mercury tetraio- ring at low speeds, a yellow precipitate of silver tetraiodo
dide ­(Ag2HgI4) (STIM) is a known inorganic thermochromic mercurate was formed and kept undisturbed for the next 4 h.
which changes its color by order–disorder transformation Finally, the deposit was filtrated using Whatman filter paper
taking place at an exact transition temperature. The differ- to separate the settled solid particles, followed by drying at
ence in the shade of ­Ag2HgI4 is caused by ion rearrangement 333 K to obtain dry pigment. It is further stored in airtight
in the crystalline structure before and after the transition containers till the coating solution is prepared.
temperature. This material was embedded into silica hybrid
materials, and their performance was studied in terms of
Preparation of thermochromic coating solution
physical properties [15]. Owing to the superionic conductiv-
ity of STIM, it was used to develop graphene nanocompos-
The coating solution was prepared in a cellulose acetate
ites and studied for its conductive performance [16]. Best of
emulsion with varying concentrations of thermochromic
our knowledge, this is the first time that STIM is being used
pigment. Initially, 10 mass% cellulose acetate (CA), i.e., 4 g,
as a temperature indicator in the form of coated label and
emulsion was prepared in 40 g of acetone and stirred at room
examined as a smart packaging technique. To develop a coat-
temperature for 2 h. Glycerol, as a plasticizer, was added to
ing material, cellulose acetate (CA) has been chosen to act as
the CA solution at a constant 1 mass% concentration based
a binder for STIM and paper substrate. CA is proven to have
on solvent mass and continued to stir for another 10 min.
excellent film-forming abilities and is a suitable binder [17].
For uniform dissolution of glycerol, the solution was sub-
Hence, this work aims to develop a reliable temperature
jected to sonication for 10 min using a bath sonicator. Now,
indicator that changes its color instantly when exposed to
the mass concentrations of thermochromic pigment were
different temperatures and applies it as a coating on a paper
considered as 0%, 50%, 60%, 70%, 80 mass% of CA, and
substrate with adhesive backing. This developed coated
they are added to the CA solutions followed by stirring for
paper can act as a temperature indicator label that can be
20 min and are stored in air-tight containers till further use.
adhered to any surface to know the product's temperature
visually. This research will help the consumers to identify
the temperature of hot serving food, especially during food Thermochromic coating on paper sheet
delivery and ready-to-eat foods which need to be added to
boiling water. The prepared solution was coated onto an adhesive back
paper of GSM 150 using an automatic bar coater (Sheen
Automatic Film Applicator-113N). A single layer was coated
using a Meyer rod of a thickness of 50 µm. The traverse
Materials and Methods speed of the machine was maintained at 100 mm/sec. Dry-
ing was carried out at room temperature for 2 h. The sam-
Materials ples were named Neat CA, CA/STIM 50, CA/STIM 60, CA/
STIM 70, and CA/STIM 80 according to the mass percent-
Laboratory-grade Nessler's reagents(R010-125ML) were age of STIM added. Table 1 shows typical recipe for organic
purchased from HiMedia Ltd. (Mumbai, India). Silver solvent-based inks label.
nitrate powder was purchased from Rankem Laboratory
Reagents. Cellulose acetate extra pure was purchased from
Characterization of thermochromic coated label
Loba Chemie Pvt. Ltd. Acetone as solvent and glycerol as a
plasticizer were purchased from HiMedia and used without
Field emission scanning electron microscopy
any further changes to prepare the thermochromic coating.
An adhesive-backed paper of GSM 150 was bought from
To understand the surface morphology and study the effect
Jiana Papers Ltd. Saharanpur, India, and used as a coating
of varying amounts of thermochromic pigment in the
substrate.

13
Novel temperature‑sensitive label based on thermochromic ink for hot food packaging and serving…

Table 1  Typical recipe for organic solvent-based inks label the color component were measured using an IGENE LAB-
Sample Cellulose Pigment/g Glycerol/g Solvent/g
SERVE portable Spectro-colorimeter (IG-210CS). The CIE
acetate/g Lab colorimetric system expresses value in three variables;
L, a, and b. The L represents the sample's lightness or dark-
Neet CA 2.2 0.00 0.22 20
ness, ‘a’ represents its redness or greenness, and ‘b’ denotes
CA/STIM50 2.2 1.10 0.22 20
its yellowness or blueness. The total color difference (E)
CA/STIM60 2.2 1.32 0.22 20
readings were calculated using the following Eq. 1
CA/STIM70 2.2 1.54 0.22 20
CA/STIM80 2.2 1.76 0.22 20
√
(1)
( )2 ( )2 ( )
ΔE = L∗ − L0∗ + a∗ − a∗0 + b∗ − b∗0
CA: Cellulose acetate; STIM: Silver tetraiodo mercurate
where ­L*, a*, and b* are the natural color values of the indi-
cator paper sheet and ­L0*, a0*, and b0* are the color meas-
coating solution on coated paper, it was examined under field urements of the indicator paper sheet at different tempera-
emission scanning electron microscopy (MIRA3 TESCAN, tures. Thermochromism is a physical process of changing
USA) at a voltage of 3 to 5 kV under vacuum. The samples’ the structure of a compound in the presence of temperature.
surface was initially subjected to gold plasma sputtering in a The thermochromism of the developed CA/STIM solutions
sputter coater (Quorum Mini Sputter Coater, SC7620, USA) was studied using a physical heating method. The labels
for better conductivity. The samples are then observed under were sticked to a temperature-assisted hot plate, and their
an electron microscope at different magnifications ranging temperature was increased gradually. A digital camera cap-
from 20 to 200 µm. tured an image at 283, 303, 313, 323, and 333 K to visually
represent the data.
X‑Ray diffraction analysis
Rub resistance test
Silver tetraiodo mercurate is a crystalline structure and
varies its crystallinity upon exposure to temperature. The Packaging undergoes undesired abrasion and scuffing during
phase identification of STIM after dissolving in CA solution transportation. It adversely affects the outer printing layer
to form a thermochromic coating was carried out through and printing or coating quality. It is important to under-
XRD analysis (Rigaku Ultima IV model, Japan). The dried stand the resistance of the coating to abrasion to maintain
coated samples were analyzed under 30 mA and 40 kV at a the quality. Hence rub resistance test was performed on all
wavelength of 0.154 nm using ­CuKα radiation. The diffrac- samples using a universal digital rub tester (Lloyds Research
tometers were collected from the 20 to 80° range of 2θ. For Foundation Inc, Mumbai, India). A 2-pound load was put on
peak identification, JCPS standards were used. the ink-printed paper sheet and rubbed back and forth for
20 cycles. Image analysis (mark on the surface) of the ink-
Thermal analysis coated paper sheet was used to quantify the rub resistance
before and after rubbing.
The thermal degradation of the coated samples needs to be
analyzed to understand the thermal behavior of ink in coated Adhesion test
form and cellulose acetate. For this purpose, the samples
were subjected to a temperature ranging from 298 to 1073 K Tape test adhesion findings were achieved by firmly apply-
using thermos gravimetric analysis (TGA, TA Instruments, ing a portion of Scotch® Cellophane Film Tape 610 to the
USA). The ramp set for the experiment was 283 K ­min-1 coated surface and then removing it in a single fast pull after
with a nitrogen atmosphere (Flow rate: 200 mL ­min-1). Plati- allowing it to rest for 24 h. The extent of coating withdrawal
num pan was used for conducting the thermal degradation was visually assessed on the print. The rating scale is from
study. Initially, 10 mg of each sample was loaded onto the 0 to 5, with 5 indicating a uniform coating of inks with no
platinum pan. The degradation or mass loss of the samples delamination and 0 showing complete delamination. After a
was recorded as a function of temperature. 24-h rest period, the second piece of tape was implemented
and tested similarly. Passable efficiency in this study is
Colorimetric analysis and thermochromism of coated label defined as anything rated a 3 or higher in initial testing with
good adhesion.
Color strength of the paper sheet after coating with ther-
mochromic ink on 150 GSM labels was measured to study
color value variation as the function of temperature. Pigment
concentration varied from 50 to 80%. CIE Lab values of

13
 J. Kumar et al.

Solid content test the base solution, the density of solids settled on the sur-
face has gradually increased. The coating with 80% (w/w)
To calculate the percentage of solid content, 2 g of of STIM has maximum aggregated particles on the surface.
organic-based thermochromic ink was placed in a Petri This could either be because of the nonuniform dispersion of
dish and dried to a constant mass at 105 °C. The following STIM in CA solution leading to observable micro-clusters or
Eq. 2 was used to calculate the solid content (percentage): the etched top most layer due to the plasma sputtering. The
conductive nature of STIM could be responsible for the latter
A0
Solid contents% = × 100 (2) phenomenon. Our result was similar to T.A. Hameed et al.
A [19], who characterized A ­ g2HgI4 films . From the micro-
where A0 represents the ink mass after drying, and A denotes graphs, it can be concluded that, although there is the micro
the mass of ink before drying. aggregation of STIM particles, the surface has not had any
phase separation; instead seems to be having excellent adhe-
sion despite agglomerates.
Statistical analysis

Statistical analysis for all the experimental data was per- XRD
formed using SPSS ver.25 (IBM Corporation, Germany).
A one-way analysis of variance was calculated for the trip- The diffractograms of all the coated samples along with
licate data, and the results were shown as a mean ± stand- STIM powder were represented in Fig. 2. It was observed
ard deviation value. Tukey post hoc test (p < 0.05) was that pure STIM has a peak at 2Ө = 39.5°, corresponding to
used for testing significant differences. the (220) crystallographic plane. STIM powder has a crys-
talline tetragonal phase at room temperature (JCPDS No.
74–0168) and has traces of impurities like ­HgI2 and AgI.
Results and discussion The triplet and doublet peaks observed at 30° and 50° cor-
respond to those impurities [20]. The dominant orientation
Solid content test in powder is seen at the (311) plane, whereas the coating’s
dominant orientation has shifted to 23°. It is also seen that
The strict laws follow for the utilization and emission of with the addition of STIM to cellulose acetate, the intensity
volatile organic compounds, so the coating industry con- of peaks at 23° and 24° has been increasing. This sharp peak
stantly reduces the ink's volatile content and increases solid is attributed to the presence of pure STIM in the tetragonal
content [18]. The solid content of the thermochromic ink phase. The diffractograms confirmed that the thermochromic
was estimated by using the moisture analyser VPB-10 with pigment had retained its crystalline structure even after coat-
halogen heating. A standard mass of 2 g organic solvent- ing at room temperature. The broad peak observed at 21°
based thermochromic pigment was placed in the equipment in neat CA results from the amorphous nature of cellulose
at 105 °C on a petri plate until the equilibrium mass was acetate[21].
achieved. In 5 min, the equilibrium mass was achieved, and
solid content of 16.93% in the organic-based thermochromic Thermal analysis
was observed. The higher solid content of the coating influ-
ences the viscosity, which can affect the drying rate, shades, The thermal degradation pattern of Neat CA and CA STIM
and printing speed. with different loadings of STIM Pigment was shown in
Fig. 3. The thermal degradation of Neat CA and CA STIM-
50, 60, 70, and 80 occurs in three different regions, as illus-
Field emission scanning electron microscopy trated in DTG curves. The loss in mass below 200 °C was
due to the evaporation of volatile materials like moisture
The microstructure of the coated surface was captured under and solvent residues from the coated paper. The main deg-
field emission scanning electron microscopy at a magnifi- radation takes place in the range of 270–350 °C, which was
cation of 100 µm and represented in Fig. 1. As seen in the the disintegration of the macromolecular polymeric chain
figure, the coating of cellulose acetate has formed a smooth of cellulose acetate and the evaporation of ­HgI2 impurities.
and fine coating on the paper’s surface. This confirms that The last stage of loss in mass was due to the carbonization
the cellulose acetate has formed a homogenous coating of the left-out products into ash at ~ 600 °C [22]. There was
solution that can adhere to the surface without any phase a decrement in Neat CA's thermal stability, as seen in Fig. 3.
separation. With the addition of thermochromic pigment to This may be a result of an increase in the loading of STIM.
It was depicted from the DTG curve, Fig. 3, that the Tmax

13
Novel temperature‑sensitive label based on thermochromic ink for hot food packaging and serving…

Fig. 1  Surface morphology of thermochromic pigment coated labels tate/ silver tetraiodomercurate 70 and e cellulose acetate/ silver tetra-
a Neat cellulose acetate, b cellulose acetate/ silver tetraiodomercurate iodomercurate 80
50, c cellulose acetate/ silver tetraiodomercurate 60, d cellulose ace-

Neat CA 0
CA/STIM 50
CA/STIM 60
Deravitave mass% min–1

CA/STIM 70
–4
CA/STIM 80
Intensity/a.u

Exo
–8

Neat CA
CA/STIM 50
– 12
CA/STIM 60
CA/STIM 70
CA/STIM 80
– 16
273 473 673 873 1073
Temperature/K
20 30 40 50 60 70 80
2θ
Fig. 3  Differential thermogravimetric curves of neat cellulose acetate
coated label and labels with varying concentrations of silver tetraio-
Fig. 2  Diffractograms of coated labels with different loading of sil- domercurate. Arrow indicates Exo (exothermic) direction on the DTG
ver tetraiodomercurate in cellulose acetate and neat cellulose acetate scale
coated label

13
 J. Kumar et al.

for the Neat CA, CA STIM-50, 60, 70, and 80 was 340 °C,
330 °C, 328 °C, 330 °C, 332 °C, respectively. The Tmax was
slightly modified with the addition of thermochromic ink.
These results illustrated that the Tmax for the CA STIM-50
Scuffed area
and CA STIM-60 was decreased and for CA STIM-70 and
CA STIM-80 increased, but the value of Tmax for different
loadings of STIM was less than Neat CA, which implies that
thermal stability decreased. Similar results were found by
Before After
Bruna et al. (2014), where the thermal stability of cellulose
acetate decreased by the presence of ­MtCu2+ [23]. The char
Fig. 4  Rub resistance analysis performed on cellulose acetate and sil-
was observed in the highest quantities for CA/STIM 70%,
ver tetraiodomercurate 70 coated label before and after 20 cycles of
depicting that there might be excess coat mass compared to testing
the other coatings.

Rub resistance test coated on the paper sheet was 86%, indicating that the devel-
oped inks had good adhesion properties to the paper sheet.
Rub resistance is an essential characteristic of ink that The enhanced intermolecular interactions among the cellu-
ensures the clarity of printed objects or even the visibil- lose acetate resin chain might have improved the adhesion
ity of any flaws in printing design. They are subjected to property. The surface irregularity of the paper sheet and the
exposure to vibration, impacts, abrasion, continuous inter- low surface energy difference between the paper sheet and
action with one another, and rubbing inside the printed roll the produced ink may also work as anchoring between ink
itself during the shipping of the products. Coated label and surface. Young-In Lee et al. (2012) depict a similar test
adhered to the package must be durable in all conditions. result and method in their study of adhesion enhancement
A digital camera was used to take photographs of the of ink-jet printed conductive copper patterns on a flexible
rubbed paper surface of the thermochromic coating on a substrate [26].
paper sheet after 20 rub cycles. The change in color in the
rubbed surface area of the thermochromic coated test sam- Colorimetric analysis
ple can be used to demonstrate the rub resistance of the
coated paper sheet, which can be analyzed by the images Color values are extremely important in the customer's
given in Fig. 4. The obtained results indicate no signifi- acceptance of a packaging product. L, a, and b values can
cant signs on the rubbed thermochromic ink-coated paper quantify the color of any ink. The color of coated labels
sheet, demonstrating the produced inks' outstanding rub before and after exposure to varying temperatures was ana-
resistance property. Our finding has similar to B. Sharma lyzed using Spectro-colorimeter (CIE Lab Values). The color
et al. and K. H. Nielsen et al., in their study of Waterborne of the labels at room temperature is determined as yellow by
acrylic copolymer resin preparation as a binding agent to visual examination. But with the increasing concentration
develop water-based inks in the printing application and of STIM, it was presumed that the yellow color's intensity
silica films on glass surfaces [24, 25]. would also increase. As presented in Table 2, The neat CA
label has the highest L value of 89.77, and the label with
80% STIM has the lowest of 67.26. As the concentration
Adhesion test of thermochromic ink increased, the yellowness (+ b value)
was seen to be increasing from 0.37 to 62.95. Surprisingly,
The primary cause of organic solvent-based thermochro- CA/STIM 70 has the highest b value, possibly because of the
mic ink failure is poor printability toward paper-based increased coat mass as understood from the thermogravimet-
substances and polymeric films due to the large surface ric analysis. When exposed to increasing temperature, there
energy gap between paper-based polymeric films and ink. It was a noticeable change in a* values as the color changed
is challenging to maintain sufficient adhesion between the from yellow to orange or reddish-orange. It has gradually
polymeric film and ink. Various additives are also respon- increased with temperature for all the samples. As seen from
sible for the ink's excellent adhesion properties. Winder, Fig. 5., at every temperature, the sample with 70% STIM has
also known as resin, is important in imparting ink and dye shown the highest + a value. The graphs conclude that the
adhesion properties. Because of the high surface energy of coated samples were changing their color gradually from
organic solvent acetone used as a vehicle for ink transfer, yellow to orange when exposed to higher temperatures and
it is tough to maintain the variation in surface energy. The that change was significant enough to know whether the
adhesion significance for yellow color thermochromic inks

13
Novel temperature‑sensitive label based on thermochromic ink for hot food packaging and serving…

Table 2  Colorimetric analysis for observed change in color of neat packaging had reached a temperature of more than 323 K if
cellulose acetate coated label and labels coated with different silver applied on ready-to-eat retard pouches.
tetraiodomercurate loading solutions when exposed to varying tem-
peratures ranging between 10 ℃ and 60 ℃
Thermochromism of coated label
Sample Tempera- L a* b*
ture/℃
As seen in Fig. 6., it is clear that the coated label changes
Neat CA 10 89.97 1.74 − 2.53 its color when exposed to different temperatures, and its
CA/STIM50 63.64 − 0.84 40.84 intensity has varied by the concentration of STIM. As
CA/STIM60 69.48 1.02 55.97 discussed in Sect. 3.5., the initial color of all coated sam-
CA/STIM70 68.99 1.26 58.76 ples was yellow, and the intensity of the yellow color is
CA/STIM80 66.08 0.65 50.36
Neat CA 30 89.77 1.18 0.37 Temperature 282 K 303 K 313 K 323 K 333 K
CA/STIM50 63.59 0.97 44.54
CA/STIM60 71.29 0.24 61.53 Neat CA
CA/STIM70 68.66 3.37 62.95
CA/STIM80 67.26 0.24 55.56
Neat CA 40 89.76 1.06 − 0.27
CA/STIM 50
CA/STIM50 64.84 1.32 47.34
CA/STIM60 69.77 3.78 63.1
CA/STIM70 64.79 1.3 56.88
CA/STIM 60
CA/STIM80 66.19 2.16 56.67
Neat CA 50 89.53 1.05 − 0.19
CA/STIM50 67.53 2.44 46.73
CA/STIM 70
CA/STIM60 65.72 9.67 57.71
CA/STIM70 64.94 12.3 55.82
CA/STIM80 65.47 7.7 53.27
CA/STIM 80
Neat CA 60 89.69 1.26 − 0.2
CA/STIM50 64.69 2.94 46.39
CA/STIM60 64.21 11.18 54.35
Fig. 6  Thermochromism observed in cellulose acetate and silver
CA/STIM70 63.01 16.48 59.61 tetraiodomercurate (varying concentrations) coated labels when
CA/STIM80 61.48 9.37 50.61 exposed to 283, 303, 313, 323, and 333 K

Neat CA CA/STIM 50 CA/STIM 60

1.8 68 48 72 64
L a* b*
90.0 L a* b* 0.5 L a* b* 3.0 12
1.7 47 71
0.0 2.5 62
67 70 10
89.9 1.6 46
2.0
– 0.5 69 8
1.5 60
1.5 45
89.8 66
1.4 – 1.0 68
44 6
L

1.0
58
89.7 1.3 – 1.5 67
65 0.5 43 4
1.2 – 2.0 0.0 66
89.6 56
42
64 2
1.1 – 0.5 65
– 2.5
41
89.5 0 54
1.0 – 1.0 64
– 3.0 63 40
270 280 290 300 310 320 330 340 270 280 290 300 310 320 330 340 270 280 290 300 310 320 330 340
Temperature/K Temperature/K Temperature/K

CA/STIM 70 18 64
CA/STIM 80
68
L a* b* L a* b* 57
69 16 63 10
67
56
14 62
68 8
66
12 61 55

10 60 65 6 54
67

8 59 64 53
4
66
6 58
63 52
4 57 2
65 51
62
2 56
0
50
64 0 55 61
270 280 290 300 310 320 330 340 270 280 290 300 310 320 330 340
Temperature/K Temperature/K

Fig. 5  Colorimetric analysis for observed change in color of neat cellulose acetate coated label and labels coated with different silver tetraio-
domercurate loading solutions when exposed to varying temperatures ranging between 283 and 333 K

13
 J. Kumar et al.

maximum for 80% STIM. At room temperature, the sam- Acknowledgements Author Kirtiraj K. Gaikwad would like to sin-
ple with 50% STIM was more greenish-yellow in color, cerely thank the Science and Engineering Research Board (SERB),
Government of India, for the financial support provided under the Start-
and at 80%, yellow was prominently visualized. With the Up Research Grant (SRG) (SRG/2021/001549).
increase in temperature, the sample with 70% STIM has
shown reddish-brown color at 313 K and the highest a* Author contribution JK: Investigation, Formal analysis, Visualization,
value indicating the dominant reddish-orange color. The Data curation, Writing—Original Draft, KA: Investigation, Formal
analysis, Visualization, Data curation Pardeep Kumar: Investigation,
reason behind this color change is the change in the crystal Formal analysis Experimental, Resources, RKDe: Experimental, KK.
lattice structure of STIM accompanied by electrical and Gaikwad: Conceptualization, Methodology, Resources, Writing—
ionic conductivities when exposed to elevated tempera- Original Draft, Manuscript editing and review, Supervision, Project
tures. The structure of STIM has a huge number of inter- administration, Funding acquisition.
stitial spaces which are connected tridimensionally and
Declarations
allow the movement of cations for ionic conductivity. At
lower temperatures, STIM has an ordered tetragonal shape Conflict of interest The authors declare that there are no conflicts of
called β- the phase, and at high temperatures, it turns into interest.
a disordered pseudo-cubic α- phase. The thermochromic
transition occurs as a consequence of the order–disorder
transition. This change occurs at a particular tempera-
ture called phase change temperature, typically 323 K for References
STIM [27]. This change is reversible in nature, and the
1. Deshmukh RK, Akhila K, Ramakanth D, Gaikwad KK. Guar gum/
color changes from yellow to orange to red. These images carboxymethyl cellulose based antioxidant film incorporated with
confirm that STIM in a coated label form changes its color halloysite nanotubes and litchi shell waste extract for active pack-
and can be used as a thermochromic label for smart pack- aging. Int J Biol Macromol. 2022;201:1–13.
2. Ramakanth D, Akhila K, Gaikwad KK, Maji PK. UV-activated
aging applications.
oxygen scavenging system based on natural rubber latex from
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