Article

Bio-Inspired Self-Adhesive Bright Non-

iridescent Graphene Pigments
Yuxiao Liu, Changmin Shao, Yu
Wang, Lingyu Sun, Yuanjin Zhao
yjzhao@seu.edu.cn

HIGHLIGHTS
A kind of multi-shell GO and PDA-
encapsulated silica nanoparticles
is presented

Bright and stable non-iridescent

pigment can be generated from
simple spraying

The pigment-derived inverse opal

hydrogel shows photothermal
responsiveness

The pigment-derived inverse opal

hydrogel has self-healing capacity

Inspired by feathers’ brightness and mussels’ adhesivity, we develop

polydopamine (PDA)-adhered multi-shell graphene oxide (GO)-encapsulated
silica nanoparticles. Their derived non-iridescent pigments through spraying
demonstrate amorphous structure and brighter structural color that is not easily
damaged, due to the existence of GO (serving as dark element to improve color
saturation) and PDA (providing color stability by self-adhesivity). The inverse opal
hydrogel generated from the pigment template also shows vivid structural color,
as well as photothermal responsiveness and self-healing capacity.

Liu et al., Matter 1, 1–11

December 4, 2019 ª 2019 Elsevier Inc.
https://doi.org/10.1016/j.matt.2019.08.018
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10.1016/j.matt.2019.08.018

Article
Bio-Inspired Self-Adhesive
Bright Non-iridescent Graphene Pigments
Yuxiao Liu,1 Changmin Shao,1 Yu Wang,1 Lingyu Sun,1 and Yuanjin Zhao1,2,*

SUMMARY Progress and Potential

Owing to the unique features of angle independence and wide-angle display, Non-iridescent materials have
non-iridescent materials have attracted increasing interest in coating, decora- emerged as an important aspect
tion, and anti-counterfeiting. However, there are still some defects that limit of structural-color materials,
their applications, such as relatively pale colors and suboptimal stability. although some of the inherent
Inspired by mussels’ super-adhesivity and feathers’ brightness, we present a defects like pale color and
graphene-doped non-iridescent pigment to overcome the aforementioned lim- instability have limited their
itations. The elementary unit of the pigments is polydopamine-adhered multi- further application. Here, we
shell graphene oxide-encapsulated silica nanoparticles. These nanoparticles present a form of multi-shell
form into microspheres after simple spraying, and the obtained angle-indepen- graphene oxide (GO) and
dent patterns are imparted with higher color saturation and excellent self- polydopamine (PDA)-
adhesivity compared with traditional non-iridescent materials. Moreover, our encapsulated silica nanoparticles
pigments can also be employed as templates for negative replication, and the to create non-iridescent
resultant inverse opal hydrogels are endowed with the same amorphous fea- pigments. The designed
tures and even some additional functions such as photothermal responsiveness nanoparticles not only have GO
and self-healing capacity. These features indicate promising prospects for our encapsulated in the outer layer,
designed pigments. which serves as a dark element to
provide brighter structural color,
but the PDA intercalated between
INTRODUCTION
the GO layers also imparts these
With the typical advantages of fastness, non-toxicity, and environmental protection, nanoparticles with good self-
structural-color materials have been broadly applied in the fields of decoration, anti- adhesivity that makes the
counterfeiting, functional materials, and biological or chemical detection.1–13 In resultant pigments much more
particular, the discovery and development of non-iridescent structural-color mate- robust and stable. In addition, the
rials has expanded their potential values, based on the special features of angle in- derived pigments can also be
dependence and wide-angle display, which are attributed to the characteristic long- employed as a template for
range disorder assembly of those component colloidal nanoparticles.14–17 However, generating inverse opal hydrogels
due to the lack of absorbing materials to decrease the incoherent scattering that with typical non-iridescent
leads to insufficient color saturation, common non-iridescent colors are often shown structural color, photothermal
to be pale and insufficiently bright.18,19 In addition, because of the relatively weak responsiveness, and even self-
interaction force between the colloidal particles and their absence of effective or healing capacity, thus
active surface, the adhesivity of most existing non-iridescent materials is undesir- demonstrating the broader
able.20,21 These disadvantages greatly limit the practical application of non-irides- application prospects of these
cent materials as painting or coating pigments. Thus, non-iridescent materials nanoparticles.
with more practical properties are urgently anticipated.

In this article, inspired by the natural phenomena of super-adhesive mussels and

bright feathers, we present a non-iridescent graphene oxide (GO) pigment with
the desired features of self-adhesivity and brightness, as shown in Figure 1. Mussels
are super-self-adhesive creatures in nature that can be found on wet and slippery
rocks. Such an interesting feature is attributed to their self-produced mussel adhe-
sive proteins whose main component is dopamine (DA). Many researchers have

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Figure 1. Schematic Diagram

Schematic of the generation process of the designed non-iridescent pigments.

demonstrated the integration of mussels (i.e., DA) into functional materials for
achieving adhesive features.22–25 Thus, when the structural-color materials are com-
bined with DA, they are imparted with good adhesion. Furthermore, feathers of
many kinds of birds often display vivid and bright structural colors. This characteristic
brightness is derived from their specific microstructure and the existence of melano-
somes, which provide the high refractive index and broadband light absorption.26–29
To mimic this phenomenon, various dark elements have been applied to enhance
the saturation of the structural colors. Among these elements, GO has significant
features of high refractive index, good photothermal effect, relatively large specific
surface area, and abundant functional groups on the surface.30–35 Therefore, if DA
and GO can be effectively integrated into artificial non-iridescent structural-color
materials, a superior type of material is expected to develop.

For this purpose, we synthesized a form of multi-shell GO-encapsulated colloidal

nanoparticles with the assistance of polydopamine (PDA). We demonstrate herein
that these multi-shell nanoparticles can be assembled into non-iridescent micro-
spheres through simple spraying. Due to the existence of GO, the microsphere pig-
ments show vivid and brighter colors with high color saturation. In addition,
benefiting from the mass PDA groups on the surface, these pigments are imparted
with high adhesivity, which provides excellent stability to the resultant coatings or
patterns. As the pigments have an amorphous nano-arrangement and spherical
structures, they show angle-independent structural colors at different viewing or illu-
mination angles. More attractively, by employing the pigments as a template, the 1State Key Laboratory of Bioelectronics, School of
replicated inverse opal hydrogels are also endowed with angle-independent struc- Biological Science and Medical Engineering,
tural colors and additional functions such as photothermal responsiveness and self- Southeast University, Nanjing 210096, China
2Lead
healing capacity. These features of the non-iridescent GO pigments and the derived Contact
hydrogels indicate their great value in the fields of coating, display, sensing, and *Correspondence: yjzhao@seu.edu.cn
monitoring, among others. https://doi.org/10.1016/j.matt.2019.08.018

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Figure 2. Characterizations of the Designed Nanoparticles and Their Derived Microspheres

(A) Schematic of the generation process of the multi-shell nanoparticles.
(B–D) TEM images of silica nanoparticles (B), silica nanoparticles with one GO layer (C), and silica nanoparticles with five GO layers (D).
(E–G) SEM images of the nanoparticle-derived microspheres (E), and the surface (F) and cross-section (G) of the microspheres.
Scale bars, 200 nm (B–D), 5 mm (E), 1 mm (F), and 2 mm (G).

RESULTS AND DISCUSSION

In a typical experiment, the elementary units of our designed pigments, i.e., the spe-
cific multi-shell nanoparticles, were generated by using PDA to encapsulate the SiO2
nanoparticles and adhere GO as outer layer simultaneously, as shown in Figure 2A.
Figures 2B–2D clearly show via transmission electron microscopy (TEM) that the SiO2
nanoparticles were encapsulated by the GO layer. In addition, by repeating the
coating process of PDA and GO, nanoparticles with different numbers of GO layers
could be easily formed, as shown in Figure 2D. Moreover, to make the nanoparticles
more self-adhesive and suitable for the subsequent applications, we usually coated
these nanoparticles with PDA in the outermost layer after finishing GO encapsula-
tion. These resultant multi-shell nanoparticles were then dispersed in absolute
ethanol, which is non-toxic and easily evaporates. We observed that the nanopar-
ticle dispersion was formed into microspheres with different sizes after spraying un-
der near-infrared (NIR) radiation, as shown in Figure 2E. Although some of the nano-
particles were not totally assembled into a spherical shape due to the incomplete
evaporation of the solvent during the spraying process, this deficiency could be
avoided by adjusting the spraying distance, radiation intensity, or solvent types.
The generated microspheres demonstrated a typical amorphous feature, which
could be confirmed by scanning electron microscopy (SEM) images of their surface
and interior and the corresponding results of two-dimensional (2D) Fourier analysis

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Figure 3. Reflection Spectra of Different Nanoparticles

(A) Reflection spectra of nanoparticles with one GO layer and different silica cores. The sizes of
silica cores were 220, 228, 235, 243, and 255 nm, respectively, from left to right.
(B) Reflection spectra of nanoparticles with 235-nm silica cores and different GO layers (0–5 layers,
from top to bottom).

(Figures 2F, 2G, and S1). It was apparent that the nanoparticles did not form a highly
ordered crystalline structure, and the 2D Fourier analysis showed a circular pattern.
This result was totally different from the diffraction pattern with regular spot array
(Figure S1A) derived from the SEM image of orderly arranged silica nanoparticles,
which meant there was no long-range ordered arrangement in the nanoparticle ar-
rays of the resultant spheres. This phenomenon could be ascribed to the rapid evap-
oration of the ethanol in the nanoparticle dispersion during the spraying process,
and the light energy of the NIR being converted into thermal energy due to the pho-
tothermal conversion capability of GO, which could also contribute to the heating
and evaporation of the particle solution. Therefore, there was insufficient time for
the nanoparticles to crystallize.

The optical properties of the nanoparticle-derived microsphere were further inves-

tigated. It was found that the reflection peak of the microsphere could be regulated
through two factors of the component multi-shell nanoparticles, i.e., the size of the
SiO2 core and the number of GO layers. As shown in Figure 3A, the reflection peaks
were gradually red-shifted with the increasing size of the SiO2 cores, which could be
ascribed to the growing center-to-center distance between adjacent nanoparticles.
In addition, it was demonstrated that the greater the number of GO layers, the
greater the red shift obtained by the reflection peak (Figure 3B). This phenomenon
could be explained by two reasons: the increasing distance between nanoparticles,
and the change in refractive index. It is well known that GO has a much higher refrac-
tive index than SiO2; thus, the integral refractive index of the multi-shell nanoparticle
grew with the increasing GO layers. Moreover, due to the excellent ability of broad-
band light absorption of GO, a decrease in reflection intensity was observed when
the doped amount of GO increased, as illustrated in Figure 3B.

We further studied the films composed of the aforementioned microspheres. The

color and brightness of the films were greatly influenced by the optical properties
of the single microsphere. Figure 4A shows that the colors of the films were appar-
ently blue-shifted when the size of SiO2 nanoparticles decreased, corresponding to
the reflection spectrum of the microsphere (Figure S2). We also compared the per-
formances between films with and without GO doping. It was found that the films
derived from unmodified SiO2 nanoparticles exhibited a paler color, while the films
derived from designed multi-shell nanoparticles were a much brighter color, and
their colors were also red-shifted correspondingly compared with unmodified films

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Figure 4. Characterizations of Films Composed of Different Microspheres

(A) Patterns prepared by microspheres derived from different sizes of unmodified silica
nanoparticles (263, 239, 228, and 200 nm from left to right).
(B) Patterns prepared by microspheres derived from designed multi-shell nanoparticles of the same
sizes of silica nanocores as in (A).
(C) Patterns prepared by microspheres derived from different sizes of unmodified silica
nanoparticles (270, 245, 228, and 200 nm from left to right).
(D) Patterns prepared by microspheres derived from designed multi-shell nanoparticles of the
same sizes of silica nanocores as in (C).
The damaging processes in (C) and (D) were (from left to right) finger wiping, knife scratching,
emery paper wiping, and watering. Scale bar, 0.5 cm.

composed of SiO2 nanoparticles of the same size (Figures 4A and 4B). The same
conclusion could be reached from the corresponding reflection spectra, as shown
in Figure S2. Moreover, because of the involvement of PDA and its characteristic
self-adhesivity, our designed films were also self-adhesive and thus presented a bet-
ter robustness than the normal non-iridescent pigments. As shown in Figures 4C and
4D, we compared the robustness of the two different types of films through finger
wiping, knife scratching, emery paper wiping, and watering. The results clearly indi-
cated that the films composed of the microsphere derived from our designed multi-
shell nanoparticles had a much better performance after such damaging operations.
This feature promises advantages for our designed pigments in future applications.

One significant feature of the non-iridescent materials is their angle independence,

and in this regard we studied the performances of our pigments. We used designed
pigments with different colors (derived from SiO2 cores with different sizes) to orga-
nize colorful patterns, such as a Chinese dragon, goldfish, and group of letters.
When these patterns were observed from different viewing angles their colors re-
mained constant, as shown in Figure 5. In addition, we measured the corresponding
reflection spectra, which showed no obvious changes in their peak positions (Fig-
ure S3). These data further confirmed that our pigments possessed the properties
of the angle independence and wide-angle display. As is well known, the long-range
order structures of the colloidal crystals result in their iridescent characteristic
and angle dependence.36–38 Therefore, once the long-range order has been

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Figure 5. Angle Independence of the Designed Pigments

(A) Schematic of the angle-independent characteristic of the pigments.
(B–N) Images of different patterns observed from different viewing angles. (B–F) Chinese dragon; (G–J) goldfish; (K–N) group of letters. Scale bars, 1 cm
(B–J), and 0.5 cm (K–N).

transformed into a short-range order and the arrangement of nanoparticles be-

comes an amorphous state, a non-iridescent and angle-independent material will
be obtained.19,20 The amorphous feature of our pigments was verified through
the SEM images and their corresponding 2D Fourier analysis, as shown in Figure S1.
Moreover, because of the rapid generation of microspheres during the spraying pro-
cess, the component of the pigments had clearly spherical morphology, which could
also contribute to the angle-independent property. These two reasons could
comprehensively explain the angle independence of the designed pigments.

To broaden the applications of our pigments, we employed them as a template for

the negative replication of hydrogels. As displayed in Figures 2E–2G, there were
obvious nanovoids among the multi-shell nanoparticles and microvoids between
the nanoparticle-formed microspheres. Due to the existence of these voids, the

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pregel solution of hydrogels filled in the voids and the hydrogel with the inverse opal
structure of the pigments was able to be obtained after pregel polymerization and
hydrofluoric acid corrosion (Figure S4A). Interestingly, the GO shells remained in
the hydrogel since the corrosion had little impact on them, which could endow the
resultant inverse opal hydrogel with some advanced features. Specifically, N-isopro-
pylacrylamide (NIPAM), a typical thermoresponsive hydrogel, was employed as the
model hydrogel for our subsequent experiments. It has been demonstrated that
the NIPAM hydrogel will shrink when the temperature is higher than its lower critical
solution temperature, whereas when heating is stopped, the hydrogel will gradually
swell and finally be restored to its original shape.39,40 The NIPAM inverse opal hydro-
gel patterns with different colors were generated from the designed pigments, as
shown in Figure S4B. Because of the inverse opal structure of the hydrogel generated
from negatively replicating the template pigments, the resultant inverse opal hydro-
gel also had an amorphous structure, which led to a non-iridescent feature. Thus, the
hydrogel would have the characteristic of angle dependence, and this deduction was
further confirmed by the subsequent observations, as shown in Figures S5A–S5E. It
was demonstrated that the color of the inverse opal hydrogel remained unchanged
from different observation angles. Moreover, since GO was also doped in the hydro-
gel, the resultant hydrogel was imparted with certain features of GO such as photo-
thermal responsiveness, which made the hydrogel more intelligent. We found that
the temperature of the resultant hydrogel could gradually increase under NIR radia-
tion, as demonstrated in Figure S6. With the increase in temperature, the inverse opal
NIPAM hydrogel showed a corresponding shrinking process (Figures S5F–S5I and 6).
In addition, it was apparent that the color of the hydrogel was blue-shifted during the
shrinking process and partially turned white in the end. This phenomenon could be
attributed to the decreasing diameters of the nanovoids and the water discharge
caused by hydrogel shrinkage. Furthermore, the shrinkage of the hydrogel could
lead to a corresponding bending action of the human-shaped hydrogel by fixing
the ‘‘feet’’ to the bottom of the dish, giving the impression of carrying out controllable
sit-ups, as illustrated in Figures 6B–6D and S7.

Besides the sensing features, the negatively replicated inverse opal hydrogels could
also be imparted with self-healing capacity if an appropriate hydrogel was chosen.
To this end we used gelatin, a common thermal reversible gel that can be melted
by heat and turned back into a gel state when the temperature falls, to replicate
the template pigments so as to investigate its self-healing performance. The gener-
ating process of the gelatin inverse opal hydrogel was similar to that of the afore-
mentioned NIPAM hydrogel. It was found that the gelatin hydrogel was also en-
dowed with non-iridescent structural colors due to their characteristic
microstructures (Figure 6E). We separated the hydrogel flowers and pieced together
the petals with different colors. After radiating the seam joint with NIR light, the
petals gradually merged together and became a complete flower with two different
colors, as shown in Figure 6E. This phenomenon could be ascribed to the photother-
mal conversion of the GO remaining in the hydrogel and the sol-gel transition prop-
erty of the gelatin. When the gelatin hydrogel was exposed under NIR, GO could
convert the light energy into heat, which caused the gelatin at the seam joint to
transform into the melting state. When NIR was removed, the sol began to turn
back into the gel state due to gradual temperature reduction. Finally, the hydrogel
resolidified and became whole, thereby completing the entire self-healing process.
In a nutshell, due to the significant features of this derived inverse opal hydrogel, the
applications of our designed pigments would be definitively broadened, since the
hydrogels with intelligent responsive ability and self-healing capacity are urgently
needed in various fields such as medicine, sensing, and electronics.

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Figure 6. Applications of Inverse Opal Hydrogels

(A) Schematic of the photothermal responsiveness of the NIPAM inverse opal hydrogel.
(B–D) Side views of shrinking process and controllable movement of the human-shaped NIPAM hydrogel.
(E) Self-healing process of the gelatin inverse opal hydrogel.
Scale bars, 0.5 cm.

Conclusion
In conclusion, inspired by natural creatures, we developed a GO-doped non-irides-
cent pigment with excellent brightness and self-adhesivity. The elementary unit of
this kind of pigment was the multi-shell nanoparticles generated from SiO2 nanopar-
ticles, GO, and PDA. Compared with most of the previously presented multi-shell
nanoparticles that focused only on the improvement of material brightness,18,19,21
our designed nanoparticles have shown more diversified functions. In our system,
GO provided a high refractive index and broadband light absorption, which made
the color of the pigments brighter, while the involvement of PDA imparted the

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pigments with significant self-adhesivity. It was demonstrated that the elementary

multi-shell nanoparticles could form into microspheres with various sizes after simple
spraying, and, because of the amorphous and spherical structure, the resultant pig-
ments showed characteristic angle independence and wide-angle display. More
importantly, the pigments could be employed as a template for the negative repli-
cation of hydrogels. Due to the distinct structure and composition of the pigments,
the obtained inverse opal hydrogel could be endowed with more advanced features
such as photothermal responsiveness and self-healing capacity. Therefore, our de-
signed non-iridescent pigments are endowed with promising prospects for future
applications.

EXPERIMENTAL PROCEDURES
Materials
The silica (SiO2) nanoparticles were purchased from Nanjing Dongjian Biological Tech-
nology. Dopamine hydrochloride was purchased from Sigma-Aldrich. GO dispersion
(XF224-1, 5 mg/mL) was purchased from Nanjing XFNANO Materials. Tris base was pur-
chased from Sigma-Aldrich. Hydrochloric acid was purchased from Sinopharm Chemical
Reagent, as was absolute ethanol. N-Isopropylacrylamide, N-methylolacrylamide
(NMA), and 2-hydroxy-2-methylpropiophenone (HMPP) were purchased from Sigma-
Aldrich. Hydrofluoric acid was purchased from Aladdin Industrial (Shanghai, China).
Deionized water with a resistivity of 18.2 MU$cm 1 was obtained from a Millipore
Milli-Q system. All other chemical reagents were of the best grade available and used
as received, and deionized water was used in all experiments. The purity of all chemical
reagents used was analytical grade.

Generation of the Multi-shell Nanoparticles

The original silica nanoparticles were prepared in an aqueous solution at a concentration
of 0.1 g/mL. Silica nanoparticles of different sizes (200, 220, 228, 235, 239, 243, 245, 255,
263, and 270 nm) were used. Dopamine hydrochloride was prepared in an aqueous so-
lution at a concentration of 13.3 mg/mL. (1) The volume of the whole reaction system was
10 mL, which contained 1.5 mL of dopamine solution (13.3 mg/mL), 2.03 mL of silica
nanoparticles solution (0.1 g/mL), 5 mL of Tris base (0.1 mol/L), and 1.47 mL of HCl
(0.1 mol/L). The entire reaction system was alkaline, and the pH was 8.5. The system
was put in a glass bottle and stirred for 6 h, at which point the polydopamine adhered
to the surface of the silica nanoparticles. The system was then centrifuged at 6800 rpm
for 10 min. (2) After discarding the supernatant, the dopamine-adhered nanoparticles
were resuspended by GO dispersion (0.5 mg/mL). The resuspension was then stirred
for 6 h to obtain the GO-encapsulated silica nanoparticles. After this process, step (1)
was repeated so as to cover the nanoparticles with dopamine and improve the adhesivity
of the nanoparticles. The nanoparticles with multi-GO shells were obtained by repeating
steps (1) and (2) in sequence. The microstructure of the nanoparticles was obtained by a
transmission electron microscope (JEOL, JEM-2100). Reflection spectra of the nanopar-
ticles were measured by an optical microscope (Olympus BX51) equipped with a fiber-
optic spectrometer (Ocean Optics QE65000).

Generation of the Non-iridescent Structural Colored Pigments

The multi-shell nanoparticles were dispersed in the absolute ethanol to obtain the
nanoparticle dispersion, which was then sprayed under NIR radiation. At this point,
the NIR light was provided by an infrared incandescent reflector lamp (Philips Incan-
descent BR125; 230–250 V). Different nanoparticles were used to obtain patterns
with different colors and brightness. The images of the pigments were photo-
graphed by a light microscope (Olympus BX51) equipped with a color CCD camera
(Media Cybernetics Evolution MP 5.0). The images of the patterns at different

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viewing angles were captured by the camera of an iPhone 6S. The corresponding
reflection spectra were measured by the microscope (Olympus BX51) equipped
with a fiber-optic spectrometer (Ocean Optics QE65000). The microstructures of
the pigments were captured by a scanning electron microscope (Hitachi S-300N).
The 2D Fourier analysis was conducted by the software DigitalMicrograph.

Generation of the Inverse Opal Hydrogel from the Pigments

The pregel solution was composed of 10% NIPAM and 1% HMPP, in which the mass ra-
tio between NIPAM and NMA was 30:1. The patterns were infiltrated by the pregel so-
lution for several minutes, then the pregel was polymerized under a UV light. Different
patterns of hydrogel were obtained through using mask plates with different patterns.
Hydrofluoric acid was used to remove the silica elements of the nanoparticles while
the GO shells remained in the hydrogel. The resultant inverse opal hydrogel was then
placed under NIR radiation (808 nm; Xi Long Tech, China) to observe the shape and co-
lor changes of the hydrogel; the radiation intensity of NIR light was 0.5 W cm 2. When
the experiment with human-shaped hydrogel was conducted, the hydrogel was first
fixed to the bottom of the dish by epoxy resin (Devcon 5 Minute Epoxy). The images
were captured by the camera of an iPhone 6S and a thermal imager.

Self-Healing Capacity of the Gelatin Inverse Opal Hydrogel

Gelatin (8%) was chosen to generate inverse opal hydrogel, and the generation
method was the same as for NIPAM hydrogel. The gelatin hydrogels were separated
into pieces and the petals with different colors were put together. NIR light (808 nm;
Xi Long Tech) was employed to radiate the seam joint of the stitching flower at radi-
ation intensity of 0.5 W cm 2. After a period of radiation, the gelatin at the seam joint
was transformed into the melting state. The NIR was then removed, the sol resolidi-
fied, and the entire self-healing process was completed.

SUPPLEMENTAL INFORMATION
Supplemental Information can be found online at https://doi.org/10.1016/j.matt.
2019.08.018.

ACKNOWLEDGMENTS
This work was supported by the National Natural Science Foundation of China (grant
nos. 61927805 and 51522302), the NSAF Foundation of China (grant no. U1530260),
the Natural Science Foundation of Jiangsu (grant no. BE2018707), the Scientific
Research Foundation of Southeast University, and the Scientific Research Founda-
tion of the Graduate School of Southeast University (grant no. YBPY1873).

AUTHOR CONTRIBUTIONS
Y.Z. conceived the idea and designed the experiment; Y.L. carried out the experi-
ments; Y.L. and Y.Z. analyzed data and wrote the paper; C.S., Y.W., and L.S. contrib-
uted to scientific discussion of the article.

DECLARATION OF INTERESTS
The authors declare no competing interests.

Received: July 8, 2019

Revised: August 5, 2019
Accepted: August 22, 2019
Published: October 2, 2019

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