RESEARCH ARTICLE

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Implantable Wet-Adhesive Flexible Electronics with

Ultrathin Gelatin Film
Ximin Yuan, Weicheng Kong, Pengcheng Xia, Zhenjia Wang, Qing Gao, Jie Xu,*
Debin Shan, Qingqiang Yao, Zhiyong Ma,* Bin Guo, and Yong He*

development is still constrained by a se-

Implantable flexible electronic has attracted significant research interest in ries of challenges. These challenges include
various fields. However, it still faces the challenge of simultaneously achieving the need for long-term tissue adhesion, im-
tight adhesion to tissues in a mildly wet environment and possessing provement of contact surface conformity,
excellent biocompatibility to reduce immune rejection reactions after feasibility of in vivo degradation, and ad-
dressing the fatigue resistance of flexi-
implantation. Here, a degradable wet-adhesive flexible electronic device based
ble electrodes in high-strain environments.
on liquid metal and ultrathin gelatin film is developed. The ultrathin gelatin The current main approach to address-
film forms numerous hydrogen bonds with tissue in a slightly humid ing these challenges involves using flexible
environment, rapidly constructing a wet-adhesive interface without damaging and stretchable materials to improve shape
tissue structure. Inkjet printing is utilized to pattern the mixture of liquid conformity. For instance, flexible electronic
devices have been developed using compos-
metal and PVP on the surface of the ultrathin gelatin to create flexible patch.
ite materials composed of conductive nano-
With the excellent conductivity of liquid metal, low toxicity, and similarity to materials and polymers,[5,6] organic con-
natural tissue components of gelatin, flexible patch exhibits outstanding ductive polymers,[7,8] and organic thin-film
biocompatibility and fatigue resistance. It can be implanted in the body for up crystals.[9,10] These devices were widely used
to 6 weeks, retaining monitoring capabilities and resisting 1 000 000 cycles of for surface and in vivo monitoring. How-
bending fatigue. This study provides a novel strategy for the future ever, several key challenges persist with
these technologies. First, traditional meth-
development of implantable flexible electronics.
ods for achieving stable contact between
the device and the interface involve su-
turing the device to the tissue, leading
1. Introduction to localized damage, significant bleeding, acute/chronic inflam-
mation, and, in severe cases, life-threatening complications.[11,12]
Implantable flexible electronic devices have garnered widespread Second, the conductivity of current conductive materials is rela-
research interest in recent years due to their unique ability to tively low, and exposure to the wet environment inside the body
establish a direct interface with biological tissues or organs.[1,2] leads to a sharp decrease in conductivity, compromising the accu-
This is achieved through the design of wavy/undulating struc- racy of electrical signal output.[13,14] Additionally, while conduc-
tures and the superior positioning of inorganic materials on tive materials can establish contact with internal tissues, the low
a neutral mechanical plane.[3,4] However, despite the poten- fluidity of conductive materials and the high modulus of the sub-
tial significance of this technology in the biomedical field, its strate result in a mismatch in modulus and lack of conformity

X. Yuan, Z. Wang, J. Xu, D. Shan, B. Guo P. Xia, Q. Yao

State Key Laboratory of Advanced Welding and Joining Department of Orthopaedic Surgery
Harbin Institute of Technology Institute of Digital Medicine
Harbin 150001, China Nanjing First Hospital
E-mail: [email protected] Nanjing Medical University
X. Yuan, Z. Wang, J. Xu, D. Shan, B. Guo Nanjing 210006, China
National Innovation Center for Advanced Medical Devices Z. Ma
Shenzhen 457001, China School of Engineering
W. Kong, Q. Gao, Y. He Huzhou University
State Key Laboratory of Fluid Power and Mechatronic Systems Huzhou, Zhejiang 313000, China
School of Mechanical Engineering E-mail: [email protected]
Zhejiang University Y. He
Hangzhou 310027, China Key Laboratory of 3D Printing Process and Equipment of Zhejiang Province
E-mail: [email protected] College of Mechanical Engineering
Zhejiang University
The ORCID identification number(s) for the author(s) of this article Hangzhou 310027, China
can be found under https://doi.org/10.1002/adfm.202404824
DOI: 10.1002/adfm.202404824

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in surface shape between the device and the tissue.[15,16] This re- implantable wet-adhesive flexible patch (Figure S2, Supporting
duces the fatigue resistance of flexible devices, significantly im- Information). EGaIn is chosen as the model liquid metal due to
pacting their lifespan. its widespread research attention. EGaIn is a commonly used liq-
To date, the materials and strategies developed for implantable uid metal with a variety of excellent properties (low melting point,
flexible electronic patches face challenges such as a lack of au- high conductivity, reproducibility, biocompatibility, etc.), making
tomatic degradation in vivo and potential damage to adhered it the focus of many studies. The wet-adhesive flexible device is
tissues. This is primarily due to significant differences in com- composed of ultrathin gelatin films and a EGaIn/PVP mixture
position and structure between the selected substrate materi- arranged in a hierarchical distribution (Figure 1b). In addition,
als and natural tissues.[17,18] Ideal implantable electronic patches the adhesive capability between the mixture of EGaIn/PVP and
should exhibit the following properties: controllable degradation the gelatin film substrate was analyzed based on a molecular dy-
time, modulus matching, non-damaging adhesion, and long- namics model. EGaIn/PVP mixture can establish adhesion inter-
term stability.[19–21] Developing materials that meet these criteria faces with gelatin films through hydrogen bonding (Figure 1c).
is crucial for advancing implantable flexible electronic patches Consequently, the gelatin film achieves wet adhesion to tissues
with improved performance and reduced impact on biological through ─OH and ─COOH interactions. When in a slightly hu-
systems. mid environment, a significant number of hydrogen bonds in the
In this study, we present an implantable flexible electronic gelatin film are released, allowing for the rapid establishment of
patch based on an ultrathin gelatin film. The gelatin film rapidly an adhesive relationship with tissues without compromising tis-
adheres to tissue surfaces within 0.13 s without causing damage sue morphology and functionality (Figure 1d).
to the tissues. Self-assembly of liquid metal with polyvinylpyrroli- Furthermore, the wet-adhesive flexible patch could be used as
done (PVP) is achieved through ultrasonic processing, allowing an implantable monitor for real-time monitoring of rat ECG and
it to adhere to the gelatin film and form a flexible electronic EEG, establishing a platform to assess the health of rats. The
patch. Even after 1 000 000 repeated bending cycles, the resis- flexible patch could degrade automatically in the body within
tance changes by <10%. The patch demonstrates excellent adhe- 6 weeks and be excreted through the kidney, avoiding bleeding
sion in wet environments, enabling effective monitoring when and inflammation caused by secondary surgeries and even life-
fully attached to the heart’s surface. Additionally, it can undergo threatening situations in severe cases (Figure 1e). To demonstrate
on-demand degradation, avoiding the harm associated with sec- the maturity and accuracy of this strategy, complex conductive
ondary surgeries. This technology provides a new approach for patterns (Great Wall and school emblem) were created based on
developing biodegradable medical electronic devices with poten- customized patterns, displaying intricate details. To further il-
tial clinical applications. lustrate the accuracy of the conductive circuit, scanning electron
microscopy was used to characterize the line width of the liquid
2. Results and Discussion metal mixture. The line diameter of the liquid metal was observed
to be ≈88 μm, maintaining high precision at the corner and con-
2.1. Preparation Mechanism sistent with the designed shape (Figure 1f).

Implantable wet-adhesive flexible electronic is a novel electronic

technology with extensive potential applications. However, it still 2.2. Mechanical Properties
faces some unresolved challenges, including stability, durability,
and biocompatibility. To address these issues, we have success- Furthermore, the transparency of the gelatin film was further ver-
fully developed biocompatible wet-adhesive flexible electronic ified (Figure 2). Surface morphology of the gelatin film was ob-
with superior performance. served through atomic force microscopy (AFM). It can be seen
Implantable wet-adhesive flexible electronic patch was ob- that the film has low surface roughness, and from the 3D struc-
tained based on the following strategy. First, a silicone film with ture diagram, it is evident that it exhibits excellent smoothness
a specific hollow size was produced using laser technology and (Figure 2a). The characterization of surface morphology using
placed on the surface of a PET film. Next, a well-mixed gelatin so- AFM has limitations. To more fully demonstrate the transparency
lution was slowly poured into the silicone film and transformed of the gelatin film, a white light interferometer was employed.
into a hydrogel through a gradual gelation process at room tem- White light interference analysis indicated that the initial metal
perature. The gelatin solution precisely filled the silicone mold surface Sa and Sq were 0.333 and 0.445 μm, respectively. After ad-
through self-leveling and self-evaporation, resulting in an ultra- hering the gelatin film to the metal surface, Sa and Sq increased
thin gelatin film that was allowed to stand at room tempera- by only 0.005 and 0.004 μm, providing further evidence of the out-
ture for 12 h (Figure S1, Supporting Information). The ultrathin standing transparency of our produced gelatin film (Figure 2b;
gelatin film obtained through this technique exhibited excellent Figure S3, Supporting Information). Sa (average roughness) rep-
transparency, allowing clear visibility of the sky, tree, and even the resents the average height deviation of a surface from a refer-
texture of leave and finger (Figure 1a). Additionally, implantable ence line (typically the mean surface). Sq (root mean square)
wet-adhesive flexible electronic was fabricated using inkjet print- height deviation, on the other hand, represents the range of
ing technology. A metal mask with a customized pattern as placed height variations on the surface. The text beneath the film can be
on the gelatin film through wet-etching, and a conductive pattern clearly seen. To precisely demonstrate its excellent light transmit-
was printed using a 3D printer with inkjet printing (the printing tance, the film underwent transparency testing and white light
material was a mixture of liquid metal and PVP pre-treated with analysis. The transmittance of the gelatin film was found to be
ultrasonic), allowing for the easy and large-scale production of 92%, with a haze of only 0.9%, as measured by a transmittance

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Figure 1. Preparation mechanism of implantable wet-adhesive flexible electronic device. a) The presentation of ultrathin gelatin film. b) The components
of an implantable wet-adhesive device. c) The adhesion mechanism of EGaIn/PVP mixture to ultrathin gelatin film. d) The adhesion mechanism between
flexible electronic and tissue in a slightly humid environment. e) Implantable wet-adhesive flexible electronic for EEG and ECG signals monitoring. f)
Complex patterns of the Great Wall and school emblem created using an inkjet printing process. Scale bar = 50 μm.

meter (Figure 2c). The gelatin film exhibits excellent mechanical (90 MPa), albeit with a reduction in its ductility (Figure 2f; Figures
properties, capable of being folded into multiple layers or curled, S5 and S6, Supporting Information). Thus, the gelatin film can
making it the thinnest reported gelatin film to date (≈573 nm, be customized according to specific requirements for ultra-thin
Figure 2d). films.
Moreover, we observed an interesting phenomenon: after mul- In order to precisely reveal the changes in the internal struc-
tiple cycles of drying and swelling treatment, the gelatin film ture of the gelatin, we conducted differential scanning calorime-
formed nano-level ordered structures (Figure 2e; Figure S4, Sup- try (DSC) to verify its stability. It is evident that with an increase
porting Information). This transition from disorder to order in the number of freeze-drying cycles, the melting peak of the
within the internal structure of gelatin resulted in an anisotropic gelatin film gradually shifted to the right, indicating a denser in-
structure, enhancing the strength of the gelatin film by 900 times ternal structure and a gradual increase in orderliness (Figure 2g;

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Figure 2. The mechanical properties of the ultrathin gelatin film. a) The surface morphology of the gelatin film. Insert is 3D morphology. b) The light
transmittance of gelatin film. c) The transparency performance of the gelatin film. d) The thickness of the gelatin film. Inserts are folding and curling of
the gelatin film. (I) is pure metal substrate. (II) is a substrate for attaching a gelatin film to the metal surface. e) SEM images of the gelatin film. f) The
mechanical properties of the enhancing gelatin film. g) The DSC characterization of the gelatin film. h) The degradation behavior of the gelatin film. i)
Comparative analysis of the overall performance between the gelatin film and other films.[22–26]

Figure S7, Supporting Information). As it is intended for in vivo ternal force is required to facilitate adhesion by pressing). This
studies later, in vivo degradation was explored. It was found that represents the shortest reported adhesion time in the literature
with an increase in film thickness, the degradation time gradu- to date. It could be lifted and even swung rapidly from side to side
ally increased, suggesting that users can choose films of different with a single-sided swing amplitude of ≈67° while maintaining a
thicknesses based on specific scenarios (Figure 2h). The ultra- strong adhesion (Figure 3b; Video S2, Supporting Information).
thin gelatin film prepared by us exhibits excellent comprehensive Furthermore, it can adhere to the surface of small (rat) or large
performance, combining strength, thinness, degradability, high (rabbit) animal hearts even under continuous washing of the wa-
transparency, and adhesiveness simultaneously, making it suit- ter. After the rinsing process, the adhesion state of the gelatin
able for a variety of use cases (Figure 2i). remains the same as the initial state (Figure 3c; Video S3, Sup-
porting Information). Taking all factors into consideration, the
ultrathin gelatin film can be optimally used as a heart adhesion
2.3. Adhesion Performance substrate, eliminating the need for detachment or failure issues,
to achieve accurate recording of cardiac signals. Even after 4 days
To demonstrate the actual adhesion of the gelatin film, it was ad- of flushing, it still maintains some adhesion (only a 20% decrease
hered to a rat heart, and it adhered firmly to the heart surface compared to the initial adhesion), suggesting its sustained in vivo
in just 0.13 s (Figure 3a; Video S1, Supporting Information) ex- adhesion (Figure 3d).

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Figure 3. The adhesion performance of ultrathin gelatin film. a) Instantaneous adhesion of the gelatin film on a rat’s heart within 0.13 s. b) Demonstration
of the adhesion force of the gelatin film. c) Wet adhesion of the gelatin film on rat and rabbit heart during washing. d) Adhesive strength of the gelatin
film. e) The mechanism diagram of the adhesion between the gelatin film and the skin in the absence of water. f) The schematic diagram of the adhesion
mechanism between the gelatin film and the skin in the presence of water. g) The binding energy of the gelatin segments. h) Perpendicular adhesion
force of different material films on the rabbit heart. i) Shear adhesion force of different material films on the rabbit heart. j) Adhesion fatigue performance
of gelatin film on rabbit heart tissue. Scale bar = 5 mm.

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To gain a deeper understanding of the adhesion mechanism bonds, and regions of enrichment for Ga and N elements over-
of gelatin film to tissues in a slightly humid environment, it has lapped (Figure 4a). Further analysis of the atomic distribution
been thoroughly investigated based on density functional the- patterns through high resolution showed that when the mass ra-
ory (DFT). The collagen peptide chain is a long chain structure tio of liquid metal to PVP was 1:1 and the ultrasonic time was
composed of 23 amino acid segments. In order to form adhe- 5 min, the coordination compound exhibited excellent crystalline
sion in the body and muscle tissue, the amino acid segments properties, appearing as a single crystal structure with dominant
need to have some charged binding sites, such as ─COOH or growth along the (011) plane. Comparatively, only the mass ratio
─NH2 . After the screening, ASP, THR, SER, GLU, GLY, ARG, of liquid metal to PVP at 1:1 with an ultrasonic time of 5 min
PRO, and HYP play a major role (Figure S8, Supporting Infor- maintained good conductivity for this coordination compound
mation). Through calculations, it is found that the peptide chain (Figure S11, Supporting Information). As observed in the SEM
of collagen is difficult to bond with muscle tissue. This is be- images, with the increase in ultrasonic time, the particle size of
cause the binding sites have electric characteristics consistent the LM gradually decreases (from ≈12 to 2 μm), and the dis-
with the molecular structure of muscle tissue, forming a clear persion increases. As the ultrasonic time increases, the parti-
vacuum layer between the two. This greatly hinders wet adhe- cle size of the LM tends to become more uniform (Figure S12,
sion. However, in a wet environment with water, small and polar Supporting Information). Furthermore, the electrical conductiv-
water molecules greatly fill the vacuum layer (Figure 3e,f). At this ity of the mixture was measured using voltammetry. It was ob-
point, collagen adheres to muscle tissue. Furthermore, the bind- served that the best conductivity was achieved when the ratio of
ing energy in dry and wet environments is also calculated. In a EGaIn to PVP was 1:1, with an ultrasonication time of 5 min
wet environment, the binding energy of GLU, ARG, PRO, and (Figure 4b; Figure S13, Supporting Information). Finally, the con-
HYP is significantly increased. Interestingly, water molecules not ductive mixture was coated on the surface of the gelatin film,
only fill the vacuum layer but also, more importantly, release the and a uniaxial reciprocating cycle was applied 1 000 000 times
stress of the peptide chain in the wet environment. The overall (Figure 4c). It was observed that at the beginning of the cycle, the
adhesion of the chain to muscle tissue is greatly improved. At mixture underwent mechanical sintering, leading to a decrease
this point, the total binding energy equals the binding energy of in resistance. However, with increasing time, the pathway for free
water filling plus the binding energy of the geometric state of the electron transfer was disrupted, resulting in a decrease in elec-
peptide chain. This results in the overall chain adhesion being tron transfer efficiency and an increase in resistance.
higher than the individual binding energy (Figure 3g). Using X-ray diffraction (XRD) techniques, we conducted a de-
Additionally, when compared to other material films (includ- tailed analysis of the crystallinity of mixture (Figure 4d). Excit-
ing commercial band-aids, PDMS, and Ecoflex), the ultra-thin ingly, optimal crystallinity was observed when the mass ratio of
gelatin film (cut into samples of the same size) exhibits signif- liquid metal to PVP was 1:1, however, with an increase in ultra-
icantly higher adhesion forces, both in the normal and tangen- sonication time, the crystallinity noticeably weakened. XRD spec-
tial directions on the surface of the rabbit heart (Figure 3h,i). The tra revealed well-defined crystalline peaks at 21.4°, 37.2°, 54.0°,
gelatin film not only exhibits excellent wet adhesion to heart tis- and 60.2°, indicating the formation of a highly ordered structure.
sue but also demonstrates remarkable adhesion to other materi- The appearance of these peaks is consistent with TEM results
als (metal, glass, paper, resin, and Teflon). Additionally, it can sup- (Figure 4a), reinforcing our understanding of the structural mor-
port a weight over 1035 times its own, indicating significant adhe- phology. The cyclic voltammetry (CV) curves effectively charac-
sive strength (Figure S9, Supporting Information). The adhesion terize the intrinsic redox properties of the material, providing in-
force of the gelatin film remains consistently high even after re- sights into the oxidation–reduction processes of the liquid metal
peated adhesion to the heart tissue for up to 1000 cycles, without versus PVP under different reference and sonication times. The
significant deterioration in adhesion performance (Figure 3j). Al- experiment employed a three-electrode system, with the liquid
though there is a decrease in adhesion force after 1000 cycles, it metal versus PVP mixture uniformly coated on a silver electrode
does not mean that the adhesion performance of the gelatin film as the working electrode. Simultaneously, a saturated calomel
is completely ineffective. It still ensures that the flexible device electrode and a platinum electrode served as the reference and
maintains stable monitoring performance (Figure S10 and Video counter electrodes, respectively. The results indicate that, with
S4, Supporting Information). In summary, ultrathin gelatin film a threshold of −1.1 V, values above it exhibit oxidative behav-
demonstrates excellent wet adhesion and underwater adhesion, ior, while values below it show reductive behavior. Within the
laying a robust foundation for the future development of in vivo −1.2–−1.3 V range, a reduction peak for the material is observed,
wet adhesion electronics. while oxidation peaks are evident in the −1.0–−1.1 V range. No-
tably, when the ratio of liquid metal to PVP reaches 1:1, the ma-
terial exhibits the strongest redox characteristics, indicating opti-
2.4. Electrical Performance mal conductivity. Furthermore, as the sonication time increases,
the redox properties decrease. This is attributed to the fact that
The conductive liquid metal (LM) mixture was obtained by ul- prolonged sonication leads to the rupture of the oxide film, hin-
trasonically dispersing the LM uniformly in polyvinylpyrrolidone dering PVP from effectively capturing the liquid metal for coordi-
(PVP, Figure 4). The nanostructure of the liquid metal/PVP nated bonding. Consequently, the material exhibits a significant
mixture was analyzed using TEM and equipped with EDS. Af- decrease in conductive performance, resembling an open circuit
ter ultrasonic treatment, In and Ga elements were separated, (Figure 4e; Figure S14, Supporting Information).
forming naturally occurring nano-microsphere structures. Ga To reveal the stability of the material system, 100 cycles were
elements reacted coordinately with PVP, forming coordination conducted. During this process, when the material underwent

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Figure 4. Conductivity of the liquid metal-PVP mixture. a) TEM images of the mass ratio of EGaIn to PVP is 1:1, with an ultrasonic time of 5 min. Scale
bar = 50 nm. b) The voltammetric curves of the mixture at different treatment methods. c) Cycle fatigue of the mixture coated on the gelatin film. d)
XRD curves of the mixture at different treatment methods. e) The C–V thermal map of the mixture at different scan rates. f) Raman characterization of
mixtures with different ultrasonic times. g) XPS curves of mixtures with different sonication times. h) DFT theoretical models of mixtures with different
sonication times.

breakage in the cyclic reaction, a silver foil oxidation satellite peak ance of cracks but still exhibiting a satellite peak of the base sil-
appeared to the left of the liquid metal oxidation peak on the ver foil. On the other hand, EGaIn:PVP = 1:1, due to its stable
surface coated with the material. The results indicated that the structure formed by good coordination, did not undergo break-
sample with EGaIn:PVP = 2:1 exhibited its oxidation peak first. age after 100 cycles (Figure S15, Supporting Information). More-
Meanwhile, in the case of EGaIn:PVP = 1:2, where adequate co- over, with an increase in ultrasonic time, the stability of the ma-
ordination was not formed, the excess PVP could not withstand terial decreased. However, the increased ultrasonic time led to
the degradation of the cyclic current, resulting in a later appear- an increase in the oxidation film. The Nyquist plot was used to

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evaluate the chemical behavior of the material in a wet environ- 2.5. Brain Signal Recording
ment. The results indicate that all five samples exhibit a clear
second-time response simulated circuit. EGaIn:PVP = 1:1 shows The excellent biocompatibility and high conductivity of im-
a simulated circuit of Rs(QR)(QR), while the others show a sim- plantable wet-adhesive flexible electronics make them a promis-
ulated circuit of Rs(CR)(QR). It is evident that Rs is the solu- ing device for long-term recording of deep brain neural signals.
tion resistance, and (QR) corresponds to the liquid metal. In The device is designed with a fork-shaped electrode configuration
EGaIn:PVP = 1:1, PVP corresponds to (QR), while in the other due to its excellent features, including enhanced sensor sensitiv-
samples, PVP corresponds to (CR). PVP, exhibiting capacitive ity, reduced interference effects, rapid response time, and high
properties, transforms into a constant phase angle element af- controllability.[29–31] In this regard, our implantable wet-adhesive
ter adding an appropriate amount of liquid metal, leading to an patch demonstrates excellent performance in adhering to the tis-
improvement in conductivity (Figure S16, Supporting Informa- sue surface within 3 s (traditional suturing may take several tens
tion). The homogeneity of liquid metal itself appears as a con- of minutes). This is achieved through a layer-by-layer process and
stant phase angle element (denoted as Q) in the electrochem- inkjet technology to construct implantable wet-adhesive bioelec-
ical impedance spectroscopy detection process. However, un- tronic patch. Based on inkjet technology, conductive patch was
der different process parameters, the morphology of PVP on created on the surface of the ultrathin gelatin film, and then
the surface of liquid metal will exhibit either a charge trans- gelatin solution was spin-coated for sealing. The total thickness
fer resistance (CR) or a constant phase angle element (QR) of the patch is ≈90 μm (Figure 5a,b; Figure S21, Supporting In-
form, indicating that PVP appears as a capacitance. The deter- formation). The biocompatibility of the conductive patches was
mining factors for this variation are the ultrasonic time and validated through co-culture with C2C12 cells. After 3 days of ob-
material ratio. The research results indicate that under condi- servation, the co-cultured cells exhibited good activity (green indi-
tions of 5 min and a 1:1 ratio, a stable gradient of PVP is cates live cells, and a higher proportion of green indicates higher
formed, while other parameters may result in the heterogeneity cell proliferation and activity). To further accurately demonstrate
of PVP, appearing in a capacitance form (Figure S17, Supporting the biocompatibility of the conductive patches, we analyzed their
Information). cell proliferation data. Cell proliferation was assessed through
The formation of coordination bonds may introduce energy OD values, and the cell proliferation of the conductive patches
gaps or alter the localized states of electrons, thereby reduc- was even higher than that of the blank group, mainly due to
ing conductivity. Furthermore, coordination bonds may cause the hydrogel providing some of the conditions necessary for cell
electrons to transfer from the surface of the liquid metal to growth. Furthermore, after 3 days, the cells maintained excellent
the ligand, potentially reducing the availability of conductive activity, suggesting that the patches have excellent biocompatibil-
electrons in the liquid metal.[27,28] FTIR and Raman charac- ity (Figure S22, Supporting Information).
terization results indicate that with increasing ultrasonic time, Brainwaves are electrical signals generated by the activity of
the peak intensity of C═O gradually decreases, indicating the neurons in the brain. Depending on their frequency, brainwaves
formation of coordination bonds between C═O and Ga over are categorized into different bands. Delta waves (𝛿, 0.5 to 4 Hz)
time (Figure 4f; Figure S18, Supporting Information). In con- typically occur during deep sleep and are associated with the reg-
clusion, the increase in resistance with increasing ultrasonic ulation of both dreaming and non-dreaming sleep phases. Theta
time is a complex process involving surface chemical reac- waves (𝜃, 4 to 8 Hz) are usually linked to deep relaxation, medita-
tions, particle aggregation, and structural changes. These fac- tion, and light sleep stages. They also play a role in creative think-
tors interact, causing the resistance to gradually increase over ing and learning. Beta waves (𝛽, 13 to 30 Hz) typically appear dur-
time. ing alertness and concentrated states of attention, for example,
In the early stages of ultrasonic processing, PVP may aid in when awake, thinking, or engaged in daily activities. When the
dispersing the LM particles, reducing aggregation between par- rat first enters the surgical state and is in deep sleep, the thermal
ticles. However, with prolonged ultrasonic time, PVP may de- map in the frequency range of delta waves (𝛿, visible in red) is
grade or separate to some extent, causing particles to re-aggregate prominent. Therefore, delta waves dominate, while theta waves
and increasing resistance. Additionally, the high-intensity oscilla- (𝜃) and beta waves (𝛽) are in a secondary position. As the surgery
tion of ultrasonic may promote chemical reactions between PVP progresses and the effects of anesthesia gradually diminish, the
and the LM surface, forming coordination bonds. These surface rat gradually regains consciousness, entering a state of regu-
reactions can reduce electronic conductivity, leading to an in- lar thinking or alertness, where theta waves and beta waves be-
crease in resistance. This result was further explored based on come dominant (energy on the thermal map gradually increases).
DFT. It was found that ultrasonic processing can cause C═O This phenomenon is attributed to the crucial role of synchro-
in PVP to coordinate with Ga in LM, forming a C─O─Ga co- nized neural activity in maintaining and terminating deep sleep
ordination bond (Figure 4g; Figure S19, Supporting Informa- (Figure 5c–e; Figures S23 and S24, Supporting Information). Fur-
tion). After DFT calculation, it was found that liquid metal and thermore, the relationship between the diameter of the lines in
PVP are two separate substances without ultrasonication. After flexible electronic devices and the amplitude of the transmitted
proper ultrasonication, liquid metal and PVP will crosslink to signal has been explored. It has been observed that as the line di-
form C─O─Ga coordination bonds. However, with excessive ul- ameter increases, the signal amplitude gradually decreases. This
trasonication, the coordination bonds will break, increasing the phenomenon may be attributed to the increase in line diameter,
exposure of oxides, further leading to an increase in resistance, leading to enhanced rigidity of the device, thereby weakening the
consistent with Figure 4g (Figure 4h; Figure S20, Supporting interface relationship established with tissues (Figure S25, Sup-
Information). porting Information). For comparison, commercial patches and

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Figure 5. The recording of EEG signal was based on implantable wet-adhesive flexible electronic. a) The schematic for rat EEG monitoring. b) Adhesion
of wet-adhesive flexible electronics to the brain. c) Recording of brain waves in the 𝛿-band with the extension of surgery time. d) Recording of brain
waves in the 𝜃-band with the extension of surgery time. e) Recording of brain waves in the 𝛽-band with the extension of surgery time. f) Recording the
amplitude of signals with different patches. g) The attenuation of signals recorded by different patches increases with the extension implantation time.
h) Fitting of EEG signal.

PDMS patches were prepared and used to record rat EEG signals ductivity of commercial patches or PDMS patches. Additionally,
under the same conditions. However, both commercially avail- there is a significant mismatch in modulus between commer-
able patches and PDMS patches exhibit a significant difference cial patches or PDMS patches and brain tissue, preventing them
from the conductivity patches we produced, whether in terms of from adhering perfectly to the surface of brain tissue. This leads
sensitivity or in vivo stability. Our conductive patches can stably to cell migration around the patch, forming a glial sheath, which
exist in vivo for 6 weeks while maintaining excellent monitor- severely hinders electron transfer and causes a gradual weaken-
ing performance (Figure 5f,g; Figure S26, Supporting Informa- ing of signals over time. However, the wet-adhesive flexible elec-
tion). This is mainly due to the poor biocompatibility and con- tronics we produced exhibit excellent biocompatibility and high

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Figure 6. In vivo signal recording on the rat heart. a) Schematic diagram of epicardial signal recording. b) Conformal adhesion capability of the conductive
patch on the heart. c) Recording of ECG signal within 60 s. d) Spatiotemporal biopotential map of ECG signals within 60 s. e) Statistical analysis of signal
SNR. f) Statistical analysis of signal amplitude. g) Spatiotemporal stability of ECG signal. h) Spatiotemporal biopotential map of a rhythm.

conductivity, addressing these challenges effectively. Addition- 2.6. Conformal Monitoring with Conductive Patch
ally, with the increase in time, the conductive patches undergo
varying degrees of degradation. The degradation of the conduc- Suturing is a typical tissue engineering fixation technique, en-
tive patches in vivo was observed using H&E and SR staining abling traditional ECG devices to provide monitoring data of
techniques (pink in H&E represents conductive patches, red in electrocardiographic signals. However, critical challenges such as
SR represents conductive patches, and black represents the mix- complex organ shapes, intricate surgeries, and issues like bleed-
ture of liquid metal and PVP). It can be observed that the conduc- ing or inflammation during the process severely hinder surgeries
tive mixture of liquid metal and PVP begins to peel off slightly inside animals (Figure 6a).
and spontaneously degrade after 3 weeks. Furthermore, due to The rat heart was selected as the model system to evaluate the
their self-degradation characteristics, the ultra-thin gelatin film monitoring performance of the implantable wet-adhesive flexi-
also spontaneously becomes thinner over time after 6 weeks, ble electronic patch. The chest was opened to expose the heart,
and the liquid metal mixture also begins to gradually decompose and the conductive patch was fixed on the surface of the heart.
(Figure S27, Supporting Information). During the contraction and expansion of the heart, the conduc-
Furthermore, by combining theoretical values with actual re- tive patch was able to maintain conformal and stable contact
sults, as the surgery progresses, the deep sleep signals of rats with the heart (Figure 6b). Successful acquisition of ECG sig-
gradually weaken, while the signals of light sleep or alertness nal was achieved. In comparison with commercial and PDMS-
gradually increase, indicating that the rats are about to wake up. based patches, the implantable conductive patch demonstrated
This significantly helps surgical staff in carrying out the proce- significantly improved stability in recording signals, with high
dure effectively (Figure 5h). We believe that studying brainwaves uniformity (Figure 6c,d). The use of the gelatin film effectively en-
contributes to understanding the relationship between brain ac- hanced the wet adhesion performance on dynamic tissues, lead-
tivity and cognitive function. Moreover, in the medical field, espe- ing to a substantial improvement in recording quality in terms
cially in neuroscience and neurology, the measurement of brain- of signal-to-noise ratio (SNR) from 8 to 45 and the amplitude
waves has crucial applications. Our implantable wet-adhesive from 3.1 to 4.2 mV (Figure 6e,f). To assess the stability of the
flexible conductive patch fills this gap perfectly. heart rate, a statistical analysis of the amplitude stability within a

Adv. Funct. Mater. 2024, 34, 2404824 2404824 (10 of 12) © 2024 Wiley-VCH GmbH
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unit pulse time was conducted. It was observed that the conduc- the film surface using masking tape (to avoid damaging the film later).
tive patch exhibited excellent stability compared to commercial Conductive ink was then jetted onto the mask using an inkjet printer. Sub-
patches and PDMS patches (Figure 6g). Based on the precise and sequently, the masking tape and mask were removed to create a specific
pattern. Finally, a layer of gelatin was spin-coated onto the pattern using
reliable monitoring performance of the conductive patch, a spa-
a spin coater to encapsulate the pattern, resulting in the production of
tiotemporal map of cardiac potentials was established, revealing wet-adhesive flexible electronic devices.
the horizontal propagation of cardiac activation from left to right Micromorphology and Bond Characterization: The microstructure of
during the heart-beating process (Figure 6h). the gelatin film was characterized by atomic force microscopy (AFM,
Bruker Dimension ICON), white light interferometry (zygo, middlefield,
CT 06 455, USA), and scanning electron microscopy (SEM, Thermal Field
3. Conclusion Emission Scanning Electron Microscope, Zeiss, Gemini SEM 300, Ger-
many). The transmittance and haze analyzer (SGW-820, Shanghai Yidi
In this study, we have successfully developed a novel patch for im- Physical Optics Instrument Co., Ltd.) was characterized using a light trans-
plantable signal monitoring. Through the utilization of advanced mittance/haze tester. The stability of the gelatin film was characterized us-
materials and techniques, stable and reliable detection of electro- ing differential scanning calorimetry (DSC) and thermogravimetric analy-
sis (TGA, Mettler-Toledo Corporation, TGA2). The results of the mixture of
cardiogram (ECG) and electroencephalogram (EEG) signals has liquid metal and PVP were characterized through SEM, HRTEM with EDS
been achieved, demonstrating the reliability of the patch under (FEI Tecnai F20). Surface chemical composition was detected by XPS (X-
various environmental conditions. The results of the study sug- ray photoelectron spectroscopy, Escalab 250Xi, Thermo Fisher Scientific
gest promising clinical applications for the patch, enabling long- Inc).
term in-body monitoring and disease diagnosis. Future work will Electromechanical Characterization: The mechanical properties of the
focus on further optimizing the design and performance of the gelatin film were tested using an electronic universal testing machine
(UTM2102, Shenzhen Sun Technology Co., Ltd.) with a 20 N load cell.
patch to meet the requirements of different application scenarios
The gelatin film was cut into a rectangular shape (length 50 mm, width
and exploring its widespread utilization in the healthcare sector. 10 mm), with one end fixed to the electronic universal testing machine.
The other end was in contact with the rabbit’s heart for testing adhesion
performance. To assess adhesion fatigue properties, the gelatin film was
affixed to the surface of rabbit heart tissue by first attaching it to the sub-
4. Experimental Section strate and then subjecting it to the electronic universal testing machine
Materials: Phosphate buffered saline (PBS) and Penicillin– (the tensile test was carried out at 50 mm min−1 under displacement con-
streptomycin liquid (PSL, 100X, reagent grade, with 10 000 units trol conditions).
penicillin and 10 000 units streptomycin) were acquired from Zhejiang The gelatin film was cut into a rectangular shape measuring 50 mm in
Jinuo Biomedical Technology Co., Ltd. Gelatin (G108395 Gelatin, used length and 10 mm in width. One end was held by tweezer, while the other
in microbiology, gel strength ≈250 g Bloom) was bought from Aladdin. end was directly in contact with the heart. To achieve rapid adhesion, ex-
Liquid metal (Ga25 In75 ) was acquired from Fanyada Electronic Technol- ternal force (finger) was applied quickly when the film contacts the heart,
ogy Co., Ltd. Polydimethylsiloxane (PDMS, Dow Corning) was from Dow allowing the film to adhere rapidly. The entire process was recorded us-
Corning. Ethanol (95%) was acquired from Shanghai Lanqing Industrial ing a high-precision camera (see Video S1, Supporting Information), and
Co., Ltd. Calcein-AM (bioreagent, ≥95.0%), Polyvinylpyrrolidone (PVP, the video was meticulously analyzed for adhesion time using professional
Mw ≈1 300 000) and propidium iodide (PI, ≥94%) were purchased from software such as Adobe.
Sigma–Aldrich; fetal bovine serum (FBS, Biological Industries, 04-001-1A) The electrical resistance of the mixture of liquid metal and PVP was
was acquired from Hyclone, Hong Kong. Deionized (DI) water was verified using the four-probe method. The conductivity of the mixture was
prepared by using a laboratory water purification system. characterized by the voltammetry method. In brief, different voltages were
Fabrication of Gelatin Solution: First, prepared a 2% PSL solution us- applied to the mixture using a DC power source, and the resulting output
ing PBS; Next, added 1 g of gelatin to a pointed bottom centrifuge tube currents were measured to characterize its conductivity. During the electri-
(50 mL), took 25 mL of PSL solution and poured it into it, then placed cal test, the resistance was measured with a resistance scanner (TH2518A,
the centrifuge tube in a 50 °C constant temperature water bath until com- Changzhou Tenhui Electronics Co., Ltd.) by connecting the measurement
pletely dissolved, then added 0.04 g of genipin and continued stirring for cable to the leads of the wet-adhesive flexible electronics.
30 min to complete the preparation of the gelatin solution. Electrochemical performance was tested through an electrochemical
Fabrication of Gelatin Film: A 50 μm thick soft silicone rubber was cut workstation (CHI 660D, Shanghai). A flexible electronic was used as the
into a suitable hollow rectangle and used as a mask, which was then at- working electrode, with Ag/AgCl as the reference electrode and the oppo-
tached to the surface of a PET film. Subsequently, an appropriate amount site electrode. All electrochemical tests were performed in aqueous solu-
of gelatin solution was poured into the mask until it spontaneously dif- tion of PBS.
fuses and fills the mask. This prevents horizontal (XY) contraction, allow- In Vitro Studies: The C2C12 cells were used to assess the in vitro toxi-
ing only slow contraction along the vertical (Z) axis. After standing at room city of wet-adhesive flexible electronics according to ISO 10993–5:2009(E)
temperature for 24 h, the nanofilm could be obtained. standards. In brief, RSC-96 cells were added with 10% FBS and 1% PS,
Fabrication of Mask: First, a film was prepared based on the pattern. seeded in a 24-well plate. After 24 h of cultivation, the culture medium
Next, ink was printed twice, followed by immediate exposure of the film was removed, and 1 mL of fresh culture medium was added. Finally, wet-
for an appropriate duration using an exposure machine. The pattern was adhesive flexible electronics were added to the 24-well plate to assess its
then revealed using a developer machine. The film was then applied to toxicity. All samples were cultured in a 5% CO2 incubator at 37 °C.
the stainless steel surface to protect the portions that need to be retained. After 24/72 h of cultivation, cell viability and proliferation were evalu-
Subsequently, the areas not protected by the mask were etched using hy- ated using live/dead cell staining and CCK-8 assay, respectively. In sum-
drofluoric acid etchant to create the desired pattern. Once the etching was mary, according to the manufacturer’s protocol, staining solution con-
complete, the mask was removed, and the stainless steel surface was thor- taining calcein AM (5%) and propidium iodide (5%) in PBS was added
oughly cleaned to remove any residue. and incubated in the dark for 30 min. After multiple washes with PBS,
Fabrication of Implantable Wet-Adhesive Flexible Conductive Patch: The the results were examined using a fluorescence microscope (Nikon Ti
liquid metal was subjected to ultrasonic treatment with PVP, and the pre- microscope, Japan). Metabolic activity of the cells was detected us-
cipitate was collected by centrifugation (1500 rpm, 5 min). A customized ing a microplate reader (BioTek, USA) at an absorbance wavelength of
mask was placed on the surface of the gel film and immediately fixed to 450 nm.

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