Tough gelatin-based biogels for wearable sensors
0 Abstract
Flexible wearable sensors that can intimately adhere to the human body for real-time monitoring of human activities and physiological signals have attracted great attention owing to their potential in personalized healthcare and human-machine interfaces. Gelatin-based biogels are promising materials in wearable sensors due to their good biocompatibility, biodegradability, and sustainability. However, conventional gelatin-based biogels are usually weak and brittle (tensile strength < 10 kPa and stretchability < 50%), and thus cannot be applied in flexible wearable devices. Therefore, further efforts are needed to engineer tough gelatin-based biogels that meet the demands of flexible wearable sensors. In this perspective, we summarize recent progress in designing tough gelatin-based biogels and their wide applications in wearable sensing devices, while highlighting potential future directions in this field.
Keywords
INTRODUCTION
Flexible wearable sensors have undergone rapid development in recent decades due to their significant role in personalized healthcare, precision medicine, and human-machine interfaces[1-3]. However, different from inherently soft human tissues, conventional wearable devices are usually made with rigid materials, causing unstable integration with tissues and discomfort[4]. Polymer gels, composed of three-dimensional polymer networks and dispersion media, have brought many opportunities to wearable sensors by harnessing their mechanical flexibility, structural permeability, and tissue resemblance[5,6]. However, general synthetic polymer gels have poor biocompatibility and non-degradability, leading to severe immune response and a serious threat to environmental sustainability[7].
Biogels derived from natural biopolymers (such as alginate, cellulose, and gelatin) are gaining research interest as building blocks for wearable sensors, ascribing to their biocompatibility and environmental sustainability[8-11]. The biogels’ biocompatibility enables long-term skin contact without irritation or inflammation, while their environmental degradability presents a sustainable approach to mitigating electronic waste. Gelatin, as a hydrolyzed product of natural collagen, is a type of protein composed of polypeptides. Collagen is generally water-insoluble, composed of three long helix-shaped chains of amino acids [Figure 1A][12]. Compared to collagen, gelatin is a mixture of single- and multi-chain polypeptides composed of amino acids such as alanine, proline, and 4-hydroxyproline with good water solubility. The unique advantages of gelatin, including excellent biocompatibility, non-immunogenicity, biodegradability, and multiple reactive sites for functionalization, make it a promising candidate for constructing soft biogels as wearable sensors [Figure 1B][13,14]. Although gelatin-based hydrogels can be formed by cooling a hot gelatin solution to convert partial gelatin chains from random coil structures to triple-helix configuration, the obtained hydrogel is fragile with low toughness, which makes it difficult to apply in flexible sensing devices[12,15].
Figure 1. (A) Schematic diagram of processing collagen to gelatin and the mechanism of sol-gel transition of gelatin hydrogel upon heating and cooling[12]. Reprinted with permission. Copyright 2019, Multidisciplinary Digital Publishing Institute; (B) Chemical structure and properties of gelatin[13]. Reprinted with permission. Copyright 2021, Wiley-VCH; (C) Fabrication; and (D) photos and tensile stress-strain curves of high-strength gelatin-ammonium sulfate hydrogels via the Hofmeister effect[19]. Reprinted with permission. Copyright 2018, WILEY-VCH; (E) Schematic of formation, structure, and non-covalent interactions in gelatin organohydrogels; and (F) Photos showing the high mechanical performances of gelatin organohydrogels[22]. Reprinted with permission. Copyright 2019, ACS Publications.
DESIGN OF TOUGH GELATIN-BASED BIOGELS FOR WEARABLE SENSING DEVICES
A general design principle for tough gels is the incorporation of energy dissipation domains within stretchable polymer networks[16]. The molecular engineering and structural engineering, including molecular interactions and topological network structures, are proposed to fabricate robust gels with high stretchability, mechanical strength, and toughness[17]. By manipulating functional groups at the molecular level, diverse crosslinking interactions (including permanent or reversible dynamic bonds) can be engineered within the polymer network for energy dissipation. Structural engineering mainly involves introducing high-order structure (such as phase separation and hierarchical structure) into polymer networks for strengthening and toughening gels. Various combinations of these effective strategies have been explored for designing tough gelatin-based biogels[18]. Considering the abundant functional groups in gelatin chains, an effective strategy for toughening gelatin biogels is to regulate non-covalent associations between gelatin chains[19-21]. For example, hydrophobic interaction domains and microphase separation regions were introduced into the gelatin network through the Hofmeister effect by soaking virgin gelatin gel in a (NH4)2SO4 solution [Figure 1C][19]. The resulting gelatin hydrogels could withstand large tensile and compressive forces with tensile strength of ca. 3 MPa when stretching to 500% [Figure 1D]. Besides, introducing crosslinkers such as tannic acid (TA), sodium citrate, and sodium phytate to build non-covalent crosslinks with gelatin chains is another effective way to enhance the mechanical properties of gelatin-based biogels[22-25]. For example, Qin et al. reported a gelatin supramolecular organohydrogel by immersing a gelatin pre-hydrogel in citrate (Cit) water-glycerol mixture solution [Figure 1E][22]. Due to the formation of hydrophobic aggregation, ionic interactions between the -NH3+ of gelatin and Cit3- anions, the organohydrogel exhibited high strength and toughness [Figure 1F]. Additionally, chemical modifications of gelatin chains with crosslinkable groups (such as methacrylate and dopamine) have also been investigated to create dually crosslinked structures for improving the mechanical properties of gelatin-based biogels[26,27]. With significant advances in mechanical enhancement, compared with the synthetic polymer gels (such as polyacrylamide-based and polyvinyl alcohol-based gels), gelatin-based biogels possess the unique advantages of biocompatibility, biodegradability, mechanical tunability, sustainability and multifunctionality [Figure 2], showcasing superior balance of these properties, which make them an outstanding material for wearable sensor applications.
Figure 2. Radar chart comparing performance metrics of gelatin-based biogels with typical synthetic polymer gels.
For applications in wearable sensors, tough gelatin biogels are typically employed in two key ways: as soft, stretchable substrates for flexible electronic devices, and as active sensing materials that respond to external stimuli. The performance of representative tough gelatin-based biogels and their application in wearable sensors are summarized in Table 1. The appealing features of mechanical robustness, good biocompatibility, and biodegradability make tough gelatin biogels a promising substrate for wearable devices on which functional sensing elements are integrated[28-30]. The fabrication of such flexible electronics is achieved by integrating individual sensing units via patterned conductive circuits embedded within or printed onto tough biogels. For example, a versatile gelatin biogel with self-adhesive, stretchable, self-healing, and fully degradable properties was fabricated by combining gelatin with sugars as extensibility promoters and water/glycerol as dispersion medium. The elastic modulus of this biogel can be widely regulated by modifying gelatin content. By utilizing rapid healing ability, biogels with different elastic moduli were assembled into graded modulus gels as tailored and sophisticated substrates for stretchable electronics [Figure 3A][28]. By integrating temperature, humidity, and strain sensors with a reusable flexible printed circuit board (PCB) on the biogel substrate, a stretchable and biodegradable on-skin electronic device was successfully fabricated, demonstrating potential as sustainable wearable electronics for real-time physiological monitoring [Figure 3B]. In another example, a transparent, robust, and recyclable biogel was fabricated via a sol-gel transition of a gelatin and alginate mixture dissolved in a water/glycerol solvent. Using this biogel as the substrate, a modulable and sustainable e-skin was developed by integrating sensing elements and patterned liquid metal as a soft conductor [Figure 3C][30].
Figure 3. (A) Assembly of graded modulus gel and tensile test of a modulus-graded gel compared with its finite element modeling simulation[28]. Reprinted with permission. Copyright 2020, Springer Nature; (B) Construction of soft e-skin on biogel substrate attached to a human arm[28]. Reprinted with permission. Reprinted with permission. Copyright 2020, Springer Nature; (C) Illustration of integrated soft electronics with gelatin-alginate as biogel substrate[30]. Reprinted with permission. Reprinted with permission. Copyright 2022, WILEY-VCH; (D) Illustration of multiresponsive metal-crosslinked alginate/gelatin organohydrogel (MAlgGel) on skin for thermal, photo, humidity, and strain sensing applications[34]. Reprinted with permission. Copyright 2022, WILEY-VCH; (E) Schematic illustration of the ionic biogel fabrication process and its versatility[38]. Reprinted with permission. Copyright 2024, WILEY-VCH; (F) Schematic illustration of the preparation of the MCG organohydrogel[43]. Reprinted with permission. Copyright 2022, Elsevier; (G) Chemical composition, liquid-to-solid transformation, and application of in situ biogel[45]. Reprinted with permission. Copyright 2025, Springer Nature. PEDOT: poly(3,4-ethylenedioxythiophene); PSS: poly(styrenensulfonate); DES: deep eutectic solvent; MCG: MXene-composited gelatin.
Performance comparison and their application in wearable sensors of representative gelatin-based tough biogels
| Composition | Mechanical property | Conductivity | Function | Admirable performance | Application | Ref. | |
| Strength | stretchability | ||||||
| Gelatin/citric acid/sugar/glycerol | 10-140 kPa | 180%-325% | / | Substrate | Self-healing; Adhesion; Recycling; | Integrated multimodal e-skin | [28] |
| Gelatin/glycerol | / | Flexible | / | Substrate | Recycling; | Capacitive touch sensors | [29] |
| Gelatin/alginate/glycerol | ~ 2.0 MPa | 540% | / | Substrate | Self-healing; Recycling; | Integrated multifunctional soft electronics | [38] |
| Gelatin/alginate/glycerol/metal cations | 0.64-1.88 MPa | 45-150% | 0.17-6.1 mS m−1 | Active sensing material | / | Thermal, humidity, strain sensors; Photodetector | [34] |
| Gelatin/betaine-[Fe(CN)6]3-/4- | 0.44 MPa | 247% | 4.04 S m-1 | Active sensing material | Self-healing | Thermal sensor array | [35] |
| Gelatin/citric acid/NaCl | ~ 0.8 MPa | ~ 460% | ~ 155 ohms at 100 Hz | Active sensing material | Temperature-controlled phase transition; Adhesion | On-skin bioelectrode for EEG recording | [36] |
| Gelatin/sodium pyrrolidone carboxylic acid | ~ 0.18 MPa | 256% | 25 mS cm-1 | Active sensing material | Adhesion; Temperature-controlled phase transition; Self-healing | Bio-interface for recording electrophysiology signals | [38] |
| Gelatin/MXene/tannic acid/glycerol | 1.81 MPa | 330% | ~ 80 mS cm-1 | Active sensing material | Adhesion | Thermal, strain sensors | [43] |
| Gelatin/PEDOT:PSS/glycerol-choline chloride | ~ 1-3 MPa | 200-375% | 0.29-0.91 S/m | Active sensing material | Adhesion | Bioelectrode for ECG and EMG signal detection | [45] |
Aside from the use as flexible substrates for wearable devices, conductive compositions such as conductive fillers and mobile ions have been integrated into gelatin matrix to prepare conductive tough biogel as active sensing materials. In biological systems, ion conduction is ubiquitous and extremely important for tactile perception. Inspired by this, ionically conductive gelatin biogels, a class of conductive biogels containing mobile ions within their network to enable electrical signal conduction via ion migration, have been developed by introducing various types of mobile ions[31]. Early studies developed ionically conductive gelatin-based biogels with excellent stretchability and environmental stability by constructing non-covalent interactions and incorporating hygroscopic agents such as glycerol, and ionic liquids[32-35]. These biogels have been effectively used as epidermal sensors to monitor strain, pressure, temperature, and humidity. Tordi et al.[34] reported gelatin-based organohydrogel by incorporating metal cations-crosslinked alginate into a stretchable gelatin network in water/glycerol binary solvent. The introduction of various metal cations could modulate ionic conductivity and mechanical properties, while glycerol enhanced long-term stability. The resulting organohydrogels exhibited high ionic conductivity and stretchability, with sensitivity to temperature, visible light, humidity, and strain, enabling the monitoring of environmental and physiological parameters [Figure 3D]. Lately, based on the reversibility of non-covalent crosslinking, tough, self-adhesive, and ionic-conductive gelatin-based biogels with the temperature-controlled reversible fluid-gel transition have been designed for electrophysiological monitoring [36-38]. For instance, Lan et al. developed ionic biogels by introducing sodium pyrrolidone carboxylic acid (PCA-Na) to gelatin hydrogel [Figure 3E][38]. This biogel exhibited good stretchability, high ionic conductivity and water retention ability. Besides, the temperature-controlled reversible sol-gel transition, enabling in situ gelation on various surfaces with strong adhesion, making it an effective interface for high-quality electrophysiological signal recording.
Though ion-conductive biogels possess advantages of optical transparency and bionic ion transport, some intrinsic drawbacks also exist, such as low conductivity and low sensitivity. Electronically conductive gelatin biogels that enable electrical conduction primarily through electron transport mechanisms have been widely investigated by incorporating conductive fillers into gelatin gel matrices. Different conductive materials, such as metal-based materials, carbon nanomaterials, and conducting polymers, are used to impart biogels with the required electrical conductivity[39-41]. To achieve high electrical conductivity, sufficient content of conductive fillers must be incorporated to establish continuous percolation pathways. However, the hydrophobic conductive fillers, including carbon nanotubes and graphene, usually have poor dispersion in the gel network, making it difficult to form an interconnected conductive network. Recently, MXene, a two-dimensional (2D) transition metal carbide or carbonitride with metallic conductivity, excellent hydrophilicity, and abundant functional groups, has emerged as a promising conductive filler for fabricating electronically conductive biogels[42]. For example, Wang et al. developed a conductive MXene-composited gelatin (MCG) organohydrogel by soaking a preformed MCG hydrogel in a TA water/glycerol solution
CHALLENGE AND PERSPECTIVES
Despite significant advancements in the design of tough and functional gelatin-based biogels for wearable applications, several critical challenges remain to be addressed.
First, although various strategies have been employed to enhance the mechanical properties of gelatin-based biogels, their performance still lags behind that of synthetic polymer gels, particularly in terms of fracture toughness. It remains a great challenge to construct a gelatin-based biogel with the comprehensive performances of high strength, toughness, and fracture-resistance capability due to the insufficient crosslinking structure. Owing to the tunable configuration of gelatin chains and the presence of multifunctional groups, recent strategies for strengthening and toughening synthetic polymer hydrogels, such as highly entangled chain structures and solvent-induced toughening, may provide effective approaches to further enhance the mechanical properties of gelatin hydrogels. Enhanced mechanical performance will broaden the application scope of biogel-based wearable sensors in demanding mechanical environments.
Second, despite the introduction of conductive fillers and mobile ions into gelatin matrix endowing the biogel with conductivity, the conductivity of these tough gelatin-based biogels is lower than 1 s/m, which is insufficient for applications as active sensing materials, particularly in bioelectrodes. The low conductivity primarily arises from the intrinsically insulating nature of gelatin, which constitutes the bulk of the biogel and impedes the formation of continuous conductive pathways. To overcome this limitation, innovative strategies such as constructing dual-phase structures-comprising a conductive component-rich phase embedded within the gelatin matrix-may enable the high conductivity (> 1 s/cm) in gelatin-based biogels, realizing a material revolution in wearable bioelectronics.
Additionally, enhancing the multifunctionality of gelatin biogels, such as incorporating antibacterial or drug-releasing capabilities, could broaden their scope of application in health monitoring and therapeutic systems. By combining advanced material design with bioinspired functionality, these functionalized biogels will hold great promise for the development of next-generation flexible wearable bioelectronics that integrate sensing and therapeutic functions.
DECLARATIONS
Authors’ contributions
Wrote the original draft: Yin, J. J.; Li, Y.
Supervised, reviewed, and revised the manuscript: Sun, X.; Qin, Z. H.
Availability of data and materials
Not applicable.
Financial support and sponsorship
The authors would like to acknowledge the support of the National Natural Science Foundation of China under Grant No. 22102139.
Conflicts of interest
Yin J. and Li Y. are affiliated with Xi’an Rare Metal Materials Institute Co., Ltd., while the other authors have declared that they have no conflicts of interest.
Ethical approval and consent to participate
Not applicable.
Consent for publication
Not applicable.
Copyright
© The Author(s) 2025.
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