Key Takeaways & Executive Findings
- •• A versatile surfactant-free emulsion construction strategy is proposed to customize functional hydrogels. • The synergistic emulsification mechanism between amphiphilic polymers and MXene is comprehensively elucidated. • Programmable functional structures confer hydrogels with excellent EMI shielding and water evaporation performance. • The hydrogels exhibit high EMI shielding efficiency (~64 dB) and superior solar evaporation rate (~3.5 kg m⁻² h⁻¹) with salt tolerance.
Abstract
Flexible and conformable nanomaterial-based functional hydrogels find promising applications in various fields. However, the controllable manipulation of functional electron/mass transport networks in hydrogels remains rather challenging to realize. We describe a general and versatile surfactant-free emulsion construction strategy to customize robust functional hydrogels with programmable hierarchical structures. Significantly, the amphipathy of silk fibroin (SF) and the reinforcement effect of MXene nanosheets produce sable Pickering emulsion without any surfactant. The followed microphase separation and self-cross-linking of the SF chains induced by the solvent exchange convert the composite emulsions into high-performance hydrogels with tunable microstructures and functionalities. As a proof-of-concept, the controllable regulation of the ordered conductive network and the water polarization effect confer the hydrogels with an intriguing electromagnetic interference shielding efficiency (~64 dB). Also, the microstructures of functional hydrogels are modulated to promote mass/heat transfer properties. The amino acids of SF and the surface terminations of MXene help reduce the enthalpy of water evaporation and the hierarchical structures of the hydrogels accelerate evaporation process, expecting far superior evaporation performance (~3.5 kg m⁻² h⁻¹) and salt tolerance capability compared to other hydrogel evaporators. Our findings open a wealth of opportunities for producing functional hydrogel devices with integrated structure-dependent properties.
1. Introduction
Flexible and robust functional hydrogels find widespread applications in soft robotics, flexible electronics, electromagnetic radiation protection, and energy conversion. Beyond conventional ionic and conductive polymer-based hydrogels, various composite hydrogels produced by including different conductive nanomaterials, such as graphene, MXene, carbon nanotubes, and metallic nanomaterials, offer more newfangled attributes and promising candidates for different applications. Fundamentally, the functionality realization of these nanomaterials depends on the type of nanofillers, their distribution in the matrix, and the microstructures of the hydrogel themselves. Recently, researchers make great efforts to address the interfacial incompatibility between conductive fillers and polymer matrices, which severely impedes the uniform dispersion, and modulation of hierarchical architectures in the hydrogels. For example, some attempts adopt directional freezing, sacrificial templates, and cononsolvency strategies to form directional channels and anisotropic pores in the composite hydrogels. However, these methods largely change the structures of hydrogels by additional procedures (e.g., ice crystal template and microphere template etching) and neglect the effect of the microstructures of hydrogel components, limiting the flexible regulation of functionality for hydrogels. Importantly, although massive randomly dispersed nanomaterials can form functional structures in the composite hydrogels, severe agglomeration and early gelation phenomena inevitably deteriorate their comprehensive performance.
Inspired by the exclusion effect in immiscible polymer blends, it is possible to modulate the phase structures and filler distribution for constructing functional structures. Similarly, Pickering emulsions, consisting of a tunable dispersed phase and a continuous phase, offer a feasible and versatile platform for the structure design and performance regulation of hydrogels. For example, the interfacial assembly of nanomaterials at the two-phase interfaces, rather than random dispersion in individual phases of emulsions, can enable almost all nanomaterials to construct connected architectures, resembling the select distribution of fillers in the polymer composites. Significantly, the micro-structure characteristics, including phase structure, continuity, and distribution, of the derived functional hydrogels can be freely tuned on-demand for specific applications. Despite the promising prospects, some challenges remain.
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Guang Yin, Jing Wu, Chengzhang Qi, Xinfeng Zhou, Zhong-Zhen Yu, Hao-Bin Zhang (2025). Pickering Emulsion-Driven MXene/Silk Fibroin Hydrogels with Programmable Functional Networks for EMI Shielding and Solar Evaporation. Nano-Micro Letters. https://doi.org/10.1007/s40820-025-01818-w
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Frequently Asked Questions
What is the main innovation of this study?
The study proposes a surfactant-free Pickering emulsion strategy to fabricate MXene/silk fibroin hydrogels with programmable hierarchical structures, enabling tunable EMI shielding and solar evaporation performance.
How do the hydrogels achieve high EMI shielding efficiency?
The ordered conductive network formed by MXene nanosheets and the water polarization effect contribute to an EMI shielding efficiency of approximately 64 dB.
What makes the hydrogels suitable for solar evaporation?
The hierarchical structures and the presence of amino acids from silk fibroin and surface terminations of MXene reduce the enthalpy of water evaporation, leading to a high evaporation rate of about 3.5 kg m⁻² h⁻¹ and good salt tolerance.
Why is a surfactant-free approach advantageous?
The surfactant-free approach avoids potential toxicity and complexity, while the amphiphilic silk fibroin and MXene nanosheets synergistically stabilize the Pickering emulsion, simplifying the fabrication process.
What applications could these hydrogels have?
These hydrogels could be used in flexible electronics, electromagnetic radiation protection, and solar-driven water purification, among other applications requiring integrated functional networks.
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