Meso-Reconstruction of Wool Keratin 3D "Molecular Springs" for Tunable Ultra-Sensitive and Highly Recovery Strain Sensors.

Wool keratin (WK) consists of a large number of α-helices, which are just like many molecular-scale springs. Herein, the construction of 3D WK molecular spring networks are reported by cross-linking individual WK molecules via a Michael addition reaction. The as-prepared springs display a superior recovery capability with unusual nonlinear elasticity, very low dissipative energy, and turntable elastic constant achieved by adjusting the chemical crosslinking density of WK networks. Owing to these unique characteristics, the 3D WK networks based flexible strain sensors reveal a high sensitivity, broad sensing ranges, and extremely long and stable performance. While normal highly sensible strain sensors, obtained by highly sophisticated surface or bulk patterning, often exhibit a relatively narrow range of measurements and limited life cycles. Such the WK mediated sensing materials have widespread applications in wearable electronics, such as detection and tracking of different human motions, and even discern voice during speaking.

From Molecular Reconstruction of Mesoscopic Functional Conductive Silk Fibrous Materials to Remote Respiration Monitoring.

Turning insulating silk fibroin materials into conductive ones turns out to be the essential step toward achieving active silk flexible electronics. This work aims to acquire electrically conductive biocompatible fibers of regenerated Bombyx mori silk fibroin (SF) materials based on carbon nanotubes (CNTs) templated nucleation reconstruction of silk fibroin networks. The electronical conductivity of the reconstructed mesoscopic functional fibers can be tuned by the density of the incorporated CNTs. It follows that the hybrid fibers experience an abrupt increase in conductivity when exceeding the percolation threshold of CNTs >35 wt%, which leads to the highest conductivity of 638.9 S m-1 among organic-carbon-based hybrid fibers, and 8 times higher than the best available materials of the similar types. In addition, the silk-CNT mesoscopic hybrid materials achieve some new functionalities, i.e., humidity-responsive conductivity, which is attributed to the coupling of the humidity inducing cyclic contraction of SFs and the conductivity of CNTs. The silk-CNT materials, as a type of biocompatible electronic functional fibrous material for pressure and electric response humidity sensing, are further fabricated into a smart facial mask to implement respiration condition monitoring for remote diagnosis and medication.

Using highly water-stable wool keratin/CsPbBr3 nanocrystals as a portable amine-responsive fluorescent test strip for onsite visual detection of food freshness.

Perovskite nanocrystals (PNCs) have emerged as promising candidates for fluorescent probes owing to their outstanding photoelectric properties. However, the conventional CsPbBr3 (CPB) NCs are extremely unstable in water, which has seriously limited their sensing applications in water environment. Herein, we present a powerful ligand engineering strategy for fabricating highly water-stable CPB NCs by using a biopolymer of wool keratin (WK) as the passivator and the polyaryl polymethylene isocyanate (PAPI) as the cross-linking agent. In particular, WK with multi-functional groups can serve as a polydentate ligand to firmly passivate CPB NCs by the ligand exchange process in hot toluene; and then the addition of PAPI can further encapsulate CPB NCs by the crosslinking reaction between PAPI and WK. Consequently, the as-prepared CPB/WK-PAPI NCs can maintain âˆ¼ 80 % of their relative photoluminescence (PL) intensity after 60 days in water, and they still maintain âˆ¼ 40 % of their relative PL intensity even after 512 days in the same environment, which is one of the best water stabilities compared previously reported polymer passivation methods. As a proof-of their application, the portable CPB/WK-PAPI NCs-based test strips are further developed as a fluorescent nanoprobe for real-time and visual monitoring amines and food freshness. Among various amine analytes, the as-prepared test strips exhibit higher sensitivity towards conjugated amines, achieving a remarkable detection limit of 18.3 nM for pyrrole. Our research not only introduces an innovative strategy involving natural biopolymers to enhance the water stability of PNCs, but also highlights the promising potential of PNCs for visually and portably detecting amines and assessing food freshness.

Bioinspired structural hydrogels with highly ordered hierarchical orientations by flow-induced alignment of nanofibrils.

Natural structural materials often possess unique combinations of strength and toughness resulting from their complex hierarchical assembly across multiple length scales. However, engineering such well-ordered structures in synthetic materials via a universal and scalable manner still poses a grand challenge. Herein, a simple yet versatile approach is proposed to design hierarchically structured hydrogels by flow-induced alignment of nanofibrils, without high time/energy consumption or cumbersome postprocessing. Highly aligned fibrous configuration and structural densification are successfully achieved in anisotropic hydrogels under ambient conditions, resulting in desired mechanical properties and damage-tolerant architectures, for example, strength of 14 ± 1 MPa, toughness of 154 ± 13 MJ m-3, and fracture energy of 153 ± 8 kJ m-2. Moreover, a hydrogel mesoporous framework can deliver ultra-fast and unidirectional water transport (maximum speed at 65.75 mm s-1), highlighting its potential for water purification. This scalable fabrication explores a promising strategy for developing bioinspired structural hydrogels, facilitating their practical applications in biomedical and engineering fields.

Using Wool Keratin as a Structural Biomaterial and Natural Mediator to Fabricate Biocompatible and Robust Bioelectronic Platforms.

The design and fabrication of biopolymer-incorporated flexible electronics have attracted immense interest in healthcare systems, degradable implants, and electronic skin. However, the application of these soft bioelectronic devices is often hampered by their intrinsic drawbacks, such as poor stability, inferior scalability, and unsatisfactory durability. Herein, for the first time, using wool keratin (WK) as a structural biomaterial and natural mediator to fabricate soft bioelectronics is presented. Both theoretical and experimental studies reveal that the unique features of WK can endow carbon nanotubes (CNTs) with excellent water dispersibility, stability, and biocompatibility. Therefore, well-dispersed and electroconductive bio-inks can be prepared via a straightforward mixing process of WK and CNTs. The as-obtained WK/CNTs inks can be directly exploited to design versatile and high-performance bioelectronics, such as flexible circuits and electrocardiogram electrodes. More impressively, WK can also be a natural mediator to connect CNTs and polyacrylamide chains to fabricate a strain sensor with enhanced mechanical and electrical properties. With conformable and soft architectures, these WK-derived sensing units can be further assembled into an integrated glove for real-time gesture recognition and dexterous robot manipulations, suggesting the great potential of the WK/CNT composites for wearable artificial intelligence.

Recent advances in flexible and wearable chemo- and bio-sensors based on two-dimensional transition metal carbides and nitrides (MXenes).

Flexible and wearable devices have drawn great attention due to their promising applications from physiological signal detection to disease diagnosis. As a critical element of flexible and wearable devices, chemo- and bio-sensors have been widely merged with advanced nanomaterials. MXenes, a type of nanomaterial from the family of two-dimensional transition metal carbides, carbonitrides and nitrides, have been intensively explored in sensors, energy storage, electromagnetic interference shielding, biomedical engineering, and catalysis, owing to their fascinating structures and outstanding properties. In this review, we focus on recent advances in various flexible and wearable chemo- and bio-sensors derived from pristine MXenes or their nanocomposites. We first present the preparation strategies, surface modification, and performances of MXenes. Then, diverse chemo- and bio-sensors developed based on the MXenes are elaborated, including their unique properties, high sensitivity, and selectivity. Furthermore, we illustrate the related applications in the biomedical field and integrated biosensing platforms. In the end, the current challenges and future perspectives for MXene-based chemo- and bio-sensors are discussed.

Recent Advances in Patterning Natural Polymers: From Nanofabrication Techniques to Applications.

The development of a flexible and efficient strategy to precisely fabricate polymer patterns is increasingly significant for many research areas, especially for cell biology, pharmaceutical science, tissue engineering, soft photonics, and bioelectronics. Recent advances of patterning natural polymers using various nanofabrication techniques, including photolithography, electron-beam lithography, dip-pen nanolithography, inkjet printing, soft lithography, and nanoimprint lithography are discussed here. Integrating nanofabrication techniques with naturally derived macromolecules provides a feasible route for transforming these polymer materials into versatile and sophisticated devices while maintaining their intrinsic and excellent properties. Furthermore, the corresponding applications of these natural polymer patterns generated by the above techniques are elaborated. In the end, a summary of this promising research field is offered and an outlook for the future is given. It is expected that advances in precise spatial patterns of natural polymers would provide new avenues for various applications, such as tissue engineering, flexible electronics, biomedical diagnosis, and soft photonics.

Wool Keratin Photolithography as an Eco-Friendly Route to Fabricate Protein Microarchitectures.

Herein, we present an eco-friendly route to construct protein microarchitectures by using wool keratin (WK) as a green biophotoresist. The photoactive WK was extracted from wool with a method of alkaline hydrolysis and reacted with 2-isocyanatoethyl methacrylate (IEM). The whole process can avoid the use of surfactant and does not cause apparent changes in the structure and function of WK. With the aid of direct-write photolithography, "photoresist-like" WK can be further used for fabricating well-defined and high-performance patterns at a low micron-scale (µm) without high temperature, complicated process, long time, and high production cost.

Continuous and Scalable Manufacture of Hybridized Nano-Micro Triboelectric Yarns for Energy Harvesting and Signal Sensing.

Textile-based triboelectric nanogenerators (TENG) that can effectively harvest biomechanical energy and sense multifunctional posture and movement have a wide range of applications in next-generation wearable and portable electronic devices. Hence, bulk production of fine yarns with high triboelectric output through a continuous manufacturing process is an urgent task. Here, an ultralight single-electrode triboelectric yarn (SETY) with helical hybridized nano-micro core-shell fiber bundles is fabricated by a facile and continuous electrospinning technology. The obtained SETY device exhibits ultralightness (0.33 mg cm-1), extra softness, and smaller size (350.66 µm in diameter) compared to those fabricated by conventional fabrication techniques. Based on such a textile-based TENG, high energy-harvesting performance (40.8 V, 0.705 µA cm-2, and 9.513 nC cm-2) was achieved by applying a 2.5 Hz mechanical drive of 5 N. Importantly, the triboelectric yarns can identify textile materials according to their different electron affinity energies. In addition, the triboelectric yarns are compatible with traditional textile technology and can be woven into a high-density plain fabric for harvesting biomechanical energy and are also competent for monitoring tiny signals from humans or insects.

All-Textile Electronic Skin Enabled by Highly Elastic Spacer Fabric and Conductive Fibers.

Electronic fabrics that combine traditional fabric with intelligent functionalities have attracted increasing attention. Here an all-fabric pressure sensor with a wireless battery-free monitoring system was successfully fabricated, where a 3D penetrated fabric sandwiched between two highly conductive fabric electrodes acts as a dielectric layer. Thanks to the good elastic recovery of the spacer fabric, the capacitance pressure sensor exhibits a high sensitivity of 0.283 KPa-1 with a fast response time and good cycling stability (≥20 000). Water-soluble poly(vinyl alcohol) template-assisted silver nanofibers were constructed on the high-roughness fabric surface to achieve high conductivity (0.33 Ω/sq), remarkable mechanical robustness, and good biocompatibility with human skin. In addition, the coplanar fabric sensor arrays were successfully designed and fabricated to spatially map resolved pressure information. More importantly, the gas-permeable fabrics can be stuck on the skin for wireless real-time pressure detection through a fiber inductor coil with a resonant frequency shift sensitivity of 6.8 MHz/kPa. Our all-fabric sensor is more suitable for textile technology compared with traditional pressure sensors and exhibited wide potential applications in the field of intelligent fabric for electronic skin.

Using Wool Keratin as a Basic Resist Material to Fabricate Precise Protein Patterns.

The ability to pattern natural polymers at different scales is extremely important for many research areas, such as cell culture, regenerative medicine, bioelectronics, tissue engineering, degradable implants, and photonics. For the first time, the use of wool keratin (WK) as a structural biomaterial for fabricating precise protein microarchitectures is presented. Through straightforward biochemical processes, modified WK proteins become intrinsically photoreactive without significant changes in protein structure or function. Under light irradiation, intermolecular chemical crosslinking between WK molecules can be successfully initiated by using commercially available photoinitiators. As a result, high-performance WK patterning on the micrometer scale (µm) can be achieved through a combination of water-based photolithography techniques. By simply mixing with nanoparticles, enzymes, and other dopants, various "functional WK resists" can be generated. In addition, without the addition of any cell-adhesive ligands, these patterned protein microstructures are demonstrated as bio-friendly cellular substrates for the spatial guidance of cells on their surface. Furthermore, periodic microfabricated WK structures in complex patterns that display typical iridescent behavior can be designed and formed over macroscale areas (cm).