Conductive hydrogels for bioenergy harvesting and self-powered application

The advent of self‐powered wearable electronics will revolutionize the fields of smart healthcare and sports monitoring. This technological advancement necessitates more stringent design requirements for triboelectric materials. The triboelectric aerogels must enhance their mechanical properties to address the issue of structural collapse in real‐world applications. This study fabricates stiff nanocellulosic triboelectric aerogels with multiscale structures induced by the Hofmeister effect. The aggregation and crystallization of polymer molecular chains are enhanced by the Hofmeister effect, while ice crystal growth imparts a porous structure to the aerogel at the micron scale. Therefore, the triboelectric aerogel exhibits exceptional stiffness, boasting a Young's modulus of up to 142.9 MPa and a specific modulus of up to 340.6 kN m kg–1, while remaining undeformed even after supporting 6600 times its weight. Even after withstanding an impact of 343 kPa, highly robust wearable self‐powered sensors fabricated with triboelectric aerogels remain operational. Additionally, the self‐powered sensor is capable of accurately detecting human movements, particularly in abnormal fall postures detection. This study provides considerable research and practical value for promoting material design and broadening application scenarios for self‐powered wearable electronics.

Multiscale Structural Nanocellulosic Triboelectric Aerogels Induced by Hofmeister Effect

Wearable electronics based on conductive hydrogels (CHs) easily suffer from prolonged response times, reduced wearing comfort, shortened service lives, and impaired signal accuracy in cold environments, because conventional CHs tend to freeze at subzero temperatures and lose their flexibility, adhesion, transparency, and conductivity, which will limit their applications in extreme environments. Inspired by the way psychrotolerant creatures and superabsorbent materials interfere with the hydrogen bonding networks of water, a freeze‐resistant conductive organohydrogel (COH) is facilely fabricated. The synergy effect between charged polar terminal groups and a binary solvent system of water–ethylene glycol weakens the hydrogen bonding between water molecules and endows the COH with remarkable freezing tolerance (−78 °C). Additionally, the obtained COH is ultra‐stretchable (≈6185%), tough (9.2 MJ m−3), highly transparent (≈99%), self‐adhesive (10.2–27.8 kPa), and biocompatible. This versatile COH is assembled into a strain sensor and a well‐designed bracelet electrocardiogram sensor. Benefiting from the exceptional low‐temperature tolerance of the prepared COH, these devices exhibit fast response with delay‐free signals even at −40 °C. Overall, this work proposes a strategy to develop multifunctional COHs for supporting human health in cold environments.

A Freeze‐Resistant, Highly Stretchable and Biocompatible Organohydrogel for Non‐Delayed Wearable Sensing at Ultralow‐Temperatures

Abstract Ideal hydrogel fibers with high toughness and environmental tolerance are indispensable for their long-term application in flexible electronics as actuating and sensing elements. However, current hydrogel fibers exhibit poor mechanical properties and environmental instability due to their intrinsically weak molecular (chain) interactions. Inspired by the multilevel adjustment of spider silk network structure by ions, bionic hydrogel fibers with elaborated ionic crosslinking and crystalline domains are constructed. Bionic hydrogel fibers show a toughness of 162.25 ± 21.99 megajoules per cubic meter, comparable to that of spider silks. The demonstrated bionic structural engineering strategy can be generalized to other polymers and inorganic salts for fabricating hydrogel fibers with broadly tunable mechanical properties. In addition, the introduction of inorganic salt/glycerol/water ternary solvent during constructing bionic structures endows hydrogel fibers with anti-freezing, water retention, and self-regeneration properties. This work provides ideas to fabricate hydrogel fibers with high mechanical properties and stability for flexible electronics. 

Spider-silk-inspired strong and tough hydrogel fibers with anti-freezing and water retention properties

Conductive hydrogel (CH) has drawn widespread interest in flexible electronics, human–computer interaction, and electronic skins (e-skins). However, it is challenging to integrate satisfactory self-adhesion, self-healing, environmental stability, and multi-stimulus response into a single CH system. Herein, a conductive nanocomposite organohydrogel with the above characteristics is well-designed and developed via incorporating carboxylic cellulose nanofibers-carrying carboxylic carbon nanotubes (C-CNTs) and phytic acid (PA) into polyacrylamide network through free-radical polymerization plus glycerol solvent displacement strategy, aiming for a high-performance multimodal sensing platform. Here, the coupling of C-CNTs and ionization of PA contributes a favorable conductivity, and the coexistence of glycerol and PA is beneficial for the formation of amounts of hydrogen bonds that endow the organohydrogel with outstanding stretchability, self-healing, and favorable adhesion in a wide temperature range of −30 to 60 °C. Besides, the resultant organohydrogel can effectively detect multiple external stimuli, manifesting high strain sensitivity over a broad strain range (0–1599 %), good humidity detectability at 0–85 % RH, and reliable thermosensation capability over a wide temperature window (−30 to 60 °C). Significantly, the application of the organohydrogel as e-skins are conducted to detect full-range human activity movements even in the extreme environments, identify hand gestures, and recognize the spatial distribution of humidity in noncontact sensing. All these indicates the preponderance of our organohydrogel in the fields of flexible smart electronics. 

Highly stretchable, environmentally stable, self-healing and adhesive conductive nanocomposite organohydrogel for efficient multimodal sensing

For soft electronic applications, the simultaneous incorporation of conductivity and mechanical robustness remains a grand constraint, not to mention being able to operate at wide temperatures ranges. Herein, a novel conductive platform is proposed by designing skin‐inspired ionic organohydrogels based on Hofmeister effect and glycerol/water system, which simultaneously realize balanced conductivity, mechanical strength, and versatile properties. The comprehensive performances are broadly and simultaneously altered via tuning the aggregation states of polymer chains by kosmotropes or chaotropes. With various ions, the conductivity and mechanical strength are continuously in situ modulated over a large window: conductivity from 0.08 to 4.8 S m−1, strength from 0.01 to 17.30 MPa, toughness from 5.4 to 9236.9 kJ m−3, and modulus from 5.1 to 2258.9 kPa. The ion transport process is inseparable from the changes of water content and pore structures caused by cross‐linking density. Meanwhile, the mechanical properties greatly depend on the densification or loosing of polymer chains and crystalline domains. Furthermore, oil/water system exhibits low temperature tolerance at ≈−65–15 °C and long‐term stability. Finally, the champion organohydrogels are applied as wearable electronic sensors and artificial skins. The mechanism proposed in this work advances the understanding of the ions contribution to organohydrogels for electronic applications.

Hofmeister Effect Assisted Dual‐Dynamic‐Bond Cross‐Linked Organohydrogels with Enhanced Ionic Conductivity and Balanced Mechanical Properties for Flexible Sensors

The self-cleaning coating has both superhydrophobic physical and photocatalytic chemical self-cleaning properties, which has attracted the wide attention of researchers in recent years. First, the flower-like hollow SiO2@TiO2 spheres with oxygen vacancies (rFHSTs) were prepared by the liquid-phase reduction method, in which several different functional components were integrated. Meanwhile, the influence mechanisms of the physical structure and chemical composition on the photocatalytic properties are discussed in detail. The results proved that rFHSTs exhibited the enhanced photoresponse range and photocatalytic degradation performance in visible light because of the synergistic effect of the microstructure (internal cavity, 3D flower-like nanosheet), SiO2/TiO2 heterojunction structure, and oxygen vacancies. After that, superhydrophobic modified rFHSTs were used as fillers to fabricate PVA/PFDTS-rFHSTs composite coatings with both physical and chemical self-cleaning properties. The self-cleaning performances and principles of the composite coating were examined and explored. The results showed that the low surface energy of the hydrophobic chain segment, the inherent particle effect, and the photocatalytic activity of rFHSTs were responsible for the superhydrophobic and photocatalytic effects, finally endowing the composite coating with self-cleaning performance. In short, this study is profound for the development and application of self-cleaning coatings with both physical and chemical performances. 

Superhydrophobic and Photocatalytic Synergistic Self-Cleaning Coating Constructed by Hierarchically Structured Flower-like Hollow SiO2@TiO2 Spheres with Oxygen Vacancies.

Due to Cd(II) with highly toxic, persistent and bioaccumulative, the discharge of it into the environment brings serious pollution. Developing strategies that are efficient, low-cost, pollution-free and specific to removing Cd(II) from wastewater is therefore of great urgency and prime importance. A novel chitosan/sodium alginate ionic imprinting(IICA) hydrogels with specific adsorption capacity for Cd(II) was prepared through freeze-thaw and ion imprinting, and finally the colorimetric sensor (IICAS) was prepared via introducing Rhodamine B(RhB) and Victoria blue(VBB) by immersion to achieve visual detection of Cd(II). The IICA hydrogels with imprinted hole structure had higher adsorption capacity and better specific selectivity for Cd(II). As well as internal diffusion, coordination, ion exchange, and hydrogen bonding influenced the adsorption rate. Moreover, the IICAS exhibited good selective detection ability and linearity for Cd(II) with the fitted correlation coefficient (R2) = 0.98, limit of detection (LOD) = 35 nmol/L. Combined with the smartphone platform, portable and quantitative detection of Cd(II) can be achieved, Within the 0–100 mg/L range, R2 remained 0.94, and LOD was 75 nmol/L. This strategy of preparing a novel whole biomass IICAS integrating capture and visual detection provides a new insight into the construction of a promising candidate sensor for the removal and detection of Cd(II). 

Biomass chitosan/sodium alginate colorimetric imprinting hydrogels with integrated capture and visualization detection for cadmium(II)

Cardiovascular disease (CVD)-related mortality and morbidity are among the most critical disease burdens worldwide. CVDs encompass many diseases and involve complex pathogenesis and pathological changes. While research on these diseases has advanced significantly, treatments and their efficacy remain rather limited. New therapeutic strategies and targets must, therefore, be explored. Tissue transglutaminase (TG2) is pivotal to the pathological development of CVDs, including participating in the cross-linking of extracellular proteins, activation of fibroblasts, hypertrophy and apoptosis of cardiomyocytes, proliferation and migration of smooth muscle cells (SMCs), and inflammatory reactions. Regulating TG2 activity and expression could ensure remarkable improvements in disorders like heart failure (HF), pulmonary hypertension (PH), hypertension, and coronary atherosclerosis. In this review, we summarize recent advances in TG2: we discuss its role and mechanisms in the progression of various CVDs and its potential as a diagnostic and therapeutic target. 

Roles and potential clinical implications of tissue transglutaminase in cardiovascular diseases

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Papers

Hofmeister Effect Assisted Dual‐Dynamic‐Bond Cross‐Linked Organohydrogels with Enhanced Ionic Conductivity and Balanced Mechanical Properties for Flexible Sensors

Superhydrophobic and Photocatalytic Synergistic Self-Cleaning Coating Constructed by Hierarchically Structured Flower-like Hollow SiO2@TiO2 Spheres with Oxygen Vacancies.

Biomass chitosan/sodium alginate colorimetric imprinting hydrogels with integrated capture and visualization detection for cadmium(II)

Roles and potential clinical implications of tissue transglutaminase in cardiovascular diseases