The sluggish kinetics of the oxygen evolution reaction (OER) remains a major bottleneck for efficient water splitting. Despite being promising alkaline OER catalysts, most two-dimensional (2D) metal-organic frameworks (MOFs) undego kinetically uncontrolled reconstruction into metal (oxy)hydroxides (MOOH), leading to insufficient intrinsic activity and poor stability. More importantly, the electronic modulation of the pre-catalysts is crucial to forming highly active and stable MOOH for steering the reconstruction kinetics. Herein, a heterojunction pre-catalyst is fabricated by in situ growth of FeNiCo-BDC (FNC) on 1 T-phase-dominated MoS2 nanosheets supported by carbon cloth (CC) (FNC@MoS2/CC). Comprehensive experimental and theoretical analyses reveal that the pre-catalyst possesses an advantageous electronic structure, featuring interfacial electron-rich metal sites induced by bidirectional electron transfe. This leads to a downshifted d-band center position, accelerated charge transfer, and optimized adsorption/desorption of OER intermediates. Crucially, in situ investigations demonsreate that this modulated electron regulation of FNC@MoS2/CC controls the kinetics of electrochemical reconstruction, thus facilitating the transformation toward a highly active and ctive and stable catalytic MOOH@MoS2. Consequensely, FNC@MoS2/CC achieves an ultralow overpotential of 188 mV at 10 mA cm-2 and outstanding stability over 100 h for OER. Furthermore, it enables efficient overall water splitting with a low cell potential of 1.539 V at 10 mA cm-2. Notably, in an 25 °C anion-exchange-membrane electrolyzer, a FNC@MoS2/CC (+,-) couple displays 500 mA cm-2 at only 1.87 V and operates stably over 200 h. This work highlights that engineering pre-catalysts to steer dynamic surface reconstruction is an pivotal strategy for advanced OER electrocatalysis.
Power requirements represent a critical challenge for wearable sensors. Self-powered sensing systems enabled by miniaturized energy-storage devices (MESDs) offer a promising solution. However, the proliferation of MESDs inevitably generates electronic waste (e-waste), which causes environmental concerns. Transient electronics that degrade into eco-friendly residuals provide opportunities for the development of green power sources. Herein, flexible e-waste-friendly power sources based on degradable MXene films were developed for the integration of wearable, self-powered biomedical sensors. The proposed transient MXene film-based supercapacitors (TMFSCs) possess good energy storage capability and mechanical flexibility and can be completely degraded into eco-friendly residuals within minutes. Furthermore, a wearable self-powered biomedical smart sensor was designed for real-time monitoring of pulse signals in real-life scenarios, and the obtained pulse rate is conducive to early evaluation of human health. Collectively, TMFSCs are considerably competitive for future eco-friendly flexible MESDs toward next-generation sustainable wearable and portable sensing electronics.
Zinc-organic batteries (ZOBs) based on C═N compounds arouse great interest due to wide structure, high capacity, and long cycle life. However, activation phenomenon of C═N compound is seldom discussed in ZOBs, as well as activation mechanism during charging/discharging. Herein, DPPT (Diphenazine-pyrenetetraimine) with eight C═N active sites is first synthesized for ZOBs, delivering ultralong cycling life (45 000 cycles) and good rate performance (20 C). Notably, there shows obvious activation process at beginning cycles because of the transformation of DPPT-eight proton into DPPT. In situ experiments and DFT calculations reveal co-participation mechanism of Zn2+ & H+ with optimized structure of 2DPPT-1Zn-14H deriving from 16 discharged products. Impressively, wearable NH3 sensors could be powered by as-fabricated flexible DPPT ZOBs, making it possible from the restriction of traditional power supply. Prospectively, activation mechanism of high-performing DPPT would provide methods for further design of organic structures into ZOBs and offer self-powered energy for wearable sensors.
ABSTRACT Copper‐based electrocatalysts exhibit high initial activity for formaldehyde oxidation but suffer rapid deactivation under industrially relevant current densities. While this instability has traditionally been attributed to copper self‐oxidation, the fundamental origin of performance decay remains debated. Here we show that the persistent accumulation of formate intermediates rather than Cu oxidation constitutes the primary deactivation pathway, and that this bottleneck can be overcome by establishing a dynamic conversion‐desorption equilibrium through local electronic microenvironment engineering. We develop an AgCu microsphere catalyst (AgCu‐MSs/CF) with an optimized Ag loading of 4.1 wt.%, which achieves a current density of 1068 mA cm −2 at 1.0 V versus RHE and operates stably up to 1.3 V versus RHE, well beyond the thermodynamic oxidation limit of Cu. Combined in situ spectroscopy and density functional theory reveal that Ag incorporation induces electron transfer from Ag to Cu, downshifting the d‐band center of Cu. This electronic modulation weakens formate adsorption, thus preventing active‐site blocking and ensuring the sustained catalytic activity. Leveraging this design principle, a bipolar FOR||HER electrolyzer operates stably for over 312 h. This work establishes that engineering the dynamic equilibrium between intermediate formation and removal offers a generalizable strategy to mitigate poisoning in Cu‐based catalysts for complex oxidation reactions.
The deployment of flexible electrochemical sensing architectures anchored by two-dimensional (2D) nanomaterials represents a paradigm shift in decentralized analytical chemistry, effectively transcending the spatial and temporal limitations intrinsic to conventional benchtop instrumentation. This review examines the engineering of high-fidelity sensing interfaces that exploit the unique physicochemical attributes of 2D nanomaterials, including the atomic-scale thickness, superior surface-to-volume ratios, and inherent mechanical compliance. Emphasis is placed on elucidating the fundamental structure-function correlations that govern the fabrication of conformal and portable device architectures. We emphasize material innovation and sensor integration, and illustrate the practical utility through the rapid detection of complex food matrices (e.g., contaminants and nutritional markers). Furthermore, the intersection of sensor arrays with artificial intelligence and machine learning algorithms is discussed as a pivotal advancement for predictive signal processing. This review concludes by identifying technical challenges and outlining future directions for advancing next-generation 2D material-based flexible electronics.
Organic materials with high capacity and sustainability are widely used in aqueous zinc-ion batteries (ZIBs), yet organic materials with multi-redox centers and stable structures are seldom reported. Herein, we design a novel π-conjugated organic molecule with twelve C═O and C═N active sites, BDQDT (Bisdipyrido[4,3-a:3',4'-c]quinoxaline[3,2-a:2',3'-h]-11,24-dihydrophenazine-10,12,23,25-tetraone), enabling strong electron delocalization, reinforced π-π stacking, and suppressed dissolution. As a result, BDQDT ZIBs exhibit excellent rate capability with 84.0 mAh g-1 at 20 A g-1 and outstanding cycling stability after 12 000 cycles. Besides, In situ characterizations combined with DFT calculations confirm Zn2+/H+ co-insertion mechanism. The optimized discharged structure is identified as BDQDT-1Zn-10H, binding from one BDQDT molecule with one zinc ion and ten protons. Impressively, flexible Zn-ion device of BDQDT maintains stable properties under various mechanical deformations, and could power a humidity sensor. Prospectively, this work would build molecular engineering strategies for high-capacity and stable organic ZIBs.
Smart patches based on multimodal wearable devices enable real-time physiologic monitoring and proactive interventions to promote wound healing. Herein, we describe a biodegradable wearable electrotherapy patch (E-patch) that integrates noninvasive self-powered electrical stimulation (ES) therapy for tissue regeneration and a multiplexed electrochemical biosensor array for continuous monitoring of wound status. Custom-developed supercapacitor arrays (SCs) supply stable energy for ES, and constructed wearable biosensors enable sensitive monitoring of biomarkers in the wound exudate. As-fabricated wearable E-patches degrade harmlessly after operation, significantly reducing the environmental pollution pressure associated with flexible electronics. In vitro studies demonstrated that an applied electric field (EF) significantly promotes cell-directed alignment, which is crucial for tissue regeneration and remodeling. In vivo investigations in the Sprague-Dawley (SD) rat model illustrate that combination therapy dramatically accelerates wound healing. Overall, this work provides a promising strategy toward integrated smart wound management and future feedback-assisted wearable therapeutic systems.
ABSTRACT The design of a wearable bioelectronic device for electrotherapeutic wound healing and real‐time monitoring is critical for smart healthcare. However, developing multifunctional materials remains challenging due to energy supply or sensing interface issues. Herein, a simple strategy for integrating wound dressings of battery‐free electrotherapy and wound sensors via Dopamine (DA)‐modified MXene‐silver nanowire (Ag NWs)‐bacterial cellulose (BC) (PMAB) cross‐linked interpenetrating networks has been presented. Specifically, DA and BC significantly enhanced the antioxidant and mechanical properties of MXene, while Ag NWs improved the electrical and antimicrobial activities of PMAB. The solid‐state supercapacitor fabricated upon PMAB displayed excellent energy storage properties (2.5 F cm−2), replacing conventional power for delivering electrical stimulation (ES) to accelerate wound healing. NIH 3T3 fibrolast showed rapid migration and higher proliferation rate (over 70%) under ES (1 V). Meanwhile, wound dressing of cross‐linking interpenetrating structure of MXene and BC performs superior mechanosensing properties, with internal resistance change only 1.5 times of initial resistance over 60 days, which enables monitoring physical signal stabilization for wound assessment and management. This work would provide novel ideas of smartsensors for designing battery‐free wearable wound dressings.
Smart patches based on multimodal wearable devices enable real-time physiologic monitoring and proactive interventions to promote wound healing. Herein, we describe a biodegradable wearable electrotherapy patch (E-patch) that integrates noninvasive self-powered electrical stimulation (ES) therapy for tissue regeneration and a multiplexed electrochemical biosensor array for continuous monitoring of wound status. Custom-developed supercapacitor arrays (SCs) supply stable energy for ES, and constructed wearable biosensors enable sensitive monitoring of biomarkers in the wound exudate. As-fabricated wearable E-patches degrade harmlessly after operation, significantly reducing the environmental pollution pressure associated with flexible electronics. In vitro studies demonstrated that an applied electric field (EF) significantly promotes cell-directed alignment, which is crucial for tissue regeneration and remodeling. In vivo investigations in the Sprague-Dawley (SD) rat model illustrate that combination therapy dramatically accelerates wound healing. Overall, this work provides a promising strategy toward integrated smart wound management and future feedback-assisted wearable therapeutic systems.
Electrokinetics, which explores charge transfer and mass transport under electric fields, has emerged as a vital domain in advancing energy storage and electrocatalysis. The integration of organic and inorganic components into composite materials offers unique opportunities to optimize electrokinetic properties, leveraging the structural stability and conductivity of inorganic phases alongside the functional diversity of organic elements. These synergies enhance charge transfer, ionic mobility, and catalytic activity, making these composites indispensable in applications such as batteries, fuel cells, and electrocatalytic systems. This review explores the intersection of electrokinetic phenomena and organic-inorganic composite materials, focusing on their fundamental principles, design strategies, and performance optimization. Emphasis is placed on advanced materials, including metal-organic frameworks, organic-carbon hybrids, and single-atom catalysts, and their applications such as energy storage, wearable devices and electrocatalysis. The review highlights advanced in situ and operando techniques for probing electrokinetic processes, shedding light on the interplay between structure, interface, and transport dynamics. By bridging the gap between electrokinetic theory and material design, this work aims to provide insights into the development of next-generation materials for sustainable energy technologies.
Dehydration during exercise can lead to electrolyte imbalance and cardiovascular risk. Real-time monitoring of key sweat ions, such as pH, Na+, and K+, provides a critical means of assessing hydration status. Herein, we report a wearable sweat sensor based on OAm-modified Ti3C2Tx MXene with quasi-superhydrophobic interface for stable, low-hysteresis detection of ions. The hydrophobic modification effectively suppresses water-layer formation and enhances interfacial stability. Through in-situ electrochemical impedance spectroscopy (EIS) and distribution of relaxation times (DRT) analysis, we elucidate that impedance instability is the primary cause of hysteresis in conventional solid-state sensors. The fabricated pH, Na+, and K+ sensors exhibit highly reversible responses with minimal potential drift (2.4 mV, 1.3 mV, and 0.4 mV, respectively). Integrated into a flexible patch, the sensor successfully tracks dynamic ion changes in human sweat during exercise, demonstrating reliable agreement with ex-situ analysis. This work presents a facile and effective interfacial engineering strategy for developing non-hysteretic wearable ion sensors, enabling real-time dehydration warning in athletic and healthcare scenarios.
We report an ionic thermoelectric generator (iTEG) capable of delivering continuous power and large thermal voltages under a temperature gradient. Unlike conventional thermogalvanic cells, the current in our system arises from a reversible redox reaction driven by ionic thermodiffusion-induced thermal potentials. By systematically studying electrolytes with varying thermoelectric properties, we identified that self-assembled polyethylene glycol (PEG) clusters, stabilized by alkoxide end groups, are key to enable the output current. The iTEG achieved a maximum power density of 4.2 mW m-2 with an output voltage of 100 mV under a 20 K temperature difference. These findings establish a new design principle for ionic thermoelectric devices and provide insights into charge transfer process and redox reactions at electrode interfaces, with implications for energy technologies such as ion batteries and related electrochemical systems.
Herein, a CuSe/MnSe2 heterostructure with Se vacancies is fabricated as an ultrafast anode for low-temperature sodium-ion batteries. It achieves 380.3 mAh g-1 after 1500 cycles (3.0 A g-1) and 403.6 mAh g-1 at -30 °C (0.5 A g-1), highlighting exceptional cyclability and low-temperature adaptability.
Introduction:Magnesium oxide nanoparticles (MgO NPs) as magnesium ionophores have shown potential as a therapeutic strategy for osteoarthritis. However, the rapid absorption and clearance of MgO NPs in the joint cavity and the lack of a clear underlying mechanism may limit their therapeutic efficacy. Methods:MgO@SiO2 nano capsules were synthesized as a controlled-release nanosystem to mitigate the rapid clearance and potential toxicity of MgO NPs. The physicochemical properties and surface charge of the nano capsules were examined through TEM, EDS, XRD and Zeta potential. The kinetics of nano capsule degradation were measured using using inductively coupled plasma optical emission spectrometry and pH monitoring both in vivo and in vitro. Cytotoxicity and reactive oxygen species (ROS) were monitored to assess the dose-dependent effect of MgO@SiO2 on ROS-mediated oxidative stress. Finally, ROS production and the expression of proinflammatory factors (IL-6, MMP-13, COX-2) were quantified in the cartilage of osteoarthritis samples to evaluate the potential mechanism of action of the nanocapsules for treating osteoarthritis. Results:MgO@SiO2 nano capsules extended the duration of MgO NPs release from 12 h to 3-5 days both in vivo and in vitro. MgO@SiO2 exhibited no cytotoxicity toward chondrocytes at formula concentrations <15 mM. Notably, low concentrations (5 mM) of MgO@SiO2 (and thus of MgO NPs) suppressed ROS generation in chondrocytes, whereas higher concentrations (>10 mM) increased ROS production. In a rat model of osteoarthritis, intra-articular injection of 5 mM MgO@SiO2 samples significantly alleviated cartilage degeneration and destruction. Finally, ROS levels and the expression of certain proinflammatory factors (IL-6, MMP-13, COX-2)] in articular cartilage were markedly reduced. Conclusion:As a multi-functional ROS-responsive nanosystem, MgO@SiO2 nano capsules not only slow the release of MgO NPs and reduce their cytotoxicity but also reduce ROS production and thus lessen the inflammatory response in cartilage. This dual-action mechanism achieves therapeutic efficacy for osteoarthritis, offering a promising strategy to delay or reverse osteoarthritis progression.
Transition metal selenides (TMSs), as promising anode materials for sodium ion batteries (SIBs), still face sluggish Na+ diffusion kinetics and severe volume change, resulting in undesirable cycling stability and rate capability. Heterostructure construction is an effective method to improve sodium ion storage in TMSs. Herein, a hierarchical hollow heterostructure of CoSe2@SnSe is precisely designed through a facile coprecipitation process followed by a selenization strategy. The heterostructure constructed by CoSe2 and SnSe nanocrystals induces the formation of built-in electric fields and accelerates electron transfer and ion diffusion, thereby improving reaction kinetics significantly. When the as-prepared CoSe2@SnSe composites are employed as anode materials of SIBs, there exhibit ultra-fast electrochemical reaction kinetics and outstanding cycling stability with a high capacity retention of 488.9 mAh g-1 at a current density of 2.0 A g-1 after 900 cycles. In addition, there still shows an exceptional rate capability of 409.5 mAh g-1 at a high current density of 10 A g-1. This work provides an effective method for the rational designing of heterostructure anode materials for high-performance SIBs. (c) 2025 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
Owing to high theoretical capacity and abundant natural resources, transition metal selenides have been identified as promising anode materials for sodium ion batteries. However, poor conductivity and volume expansion during cycling seriously limit practical application. Herein, the growth of 2D MnSe2 nanosheets on Cu3Se2@Cu2Se nanocubes with mixed valence states has been designed by simple one-step selenization process at room temperature. As-fabricated MnSe2@Cu3Se2/Cu2Se (MCC) with hollow structure and heterostructure interfaces, can effectively alleviate volume expansion, accelerate ionic/electronic diffusion kinetics, and improve cycle stability for sodium ion batteries. The MCC anode maintains an ultrahigh-rate stability of 237.6 mAh/g at 80 A/g that is higher than reported selenide anodes, as well as long-term cycling stability after 3000 cycles at 20 A/g. Electrochemical kinetics and characterizations have effectively confirmed that the combination of heterojunction interface and microstructure is an effective way to improve the sodium storage performance of transition metal selenides.
Organophosphorus pesticides (OPs), while pivotal for agricultural productivity, pose severe environmental and health risks due to their persistence and bioaccumulation. Existing detection methods, such as chromatography and spectroscopy, face limitations in field adaptability, cost, and operational complexity. To address these challenges, this study introduces a novel dual-mode photoelectrochemical–electrochemical (PEC-EC) sensor based on a Co,N-TiO2@ZrO2/3DGH nanocomposite. The sensor synergistically integrates zirconium oxide (ZrO2) for selective OP capture via phosphate-Zr coordination, cobalt-nitrogen co-doped titanium dioxide (Co,N-TiO2) for visible-light responsiveness, and a three-dimensional graphene hydrogel (3DGH) for enhanced conductivity. In the PEC mode under light irradiation, OP adsorption induces charge recombination, yielding a logarithmic photocurrent attenuation with a detection limit of 0.058 ng mL−1. Subsequently, the EC mode via square wave voltammetry (SWV) self-validates the results, achieving a detection limit of 0.716 ng mL−1. The dual-mode system demonstrates exceptional reproducibility, long-term stability, and selectivity against common interferents. Parallel measurements revealed <5% inter-mode discrepancy, validating the intrinsic self-checking capability. This portable platform bridges the gap between laboratory-grade accuracy and field-deployable simplicity, offering transformative potential for environmental monitoring and food safety management.
The increase in the diabetic population and requirements for glucose monitoring devices accelerates the promotion of tremendous glucose biosensors. Aside from blood, alternative body fluids were explored to indicate the glucose profiles in a non-invasive manner. Sweat sensing using electrochemical biosensors offers an ideal solution for glucose monitoring, but their widespread application is now greatly hindered by the performance decreasing over the operation period. Here, we present a micro-sonobot-based decontamination strategy for the sweat glucose sensor to gently clean the sensor and achieve the recovery of its sensing activity. A screen-printed electrochemical biosensor with Cu2O decoration was proposed to detect sweat glucose and unveil the relationship between sweat and blood glucose levels. The sweat pollutant removal and sensor regeneration were realized using an acoustic manipulation platform and the bubble-powered micro-sonobots. The specified vibration mode of the acoustic manipulation platform generates the desired acoustic field for the control of bubble-powered micro-sonobots. The self-generated and swarm-enhanced acoustic streaming as well as the motion of microsonobots on the fouled sensor effectively remove the sweat pollutant and realize the renewal. The proposed decontamination method is expected to be a step toward the widespread application of sweat glucose biosensors and a general solution for the cleaning and regeneration of miniaturized surface-based biosensors.
Organic zinc-ion batteries (ZIBs) have been widely studied presently for high capacity, long lifespan, and sustainability of organic C--O/C--N materials, yet active sites storage mechanism is still unknown. Herein, a C--O/ C--N material of HATTAQ (Hexaazatriphenylene-trianthraquinone) has been designed. Through in-situ experiments and theoretical calculations, the optimal structure of HATTAQ-1Zn-10H is acquired by analyzing 10 more possible discharging products. Besides, there systemically illustrates detailed active sites during formation of HATTAQ-1Zn-10H. One inner C--N and one outer C--O bind with Zn2+ then H+ insertion. Initially, H+ insert in one C--N and one C--O in para-position followed by reaction of H+ with 4 internal C--N and 4 external C--O. As expected, HATTAQ ZIBs show long cycle life of 12,000 cycles with 91 % capacity retention. Impressively, flexible HATTAQ ZIBs with a stable capacity are firstly used in wearable sensors. Prospectively, this work would provide ideas into active sites storage mechanism of organic ZIBs.