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Photothermal responsive hydrogels are widely used in bionic soft actuators due to their remote-controlled capabilities and flexibility. However, their weak mechanical properties and limited responsiveness hinder their potential applications. To overcome this, we developed an innovative laponite/MXene/PNIPAm (LxMyPN) nanocomposite hydrogel that is mechanically robust and exhibits excellent photothermally responsive properties based on abundant hydrogen bonds. Notably, laponite clay is used as a co-cross-linking agent to improve the mechanical properties of LxMyPN hydrogel, while MXene nanosheets are added to promote the photothermal responsiveness. The resulting L3M0.4PN nanocomposite hydrogel exhibits enhanced mechanical properties, with a compressive strength of 0.201 MPa, a tensile strength of 90 kPa, and a fracture toughness of 27.25 kJ m-2. In addition, the L3M0.4PN hydrogel displays a deswelling ratio of 73.6% within 60 s and experiences an excellent volume shrinkage of 82.4% under light irradiation. Furthermore, hydrogel actuators with fast response behaviors are constructed and employed as grippers capable of grasping and releasing target objects. Overall, this high-strength and fast-responsive hydrogel actuator is beneficial to paving the way for remote controlled soft robots.
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Hierarchical porous structures and well-modulated interfacial interactions are essential for the performance of electrode materials. The energy storage performance can be promoted by regulating the diffusion behavior of the electrolyte and constructing a coupled interaction at heterogeneous interfaces. Herein, we have synthesized ultrathin NiO nanosheets anchored to nitrogen-doped hierarchical porous carbon (NiO/N-HPC) and applied it to construct aqueous potassium ion hybrid capacitors (APIHCs). The abundant and interconnected porous architecture promotes electrolyte penetration/diffusion and shortens the ion transport path, thereby accelerating storage reaction kinetics. The nitrogen-doped carbon support can achieve optimized metal oxides-carbon interaction and enhance the adsorption ability for the electrolyte ions, leading to earning higher storage capacity. Consequently, the prepared NiO/N-HPC exhibits a superior capacitance of 126.4 F g-1 at a current density of 0.5 A g-1, and the as-fabricated NiO/N-HPC//N-HPC APIHC achieves an ultra-high capacitance retention of 91.6% over 8000 cycles at a current density of 2 A g-1. Meanwhile, the APIHC device shows an excellent energy density of 21.95 W h kg-1 and a power density of 9000 W kg-1.
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High-entropy perovskite oxides are promising materials in the field of electrocatalysis due to their advantages such as large spatial composition regulation, entropy effects, and tunable material properties. However, the preparation of high-entropy perovskite oxides with stable and controllable structures still remains challenging. Herein, we fabricated a series of high-entropy perovskite oxide porous nanotubes (PNTs) by electrospinning as efficient electrocatalysts for the nitrate reduction reaction (NO3RR). We further revealed that the different diffusion and decomposition behaviors of metal ions and polymers during the calcination process are the key to the formation of high-entropy perovskite oxide PNTs. Especially, LaSrNiCoMnFeCuO3 PNTs show excellent performance of the NO3RR, achieving the maximum NH3 Faradaic efficiency of almost 100%, yield rate of 1657.5 µg h-1 mgcat.-1, and durable stability after successive cycling, being one of the best electrocatalysts for the NO3RR. The mechanism studies show that the charge redistribution induced by the multisite synergistic effect and abundant unsaturated sites in the high-entropy perovskite oxide PNTs favors the adsorption of NO3- and key intermediates and reduces the catalytic energy barrier, thus further achieving high NO3- conversion efficiency.
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Aqueous zinc (Zn) iodine (I2) batteries have emerged as viable alternatives to conventional metal-ion batteries. However, undesirable Zn deposition and irreversible iodine conversion during cycling have impeded their progress. To overcome these concerns, we report a dynamical interface design by cation chemistry that improves the reversibility of Zn deposition and four-electron iodine conversion. Due to this design, we demonstrate an excellent Zn-plating/-stripping behavior in Zn||Cu asymmetric cells over 1000 cycles with an average Coulombic efficiency (CE) of 99.95%. Moreover, the Zn||I2 full cells achieve a high-rate capability (217.1 mA h g-1 at 40 A g-1; C rate of 189.5C) at room temperature and enable stable cycling with a CE of more than 99% at -50 °C at a current density of 0.05 A g-1. In situ spectroscopic investigations and simulations reveal that introducing tetraethylammonium cations as ion sieves can dynamically modulate the electrode-electrolyte interface environment, forming the unique water-deficient and chloride ion (Cl-)-rich interface. Such Janus interface accounts for the suppression of side reactions, the prevention of ICl decomposition, and the enrichment of reactants, enhancing the reversibility of Zn-stripping/-plating and four-electron iodine chemistry. This fundamental understanding of the intrinsic interplay between the electrode-electrolyte interface and cations offers a rational standpoint for tuning the reversibility of iodine conversion.
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Creating bionic intelligent robotic systems that emulate human-like skin perception presents a considerable scientific challenge. This study introduces a multifunctional bionic electronic skin (e-skin) made from polyacrylic acid ionogel (PAIG), designed to detect human motion signals and transmit them to robotic systems for recognition and classification. The PAIG is synthesized using a suspension of liquid metal and graphene oxide nanosheets as initiators and cross-linkers. The resulting PAIGs demonstrate excellent mechanical properties, resistance to freezing and drying, and self-healing capabilities. Functionally, the PAIG effectively captures human motion signals through electromechanical sensing. Furthermore, a bionic intelligent sorting robot system is developed by integrating the PAIG-based e-skin with a robotic manipulator. This system leverages its ability to detect frictional electrical signals, enabling precise identification and sorting of materials. The innovations presented in this study hold significant potential for applications in artificial intelligence, rehabilitation training, and intelligent classification systems.
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Constructing a built-in interfacial electric field (BIEF) is an effective approach to enhance the electrocatalysts performance, but it has been rarely demonstrated for electrochemical carbon dioxide reduction reaction (CO2RR) to date. Herein, for the first time, SnO2/LaOCl nanofibers (NFs) with BIEF is created by electrospinning, exhibiting a high Faradaic efficiency (FE) of 100% C1 product (CO and HCOOH) at -0.9--1.1 V versus reversible hydrogen electrode (RHE) and a maximum FEHCOOH of 90.1% at -1.2 VRHE in H-cell, superior to the commercial SnO2 nanoparticles (NPs) and LaOCl NFs. SnO2/LaOCl NFs also exhibit outstanding stability, maintaining negligible activity degradation even after 10 h of electrolysis. Moreover, their current density and FEHCOOH are almost 400 mA cm-2 at -2.31 V and 83.4% in flow-cell. The satisfactory CO2RR performance of SnO2/LaOCl NFs with BIEF can be ascribed to tight interface of coupling SnO2 NPs and LaOCl NFs, which can induce charge redistribution, rich active sites, enhanced CO2 adsorption, as well as optimized Gibbs free energy of *OCHO. The work reveals that the BIEF will trigger interfacial accumulation and stability enhancement effects in promoting CO2RR activity and stability of SnO2-based materials, providing a novel approach to develop stable and efficient CO2RR electrocatalysts.
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Electronic skin (e-skin), a skin-like wearable electronic device, holds great promise in the fields of telemedicine and personalized healthcare because of its good flexibility, biocompatibility, skin conformability, and sensing performance. E-skin can monitor various health indicators of the human body in real time and over the long term, including physical indicators (exercise, respiration, blood pressure, etc.) and chemical indicators (saliva, sweat, urine, etc.). In recent years, the development of various materials, analysis, and manufacturing technologies has promoted significant development of e-skin, laying the foundation for the application of next-generation wearable medical technologies and devices. Herein, the properties required for e-skin health monitoring devices to achieve long-term and precise monitoring and summarize several detectable indicators in the health monitoring field are discussed. Subsequently, the applications of integrated e-skin health monitoring systems are reviewed. Finally, current challenges and future development directions in this field are discussed. This review is expected to generate great interest and inspiration for the development and improvement of e-skin and health monitoring systems.
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Dispositivos Electrónicos Vestibles , Humanos , Monitoreo Fisiológico/instrumentación , Monitoreo Fisiológico/métodos , Piel , Telemedicina/instrumentaciónRESUMEN
Prussian blue analogues (PBAs) are considered to be one of the most suitable sodium storage materials, especially with the introduction of the high-entropy (HE) concept into their structure to further improve their various abilities. However, severe agglomeration of the HEPBA particles still limits the fast charging capabilities. Here, an HEPBA (Nax(FeMnCoNiCu)[Fe(CN)6]yâ¡1-y·nH2O) with a hollow stair-stepping spherical structure has been prepared through the chemical etching process of the traditional cubic structure of HEPBA. Electrochemical characterization (sodium ion battery), kinetic analysis, and COMSOL Multiphysics simulations reveal that the nature of the high-entropy and the hollow stair-stepping spherical structure can greatly improve the diffusion behavior of Na+ ions. Moreover, the hollow structure effectively mitigates the volume change of HEPBA during SIBs operation, ultimately extending the lifespan. Consequently, the as-prepared HEPBA cathode exhibits excellent rate performance (126.5 and 76.4 mAh g-1 at 0.1 and 4.0 A g-1, respectively) and stable long-term capability (maintaining its 75.6% capacity after 1000 cycles) due to its unique structure. Furthermore, the waste of the etching process can easily be recycled to prepare more HEPBA product. This processing method holds great promise for designing nanostructures of advanced high-entropy Prussian blue analogues for sodium ion batteries.
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Metal nanoparticle (NP) cocatalysts are widely investigated for their ability to enhance the performance of photocatalytic materials; however, their practical application is often limited by the inherent instability under light irradiation. This challenge has catalyzed interest in exploring high-entropy alloys (HEAs), which, with their increased entropy and lower Gibbs free energy, provide superior stability. In this study, 3.5 nm-sized noble-metal-free NPs composed of a FeCoNiCuMn HEA are successfully synthesized. With theoretic calculation and experiments, the electronic structure of HEA in augmenting the catalytic CO2 reduction has been uncovered, including the individual roles of each element and the collective synergistic effects. Then, their photocatalytic CO2 reduction capabilities are investigated when immobilized on TiO2. HEA NPs significantly enhance the CO2 photoreduction, achieving a 23-fold increase over pristine TiO2, with CO and CH4 production rates of 235.2 and 19.9 µmol g-1 h-1, respectively. Meanwhile, HEA NPs show excellent stability under simulated solar irradiation, as well high-energy X-ray irradiation. This research emphasizes the promising role of HEA NPs, composed of earth-abundant elements, in revolutionizing the field of photocatalysis.
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Crystal-phase engineering that promotes the rearrangement of active atoms to form new structural frameworks achieves excellent result in the field of electrocatalysis and optimizes the performance of various electrochemical reactions. Herein, for the first time, it is found that the different components in metallic aerogels will affect the crystal-phase transformation, especially in high-entropy alloy aerogels (HEAAs), whose crystal-phase transformation during annealing is more difficult than medium-entropy alloy aerogels (MEAAs), but they still show better electrochemical performance. Specifically, PdPtCuCoNi HEAAs with the parent phase of face-centered cubic (FCC) PdCu possess excellent 89.24% of selectivity, 746.82 mmol h-1 g-1 cat. of yield rate, and 90.75% of Faraday efficiency for ethylamine during acetonitrile reduction reaction (ARR); while, maintaining stability under 50 h of long-term testing and ten consecutive electrolysis cycles. The structure-activity relationship indicates that crystal-phase regulation from amorphous state to FCC phase promotes the atomic rearrangement in HEAAs, thereby optimizing the electronic structure and enhancing the adsorption strength of reaction intermediates, improving the catalytic performance. This study provides a new paradigm for developing novel ARR electrocatalysts and also expands the potential of crystal-phase engineering in other application areas.
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The oligomers of carbon suboxide, known as red carbon, exhibit a highly conjugated structure and semiconducting properties. Upon mild heat treatment, it transforms into a carbonaceous framework rich in oxygen surface terminations, called oxocarbon. In this study, the abundant oxygen functionalities are harnessed as anchors to create oxocarbon-supported nanohybrid electrocatalysts. Starting with single atomic Cu (II) strongly coordinated to oxygen atoms on red carbon, the Fehling reaction leads to the formation of Cu2O clusters. Simultaneously, a covalent oxocarbon framework emerges via cross-linking, providing robust support for Cu2O clusters. Notably, the oxocarbon support effectively stabilizes Cu2O clusters of very small size, ensuring their high durability in acidic conditions and the presence of ammonia. The synthesized material exhibits a superior electrocatalytic activity for nitrate reduction under acidic electrolyte conditions, with a high yield rate of ammonium (NH4 +) at 3.31 mmol h-1 mgcat -1 and a Faradaic efficiency of 92.5% at a potential of -0.4 V (vs RHE).
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Carbon dioxide (CO2) adsorption and electron transport play an important role in CO2 reduction reaction (CO2RR). Herein, we have demonstrated a new class of diverse hollow ZnSnOx (ZSO) through the amorphization of hydroxides to enhance CO2 adsorption and accelerate electron transport. The amorphization is occurred by calcination process, as indicated by Fourier transform infrared spectroscopy and Raman spectra. In particular, the ZnSnOx hollow spheres (ZSO HSs) achieve a high Faradaic efficiency (FE) of HCOOH up to 92.7 % at best, outperforming the commercial ZSO (Comm. ZSO, 85.7 %). ZSO HSs also exhibit durable stability with negligible activity decay after 10â h of successive electrolysis. In-situ attenuated total reflectance infrared absorption spectroscopy further reveals strong adsorption of CO2 and rapid intermediate configuration transformation in amorphous ZSO HSs. This work demonstrates the practical application of ZSO for CO2RR and provides a new insight to create efficient CO2RR electrocatalysts.
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The growing interest in so-called interface coupling strategies arises from their potential to enhance the performance of active electrode materials. Nevertheless, designing a robust coupled interface in nanocomposites for stable electrochemical processes remains a challenge. In this study, an epitaxial growth strategy is proposed by synthesizing sulfide rhenium (ReS2) on exfoliated black phosphorus (E-BP) nanosheets, creating an abundance of robust interfacial linkages. Through spectroscopic analysis using X-ray photoelectron spectroscopy and X-ray absorption spectroscopy, the authors investigate the interfacial environment. The well-developed coupled interface and structural stability contribute to the impressive performance of the 3D-printed E-BP@ReS2-based micro-supercapacitor, achieving a specific capacitance of 47.3 mF cm-2 at 0.1 mA cm-2 and demonstrating excellent long-term cyclability (89.2% over 2000 cycles). Furthermore, density functional theory calculations unveil the positive impact of the strongly coupled interface in the E-BP@ReS2 nanocomposite on the adsorption of H+ ions, showcasing a significantly reduced adsorption energy of -2.17 eV. The strong coupling effect facilitates directional charge delocalization at the interface, enhancing the electrochemical performance of electrodes and resulting in the successful construction of advanced micro-supercapacitors.
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Zinc-iodine batteries (ZIBs) are promising candidates for ecofriendly, safe, and low-cost energy storage systems, but polyiodide shuttling and the complex cathode fabrication procedures have severely hindered their broader commercial usage. Herein, a protocol is developed using phospholipid-like oleylamine molecules for scalable production of Langmuir-Blodgett films, which allows the facile preparation of ZIB cathodes in less than 1 min. The resulting inhomogeneous cathode allows for the continuous conversion of iodine. Moreover, the amine group of the oleylamine molecule at the cathode is capable of producing [OA*I+]I3- charge-transfer complexes with iodine, which facilitates the rapid migration of iodine and results in a highly reversible iodine conversion process. Consequently, the as-prepared ZIBs can deliver over 2000 cycles at 0.5 mA cm-2 with a capacity retention of 75.3%. This work presents a novel, straightforward, and efficient method for the rapid construction of ZIBs.
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Aqueous rechargeable multivalent metal-ion batteries (ARMMBs) have attracted considerable attention due to their high capacity, high energy density, and low cost. However, their performance is often limited by low temperature operation, which requires the development of anti-freezing electrolytes. In this review, we summarize the anti-freezing mechanisms and optimization strategies of anti-freezing electrolytes for aqueous batteries (especially for Zn-ion batteries). Besides, we investigate the possible interactions and side reactions between electrolytes and electrodes. We also analyze the problems between electrolytes and electrodes at low temperature, and propose possible solutions. The research progress in the field of low temperature energy storage for aqueous Mg-ion, Ca-ion, and Al-ion batteries, and the challenges faced in their anti-freezing electrolytes are investigated in detail. Last but not least, the outlook on the energy storage applications of ARMMBs is provided to guide the future research.
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Lattice strain engineering optimizes the interaction between the catalytic surface and adsorbed molecules. This is done by adjusting the electron and geometric structure of the metal site to achieve high electrochemical performance, but, to date, it has been rarely reported on anti-poisoned oxygen reduction reaction (ORR). Herein, lattice-strained Pd@PdBiCo quasi core-shell metallic aerogels (MAs) were designed by "one-pot and two-step" method for anti-poisoned ORR. Pd@PdBiCo MAs/C maintain their original activity (1.034â A mgPd -1 ) in electrolytes with CH3 OH and CO at 0.85â V vs. reversible hydrogen electrode (RHE), outperforming the commercial Pd/C (0.156â A mgPd -1 ), Pd MAs/C (0.351â A mgPd -1 ), and PdBiCo MAs/C (0.227â A mgPd -1 ). Moreover, Pd@PdBiCo MAs/C also show high stability and anti-poisoning with negligible activity decay after 8000 cycles in 0.1â m KOH+0.3â m CH3 OH. These results of X-ray photoelectron spectroscopy, CO stripping, and diffuses reflectance FTIR spectroscopy reveal that the tensile strain and strong interaction between different elements of Pd@PdBiCo MAs/C effectively optimize the electronic structure to promote O2 adsorption and activation, while suppressing CH3 OH oxidation and CO adsorption, leading to high ORR activity and anti-poisoning property. This work inspires the rational design of MAs in fuel cells and beyond.
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Polyimide aerogel fibers hold promise for intelligent thermal management fabrics, but their scalable production faces challenges due to the sluggish gelation kinetics and the weak backbone strength. Herein, a strategy is developed for fast and scalable fabrication of crosslinked polyimide (CPI) aerogel fibers by wet-spinning and ambient pressure drying via UV-enhanced dynamic gelation strategy. This strategy enables fast sol-gel transition of photosensitive polyimide, resulting in a strongly-crosslinked gel skeleton that effectively maintains the fiber shape and porous nanostructure. Continuous production of CPI aerogel fibers (length of hundreds of meters) with high specific modulus (390.9 kN m kg-1) can be achieved within 7 h, more efficiently than previous methods (>48 h). Moreover, the CPI aerogel fabric demonstrates almost the same thermal insulating performance as down, but is about 1/8 the thickness of down. The strategy opens a promisingly wide-space for fast and scalable fabrication of ultrathin fabrics for personal thermal management.
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Uncontrolled dendrite growth and water-related side reactions in mild electrolytes are the main causes of poor cycling stability of zinc anodes, resulting in the deterioration of aqueous zinc-based batteries. Herein, a multifunctional fluorapatite (Ca5(PO4)3F) aerogel (FAG) interface layer is proposed to realize highly stable zinc anodes via the integrated regulation of Zn2+ migration kinetics and Zn (002) orientation deposition. Owing to the well-defined aerogel nanochannels and the rich Zn2+ adsorption sites resulting from the ion exchange between Ca2+ and Zn2+, the FAG interface layer could significantly accelerate the Zn2+ migration and effectively homogenize the Zn2+ flux and nucleation sites, thus promoting rapid and uniform Zn2+ migration at the electrode/electrolyte interface. Additionally, during the cycling process, the F atoms from FAG promote the in situ generation of ZnF2, which facilitates the manipulation of the preferred Zn (002) orientation deposition, thus efficiently suppressing dendrite growth and side reactions by combining with the above synergistic effects. Consequently, the FAG-modified Zn anode displays a stable cycle life of over 4000 h at 1 mA cm-2 and exhibits highly reversible Zn plating/stripping behavior. Meanwhile, the Zn||MnO2 full cells exhibit improved cycle stability over 2000 cycles compared with that of the bare Zn, highlighting the virtues of the FAG protective layer for highly reversible Zn anodes. Our work brings the insight in to stabilize Zn anodes and power the commercial applications of aqueous zinc-based batteries.
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Sequentially managing the coverage and dimerization of *CO on the Cu catalysts is desirable for industrial-current-density CO2 reduction (CO2R) to C2+, which required the multiscale design of the surface atom/architecture. However, the oriented design is colossally difficult and even no longer valid due to unpredictable reconstruction. Here, we leverage the synchronous leaching of ligand molecules to manipulate the seeding-growth process during CO2R reconstruction and construct Cu arrays with favorable (100) facets. The gradient diffusion in the reconstructed array guarantees a higher *CO coverage, which can continuously supply the reactant to match its high-rate consumption for high partial current density for C2+. Sequentially, the lower energy barriers of *CO dimerization on the (100) facets contribute to the high selectivity of C2+. Profiting from this sequential *CO management, the reconstructed Cu array delivers an industrial-relevant FEC2+ of 86.1% and an FEC2H4 of 60.8% at 700 mA cm-2. Profoundly, the atomic-molecular scale delineation for the evolution of catalysts and reaction intermediates during CO2R can undoubtedly facilitate various electrocatalytic reactions.