The scalable implementation of water electrolysis for sustainable hydrogen production remains critically hindered by the lack of earth-abundant electrocatalysts that can operate efficiently and stably under industrially relevant conditions. Herein, we report a hierarchically engineered, noble-metal-free electrocatalyst that delivers efficient and durable performance for the alkaline hydrogen evolution reaction (HER) at high current densities. This catalyst was synthesized by conformally growing an interwoven network of carbon nanotubes (CNTs) decorated with Co/CoOx heterojunction nanoparticles on the inner surface of carbonized wood (CW) channels via a simple combustion-reductive annealing method. Control experiments in combination with finite-element simulations revealed that the CNTs lining simultaneously enhance surface superhydrophilicity and underwater superaerophobicity, synergistically overcoming mass-transfer limitations. Furthermore, the micro-nano hierarchical architecture generates abundant accessible Co/Co3O4 heterointerfaces that actively catalyze the alkaline HER, while simultaneously providing a continuous three-dimensional conductive network for rapid electron transport. Benefiting from this synergistic multi-parameter optimization, the Co/CoOx/CNT/CW catalyst exhibits excellent electrocatalytic performance, delivering 1000 mA cm−2 at an overpotential of 253 mV and maintaining stable operation for longer than 300 h. The assembled alkaline cell using the self-supported Co/CoOx/CNT/CW cathode sustains steady hydrogen generation at 1000 mA cm−2 beyond 300 h.
Purification of C2H4 from C2H2 and CO2 mixtures is a crucial yet challenging industrial process that typically relies on energy-intensive methods. A novel cage-based MOF, {[Ni1.5(CPIA)(DPA)1.5(H2O)2]·3DMF·1.5H2O}n (Ni-MOF, CPIA = 5-((6-carboxypyridin-3-yl)oxy)isophthalic acid, DPA = di(pyridin-4-yl)amine), was successfully constructed from flexible ligands. The structure features 1D tubular channels and unique trigonal bipyramidal cages, exhibiting high adsorption capacities for C2H2 and CO2 but suppressed adsorption of C2H4 at ambient conditions. Notably, IAST calculations reveal preferential selectivities for C2H2/C2H4 (2.28-2.92) and C2H2/CO2 (2.14-7.4) mixtures, which are further confirmed by breakthrough simulations. GCMC simulations indicate that multiple host-guest interactions within the pores contribute to the preferential adsorption of C2H2 and CO2 over C2H4. These results demonstrate the potential of Ni-MOF as a promising adsorbent for efficient purification of C2H4 from binary and ternary gas mixtures.
The catalytic decomposition of hydrazine monohydrate (N2H4 center dot H2O) has attracted considerable attention as a promising on-demand hydrogen generation technology for mobile and portable applications. However, the practical implementation of N2H4 center dot H2O-based system is hindered by the low activity and poor stability of existing catalysts, particularly those based on non-precious metals. We herein report a ternary alloying strategy to simultaneously enhance catalytic activity and stability of non-precious metal catalysts. In this work, we selected Ni-Mo binary alloy, one of the best non-precious metal catalysts, as basic material and introduced Cu as an additional alloying element. An oxide-supported ternary alloy catalyst, (Ni1-xCux)10Mo/MoOy, was synthesized by a simple hydrothermal method followed by reductive annealing. Comprehensive phase/structure/chemical state analyses confirmed the formation of (Ni1-xCux)10Mo solid solution alloy, with Cu atoms substituting for Ni within the Ni10Mo lattice. The incorporation of Cu into Ni-Mo alloy resulted in nearly a fivefold increase in catalytic activity and a significant reduction in activity decay, from 11 % to less than 5 % after 10 reaction cycles. Benefiting from the Ni-Cu-Mo alloying and the construction of a hierarchical nanostructure, (Ni1-xCux)10Mo/ MoOy exhibited high activity, 100 % H2 selectivity (at 70 degrees C), and excellent stability, outperforming most reported non-precious metal N2H4 center dot H2O decomposition catalysts. Utilizing this precious-metal-free catalyst, we further developed a N2H4 center dot H2O-based hydrogen generation system featuring a high hydrogen capacity (6.3 wt%) and rapid dynamic response, demonstrating strong potential for practical hydrogen source applications.
Transition metal/transition metal oxide (TM/TMO) heterostructures have attracted extensive attention as promising catalysts for the alkaline hydrogen evolution reaction (HER), which is particularly relevant for industrial-scale hydrogen production. However, the HER activity of conventional TM/TMO catalysts is still hampered by intrinsic limitations, including poor electrical conductivity, excessively strong hydroxyl binding, and suboptimal hydrogen adsorption. Herein, we report the rational design and tailored synthesis of a Cu-Co/N-MoO(2 )heterointerface catalyst for the alkaline HER, with special focus on concurrently modulating the electronic structures of the oxide and metallic components via N-doping and Cu-Co alloying, respectively, and correlating these modifications with the adsorption/desorption properties of OH* and H* intermediates on the catalyst surface. Experimental and computational studies consistently reveal that N-doping in MoO(2 )significantly enhances electrical conductivity and weakens hydroxyl (OH*) binding, thereby mitigating site poisoning. Meanwhile, Cu-Co alloying optimizes the D-band structure of the metallic sites, enabling nearly thermoneutral H2 desorption. The synergistic modifications in electronic structure and surface chemistry, together with the construction of the Cu-Co/N-MoO(2 )heterointerface, render accelerated kinetics in all elementary steps of the alkaline HER. As a consequence, the Cu-Co/NMoO2 catalyst exhibits outstanding HER performance, requiring only 15 mV overpotential at 10 mA cm-2 and 171 mV at 10 0 0 mA cm(-2) , along with remarkable long-term stability under high current densities. When paired with a NiFe-LDH anode in an alkaline anion exchange membrane water electrolyzer, the cell achieves 10 0 0 mA cm-2 at just 1.98 V and operates stably for over 300 h with < 1% voltage decay. The findings highlight the strong potential of Cu-Co/N-MoO(2 )as a highly active, durable, and earth-abundant catalyst for industrial-scale hydrogen production. (c) 2026 Published by Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.
The practical application of potassium metal batteries (PMBs) has been hindered by serious dendrite growth and volume variation on the potassium (K) metal anode. Altering the deposition behavior of K metal by designing a three-dimensional (3D) scaffold is an ideal strategy to inhibit the dendrite growth and volume variation. Here, a self-standing and gradient-potassiophilic 3D porous scaffold composed of Ti3CN on the separator side and Ti3CN and SnF2 nanoparticles on the anode side (named 3D-T/TSF) is designed to modify the K metal anode, achieving excellent electrochemical performance. The potassiophilicity of the 3D-T/TSF scaffold increases in gradient along the direction perpendicular to the electrode, which induces the preferential deposition of K metal within the 3D-T/TSF scaffold. Such deposition behavior could fully occupy the internal pore structure of the scaffold, inhibiting the K dendrite growth and relieving the volume variation. In addition, an inorganic SEI layer rich in K-Sn alloy, SnO2, and KF is spontaneously formed at the interface between the anode and electrolyte to enhance the stability of the K anode. Consequently, the 3D-T/TSF@K//3D-T/TSF@K symmetric battery presents a long cycle lifespan of over 1200 h at 0.5 mA cm-2. The 3D-T/TSF@K//PTCDA full battery delivers a capacity retention of 88.5% after 100 cycles at 1C. The design of the gradient-potassiophilic 3D porous scaffold provides a new direction for the construction of stable K metal anodes, which is beneficial for promoting the practical application of PMBs.
The advancement of modern electronic devices toward lightweighting, high-frequency, and integrated designs has escalated the demand for multifunctional materials that can combine microwave and thermal management capabilities with mechanical load-bearing capacity. However, inherent trade-offs exist between electrical conductivity and thermal insulation, as well as between mechanical strength and lightweight properties. Herein, attempts have been made to innovatively embed lightweight, high-strength dielectric shells and highly conductive, low-infrared-emissivity metallic shells into hollow structure design. Specifically, heterogeneous dual-shell hollow microspheres (DSHM) were constructed using glass as the model dielectric material and copper as the conductive material. By optimizing the ratio of dielectric-to-conductive phases, the shell microstructure, and macroscopic structural parameters, we achieved a synergistic combination of lightweight and high strength (density: 0.4456-1.0991 g cm- 3, survival rate under 2 MPa uniaxial compression: 87.1%. Crucially, leveraging the distinct structural dependence of conductive and thermal networks, the integration of low thermal conductivity (0.1134-0.1478 W m- 1 K- 1) with broadly tunable electrical conductivity (299.6-2625.7 S cm- 1) and infrared emissivity (0.218-0.493) in a single microsphere was achieved for the first time. These properties endow the hollow microspheres with exceptional microwave attenuation and thermal regulation performance.
Optimizing catalytic performance while minimizing precious-metal usage represents a promising strategy for advancing the practical application of precious metal catalysts for formaldehyde (HCHO) oxidation. However, its implementation remains largely constrained by the limited understanding of structure-activity relationships and catalytic mechanisms. Herein, we report an experimental study of supported Pt catalysts on defect-engineered Al2O3, focusing on the modulation of surface chemistry and its correlation with catalytic activity towards HCHO oxidation. The defective Al2O3 was prepared via acetic acid (HAc) treatment of commercial Al2O3 followed by calcination, after which Pt nanoparticles were immobilized on the support using an impregnation-reduction method. The Pt/Al2O3–1.0HAc catalyst prepared under optimal conditions exhibited high activity (77.7 μmol gPt−1 s−1 at 25 °C), good stability, and excellent moisture tolerance. Notably, simply varying the HAc concentration during support preparation enabled simultaneously tuning the abundances of oxygen vacancies and coordinatively different surface hydroxyl species, as well as the electronic state of supported Pt. Correlating these surface chemical characteristics with catalytic performance revealed positive linear relationships between apparent site-normalized activity and the abundances of both oxygen vacancies and doubly-bridged hydroxyls. Furthermore, control experiments using in situ diffuse reflectance infrared Fourier transform spectroscopy coupled with online gas chromatography analysis indicated that HCHO oxidation over Pt/Al2O3-xHAc proceeds mainly via a hydroxyl-assisted pathway, in which the continuous regeneration of surface hydroxyls is critical for sustaining the catalytic cycle.
With the development of high-speed spacecraft, the equipment faces the threat of high temperatures brought about by the high speed. Hollow microspheres commonly applied in equipment may lose efficacy in extremely high-temperature circumstances. Fortunately, the thermal stability of hollow alumina microspheres (HAMs) could solve the drawbacks. However, HAMs prepared by conventional strategies encounter problems of high cost, time-consuming, and low yield. The spray drying can rapidly make soft and agglomerate-free granules on a large scale, which makes HAMs feasible in practical applications. Nonetheless, in previous work, HAMs prepared by spray drying suffer from poor mechanical performance. In this research, Al(NO3)3 was selected as the alumina source, using spray drying with heat treatment to prepare HAMs, which present low density, high isostatic strength, low thermal conductivity, and high-temperature thermal stability. Furthermore, the relationship between the preparation parameters with the morphology and properties of HAMs was explored. Based on explorations, the formation mechanism of HAMs and the factors influencing their morphology and structure were speculated. These explorations will serve as a paradigm for inspiring and guiding the development of high-performance HAMs, ultimately addressing the lightweight and high-strength demands of composite materials for aircraft under high-temperature conditions.
Potassium metal batteries (PMBs), characteristic of high energy density, environmental sustainability, and cost-effectiveness, are considered a promising alternative to lithium-ion batteries (LIBs) for next-generation electrochemical energy storage systems. However, the practical application of PMBs is hindered by uncontrolled dendrite growth and severe volume expansion of the potassium (K) metal anode. Herein, a self-standing K metal storage host composed of multi-channel carbon nanofibers (MCNFs) and Sn and Bi metal sub-nanoclusters modified MCNFs (denoted as MCNFs-Sn/Bi@MCNFs) with gradient potassiophilicity was developed through a simple layer-by-layer electrospinning method followed by subsequent thermal treatment procedures. The gradient potassiophilicity governed by the elaborate surface electronic-state modulation with Sn and Bi metal sub-nanoclusters effectively reduces the K nucleation barrier and guides bottom-up K deposition. Moreover, the three-dimensional (3D) conductive network with a multi-channel self-standing structure enhances ion transport kinetics, homogenizes electric field distribution, and mitigates volume expansion during the K plating/stripping process, synergistically suppressing K dendrite growth and electrolyte-related parasitic reactions. As a result, the symmetric cell delivers exceptional cycling stability for over 2400 h. The full cell demonstrates a high specific capacity of 122.8 mAh g−1 and excellent cycling stability for over 2500 cycles at 1000 mA g−1. This work developed a promising dual strategy by regulating gradient potassiophilicity with metal sub-nanoclusters and constructing self-standing 3D conductive networks to achieve dendrite-free K deposition and mitigate huge volume variation during the K plating/stripping process for improving the cycling stability of PMBs.
Sodium-ion batteries (SIBs) have emerged as strong alternatives for large-scale energy storage owing to their abundant availability of sodium, cost-effectiveness, and enhanced safety. However, the relatively low energy density than lithium-ion batteries remains a major challenge for large scale applications. 3D printing technology offers precise structural control and high material efficiency, has emerged as a potential solution to improve the areal capacity of electrodes and overcome the energy density limitations of SIBs. In this study, a high mass loading porous Na3V2(PO4)3 (NVP) cathode is 3D printed to enhance areal capacity and energy density, while maintaining the high rate capability and power density. The 3D printed NVP cathode with a high mass loading of 15.0 mg cm-2 delivers a specific capacity of 110.5 mAh g-1 and an areal capacity of 1.7 mAh cm-2 at 1C (1C = 117 mA g-1), maintaining 92.6 % of its initial capacity after 400 cycles. Moreover, the 3D printed Na-HC||NVP full batterie displays an initial specific capacity of 102.7 mAh g-1, which is effectively retained at 71.8 mAh g-1 after 300 cycles at 1C. It demonstrates an energy density of 177.7 Wh kg-1 and a power density of 187.9 W kg-1. This study demonstrates the potential of 3D printing for fabrication high mass loading and high areal capacity cathodes for SIBs.
Surface engineering of formaldehyde (HCHO) oxidation catalysts to enhance the mobility of active oxygen species represents a promising yet largely unexplored approach to boosting catalytic performance while minimizing precious metal usage. Herein, we demonstrate the viability of this approach using a CeO2-decorated Pt/Al2O3 catalyst, in which CeO2 functions primarily as a regulator of active oxygen species mobility. CeO2 nanoislands were introduced via a simple wet impregnation method, with their size readily tuned by controlling the solvent evaporation temperature. The Pt/Al2O3-CeO2 catalyst prepared under optimal conditions exhibited a nearly two-fold higher turnover frequency and a nearly three-fold higher mass-specific reaction rate compared to the Pt/Al2O3 reference. Combined in situ and ex situ characterization revealed that the pronounced activity improvement arises from the functional synergy among multiple components. Downsizing the CeO2 nanoislands increases Pt dispersion and expands the Pt/CeO2 interfacial area, thereby promoting O2 activation and surface migration of active oxygen species. Coupling these effects with the strong H2O adsorption strength of Al2O3 enables rapid and sustained hydroxyl regeneration, accelerating the HCHO oxidation kinetics.
Polystyrene (PS) waste recycling remains a critical challenge due to its high energy consumption and limited monomer yield. Herein, the b-ZnO catalyst with a few in-situ formed Zn sites at 270 degrees C under microwaves enhances the depolymerization of PS waste into monomers. To further improve the PS depolymerization over the bZnO catalyst, a series of Zn/b-ZnO catalysts with different metal Zn contents were prepared. Among these catalysts, the optimal 5Zn/b-ZnO achieves nearly 100 wt% PS conversion, yielding up to 0.997 g(-1) PS liquid products with 0.8 g(-1) PS styrene monomer in five cycles of experiment under microwaves. Such process greatly reduces the energy cost as compared with the conventional thermal process (0.51 vs. 0.81 kWh) and the obtained styrene monomer mixture can be repolymerized into fresh PS to complete a closed-loop recovery (80 wt% PS waste recycled). This work builds a novel microwave-assisted Zn/b-ZnO catalyst system for depolymerizing PS waste into monomers in a highly efficient way, which sheds a light on the sustainable recovery of PS waste.
Solar-driven interfacial evaporation offers a sustainable route for off-grid water purification, but achieving high evaporation efficiency and salt resistance remains a core design challenge. Herein, we propose a cross-scale integration strategy that simultaneously reduces evaporation enthalpy and enhances salt resistance. A 3D conical chitosan/polyvinyl alcohol (CSPx) aerogel-based evaporator with vertically oriented hierarchical micro-nano channels was prepared by unidirectional freezing, where polyvinyl alcohol incorporation enabled the formation of nanopores, enhanced porosity, and high-proportioned intermediate water. The optimized CSP2 achieves an evaporation rate of 2.39 kg m-2 h-1 and a solar efficiency of 100.4% under one solar intensity. For the first time, a fully coupled thermal-fluid-mass transfer COMSOL simulation revealed the surface temperature and evaporation flux distributions, clarifying the heat balance and confirming that interfacial cooling and environmental heat harvesting enable the conical structure to exceed 100% efficiency. The evaporator enables directional salt crystallization at the cone apex in 5 wt% NaCl solution and exhibits strong antibacterial activity, excellent purification performance for seawater, heavy-metal wastewater, and dye-contaminated water, as well as outstanding potential for practical applications. To sum up, this research provides insights into the performance optimization of solar evaporators and highlights the potential applications in alleviating the global freshwater crisis.
Traditional strong-solvating electrolytes exhibit high ionic conductivity but are limited by solvent-dominated solvation structures. The unstable solvent-derived electrode-electrolyte interfaces (EEIs) are detrimental to the fast-charging performance of sodium metal batteries (SMBs). Herein, a configuration-entropy-driven electrolyte with diverse solvation structures induced by a strongly solvating anion and cosolvent is proposed to realize a trade-off between high ionic conductivity and anion-enhanced solvation structures. The electrolyte possesses 75 types of Na+ solvation structure, contributing to its higher solvation configurational entropy (Delta S conf, 33.09 J mol-1 K-1) compared to the conventional strong-solvating ester electrolyte (24.28 J mol-1 K-1). The high Delta S conf facilitates ion transport and endows the electrolyte with diverse anion-coordination solvation structures, which promote the formation of inorganic-rich and stable EEIs. Therefore, the configuration-entropy-driven electrolyte with anion-enhanced solvation structures can reinforce the stability of Na metal anode and enable superior rate performances and cycling stability of Na||Na3V2(PO4)3 (NVP) cells. The modified Na||NVP cells deliver a high capacity retention of 98.2% at an ultrahigh rate of 60 C after 10 000 cycles. Even paired with high-loading NVP (approximate to 12 mg cm-2), the Na||NVP cells steadily operate for over 600 cycles. This work provides a unique insight into electrolyte design from the perspective of solvation configurational entropy.
Hollow microsphere absorbents hold great potential for lightweight and multi‐band compatible design due to their inherent low density and thermal conductivity, but it remains a great challenge to rationally control the microstructures to achieve an optimal balance of low density, high mechanical strength, impedance matching, attenuation ability, and thermal performance. In this work, bimetallic alloys and glass are selected as the model materials for the functional and supporting shells to construct lightweight yet robust hollow microspheres. The rational design and highly efficient realization of the composition and miscibility control of the bimetallic alloy are first emphasized. An in‐depth investigation is conducted on the effects of metal type and component compatibility on the microstructure of the structural units (SU), and further on the electromagnetic and thermal performances. The results confirm the necessity and effectiveness of regulating the integrity and microstructure of the electromagnetic and thermal networks via alloying‐induced migration and aggregation behavior control. The optimized product exhibits comprehensive advantages of being simultaneously thin (1.69 mm), wide (5.20 GHz), light (0.81 g cm −3 ), strong (−23.8 dB), high mechanical strength (91.87% survival rate at 20 MPa) and low thermal conductivity (0.063 W m −1 K −1 ), indicating excellent radar‐infrared stealth capabilities and structural stability.
The construction of cooperative active sites in manganese oxide catalysts has attracted ever-increasing attention as an effective strategy to enhance catalytic performance for formaldehyde (HCHO) oxidation. Herein, we report for the first time an oxygen-vacancy-rich mixed-valence MnO2 center dot MnO oxide as a highly efficient cooperative catalyst for HCHO oxidation. The MnO2 center dot MnO catalyst was synthesized via a simple one-step redox reaction between ethanol and potassium permanganate. Structural and surface chemical analyses demonstrated the formation of a single-phase nanocrystalline material with a high density of oxygen vacancies. Control experiments using in situ diffuse reflectance infrared Fourier transform spectroscopy revealed that HCHO oxidation over MnO2 center dot MnO follows a cooperative catalysis mechanism: the oxygen defect-rich MnO2 unit facilitates the dissociation of H2O into hydroxyl species, while the defective MnO unit promotes the activation of molecular O-2. Benefiting from this synergistic interaction, the MnO2 center dot MnO catalyst shows an extraordinarily high reaction rate of 0.24 mu mol m(-2) min(-1) at 70 degrees C, along with outstanding stability and moisture tolerance, surpassing previously reported non-precious metal oxide catalysts.
The 3D structure design as an available pathway is sufficiently demonstrated to improve the evaporation performance of solar evaporators. However, the evaporator with a 3D structure exhibiting high evaporation performance results in an increased rate of salt precipitation, which places a higher demand on salt resistance. Therefore, it remains a great challenge to overcome the salt accumulation at the evaporator surface, especially for a 3D cylindrical evaporator. Here, a novel 3D evaporator is developed that integrates an air-laid paper stick and chitosan/CNT (CSC) aerogel, featuring unique water transport channels designed to facilitate the radial transport of salt solution and directional precipitation towards the top edge. It is proved that increasing the height of the evaporator effectively improves the evaporation performance through experiments and thermodynamic calculations. In addition, the effect of relative humidity on the evaporation performance of the 3D interfacial evaporator was systematically studied. On this basis, the effects of including material properties, solution properties, and working environment on the salt deposition behavior are further investigated, which can guide researchers to rationally design according to specific conditions to achieve edge-directed salt deposition.
Nowadays, growing particulate matter (PM) pollution poses a serious threat to human health. Due to its biodegradability, worldwide availability, easy processability and low cost, cellulose has attracted significant attention for air filter production. However, natural cellulose-based air filters feature the intrinsic limitations, such as low removal efficiency and susceptibility to bacterial contamination. Herein, we fabricated an NH2-MIL-101@cellulose composite air filter with desirable manufacturing feasibility using the in-situ growth process combined with traditional papermaking techniques. The cellulosic substrate, rich in hydroxyls, fosters uniform NH2-MIL-101 dispersion and secure anchoring, minimizing loss. Characterization techniques and Density Functional Theory calculations verified the unique interface between NH2-MIL-101(Fe) and cellulose. At a testing wind speed of 2 m/s, the PM10 (PM2.5) filtration efficiency, pressure drop and quality factor for N101@BP-2 were 95.8 % (92.3 %), 31 Pa, and 0.102 Pa-1 (0.0827 Pa-1), respectively, harnessing fiber interception and MOF-mediated electrostatic effects. Furthermore, the antibacterial and biodegradable performance of NH2-MIL-101@cellulose composite filter were assessed. This work provides instructive guidance for the research on advanced cellulose-based materials for air purification.
Self-stacking, volume variation and sluggish ions diffusion kinetics strictly impede the application of graphene oxide (GO) in energy storage fields. Herein, an innovative molecular intercalating-chemical bonds anchoring strategy is proposed to simultaneously inhibit the self-stacking, improve the structural stability and broaden the interlayer spacing of GO, which is realized by intercalating P-Phenylenediamine (PPD) organic molecules into interlayers of GO (named PPD-GO) through strong chemical bonds. The intercalated PPD molecules between the GO layers can enhance the layered structural stability and durability by contributing both supporting pillar and tensional strain effects to the adjacent GO nanosheets. Meanwhile, the intercalated PPD molecules can broaden the interlayer spacing of GO to 0.86 nm, effectively reducing the Na+ ions migration barrier (dropping by 0.16 eV compared to GO) and remarkably improving Na+ ions diffusion kinetics. Benefiting from the aforementioned structural uniqueness, 2D layered PPD-GO delivers a decent capacity retention of 70.0 % after 10,000 cycles at 0.5 A g-1 and excellent rate capability with a specific capacity of 259.3 mAh g-1 at 5.0 A g-1. The PPD-GO//AC sodium-ion capacitor displays a decent energy density of 80.5 Wh kg-1 at the power density of 198.6 W kg-1.