High-entropy nanomaterials have attracted tremendous research attention owing to their unique physical and chemical properties. Conventional methods for the synthesis of high-entropy nanomaterials often necessitate high temperatures and struggle with achieving well-defined morphologies. Here, we report room-temperature synthesis of high-entropy metal sulfide nanobelts through sequential cation exchange reactions between the pre-synthesized cobalt sulfide nanobelts and various metal ions in aqueous solution. The cation exchange reaction follows the hard and soft acid-base theory, which guides us to design and produce a variety of binary to high-entropy octonary metal sulfide nanobelts with uniform distribution of elements. The high-entropy quinary (CoCuSnFeIn)Sx nanobelts demonstrate significantly enhanced electrocatalytic performance for the nitrate reduction reaction in comparison to low- and medium-entropy metal sulfide nanobelts, due to the increased configurational entropy and synergistic benefits of the incorporated metal elements. Our work provides a facile yet powerful synthesis platform for designing and synthesizing a diverse array of multi-metal/high-entropy sulfide nanomaterials with controlled compositions for electrocatalytic applications.

Heterogeneous photocatalytic polymerization has emerged as a promising strategy for developing greener reversible complexation-mediated polymerization (RCMP) systems. In this study, a bio-based heterogeneous photocatalyst was prepared by anchoring betaine onto hydroxyethyl cellulose via esterification, aiming to address the drawbacks of homogeneous photo-RCMP systems and inorganic support catalysts, and thereby enabling photoinduced RCMP under white LED irradiation. This system enabled the synthesis of well-defined polymethacrylates with controlled molecular weights and narrow dispersity (& Dstrok; < 1.2). Upon light exposure, photoinduced energy transfer from the catalyst to alkyl iodide initiators promoted carbon-iodine bond cleavage, generating radicals to initiate polymerization. Density functional theory calculations revealed that electrostatic interactions between the iodide anion and the quaternary ammonium cation, together with halogen bonding between the catalyst and alkyl iodide, significantly lower the bond dissociation energy, thereby enhancing polymerization efficiency. Kinetic studies and light on/off experiments confirmed good temporal control, while chain-extension experiments demonstrated high chain-end fidelity. Furthermore, the photocatalyst exhibited broad monomer compatibility, retained over 90% of its activity after three recycling cycles, and performed effectively under natural sunlight. Overall, this work provides a sustainable and recyclable strategy for visible-light-induced RCMP by integrating renewable materials with efficient photocatalytic functionality.

In this study, we explored a high-throughput automated chromatography strategy for fast screening high-performance fluorinated block copolymers as electrolyte additives for ultrastable Zn-ion batteries. The proposed polymer, synthesized through controlled reversible addition-fragmentation chain-transfer (RAFT) polymerization, features a hydrophilic oligo(ethylene glycol) methyl ether acrylate (OEGA) block to provide water solubility, and a fluorophilic perfluoropolyether (PFPE) segment as the fluorine source. Our investigations reveal that the balance between OEGA and fluorine plays a key role in modulating interactions between Zn2+ and the fluorinated polymer additives. The degree of polymerization (DP) of OEGA affects both the coordination environment of Zn2+ and water and the exposure of the hydrophobic fluorinated core. Meanwhile, the fluorinated segment facilitates the formation of a protective ZnF2-rich layer, contributing to the stabilization of the solid electrolyte interphase (SEI). Benefiting from this synergistic effect, the polymer additive significantly improves battery performance, achieving stable cycling for 3800 h in symmetric Zn|Zn cells with a Coulombic efficiency (CE) of over 99.6% in Zn|Cu cells. Notably, the Zn|NVO full cell demonstrates excellent capacity retention, maintaining 98.4% of its initial capacity after 5000 cycles at 5 A g-1, with a per-cycle capacity decay as low as 0.00032%. In addition, the Zn|NVO pouch cell delivers stable cycling with a capacity retention of 92% after 700 cycles. This work highlights the important role of composition balance in developing fluorinated polymer additives, puts forward valuable molecular design guidelines for functional additives for practical energy storage applications.

Flexible porous carbon fiber composite electrodes (Pt@C-PES cathode/RuO2@C-PES anode) for hydrogen and chlorine evolution reactions (HER/CER) in acidic NaCl electrolyte (1 M HCl + 5 M NaCl) were developed in this work. Functionalized with Pt and RuO2via electrodeposition and drop-coating, the electrodes demonstrated low overpotentials of 71 mV@25 mA cm-2 (HER) and 77 mV@25 mA cm-2 (CER). When applied in a two-electrode H-cell system, faradaic efficiencies of 99.14% (HER) and 98% (CER) were achieved at a current density of 25 mA cm-2, while 30 mL of iodine solution (66.25 mmol L-1) was obtained within 5 hours for extensive sterilization (5 types of bacteria). As antibacterial electrodes, in situ generated active chlorine enabled 100% inactivation of Staphylococcus aureus within 30 minutes. The porous structure, good hydrophilicity and mechanical flexibility of the electrodes enhanced electrolyte penetration, catalytic activity and wearability. This study provides a high-performance flexible electrode for acidic NaCl electrolysis, reducing energy consumption while broadening applications in hydrogen/chlorine production and antibacterial applications.

The development of aqueous Zn metal batteries (AZMBs) as a promising energy storage device has been hindered by dendrite growth and parasitic reactions. Here, the potential of a low-cost additive, maltodextrin (MD), to enhance the performance of AZMBs by modulating the typical 2 M ZnSO4 electrolyte is explored. Through a combination of experimental characterizations and theoretical calculations, it has been demonstrated that, MD exhibits a stronger propensity to absorb on Zn (002), Zn (100) and Zn (101) planes compared to H2O, thereby suppressing side reactions induced by active H2O molecules. Concomitantly, MD additive has been shown to be capable of weakening the interaction between Zn2+ and H2O, thereby accelerating the de-solvation process of Zn2+-solvation structure at Zn anode/electrolyte interface. As a proof of concept, Zn||Zn symmetric batteries, Zn||Cu asymmetric batteries and Zn||NVO full batteries with 2 M ZnSO4 + 8% MD electrolyte have been shown to achieve enhanced stability in comparison with those utilizing 2 M ZnSO4 electrolyte.

Alkaline water electrolysis (AWE) plays a leading role in green hydrogen production due to its scalability and cost-effectiveness, but suffers from low current density and gas-crossover issues. This study demonstrates substantial progress in AWE performances through synergistic membrane-electrode optimization. Zirconiapolysulfone (Z-PSU) and zirconia-polyethersulfone (Z-PESf) membranes were prepared using a phase-inversion casting method. The Z-PSU composite membrane exhibits exceptional thermal stability and chemical durability, outperforming Z-PESf. Controlled in-situ growth of Ni(OH)(2) via hydrothermal treatment enhances membrane performance, achieving a 33 % increase in bubble point pressure (3.53 bar), 48 % reduction in contact angle (48.7 degrees), while maintaining low area resistance (0.23 Omega cm(2)). When integrated with a Raney Ni cathode and nickel-deposited stainless-steel anode, the cell delivers 2.25 A cm(-2) at 2 V in 80 degrees C@30 wt% KOH electrolyte. This membrane-electrode co-design strategy establishes an effective approach for industrial-scale green hydrogen production, combining robust material durability with high catalytic efficiency.

Traditional photocatalytic systems often face significant challenges in nanocatalyst recovery from aqueous solutions, hindering their practical implementation in industrial-scale wastewater remediation. In this study, graphitic carbon nitride (g-C3N4) metal-free heterostructure film was spontaneously coassembled at the gas-liquid interface, with a uniform film structure of g-C3N4, well-stacked graphene oxide, and hexagonal boron nitride over centimeters in size. The van der Waals heterostructure film exhibits excellent photocatalytic performance behavior and broadband photoperception from 450 to 550 nm. Moreover, the optimized reaction rate of the film is 7.2 times higher than that of the pure g-C3N4 powder control system. Under visible light irradiation, the film achieves ca. 92% degradation rate for RhB and exhibits a degradation efficiency of up to 76% for 2,4-DCP. The robust structural integrity maintained during prolonged cycling tests, coupled with its efficient solar-driven and charge carrier dynamics performance, renders this thin-film architecture particularly promising for industrial-scale implementation through incorporation into fixed-bed photocatalytic reactor systems.

Lithium-sulfur batteries due to high theoretical specific capacity and quality of energy density, low-cost advantages are thought to be most likely to next-generation lithium-ion batteries for its production, but its development is shuttle effect, reaction kinetics hysteresis problems such as serious obstacles, the study found that for a moderate amount of polysulfide adsorption and fast catalytic conversion is the key to improve the battery performance. Herein, we synthesized a modified lithium sulfur battery separator for high entropy oxidesy((FeCoNiCrMn)(3)O-4). The synergistic effect between multiple active sites and multi-components of (FeCoNiCrMn)(3)O-4 can strong anchor and catalytic ability for polysulfides, thus can improve the utilization efficiency of sulfur. As (FeCoNiCrMn)(3)O-4 was utilized to modify the separators, the resulting Li-S battery showed an excellent battery performance.

Hydrogen-transporting membrane reactors play active roles in ammonia (NH3) 3 ) decomposition and carbon dioxide (CO2) 2 ) reduction by combining reaction and separation in one unit, simplifying the processes and reactor design and therefore saving the cost. These important reactions normally occur at high temperatures and in reducing and acidic atmosphere, thus posing great challenges on the membrane stability. Previous effort was devoted to thin Pd membranes, which however, suffer the shortcomings of hydrogen embrittlement, CO poisoning and high costs. Herein, we develop a H2-COx-tolerant 2-CO x-tolerant and non-noble metal-ceramic dual-phase hydrogen permeable membrane reactors with a nominal composition of 60 vol% Ni-40 vol% La 5.5 WO 11.25-delta (Ni-LWO). NH3 3 decomposition and hydrogen permeation was observed via the developed mixed protonic and electronic conducting membrane. A considerable production of CO in the sweep (CO2) 2 ) side could also be achieved from CO2 2 reduction when the membrane was coupled by NH3 3 decomposition where the permeated hydrogen can consume the produced oxygen from favorable CO2 2 decomposition. Furthermore, we systematically investigated the performance of NiO-CeO2 2 catalyst coated Ni-LWO membrane reactor for CO2 2 reduction. Noteworthy that the CO generation rate obtained from Ni-LWO membrane reactor was increased in the presence of NiO-CeO2 2 catalysts. Hydrogen separation process coupled with surface reactions is jointly controlled by hydrogen surface exchange and bulk diffusion kinetics. These findings reveal a vital step towards the development of efficient hydrogen-transporting membrane reactor for the integration of chemical reactions and separation processes.

Nitrous oxide (N2O) emissions sourced from agricultural and industrial activities have gained much attention because of their contribution to the global greenhouse effect and ozone layer depletion. Significant efforts have been devoted to developing the cost-effective and highly efficient technologies for N2O removal. The direct N2O decomposition is limited by the thermodynamic equilibrium at high temperatures. Recently, catalytic reduction of N2O with carbon-free hydrogen derived from in situ ammonia decomposition is considered as an ideal approach. Herein, thermal decomposition of N2O is investigated by employing a BaCe0.85Fe0.15O3-delta-BaCe0.15Fe0.85O3-delta (BCF8515-BCF1585) hydrogen-transporting membrane or a Ce0.85Sm0.15O1.925-Sm0.6Sr0.4FeO3-delta (SDCSSF) oxygen-transporting membrane respectively. It is noted that the membrane catalysis of N2O decomposition by reacting with permeated hydrogen or via in-situ oxygen removal displayed significant advantages over the direct thermal decomposition of N2O under a fixed bed condition. Moreover, the N2O conversion as well as hydrogen/oxygen permeability of such membranes were greatly improved by the introduction of porous Ni-CeO2 or SDC-NCO layers due to the increased catalytic activities and hydrogen/oxygen surface exchange kinetics.

The architecture of anode materials is an essential factor in improving the performance of energy storage devices, which meets the increasing demand for energy storage and helps achieve environmental sustainability targets. Atomic manufacturing allows the makeup of electrodes to be changed precisely at the atomic level. This facilitates the creation of electrode materials with specific physical properties and enhanced performance. This Perspective reviews the details of how the microstructure design influences key electrode material characteristics. Finally, we anticipate the potential of materials and manufacturing techniques for materials microstructure in the future. A thorough grasp of the materials microstructure in electrode materials is offered by this article.

Surface-enhanced Raman spectroscopy (SERS), well acknowledged as a fingerprinting and sensitive analytical technique, has exerted high applicational value in a broad range of fields including biomedicine, environmental protection, food safety among the others. In the endless pursuit of ever-sensitive, robust, and comprehensive sensing and imaging, advancements keep emerging in the whole pipeline of SERS, from the design of SERS substrates and reporter molecules, synthetic route planning, instrument refinement, to data preprocessing and analysis methods. Artificial intelligence (AI), which is created to imitate and eventually exceed human behaviors, has exhibited its power in learning high-level representations and recognizing complicated patterns with exceptional automaticity. Therefore, facing up with the intertwining influential factors and explosive data size, AI has been increasingly leveraged in all the above-mentioned aspects in SERS, presenting elite efficiency in accelerating systematic optimization and deepening understanding about the fundamental physics and spectral data, which far transcends human labors and conventional computations. In this review, the recent progresses in SERS are summarized through the integration of AI, and new insights of the challenges and perspectives are provided in aim to better gear SERS toward the fast track.

The Ag/h-BN/Bi2O3 ternary composite was facilely fabricated via self-assembly combined with in situ reduction. Characterization results showed that the as-prepared Ag/h-BN/Bi2O3 possessed distinct surface plasma resonance (SPR) and Mott-Schottky heterostructure, resulting in significant enhancement of catalytic activity for RhB removal, the reaction rate constant (2.26x 10 (2) min 1) is 2.5 times that of h-BN/Bi2O3 under visible-light irradiation for 2 hours, which was mainly ascribed to the SPR and Mott-Schottky heterostructure result in Ag/h-BN/Bi2O3 enhanced visible-light harvesting capacity and the effectual spatial separation of photoinduced carriers. The quenching process of reactive species indicated that h(+) and *O-2 play dominant role in the degradation for pollutants. This work demonstrates that Ag/h-BN/Bi2O3 is a promising stability photocatalyst for water purification.

Ammonia（NH 3 ） decomposition to release CO x -free hydrogen（H 2 ） over non-noble catalysts has gained increasing attention.In this study,three nanostructured CeO 2 with different morphologies,viz.rod（R）.sphere（Sph）,and spindle（Spi）,were fabricated and served as supports for Ni/CeO 2 catalyst.The CeO 2 supports are different in particle sizes,specific surface area and porosity,resulting in the formation of Ni nanoparticles with distinguished sizes and dispersions.The surface properties of the Ni/CeO 2 catalysts are not only distinct but also influential,affecting the adsorption and desorption of NH 3 ,N 2 ,and/or H 2 molecules.The Ni/CeO 2 -R catalyst shows superior catalytic activity compared to the other two,owing to its smaller Ni crystallite size and larger BET surface area.The most abundant strong basic sites are observed for Ni/CeO 2 -Spi catalyst based on its exposed CeO 2 （110） planes,which facilitates the donation of electrons to the Ni particles,benefiting the associative desorption of N atoms.Thus,Ni/CeO 2 -Spi shows higher catalytic activity than Ni/CeO 2 -Sph,despite their almost identical Ni crystallite sizes.

In this study, we prepared SrR2O4+δ (SRO, R=Y, Yb, Gd, Sm) of brownmillerite structure. Among the four n-type SRO semiconductors, SYO is the most negative in conduction band and the smallest in band gap. As a result, the SYO-based SOFC can offer a maximum power density (MPD) of 1.03W/cm-2 at 800°C, which is higher than that based on the other three SRO oxides. The introduction of larger Sr2+ at the B sites of Sr1+xY2-xO4+δ [SYO(x)] causes decrease of band gap, resulting in a 4-fold increase of electronic conductivity. The foreign Sr2+ creates surface oxygen vacancies to boost interfacial transport. The measurement of oxygen transport reveals that SYO(0.10) exhibits a bulk diffusion coefficient 500 folds higher than that of LSM. An anode supported Ni-YSZ|YSZ|SYO(0.10)-60YSZ DA-SOFC yields an MPD of 0.24W/cm2 at 600°C and 1.21 W/cm2 at 800°C with remarkable stability, about 1.73- and 1.29-folds higher than that of LSM-based SOFC, respectively.

In this study, pyrochlore Pr2B2O7 oxides (B--Zr, ZrSn, Sn, PZO/PZSO/PSO) and perovskite (B--Ti, PTO) were prepared as direct ammonia solid oxide fuel cell (DA-SOFC) cathode with oxygen reduction reaction activity induced by B-site cationic defects. Compared with PTO, the pyrochlore PBO with unoccupied 8a-oxygen sites are high in inherent oxygen vacancies (ca. 12.5%), leading to enhanced migration of lattice oxygen. Among the ntype semiconductors, PZO is with a more negative flat-band potential and is more effective in terms of overcoming energy barriers. As a result, the conductivity of PZO is two orders of magnitude higher than that of PTO at 800 degrees C. The oxygen transport performance reveals that the surface exchange coefficient of PZO is about one order of magnitude higher than that of La0.7Sr0.3MnO3-delta at 900 degrees C. Owing to high conductivity, fast oxygen transport, and matched thermal expansion coefficient, an anode-supported DA-SOFC using the PZO-based cathode can offer a maximum power density of 0.25 W cm-2 at 600 degrees C and 1.22 W cm-2 at 800 degrees C, operating continuously over 100 h without obvious degradation. The electrochemical performance is 2.3 folds higher than those of SOFCs using other PBO-based cathode, and higher than most reported SOFCs with the cathodes using A-site Pr.

With high energy density both by weight and volume, ammonia (NH3) is a promising hydrogen carrier. Furthemore, NH3 has a mature industrial background, and in liquid form storage and transportation is not a problem. Adding the merit of zero CO2 emission, NH3-to-power by direct ammonia solid oxide fuel cells (DA-SOFCs) is an acceptable strategy to facilitate hydrogen usage. Nonetheless, to achieve efficacy, a high compatibility between operating temperature and catalytic materials for NH3 decomposition is needed. In this work, we developed a tubular DA-SOFC with an output power capability of > 3 W. By combining experimental measurements and multi-physics simulation, we comprehensively studies the related intrinsic processes. Based on experimental data, we developed a two-dimensional multi-scale electro-thermo model of tubular DA-SOFC. Separately we evaluated the effects of inlet fuel gas composition, inlet flow velocity, operating temperature, and operating voltage on the rate of NH3 catalytic decomposition and H-2 electrochemical oxidation, as well as on NH3 conversion, H atom utilization, and electrical efficiency of the tubular DA-SOFC. The results suggest that high H atom utilization could be realized by matching the rate of NH3 decomposition with that of H-2 electrochemical oxidation. It was observed that with the decrease of temperature, the rate of H-2 oxidation decreases more rapidly than that of NH3 decomposition, suggesting that the flow velocity of NH3 should be appropriately lowered to optimize H atom utilization. Finally, we established a correlation between H atom utilization, operating voltage, and electrical efficiency for synergistic optimization of operating conditions. At 0.7 V and 800 celcius, the tubular DA-SOFC fueled with NH3 of 27 mL.min(-1) is capable of offering 3.2 W, displaying an efficiency of 60%. Compared to that of a tubular H-2-SOFC (only 51% efficiency), the efficiency is significantly higher on the basis of equal voltage and fuel utilization ratio. The outcome of the present study demonstrates the potential of tubular DA-SOFC as a device for high-efficiency power generation.

Ammonia has been considered as a promising hydrogen carrier with high energy storage density and easy transport. Here, we report the ruthenium (Ru) nanoparticles supported on LaAlO3, a typical ABO3 perovskite oxide, as an efficient catalyst for ammonia decomposition. By tailoring the cation substitution of La3+ by Sr2+, the electronic properties of support materials were modulated, which exerts an impact on the electronic state of Ru active sites. It is found that the Ru/La0.8Sr0.2AlO3 catalyst has a high hydrogen formation rate and low activation energy. In situ spectroscopic investigation and NH3 temperature programmed desorption (NH3-TPD) analyses indicate the electron-rich state of metallic Ru on the La0.8Sr0.2AlO3 support, which promotes associative desorption of N atoms and accelerates NH3 decomposition reactions. This study provides a universal strategy of aliovalent cation substitution to engineer the electronic properties of metal/oxide catalysts as well as their catalytic activities. (c) 2022 Elsevier Ltd. All rights reserved.

Cognizing the structural characteristics of a heterointerface is significant to understand the growth mechanism of heterostructured nanowires. Here, the structural characteristics of a heterointerface in GaAs-GaAsSb heterostructured nanowires were investigated by employing spherical aberration (C-S)-corrected transmission electron microscopy (TEM). It is found that some unusual dislocations are formed at the heterointerface, leading to the bending of nanowires. Further, the atomically inhomogeneous distribution of Sb content near the heterointerface is revealed, which is responsible for the formation of dislocations. By applying a thermal electric system equipped in the Cs-corrected TEM, a direct observation of structural evolution at the heterointerface was enabled and the stability of GaAs-GaAsSb heterostructured nanowires was evaluated. In situ high-resolution TEM imaging indicates that the destabilization of the heterointerface occurs during nanowire annealing. This study builds a direct correlation between the nanowire heterointerfacial structure with nanowire growth behavior and its stability, which is of importance for heterostructured nanowire design for practical use.