Phase and Orbital Engineering Effectuating Efficient Adsorption and Catalysis toward High-Energy Lithium-Sulfur Batteries.

The delicate construction of electrocatalysts with high catalytic activity is a strategic method to enhance the kinetics of lithium-sulfur batteries (LSBs). Adjusting the local structure of the catalyst is always crucial for understanding the structure-activity relationship between atomic structure and catalyst performance. Here, in situ induction of electron-deficient B enables phase engineering MoC, realizing the transition from hexagonal (h-MoC) to cubic phase (c-B-MoC).

Exploring interfacial electrocatalysis for iodine redox conversion in zinc-iodine battery.

The challenges posed by the non-conductive nature of iodine, coupled with the easy formation of soluble polyiodides in water, impede its integration with zinc for the development of advanced rechargeable batteries. Here we demonstrate the in-situ loading of molybdenum carbide nanoclusters (MoC) and zinc single atoms (Zn-SA) into porous carbon fibers to invoke electrocatalytic conversion of iodine at the interface. The electronic interactions between MoC and Zn-SA lead to an upshift in the d-band center of Mo relative to the Fermi level, thus promoting the interfacial interactions with iodine species to suppress shuttle effects.

Alloying Strategy Regulating Size and Electronic Structure of MoNbSe to Achieve High-Performance Lithium-Sulfur Batteries.

The utilization of catalysts in lithium--sulfur batteries has proven to be an efficacious avenue for enhancing the kinetics of polysulfide conversion. Specially, the size and electronic structure of catalysts play a pivotal role in harnessing the active sites and intrinsic catalysis activity. Outstanding MoSe and NbSe are were selected from 16 universal transition metal selenides based on the proposed binary descriptor.

Interfacial coupling of Ce-CoSe nanoneedle arrays with MXene for efficient overall water splitting.

Designing highly effective, low-cost bifunctional electrocatalysts without noble metals for overall water splitting remains a significant challenge. In this work, interfacial coupling of Ce-doped CoSe nanoneedle arrays with MXene (Ce-CoSe/MXene) is developed via the facile hydrothermal and selenization methods. The extensive specific surface area and favorable hydrophilicity of TiAlC, combined with the optimized electronic structure and abundant active sites from Ce-doping and selenization, contribute to the exceptional bifunctional electrocatalytic performance of the Ce-CoSe/MXene electrode.

Spatial Structure of Electron Interactions in High-entropy Oxide Nanoparticles for Active Electrocatalysis of Carbon Dioxide Reduction.

High-entropy oxides (HEOs) exhibit distinctive catalytic properties owing to their diverse elemental compositions, garnering considerable attention across various applications. However, the preparation of HEO nanoparticles with different spatial structures remains challenging due to their inherent structural instability. Herein, ultrasmall high-entropy oxide nanoparticles (less than 5 nm) with different spatial structures are synthesized on carbon supports via the rapid thermal shock treatment.

Molten-salt-assisted preparation of porous carbon foams for efficient oxygen electrocatalysis in zinc-air batteries.

To enhance the reversible electrolytic conversion of oxygen in zinc-air batteries, a molten-salt-assisted method was demonstrated to synthesize highly porous carbon foams with anchoring of metal sites. These electrocatalysts improved the electrolysis for oxygen reduction and evolution reactions, thus leading to the fabrication of advanced zinc-air batteries.

Thermal-Driven Dispersion of Bismuth Nanoparticles among Carbon Matrix for Efficient Carbon Dioxide Reduction.

The poor electrocatalytic stability and rapid deactivation of metal electrocatalysts are always present in the electrocatalytic conversion of carbon dioxide (CO) due to the harsh reduction condition. Herein, we demonstrate the controllable dispersion of ultrafine bismuth nanoparticles among the hollow carbon shell (Bi@C-700-4) simply by a thermal-driven diffusion process. The confinement effect of nitrogen-doped carbon matrix is able to low the surface energy of bismuth nanoparticles against the easy aggregation commonly observed for the thermal treatment.

Bimetal-bridging Nitrogen Coordination in Carbon-based Electrocatalysts for pH-universal Oxygen Reduction.

Electrocatalysts with atomically dispersed metal sites (e.g., metal-nitrogen-carbon) have been deemed as promising alternatives for noble-metal catalysts in couples of electrocatalytic reactions.

Strong p-d Orbital Hybridization on Bismuth Nanosheets for High Performing CO Electroreduction.

Single-atom alloys (SAAs) show great potential for a variety of electrocatalytic reactions. However, the atomic orbital hybridization effect of SAAs on the electrochemical reactions is unclear yet. Herein, the in situ confinement of vanadium/molybdenum/tungsten atoms on bismuth nanosheet is shown to create SAAs with rich grain boundaries, respectively.

Bionic Mineralization toward Scalable MOF Films for Ampere-Level Biomass Upgrading.

With significant advances in metal-organic framework (MOF) nanostructure preparation, however, the facile synthesis of large-scale MOF films with precise control of the interface structure and surface chemistry is still challenging to achieve with satisfactory performance. Herein, we introduce a universal strategy bridging metal corrosion chemistry and bionic mineralization to synthesize 16 MOF films on 7 metal supports under ambient conditions. The robustness to explore unlimited libraries of MOF films (e.

Coordination modulation of hydrated zinc ions to enhance redox reversibility of zinc batteries.

The dendrite growth of zinc and the side reactions including hydrogen evolution often degrade performances of zinc-based batteries. These issues are closely related to the desolvation process of hydrated zinc ions. Here we show that the efficient regulation on the solvation structure and chemical properties of hydrated zinc ions can be achieved by adjusting the coordination micro-environment with zinc phenolsulfonate and tetrabutylammonium 4-toluenesulfonate as a family of electrolytes.

Atomic bismuth induced ensemble sites with indium towards highly efficient and stable electrocatalytic reduction of carbon dioxide.

Structural reconstruction is commonly observed during electrocatalytic CO reduction (CORR) process. However, the proper modulation of interface and defect sites remains challenging with the mechanism understanding to realize the favorable electrocatalysis. Herein, the atomic bridging of bismuth with indium atoms is elaborately designed for improving electrocatalysis of CORR via electrochemical reduction and in situ anchoring strategy.

Physicochemical Confinement Effect Enables High-Performing Zinc-Iodine Batteries.

Zinc-iodine batteries are promising energy storage devices with the unique features of aqueous electrolytes and safer zinc. However, their performances are still limited by the polyiodide shuttle and the unclear redox mechanism of iodine species. Herein, a single iron atom was embedded in porous carbon with the atomic bridging structure of metal-nitrogen-carbon to not only enhance the confinement effect but also invoke the electrocatalytic redox conversion of iodine, thereby enabling the large capacity and good cycling stability of the zinc-iodine battery.

Microsized Gray Tin as a High-Rate and Long-Life Anode Material for Advanced Sodium-Ion Batteries.

Sodium-ion batteries (SIBs) are developed to address the serious concern about the limited resources of lithium. To achieve high energy density, anode materials with a large specific capacity and a low operation voltage are highly desirable. Herein, microsized particles of gray Sn (α-Sn) are explored as an anode material of SIBs for the first time.

Interface Molecular Functionalization of CuO for Synchronous Electrocatalytic Generation of Formate.

The electrocatalytic generation of valuable fuels and chemicals from carbon dioxide (CO) and others with the assistance of clean solar energy is a highly promising way to realize the carbon-neutral cycle, which invokes the systematic development of advanced electrocatalysts for efficient and selective redox reactions of feedstocks. Herein, we demonstrate the interface modification of cuprous oxide with polyvinylpyrrolidone (PVP) to improve the electrocatalytic efficiency for the synchronous formate generation. Density functional theory calculations reveal that the interfacial properties can be effectively regulated by the PVP functionalization for the favorable formation of intermediates to improve the selectivity of formate generation.

Interface Coordination Stabilizing Reversible Redox of Zinc for High-Performance Zinc-Iodine Batteries.

Aqueous Zn batteries (AZBs) have attracted extensive attention due to good safety, cost-effectiveness, and environmental benignity. However, the sluggish kinetics of divalent zinc ion and the growth of Zn dendrites severely deteriorate the cycling stability and specific capacity. The authors demonstrate modulation of the interfacial redox process of zinc via the dynamic coordination chemistry of phytic acid with zinc ions.

Atomic Bridging Structure of Nickel-Nitrogen-Carbon for Highly Efficient Electrocatalytic Reduction of CO.

To meet strategic applications, electrochemical reduction of CO into value-added chemical molecules would be improved by the rational design of advanced electrocatalysts with atomically dispersed active sites. Herein an electrospun-pyrolysis cooperative strategy is presented to not only modulate the porous structure of the carbon support for favorable charge and mass transfer, but also adjust the bridging structure of atomically dispersed metal species. Typically, the experimental results and theoretical calculations revealed that the unique chemical structure of binuclear nickel bridging with nitrogen and carbon atoms (namely Ni -N -C ) tunes the electronic nature of the d-states for the optimal adsorption of carbon dioxide and intermediates, thus inducing the substantial enhancement of CO reduction via the thermodynamically more favorable pathway.

Iodine Redox Chemistry in Rechargeable Batteries.

Halogens have been coupled with metal anodes in a single cell to develop novel rechargeable batteries based on extrinsic redox reactions. Since the commercial introduction of lithium-iodine batteries in 1972, they have shown great potential to match the high-rate performance, large energy density, and good safety of advanced batteries. With the development of metal anodes (e.

Preparation of Hierarchical Cube-on-plate Metal Phosphides as Bifunctional Electrocatalysts for Overall Water Splitting.

To rationally design efficient and cost-effective electrocatalysts, a simple but efficient strategy has been developed to directly anchor prussian blue analogue (PBA) nanocubes on cobalt hydroxide nanoplates (PBA@Co(OH) ) via the in-situ interfacial precipitation process. Subsequently, the thermal treatment in the presence of sodium hydrogen phosphite enabled the successful transition into metal phosphides with the hierarchical cube-on-plate structure. When used as electrocatalytsts, the obtained bimetal phosphides exhibited good bifunctional electrocatalytic activities for hydrogen and oxygen evolution reactions with good long-term stability.

A 3D and Stable Lithium Anode for High-Performance Lithium-Iodine Batteries.

Lithium metal is considered as the most promising anode material due to its high theoretical specific capacity and the low electrochemical reduction potential. However, severe dendrite problems have to be addressed for fabricating stable and rechargeable batteries (e.g.

A rechargeable iodine-carbon battery that exploits ion intercalation and iodine redox chemistry.

Graphitic carbons have been used as conductive supports for developing rechargeable batteries. However, the classic ion intercalation in graphitic carbon has yet to be coupled with extrinsic redox reactions to develop rechargeable batteries. Herein, we demonstrate the preparation of a free-standing, flexible nitrogen and phosphorus co-doped hierarchically porous graphitic carbon for iodine loading by pyrolysis of polyaniline coated cellulose wiper.

Cation Intercalation in Manganese Oxide Nanosheets: Effects on Lithium and Sodium Storage.

The rapid development of advanced energy-storage devices requires significant improvements of the electrode performance and a detailed understanding of the fundamental energy-storage processes. In this work, the self-assembly of two-dimensional manganese oxide nanosheets with various metal cations is introduced as a general and effective method for the incorporation of different guest cations and the formation of sandwich structures with tunable interlayer distances, leading to the formation of 3D Mx MnO2 (M=Li, Na, K, Co, and Mg) cathodes. For sodium and lithium storage, these electrode materials exhibited different capacities and cycling stabilities.

Silver-modified mesoporous TiO2 photocatalyst for water purification.

Mesoporous anatase (TiO(2)) was modified with silver (Ag) nanoparticles using a photoreduction method. Performance of the resulting TiO(2)-Ag nanocomposites for water purification was evaluated using degradation of Rhodamine B (RhB) and disinfection of Escherichia coli (E. coli) under ultraviolet (UV) irradiation.

Photocatalytic degradation of dyes over graphene-gold nanocomposites under visible light irradiation.

Graphene modified with gold nanoparticles displayed an excellent visible-light photocatalytic performance in degrading dyes in water.