Single Atom-Substituted Chalcogenides with Anion Vacancy Bonded on Graphene Nanotubes for Achieving "1+1+1>3" Synergistic Enhanced Sodium Storage.

Developing distinctive composite anodes with multiple active components is critical for enhancing the charge storage capability of sodium-ion hybrid capacitors (SIHCs). Herein, In single atom-substituted SnS with moderate sulfur vacancies in situ bonded on N-doped graphene nanotubes (In─SnS@NG) is ingeniously engineered as a superior anode. Theoretical calculations and in situ/ex situ characterizations illustrate that the introduced Sn(In)─N interfacial bonds immensely strengthen composites integration and boost charge transfer, then In single atom substitution effectively elevates d band center and enhances Na adsorption.

Corrosion-Regulated Surface Reconstruction for High-Performance Oxygen Evolution Electrocatalysts.

Surface reconstruction is a common phenomenon during electrode processes, occurring on the surface of electrocatalysts. While corrosion-engineering approaches show promise in this reconstruction, the precise control of surface reaction kinetics remains a significant challenge. In this work, a corrosion kinetics-controlled strategy using a hypophosphite corrosion inhibitor was proposed to achieve a uniform nickel-iron oxyhydroxide (p-(Fe,Ni)OOH) layer through controlled corrosion-induced reconstruction.

Sulfur form regulation and dual-interface effect: catalytic mechanism of nickel-based catalyst in ethanol electrooxidation.

Electrocatalytic organic oxidation emerge as energy-efficient alternatives to conventional oxygen evolution reactions (OER) for sustainable hydrogen coproduction. The design of efficient catalysts and the understanding of the underlying mechanisms of anodic nucleophilic reagent electrooxidation constitute the core of electrochemistry-driven technological advances. Herein, this paper reports a nickel sulfide heterostructure embedded in biomass carbon (NiS-NiS/CC), which exhibits great ethanol oxidation reaction (EOR) activity with a current density of 50 mA·cm at 1.

Continuous Encodable Reshaping of Gold Nanocrystals through Facet Modulation.

Shape control of nanocrystals (NCs) is crucial for tuning their assembly behavior and functional properties, yet the precise manipulation of facet composition remains challenging. Here, we present a nanocrystal reshaping strategy to control and modulate the facets of gold (Au) NCs. Our one-pot approach, conducted at room temperature, requires only initial Au NCs, Au ions, and surfactants, distinguishing it from conventional reduction-mediated "etching-and-regrowth" methods.

Bioinspired Sulfo oxygen bridges optimize interfacial water structure for enhanced hydrogen oxidation and evolution reactions.

Uncovering the dynamic structures of water at the electrode-solution interface is crucial for various electrocatalysis processes, where water acts as a proton and electron source. However, precisely controlling the state of water on complex interfaces remains challenging. Inspired by the metalloproteins in natural enzymes, we herein demonstrate that the hydrophilic sulfo-oxygen bridging between Co and Ru sites (Co-SO-Ru) optimizes interfacial water structure via a favorable hydrogen-bond network, promoting hydrogen oxidation and evolution reactions.

Selective Sieving Effect of Multi-Atomic Bismuth Interfaces for Efficient Formate Electrosynthesis and Evolution at Industrial Current Density.

Constructing multi-atomic interfaces architectures is promising for electrocatalytic CO conversion, yet their synthesis and stability under industrial current densities remain challenging. Herein, multi-atomic Bi interfaces (Bi/Bi-O moiety) were precisely engineered by embedding atomically dispersed Bi centers, encompassing Bi single atoms and Bi atomic clusters into the substrate of porous BiO nanosheets. The composite showcases outstanding CO conversion performance across a wide pH range, attaining remarkable Faradaic efficiency for formate (FE) of 96.

Atomic-Level Design of Acid-Base Pairs in Oxides for Selective Catalytic Reduction of Nitrogen Oxides with Ammonia.

Selective catalytic reduction of nitrogen oxides (NO) with NH (NH-SCR) poses considerable potential in the abatement of NO emissions. However, the efficient adsorption and speedy reaction of reactants following the specific mechanism in a favorable way is still a challenge for enhancing catalysis. Herein, we propose the strategy aimed at adjusting electronic properties of Ce-O-W acid-base pairs through constructing oxygen vacancies on Ce/WO, thereby fostering SCR activity.

An Artificial Peroxynitrite-Resistant Superoxide Dismutase for Acute Kidney Injury Alleviation.

Manganese superoxide dismutase (Mn-SOD) is the most common natural antioxidant enzyme that defends cells against oxidative stress. However, it is intrinsically vulnerable to nitration by peroxynitrite (ONOO) to result in accumulation of reactive oxygen species and inducement of acute kidney injury (AKI). Designing Mn-SOD mimics that are both active and resistant to ONOO is essential for advancing artificial enzymes and broadening the application of enzymatic catalytic therapies.

MXene-Supported Ru-Ni: A Common Active Site for Hydrolysis, Hydrogen Oxidation, and Hydrogenation.

Insights into the activation and conversion of hydrogen using a single-mode catalyst are crucial for advancing fuels and fine chemical production. In this paper, the activation and conversion of H molecules in hydrogen production and application were investigated on RuM (M = Ni, Co, Cu, Fe)-MXene catalysts. RuM (M = Ni, Co, Cu, Fe) bimetallic nanoclusters were uniformly distributed on TiC MXene.

Deciphering the N─N Coupling Mechanism Over Iron-Copper Alloy Catalysts During Ammonia Decomposition.

The production of CO-free hydrogen via the ammonia decomposition reaction (ADR) using Fe-based non-precious metal catalysts has attracted much attention. N─H bond cleavage and N─N coupling are two key steps in ADR, however, stronger Fe─N binding leads to lower activity of iron catalysts. Herein, we develop FeCu alloy catalysts with optimized metal-nitrogen binding energy by incorporating Cu, a metal with inherently weaker nitrogen affinity, into Fe-based catalysts.

Engineering Spatial Interface in Supported Molecular Complexes for Ampere-Level Electrocatalytic Oxygen Evolution.

Homogenized molecular complexes with active single sites hold great promise for electrocatalytic conversion processes. However, the influence of the spatial gap between coordination complexes and the carbon support on electron shuttling remains poorly understood. Herein, we demonstrate a supramolecular architectural strategy that leverages oxygen sites to strengthen the complex-support interactions, thereby elucidating the oxygen evolution reaction (OER) catalytic mechanism effected by the spatial gap.

Magnetic-Field-Induced Spin Transition in Single-Atom Catalysts for Nitrate Electrolysis to Ammonia.

Electrochemical nitrate reduction (NitRR) using single-atom catalysts (SACs) offers a promising pathway for sustainable ammonia production. Herein, we explore the use of external magnetic fields to regulate the spin state of Ru SACs supported on nitrogen-doped carbon (Ru-N-C), aiming to optimize their catalytic performance toward NitRR. Under magnetic field conditions, Ru-N-C exhibits a remarkable NH yield rate of ∼38 mg L h and a Faradaic efficiency of ∼95% over 200 h.

Site-Specific Spin State Modulation in Spinel Oxides for Enhanced Nonradical Oxidation.

Spinel oxides hold tremendous potential for driving advanced oxidation processes, yet the underlying mechanism for maximizing their activity remains unclear. In this study, we leverage tetrahedral and octahedral site interactions in MnCoO to modulate the spin states, specifically spin alignment and spin moment, thereby enhancing periodate (PI) activation and catalytic performance in contaminant degradation. Through combined experimental and density functional theory (DFT) analyses, we elucidate the role of spin alignment at synergetic tetrahedral and octahedral sites in facilitating quantum spin exchange interactions (QSEI) with an efficient electronic spin channel for charge transfer.

High-Entropy Environments Enable Metal Surface-Catalyzed Nucleophilic Electrooxidation.

Electrochemical biomass conversion offers a sustainable route to diverse products, minimizing environmental impact. However, conventional 5-hydroxymethylfurfural electrooxidation (HMFOR) catalysts such as Ni(OH)₂ and NiS suffer from low conductivity, poor stability, and limited active sites. This work introduces a CoNiMnMoPd high entropy alloy (HEA) to address these limitations by simultaneously maintaining high conductivity, stability, and a high Ni oxidation state, enabling nucleophilic dehydrogenation.

Phosphorus-Doped Single Atom Copper Catalyst as a Redox Mediator in the Cathodic Reduction of Quinazolinones.

The use of clean electric energy to activate inert compounds has garnered significant attention. Homogeneous redox mediators (RMs) in organic electrosynthesis are effective platforms for this purpose. However, understanding the RM's electronic structure under operational conditions, electron transport processes at the electrode surface, and substrate adsorption-desorption dynamics remains challenging.

The Cooperative Effects of the Rh-M Dual-Metal Atomic Pairs in Formic Acid Oxidation.

The continuously increasing mass activity of precious metal in formic acid oxidation reaction (FAOR) is the key to achieving the practical application of direct formic acid fuel cells (DFAFCs). Herein, Rh-based dual-metal atomic pairs supported on nitrogen-doped carbon catalysts [DAP-(M, Rh)/CN] with adjacent interatomic Rh-M (M = V, Cr, Mn, Fe, Co, Ni, Cu) have been synthesized by a "host-guest" strategy. It is discovered that DAP-(Cr, Rh)/CN shows the highest mass activity of 64.

Atomic Symbiotic-Catalyst for Low-Temperature Zinc-Air Battery.

Atomic-level designed electrocatalysts, including single-/dual-atom catalysts, have attracted extensive interests due to their maximized atom utilization efficiency and increased activity. Herein, a new electrocatalyst system termed as "atomic symbiotic-catalyst", that marries the advantages of typical single-/dual-atom catalysts while addressing their respective weaknesses, was proposed. In atomic symbiotic-catalyst, single-atom MN and local carbon defects formed under a specific thermodynamic condition, act synergistically to achieve high electrocatalytic activity and battery efficiency.

Efficient Generation of Negative Hydrogen with Bimetallic-Ternary-Structured Catalysts for Nitrobenzene Hydrogenation.

Transition metal-catalyzed transfer hydrogenation (TH) with in situ negative hydrogen (H) has received extensive attention as an alternative to conventional high-pressure hydrogenation processes. However, the insufficient activity of hydrogen production and unclear the conversion process of hydrogenation remain a great challenge. In this work, brand new bimetallic ternary-structured catalysts (RuM-TiO, M=Co, Cu, Fe, Ni) were synthesized to efficiently generate H donors from ammonia borane (AB, NHBH) for nitrobenzene hydrogenation under moderate conditions.

Co Nanoparticle: An Efficient H-pump for Pt Single Atoms Towards Enhanced Hydrogen Spillover.

Introducing OH-interaction sites to accelerate water dissociation can increase hydrogen coverage on active site surfaces and thus accelerate H-spillover, leading to an enhanced hydrogen evolution reaction (HER). Recent studies on single-atom catalysts (SACs) combined with nano-metal-particles (NMPs) have developed various homologous NMP-SACs, however, synthesizing the heterologous NMP-SACs remains a significant challenge. Particularly for HER catalysts under alkaline conditions, the ideal heterologous structure requires a synergy between non-noble NMPs with strong oxophilicity and noble-metal SAs with suitable hydrogen binding energy.

Coordination-in-pipe engineering of Pt-based intermetallic compounds with nanometer to angstrom precision.

The simultaneous regulation of particle size, surface coordinated environment and composition for Pt-based intermetallic compound (Pt-IMC) nanoparticles to manipulate their reactivity for energy storage is of great importance. Herein, we report a general synthetic method for Pt-IMCs using SBA-15 for coordination-in-pipe engineering. The particle size can be regulated to 3-9 nm by carrying out the coordination in pipes with different diameters and the coordination number of the interface metal atoms can be adjusted by altering the N source.

Ultralow Coordination Copper Sites Compartmentalized within Ordered Pores for Highly Efficient Electrosynthesis of -Propanol from CO.

Coordinatively unsaturated copper (Cu) has been demonstrated to be effective for electrifying CO reduction into C products by adjusting the coupling of C-C intermediates. Nevertheless, the intuitive impacts of ultralow coordination Cu sites on C products are scarcely elucidated due to the lack of synthetic recipes for Cu with low coordination numbers and its vulnerability to aggregation under reductive potentials. Herein, computational predictions revealed that Cu sites with higher levels of coordinative unsaturation favored the adsorption of C and C intermediates.

Destabilization of Single-Atom Catalysts: Characterization, Mechanisms, and Regeneration Strategies.

Numerous in situ characterization studies have focused on revealing the catalytic mechanisms of single-atom catalysts (SACs), providing a theoretical basis for their rational design. Although research is relatively limited, the stability of SACs under long-term operating conditions is equally important and a prerequisite for their real-world energy applications, such as fuel cells and water electrolyzers. Recently, there has been a rise in in situ characterization studies on the destabilization and regeneration of SACs; however, timely and comprehensive summaries that provide the catalysis community with valuable insights and research directions are still lacking.

Symmetry Breaking of FeN Moiety via Edge Defects for Acidic Oxygen Reduction Reaction.

Fe-N-C catalysts, with a planar D symmetric FeN structure, show promising as noble metal-free oxygen reduction reaction catalysts. Nonetheless, the highly symmetric structure restricts the effective manipulation of its geometric and electronic structures, impeding further enhancements in oxygen reduction reaction performance. Here, a high proportion of asymmetric edge-carbon was successfully introduced into Fe-N-C catalysts through morphology engineering, enabling the precise modulation of the FeN active site.

High-Throughput Screening and General Synthesis Strategy of Single-Atom Nanozymes for Oral Squamous Cell Carcinoma Therapy.

Single-atom nanozymes (SAzymes), with their superior enzyme-like catalytic activity, have emerged as promising candidates for oncology therapeutics. The well-defined structures of SAzymes make them well predictable by experiences and theoretical calculation. However, the effects of metal center species and coordination environments on enzyme-like activity are variable, and screening catalytic activity by artificial experiments is challenging.