Asymmetric S Heteroatom Coordinated Dual‐Atom Catalysts and Coupled Anodic Sulfion Oxidation to Boost Electrocatalysis Oxygen Reduction

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 5, 2025

Abstract Considering the exceptional electronic regulation capability, p‐block elements can be used to regulate charge density of traditional transition metal catalysts. In this work, CoGa‐NS‐C dual‐atom catalysts (DACs) are successfully synthesized through co‐precipitation and post‐annealing treatment. The atomic dispersion Co Ga synergistic coordination structure CoN 3 S 1 GaN 4 confirmed by AC‐TEM, EXAFS, XPS. Due steric hindrance effect adsorbed * OH on site asymmetric heteroatom species, adsorption energy OOH intermediation neighboring is thus enhanced greatly, resulting in enhancement 2e‐ORR pathway. Besides, Co─OH intermediates detected situ FT‐IR EC‐SHINERS spectroscopy. A high H 2 O selectivity 90.3% a fast production rate 1.12 mol h −1 g reached. addition, cathodic oxygen reduction couple with sulfion oxidation reaction (SOR) instead energy‐intensive OER reaction. coupling system, SOR potential 1.31 V lower than process at current intensity 100 mA. Both proposed DACs strategy ORR‐SOR system beneficial for achieving efficient energy‐effective 2e‐ORR.

Language: Английский

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Highly selective in-situ generation of 1O2 via electronic structure regulation of single atom sites in electro-Fenton system

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: 366, P. 125040 - 125040

Published: Jan. 8, 2025

Language: Английский

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Preparation of Fe, Co, Ni-based single atom catalysts and the progress of their application in electrocatalysis

Microstructures, Journal Year: 2025, Volume and Issue: 5(1)

Published: Jan. 8, 2025

Single-atom catalysts (SACs) have garnered considerable attention owing to their profound potential in promoting the efficient utilization of metal resources and attaining atomic-level economy. Fe, Co, Ni SACs demonstrated broad application prospects electrocatalysis due tunable composition structure, as well unique electronic properties. Firstly, various preparation methods for are outlined this review, including high-temperature pyrolysis, impregnation, chemical vapor deposition, atomic layer deposition. These not only enhance efficiency atoms but also ensure stability catalysts. Subsequently, review summarizes recent progress applications electrocatalysis, with a particular focus on efficacy hydrogen evolution reaction, oxygen reduction carbon dioxide nitrogen reaction. Despite remarkable advancements, still face challenges related large-scale production, enhancement, comprehensive characterization, mechanistic exploration. Finally, discusses these proposes strategies address them order fully realize high-performance

Language: Английский

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Electrocatalytic H2O2 production paired with value-added chemicals synthesis, contaminant remediation, and electricity generation

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 159828 - 159828

Published: Jan. 1, 2025

Language: Английский

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Emerging Supported Metal Atomic Clusters for Electrocatalytic Renewable Conversions

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 2434 - 2458

Published: Jan. 27, 2025

Subnanometric supported metal atomic clusters (SMACs) composed of several to tens surface atoms have attracted increased research interest in electrocatalysis. SMACs been known show distinct properties compared their nanoparticles and single atom counterparts long developed for functional improvements. Tremendous advancements made the past few years, with a notable trend more precise design down an atomic/molecular level investigation transferring into practical devices, which motivates this timely review. To begin, review presents classifies classic latest synthetic strategies state-of-the-art characterization techniques SMACs. It then outlines discusses basic structure principles SMACs, highlighting importance organic ligands, size effect clusters, support-cluster interactions determining catalytic activity device stability. Thereafter, recent advances typical electrocatalysis processes from laboratory scale industrial are discussed obtain general understanding structure–activity correlations Current challenges future perspectives emerging field also discussed, aiming at practicing SMAC catalysts energy conversion devices.

Language: Английский

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Exploring the Catalytic Performance of Oxygen-Coordinated Single-Atom Catalysts for Nitric Oxide Electroreduction

The Journal of Physical Chemistry C, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 9, 2025

Language: Английский

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Tailoring Oxygen Reduction Selectivity for Acidic H₂O₂ Electrosynthesis on Single-Atom Co–N–C Catalyst via PEG Post-treatment

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 10, 2025

The selective two-electron oxygen reduction reaction (ORR) for H2O2 electrosynthesis provides a promising alternative to anthraquinone-based redox technology. However, atomically dispersed Co-N-C materials routinely lead the ORR process follow four-electron path via accessible Co-N4 moieties rather than terminating in competitive production. Herein, we demonstrate that by simultaneously reconstructing Co-N2-C and modifying functional groups into Co-adjacent carbon matrix through low-temperature pyrolysis with oxygen-containing molecules, Co SAC catalyst typical sites can be transformed SAC-PEG electrocatalyst high selectivity. A combination of X-ray absorption infrared spectroscopy confirmed shift selectivity from pathway originated transfer real active rigid in-plane embedded modified low-coordinated SAC-PEG. In stark contrast remarkable 4e- prototype SAC, after treatment has surprising Eonset acidic electrolytes. This study presents new avenue manipulation tailoring flexible structure single one-step post process, ultimately converting readily available directly difficult-to-obtain 2e- catalyst.

Language: Английский

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Elucidating Relay Catalysis on Copper Clusters With Satellite Single Atoms for Enhanced Urea Electrosynthesis

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: March 10, 2025

Relay catalysis represents significant efficacy in alleviating competition among different reactants during coupling reactions. However, a comprehensive understanding of the reaction mechanism underlying relay for urea electrosynthesis remains challenging. Herein, we have developed catalyst (CuAC-CuSA@NC) comprising Cu atomic clusters (CuAC) with satellite Cu─N4 single atoms (CuSA) sites on nitrogen-doped porous interconnected carbon skeleton (NC), enabling elucidation process co-reduction CO2 and NO3 -. The designed CuAC-CuSA@NC exhibits an approximately threefold higher yield rate compared to that CuSA@NC at -1.3 V versus RHE. Ex-situ experimental results in-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy analysis reveal formation sequence between *NH2 *NH2CO species increasing reduction potential. combination theoretical calculations further elucidates pathway involves "CuAC" facilitating conversion *NO3 *NOx, followed by hydrogenation form *H from water dissociation promoted "CuSA" sites, which subsequently couples *CO2 produce urea. This work provides novel insights into investigation reactions, but not limit to, synthesis.

Language: Английский

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Single-atom catalysts for electrocatalytic conversion of biomass-derived small molecules

Coordination Chemistry Reviews, Journal Year: 2025, Volume and Issue: 534, P. 216576 - 216576

Published: March 6, 2025

Language: Английский

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Tailoring Oxygen Electrocatalytic Performance via Construction of Iron‐Cobalt Oxides and FeN₄ Sites on Hierarchical Carbon Fibers for Efficient Zinc–Air Batteries

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 10, 2025

Abstract The design and fabrication of non‐precious metal materials for bifunctional oxygen electrocatalytic properties with reversible reduction reaction (ORR) evolution (OER) has been a research hotspot in the field zinc–air batteries. Herein, hierarchical carbon nanofiber immobilized iron cobalt oxide particles (FeCoO x ) Fe‐N sites catalyst is synthesized through electrostatic spinning situ polymerization pyrrole coupled pyrolysis. FeCoO /Fe─N─C demonstrates superior performance (E 1/2 = 0.91 V, η 10 350 mV). Liquid batteries employing exhibit high power 184.8 mW cm −2 more than 580 cycles stable cycling ability. Additionally, incorporation cobaltite introduces extra electrons optimizes adsorption capacity intermediates, effectively boosting inherent ORR activity. experimental results illustrate that special geometrical structure spinel ferrite provides excellent OER catalytic performance. Theoretical calculations indicate shifts d‐band center closer to Fermi level f ), thereby modulating hybridization between Fe 3d O 2p orbitals. This work offers an effective approach constructing coupling catalysts have single atoms coexisting efficient catalysis.

Language: Английский

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