Structural engineering of atomic catalysts for electrocatalysis

Chemical Science, Год журнала: 2024, Номер 15(14), С. 5082 - 5112

Опубликована: Янв. 1, 2024

This review systematically introduces how to regulate the electronic structure and geometric configuration of atomic catalysts achieve high-efficiency electrocatalysis performances by analyzing detailed electrocatalytic applications mechanisms.

Язык: Английский

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Atomic Cobalt–Silver Dual-Metal Sites Confined on Carbon Nitride with Synergistic Ag Nanoparticles for Enhanced CO₂ Photoreduction

ACS Nano, Год журнала: 2023, Номер 17(12), С. 11869 - 11881

Опубликована: Июнь 8, 2023

Photocatalytic reduction of CO2 to value-added solar fuels is great significance alleviate the severe environmental and energy crisis. Herein, we report construction a synergistic silver nanoparticle catalyst with adjacent atomic cobalt-silver dual-metal sites on P-doped carbon nitride (Co1Ag(1+n)-PCN) for photocatalytic reduction. The optimized photocatalyst achieves high CO formation rate 46.82 μmol gcat-1 70.1% selectivity in solid-liquid mode without sacrificial agents, which 2.68 2.18-fold compared that exclusive single-atom (Ag1-CN) site (Co1Ag1-PCN) photocatalysts, respectively. closely integrated situ experiments density functional theory calculations unravel electronic metal-support interactions (EMSIs) Ag nanoparticles Ag-N2C2 Co-N6-P promote adsorption CO2* COOH* intermediates form CH4, as well boost enrichment transfer photoexcited electrons. Moreover, atomically dispersed Co-Ag SA serve fast-electron-transfer channel while act electron acceptor enrich separate more photogenerated This work provides general platform delicately design high-performance catalysts highly efficient conversion.

Язык: Английский

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Advances on Axial Coordination Design of Single-Atom Catalysts for Energy Electrocatalysis: A Review

Nano-Micro Letters, Год журнала: 2023, Номер 15(1)

Опубликована: Окт. 13, 2023

Abstract Single-atom catalysts (SACs) have garnered increasingly growing attention in renewable energy scenarios, especially electrocatalysis due to their unique high efficiency of atom utilization and flexible electronic structure adjustability. The intensive efforts towards the rational design synthesis SACs with versatile local configurations significantly accelerated development efficient sustainable electrocatalysts for a wide range electrochemical applications. As an emergent coordination avenue, intentionally breaking planar symmetry by adding ligands axial direction metal single atoms offers novel approach tuning both geometric structures, thereby enhancing electrocatalytic performance at active sites. In this review, we briefly outline burgeoning research topic axially coordinated provide comprehensive summary recent advances synthetic strategies Besides, challenges outlooks field also been emphasized. present review provides in-depth understanding SACs, which could bring new perspectives solutions fine regulation structures catering high-performing electrocatalysis.

Язык: Английский

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Boosting CO₂ Electroreduction over a Covalent Organic Framework in the Presence of Oxygen

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(14)

Опубликована: Фев. 7, 2024

Herein, we propose an oxygen-containing species coordination strategy to boost CO

Язык: Английский

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Tuning Coordination Structures of Zn Sites Through Symmetry‐Breaking Accelerates Electrocatalysis

Advanced Materials, Год журнала: 2023, Номер 36(4)

Опубликована: Авг. 31, 2023

Manipulating the coordination environment of individual active sites in a precise manner remains an important challenge electrocatalytic reactions. Herein, inspired by theoretical predictions, facile procedure to synthesize series symmetry-breaking zinc metal-organic framework (Zn-MOF) catalysts with well-defined structures is presented. Benefiting from optimized microenvironment regulated symmetry-breaking, Zn-N

Язык: Английский

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Transplanting Gold Active Sites into Non-Precious-Metal Nanoclusters for Efficient CO₂-to-CO Electroreduction

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(4), С. 2152 - 2160

Опубликована: Янв. 19, 2023

Electrocatalytic CO2 reduction reaction (CO2RR) is greatly facilitated by Au surfaces. However, large fractions of underlying atoms are generally unused during the catalytic reaction, which limits mass activity. Herein, we report a strategy for preparing efficient electrocatalysts with high activities atomic-level transplantation active sites into Ni4 nanocluster (NC). While NC exclusively produces H2, Au-transplanted selectively CO over H2. The origin contrasting selectivity observed this investigated combining operando and theoretical studies, reveal that while Ni almost completely blocked intermediate in both NCs, act as CO2-to-CO electroreduction. exhibits remarkable turnover frequency activity production (206 molCO/molNC/s 25,228 A/gAu, respectively, at an overpotential 0.32 V) durability toward CO2RR 25 h.

Язык: Английский

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Electronic Structure Design of Transition Metal-Based Catalysts for Electrochemical Carbon Dioxide Reduction

ACS Nano, Год журнала: 2024, Номер 18(14), С. 9823 - 9851

Опубликована: Март 28, 2024

With the increasingly serious greenhouse effect, electrochemical carbon dioxide reduction reaction (CO2RR) has garnered widespread attention as it is capable of leveraging renewable energy to convert CO2 into value-added chemicals and fuels. However, performance CO2RR can hardly meet expectations because diverse intermediates complicated processes, necessitating exploitation highly efficient catalysts. In recent years, with advanced characterization technologies theoretical simulations, exploration catalytic mechanisms gradually deepened electronic structure catalysts their interactions intermediates, which serve a bridge facilitate deeper comprehension structure-performance relationships. Transition metal-based (TMCs), extensively applied in CO2RR, demonstrate substantial potential for further modulation, given abundance d electrons. Herein, we discuss representative feasible strategies modulate catalysts, including doping, vacancy, alloying, heterostructure, strain, phase engineering. These approaches profoundly alter inherent properties TMCs interaction thereby greatly affecting rate pathway CO2RR. It believed that rational design modulation fundamentally provide viable directions development toward conversion many other small molecules.

Язык: Английский

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Recent advances of metal suboxide catalysts for carbon‐neutral energy applications

EcoEnergy, Год журнала: 2024, Номер 2(1), С. 45 - 82

Опубликована: Фев. 22, 2024

Abstract Metal suboxides have emerged as a class of promising candidates for many electrocatalytic applications owing to their enhanced electrical conductivity and chemical activities. In this review, we summarized the recent progress metal suboxides. We firstly introduced discovery suboxides, categories according element tables. Then various synthetic methods been systematically illustrated involving solid‐state synthesis, high‐temperature low‐temperature synthesis plasma‐driven methods, etc. addition, demonstrated in field water, carbon nitrogen cycle‐based energy catalysis technologies electrochemical hydrogen evolution reaction, oxygen reduction dioxide reduction, urea oxidation methanol reaction nitrate Finally, make brief conclusion about developments giving an outlook future research challenges. These insights are expected hold promise developing suboxide catalysts toward practical applications.

Язык: Английский

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Recent advancements in noble-metal electrocatalysts for alkaline hydrogen evolution reaction

Chinese Chemical Letters, Год журнала: 2024, Номер unknown, С. 109557 - 109557

Опубликована: Янв. 1, 2024

Язык: Английский

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Multifunctional Film Assembled from N-Doped Carbon Nanofiber with Co–N4–O Single Atoms for Highly Efficient Electromagnetic Energy Attenuation

Nano-Micro Letters, Год журнала: 2024, Номер 16(1)

Опубликована: Июль 9, 2024

Single-atom materials have demonstrated attractive physicochemical characteristics. However, understanding the relationships between coordination environment of single atoms and their properties at atomic level remains a considerable challenge. Herein, facile water-assisted carbonization approach is developed to fabricate well-defined asymmetrically coordinated Co-N

Язык: Английский

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