Challenges and Perspectives of Single-Atom-Based Catalysts for Electrochemical Reactions

JACS Au, Journal Year: 2023, Volume and Issue: 3(3), P. 736 - 755

Published: Feb. 16, 2023

Single-atom catalysts (SACs) are emerging as the most promising for various electrochemical reactions. The isolated dispersion of metal atoms enables high density active sites, and simplified structure makes them ideal model systems to study structure–performance relationships. However, activity SACs is still insufficient, stability usually inferior but has received little attention, hindering their practical applications in real devices. Moreover, catalytic mechanism on a single site unclear, leading development rely trial-and-error experiments. How can one break current bottleneck sites density? further increase activity/stability sites? In this Perspective, we discuss underlying reasons challenges identify precisely controlled synthesis involving designed precursors innovative heat-treatment techniques key high-performance SACs. addition, advanced operando characterizations theoretical simulations essential uncovering true electrocatalytic an site. Finally, future directions that may arise breakthroughs discussed.

Language: 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, Journal Year: 2023, Volume and Issue: 17(12), P. 11869 - 11881

Published: June 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.

Language: Английский

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Modulating the Asymmetric Atomic Interface of Copper Single Atoms for Efficient CO₂ Electroreduction

ACS Nano, Journal Year: 2023, Volume and Issue: 17(5), P. 4619 - 4628

Published: Feb. 23, 2023

Cu single-atom catalysts (Cu SACs) have been considered as promising for efficient electrocatalytic CO2 reduction reactions (ECRRs). However, the reports on SACs with an asymmetric atomic interface to obtain CO are few. Herein, we rationally designed two different interfaces explore their catalytic performance. The catalyst of CuN3O/C delivers high ECRR selectivity FECO value above 90% in a wide potential window from -0.5 -0.9 V vs RHE (in particular, 96% at -0.8 V), while CuCO3/C poor production maximum only 20.0% RHE. Besides, exhibited large turnover frequency (TOF) up 2782.6 h-1 RHE, which is much better than 4.8 CuCO3/C. Density functional theory (DFT) results demonstrate that CuN3O site needs lower Gibbs free energy CuCO3 rate-determining step desorption, leading outstanding performance process ECRR-to-CO. This work provides strategy improve and activity via regulating by adjusting coordination atoms.

Language: Английский

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

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 15(1)

Published: Oct. 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.

Language: Английский

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

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(4)

Published: Aug. 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

Language: Английский

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