Hierarchically Ordered Pore Engineering of Carbon Supports with High-Density Edge-Type Single-Atom Sites to Boost Electrochemical CO2 Reduction

Hierarchically Ordered Pore Engineering of Carbon Supports with High-Density Edge-Type Single-Atom Sites to Boost Electrochemical CO2 Reduction

© 2024 Wiley‐VCH GmbH.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - 36(2024), 48 vom: 22. Nov., Seite e2409531
1. Verfasser: Hu, Chenghong (VerfasserIn)
Weitere Verfasser: Hong, Ximeng, Liu, Miaoling, Shen, Kui, Chen, Liyu, Li, Yingwei
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2024
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article Zn–CO2 battery edge electrochemical CO2 reduction electronic modification single‐atom catalyst
Beschreibung
Zusammenfassung:© 2024 Wiley‐VCH GmbH.
Metal sites at the edge of the carbon matrix possess unique geometric and electronic structures, exhibiting higher intrinsic activity than in-plane sites. However, creating single-atom catalysts with high-density edge sites remains challenging. Herein, the hierarchically ordered pore engineering of metal-organic framework-based materials to construct high-density edge-type single-atomic Ni sites for electrochemical CO2 reduction reaction (CO2RR) is reported. The created ordered macroporous structure can expose enriched edges, further increased by hollowing the pore walls, which overcomes the low edge percentage in the traditional microporous substrates. The prepared single-atomic Ni sites on the ordered macroporous carbon with ultra-thin hollow walls (Ni/H-OMC) exhibit Faraday efficiencies of CO above 90% in an ultra-wide potential window of 600 mV and a turnover frequency of 3.4 × 104 h-1, much superior than that of the microporous material with dominant plane-type sites. Theory calculations reveal that NiN4 sites at the edges have a significantly disrupted charge distribution, forming electron-rich Ni centers with enhanced adsorption ability with *COOH, thereby boosting CO2RR efficiency. Furthermore, a Zn-CO2 battery using the Ni/H-OMC cathode shows an unprecedentedly high power density of 15.9 mW cm-2 and maintains an exceptionally stable charge-discharge performance over 100 h
Beschreibung:Date Revised 28.11.2024
published: Print-Electronic
Citation Status PubMed-not-MEDLINE
ISSN:1521-4095
DOI:10.1002/adma.202409531