Sulfur-Bridged Asymmetric CuNi Bimetallic Atom Sites for CO2 Reduction with High Efficiency

Sulfur-Bridged Asymmetric CuNi Bimetallic Atom Sites for CO2 Reduction with High Efficiency

© 2024 Wiley‐VCH GmbH.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - 36(2024), 33 vom: 25. Aug., Seite e2404665
1. Verfasser: Sun, Zhiyi (VerfasserIn)
Weitere Verfasser: Li, Chen, Wei, Zihao, Zhang, Fang, Deng, Ziwei, Zhou, Kejia, Wang, Yong, Guo, Jinhong, Yang, Jiayi, Xiang, Zequn, Ma, Peijie, Zhai, Huazhang, Li, Shenghua, Chen, Wenxing
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2024
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article CO2 reduction reaction X‐ray absorption spectroscopy asymmetrical coordination dual‐atom catalyst sulfur bridge
Beschreibung
Zusammenfassung:© 2024 Wiley‐VCH GmbH.
Double-atom catalysts (DACs) with asymmetric coordination are crucial for enhancing the benefits of electrochemical carbon dioxide reduction and advancing sustainable development, however, the rational design of DACs is still challenging. Herein, this work synthesizes atomically dispersed catalysts with novel sulfur-bridged Cu-S-Ni sites (named Cu-S-Ni/SNC), utilizing biomass wool keratin as precursor. The plentiful disulfide bonds in wool keratin overcome the limitations of traditional gas-phase S ligand etching process and enable the one-step formation of S-bridged sites. X-ray absorption spectroscopy (XAS) confirms the existence of bimetallic sites with N2Cu-S-NiN2 moiety. In H-cell, Cu-S-Ni/SNC shows high CO Faraday efficiency of 98.1% at -0.65 V versus RHE. Benefiting from the charge tuning effect between the metal site and bridged sulfur atoms, a large current density of 550 mA cm-2 can be achieved at -1.00 V in flow cell. Additionally, in situ XAS, attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS), and density functional theory (DFT) calculations show Cu as the main adsorption site is dual-regulated by Ni and S atoms, which enhances CO2 activation and accelerates the formation of *COOH intermediates. This kind of asymmetric bimetallic atom catalysts may open new pathways for precision preparation and performance regulation of atomic materials toward energy applications
Beschreibung:Date Revised 15.08.2024
published: Print-Electronic
Citation Status PubMed-not-MEDLINE
ISSN:1521-4095
DOI:10.1002/adma.202404665