Carbon nanosheets supporting Ni–N3S single-atom sites for efficient electrocatalytic CO2 reduction. (30th June 2021)

• Record Type: Journal Article
• Authors: Zhao, Xiaoyi; Huang, Senhe; Chen, Zhenying; Lu, Chenbao; Han, Sheng; Ke, Changchun; Zhu, Jinhui; Zhang, Jichao; Tranca, Diana; Zhuang, Xiaodong
• Is Part Of: Carbon. Volume 178(2021)
• Page Start: 488
• Page End: 496
• Publication Date: 2021-06-30
• Subjects: Carbon nanosheets -- Nickel phosphorus trisulfide -- Single nickel sites -- Nitrogen and sulfur co-coordination -- Carbon dioxide reduction reaction; Carbon -- Periodicals; Carbone -- Périodiques; Koolstof; Toepassingen; Electronic journals; 546.681
• DOI: 10.1016/j.carbon.2021.03.017
• Languages: English
• ISSNs: 0008-6223

Abstract

Abstract: Of various atomically dispersed metal catalysts, those based on single Ni atoms are among the most efficient electrocatalysts for CO2 reduction. However, the activity of these catalysts is determined by the coordination environment of Ni sites. Here, N and S co-coordinated Ni sites were successfully prepared using a nickel phosphorus trisulfide two-dimensional template to form a sandwich-like conjugated microporous polymer. As-prepared Ni single atom–based porous carbon nanosheets were proved to possess N/S co-coordination via X-ray absorption spectroscopy. As electrocatalysts for CO2 reduction, the prepared porous carbon nanosheets achieved over 95% CO selectivity rate and −7.8 mA cm −2 current density (−0.8 V vs. reversible hydrogen electrode). This performance could be attributed to the sheet-like morphology of the nanosheets with long-distance conductivity and the rich single N/S-coordinated Ni atoms with high activity. The fundamental understanding of manipulating such a coordination environment revealed in this study can be used to create versatile single-metal atom–based catalysts for high-efficient energy conversion. Graphical abstract: Image 1 Highlights: Sheet-like Ni single-atom catalyst is prepared by the pyrolysis of conjugated microporous polymer covered NiPS3 flakes. The Ni single-atom catalyst features Ni–N3 S active sites, and shows good performance for CO2 electroreduction. This good performance is attributed to the rich Ni–N3 S active sites and sheet-like morphology of the catalyst.