Carbon nanosheets supporting Ni-N3S single-atom sites for efficient electrocatalytic CO2 reduction
Carbon nanosheets supporting Ni-N3S single-atom sites for efficient electrocatalytic CO2 reduction
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支持 Ni-N3S 单原子位点的碳纳米片可有效电催化 CO2 还原
DOI：
10.1016/j.carbon.2021.03.017
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发表时间：
2021
期刊：
影响因子：
10.9
通讯作者：
Zhuang Xiaodong
中科院分区：
文献类型：
--
作者：
Zhao Xiaoyi;Huang Senhe;Chen Zhenying;Lu Chenbao;Han Sheng;Ke Changchun;Zhu Jinhui;Zhang Jichao;Tranca Diana;Zhuang Xiaodong
在各种原子分散的金属催化剂中，基于单个Ni原子的催化剂是最有效的二氧化碳还原电催化剂之一。然而，这些催化剂的活性是由Ni位点的配位环境决定的。本文采用三硫化镍磷二维模板成功制备了N、S共配镍位，形成了三明治状共轭微孔聚合物。通过x射线吸收光谱分析，证明了制备的Ni单原子多孔碳纳米片具有N/S共配性。作为co2还原电催化剂，制备的多孔碳纳米片具有95%以上的CO选择性和−7.8 mA cm−2电流密度（−0.8 Vvs）。可逆氢电极)。这种性能可能归因于纳米片的片状结构，具有远距离导电性和丰富的单N/ s配位镍原子，具有高活性。本研究揭示的操纵这种配位环境的基本理解可用于制造多功能的单金属原子基催化剂，用于高效的能量转换。
Of various atomically dispersed metal catalysts, those based on single Ni atoms are among the most efficient electrocatalysts for CO2reduction. 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 CO2reduction, the prepared porous carbon nanosheets achieved over 95% CO selectivity rate and −7.8 mA cm−2current density (−0.8 Vvs.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.