协调不和Ni-N2 网站,以有效的电化学二氧化碳减排
Jian Song1,2, Xue Lei3, Jiali Mu1
1Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, 116023, China.
Small (Weinheim an der Bergstrasse, Germany)
|August 31, 2023
概括
在--碳催化剂中引入可以提高二氧化碳的减少. 新的Ni-N2Cl/C催化剂在转化二氧化碳方面显示出更高的效率和稳定性,其性能优于类似的催化剂.
科学领域:
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
- 电化学 电化学 电化学
背景情况:
- 异原子兴奋剂修改了金属--碳 (M-N-C) 单原子催化剂.
- M-N4结构通常被杂,但M-N2站点为优化提供更好的硬体接入.
- 协调不和的M-N2站点对调整催化剂电子结构具有前景.
研究的目的:
- 构建一个Ni-N2催化剂与外平面 (Cl) 原子 (Ni-N2Cl/C) 有效的二氧化碳还原反应 (CO2 RR).
- 为了研究Cl兴奋剂对Ni-N2活性部位的电子和几何效应.
- 为了评估Ni-N2Cl/C催化剂对CO2的催化性能和稳定性,RR.
主要方法:
- 功能化碳支物的合成 (C-Cl).
- 构建一个Ni-N2Cl/C单原子催化剂.
- 密度函数理论 (DFT) 计算以了解反应机制.
- 在现场拉曼光谱检测以确认中间结合.
- 电化学测试二氧化碳RR性能 (法拉代效率,电位范围,稳定性) 和转速频率 (TOF) 的确定.
主要成果:
- Ni-N2Cl/C催化剂显示了增强的CO2 RR性能.
- DFT的计算表明,COOH*形成和CO*脱吸平衡有所改善.
- 在现场,拉曼光谱证实了较低的CO结合能量,从而促进了CO脱吸.
- 在一个广泛的潜能范围内实现了>80%的CO 法拉代效率 (FE_CO) (-0.6到-1.2V与RHE相比).
- 在40小时内表现出极好的稳定性,可忽略不计FE_CO和电流下降.
- 证明了高周转频率 (TOF) 的15,808小时-1,比Ni-N2 / C.高十倍以上.
结论:
- 在Ni-N2位点进行异平的Cl兴奋剂,有效地优化了CO2 RR的电子结构.
- 与无兴奋剂对应物相比,Ni-N2Cl/C催化剂提供了更高的活性和稳定性.
- 这项工作突出了M-N2站点和战略性异构原子兴奋剂在先进的电催化剂设计中的潜力.
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