在Cu-NHx-C单原子催化剂中的近端质子源可以选择性地提高CO2到甲的电还原
Rongming Cai1,2, Hong Zhu3,4, Fei Yang5
1Guangdong Provincial Key Lab of Nano-Micro Material Research, School of Advanced Materials, Shenzhen Graduate School, Peking University, Shenzhen, 518055, China.
这项研究表明,铜单原子催化剂 (SAC) 中的N-H功能组如何增强二氧化碳还原反应 (CO2RR) 到甲. 该N-H部分作为质子化剂,提高甲生产效率.
科学领域:
- 不同质的催化剂.
- 电触媒溶解是一种电触媒.
- 材料科学 材料科学 材料科学
背景情况:
- 控制活性位点协调是同质催化剂性能的关键.
- 异质单原子催化剂 (SAC) 在精确调整协调环境方面存在挑战.
- 铜SAC对CO2RR有希望,但需要优化活跃站点.
研究的目的:
- 开发一个自下而上的策略,用于构建具有可调节的N站点功能组的铜SAC.
- 研究近端N位点功能组 (N-H与N-CH3) 对CO2RR选择性和活性的影响.
- 为了阐明增强甲生产的反应机制.
主要方法:
- 减少氧化石墨烯的自下而上的合成支持铜SACs (rGO@Cu-N(Hx) -C).
- 在现场使用N-H功能组进行二氧化碳减排的质子化.
- 运行光谱研究和理论计算来分析反应通路.
- 与-CH3替代对应物 (rGO@Cu-N-C) 的比较.
主要成果:
- 在rGO@Cu-NHx-C中的N-H部分起到in-situ质子化剂的作用,加速CO2转化为甲.
- 实现了比-CH3替代催化剂高出2.42倍的甲电流密度.
- 通过受欢迎的*OCHO路径实现了高甲法拉达效率 (77.1%).
- 证明了SACs的精确调制,以实现高效和选择性的CO2电减.
结论:
- 该N-H功能组对于增强CO2RR到甲通过in-situ质子化至关重要.
- 对于甲生产, *OCHO路径在能量方面比 *CO路径更受青.
- 这一策略使得用于有针对性的电化学二氧化碳减排应用的SAC能够合理设计.
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