对原子分散的NiN4位点进行局部压力应变调节,以增强CO2电还原到CO的电还原
Minghui Li1, DaPeng Zhang1, Kaifang Wu1
1Department of Physiology, Harbin Medical University-Daqing, Daqing, Heilongjiang 163319, China. wangpeng@hmudq.edu.cn.
Nanoscale
|September 20, 2023
概括
螺旋碳中--碳 (NiN4) 单原子催化剂的应变工程增强了二氧化碳的电还原. 这一战略提高了碳排放的选择性和流动密度,以实现可持续的化学生产.
科学领域:
- 电化学 电化学 电化学
- 材料科学 材料科学 材料科学
- 可持续化学 可持续化学
背景情况:
- 二氧化碳电还原 (CO2RR) 为化学品提供了一条可持续的途径,但在电流密度和选择性方面面临挑战.
- 精确调节CO2RR活性位点是提高效率和抑制演化反应 (HER) 的关键.
研究的目的:
- 调查应变调节对二氧化碳电还原螺旋碳框架内原子分散的NiN4活性位点的影响.
- 通过优化单原子催化剂的局部结构来提高CO2RR性能.
主要方法:
- 在螺旋状碳结构中嵌入的NiN4活性位点的合成.
- 电化学表征,包括循环电压测量和时测量.
- 密度函数理论 (DFT) 计算以了解反应机制.
主要成果:
- 催化剂在-1.4V与RHE相比,达到99.4%的CO选择性.
- 法拉代的效率 (FE_CO) 在一个广泛的电位范围内超过了85% (-0.8到-1.8V与RHE相比).
- 对于CO的最大部分电流密度达到458mA cm-2在-1.8V与RHE相比.
结论:
- 在螺旋式碳中对NiN4位点的压缩应变增强了CO2的电还原.
- 催化剂有效地产生*COOH中间体并抑制HER.
- 本书提出了一种新的策略,通过结构调节来设计单原子催化剂,以实现高效的电催化.
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