在CO2中通过快速结-奎恩奇Mössbauer光谱学可视化单Cu原子修饰SnS的催化动力学
Ruru Chen1,2, Jian Zhao1,3, Xiong Zhang1
1State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
Journal of the American Chemical Society
|August 21, 2024
概括
快速结灭Mössbauer光谱显示了电化学二氧化碳减少过程中的动态催化剂变化. 通过在现场确定Cu1/Sn活跃点,实现了高形式生产效率.
科学领域:
- 材料科学
- 电化学
- 光谱学
背景情况:
- 催化剂设计需要了解反应条件下的动态转换.
- 电化学二氧化碳减排 (CO2RR) 对于可持续能源至关重要,但催化机制是复杂的.
- 单原子催化剂具有独特的反应性,但它们的动态演变往往不清楚.
研究的目的:
- 在CO2RR过程中应用快速冷 (RFQ) 莫斯巴尔光谱法监测催化剂动态.
- 阐明单Cu原子修饰的SnS2 (Cu1/SnS2) 催化剂的结构和化学演变.
- 将催化剂动态与CO2RR性能相关联,并确定活性位点.
主要方法:
- 快速结灭 (RFQ) 119Sn莫斯尔光谱.
- 在运行拉曼光谱和ATR-SEIRAS.
- 准现场电子显微镜和XPS.
- 理论上的计算.
主要成果:
- 在CO2RR过程中,RFQ Mössbauer光谱量化跟踪了Cu1/Sn2转化为Cu1/Sn和Cu1/Sn的过程.
- 在158 mA cm-2的部分电流密度下实现了高法拉达效率 (~90.9%).
- 确定了Cu1/Sn活跃点的现场形成,加速了二氧化碳的减少,并促进了关键的中间生成 (*CO2-/*OCHO).
结论:
- 这项研究表明RFQ Mössbauer光谱是一种可视化催化动态的强大工具.
- 在现场形成的Cu1/Sn位点对于高效的二氧化碳转化至关重要.
- 了解催化剂的动态演变是设计高性能单原子催化剂的关键.
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