通过同结构铜纳米集群催化剂的单原子切换来调节CO2的产品选择性
Chao Han1, Tao Yang1, Youqiong Fang2
1Department of Materials Science and Engineering, Centre for Atomic Engineering of Advanced Materials, Institutes of Physical Science and Information Technology, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, Anhui University, Hefei, 230601, P.R. China.
将单个铜原子添加到纳米集群中,将大大改变其在减少二氧化碳中的催化性能. 14纳米集群有效地将二氧化碳转化为碳化合物,与活性较低的13不同. 这突出了单个原子操纵的重点.
科学领域:
- 催化剂是一种催化剂.
- 纳米材料科学 科学 纳米材料科学
- 电化学 电化学 电化学
背景情况:
- 单个原子的操纵显著影响了原子级催化剂的催化活性和选择性.
- 阐明单个原子的精确影响是具有挑战性的,因为复杂的催化剂中相互交织的因素.
- 原子精确的同结构纳米集群 (NCs) 为研究单原子效应提供了理想的平台.
研究的目的:
- 合成和研究一对同结构铜纳米集群 (Cu13和Cu14) 作为模型系统.
- 阐明单原子添加对电化学二氧化碳减排中的催化性能的影响.
- 了解控制催化反应的结构-活性关系.
主要方法:
- 同结构Cu13和Cu14纳米集群的合成.
- 电化学二氧化碳还原反应 (CO2RR) 实验.
- 晶体分析,计算建模,现场表征和运动实验.
主要成果:
- 13在将二氧化碳减少为二氧化碳方面表现出较低的活性 (13%的法拉代效率在-1.1 V).
- 14表现出增强的二氧化碳深度降解到碳化合物 (CH4和C2H4),在-1.2V时具有54.3%的FE.
- Cu14中额外的Cu原子优化了电子结构,促进了CO2激活和H2O解离.
结论:
- 在同结构纳米集群中单原子操纵可以切换催化反应.
- 额外的Cu原子引起的结构和电子修改是提高性能的关键.
- 这项研究提供了通过精确的原子控制控制催化物的基本见解.
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