通过调节/铜催化剂的二聚化和质子化,将CO2电还原转换为C2+产品和CH4产品
Tailei Hou1, Jiexin Zhu2, Hongfei Gu1
1Beijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green Applications, MOE Key Laboratory of Cluster Science, MIIT Key Laboratory of Medical Molecule Science and Pharmaceutical Engineering, School of Chemistry and Chemical Engineering, School of Materials Science & Engineering, Beijing Institute of Technology, Beijing, 100081, China.
改铜催化剂精确控制关键中间体,以有效减少二氧化碳排放. 这一战略提高了对C2+产品和甲的选择性,提供了针对目标CO2转换的催化剂设计的见解.
科学领域:
- 电化学 电化学 电化学
- 催化剂是一种催化剂.
- 材料科学 材料科学 材料科学
背景情况:
- 基于铜 (Cu) 的催化剂对于电化学二氧化碳还原反应 (CO2RR) 至关重要,但通过关键中间体 (* CO 和 * H) 控制选择性仍然具有挑战性.
- 开发多功能策略来管理中间覆盖是优化CO2RR产品分销的必要条件.
研究的目的:
- 设计和研究 (Pt) 改性Cu催化剂,以精确调节CO2RR中的关键中间体.
- 了解Pt单个原子 (Cu-Pt1) 和Pt纳米粒子 (Cu-PtNPs) 如何影响反应通路和产品选择性.
主要方法:
- 合成和表征Pt修饰的Cu催化剂 (Cu-Pt1和Cu-PtNP).
- 电化学二氧化碳减排反应 (CO2RR) 性能评估,包括法拉第效率 (FE) 测量.
- CO剥离实验和现场光谱分析.
- 理论计算以阐明界面部位的反应机制.
主要成果:
- -Pt1催化剂实现了高FE的C2+产品 (高达70.4%),归因于增强的*CO吸附和*OCCO中间体形成.
- Cu-PtNPs催化剂显示CH4的高FE (高达57.7%),与抑制*CO耐受性相关,并通过水解离促进*CHO形成.
- 实验和理论研究证实了Pt单个原子和纳米粒子在管理中间覆盖和反应路径方面的独特作用.
结论:
- 具有工程关键中间覆盖的原子设计活性站点为有针对性的二氧化碳转化提供了有效的战略.
- 催化剂的Pt修改提供了一种多功能方法,可以从二氧化碳减排中选择性地产生C2+产品或甲.
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