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Size-dependent activity and selectivity of atomic-level Cu nanoclusters during CO/CO2 electroreduction.
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-09-18 , DOI: 10.1002/anie.202011836
Weifeng Rong 1, 2 , Haiyuan Zou 1, 3 , Wenjie Zang 4 , Shibo Xi 5 , Shuting Wei 1 , Baihua Long 1 , Junhui Hu 1 , Yongfei Ji 6 , Lele Duan 1
Affiliation  

As a favorite descriptor, the size effect of Cu‐based catalysts has been regularly utilized for activity and selectivity regulation toward CO2/CO electroreduction reactions (CO2/CORR). However, little progress has been made in regulating the size of Cu nanoclusters at the atomic level. Herein, the size‐gradient Cu catalysts from single atoms (SAs) to subnanometric clusters (SCs, 0.5–1 nm) to nanoclusters (NCs, 1–1.5 nm) on graphdiyne matrix are readily prepared via an acetylenic‐bond‐directed site‐trapping approach. Electrocatalytic measurements show a significant size effect in both the activity and selectivity toward CO2/CORR. Increasing the size of Cu nanoclusters will improve catalytic activity and selectivity toward C2+ productions in CORR. A high C2+ conversion rate of 312 mA cm−2 with the Faradaic efficiency of 91.2 % are achieved at −1.0 V versus reversible hydrogen electrode (RHE) over Cu NCs. The activity/selectivity‐size relations provide a clear understanding of mechanisms in the CO2/CORR at the atomic level.

中文翻译:

CO / CO2电还原过程中原子级Cu纳米团簇的尺寸依赖性活性和选择性。

作为最喜欢的描述词,通常将铜基催化剂的尺寸效应用于对CO 2 / CO电还原反应(CO 2 / CORR)的活性和选择性调节。然而,在原子水平上调节Cu纳米团簇的尺寸方面进展甚微。在这里,可以通过乙炔键合定点制备在石墨二炔基质上从单原子(SAs)到亚纳米簇(SCs,0.5-1 nm)到纳米团簇(NCs,1-1.5 nm)的尺寸梯度Cu催化剂。诱捕方法。电催化测量显示出对CO 2 / CORR的活性和选择性均具有明显的尺寸影响。增加Cu纳米团簇的尺寸将改善催化活性和对C 2+的选择性CORR中的作品。与Cu NCs上的可逆氢电极(RHE)相比,在-1.0 V时可实现312 mA cm -2的高C 2+转化率和91.2%的法拉第效率。活性/选择性-尺寸之间的关系提供了对原子级CO 2 / CORR中机理的清晰理解。
更新日期:2020-09-18
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