Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 1, Pages 466-472Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202011836
Keywords
CO electroreduction; CO2 electroreduction; copper nanoclusters; graphdiyne; size dependence
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Funding
- National Natural Science Foundation of China [21771098, 21903016]
- Science and Technology Innovation Commission of Shenzhen Municipality [JCYJ20170817111548026]
- Shenzhen Clean Energy Research Institute [CERI-KY-2019-003]
- Guangdong Provincial Key Laboratory of Energy Materials for Electric Power [2018B030322001]
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This study investigated the impact of size-gradient Cu catalysts on CO2/CO electroreduction reactions, revealing that increasing the size of Cu nanoclusters can enhance catalytic activity and selectivity. The findings provide a clear understanding of mechanisms in the CO2/CORR at the atomic level.
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.
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