Abstract
AbstractThe electrochemical CO2 reduction to high-value-added chemicals is one of the most promising and challenging research in the energy conversion field. An efficient ECR catalyst based on a Cu-based conductive metal-organic framework (Cu-DBC) is dedicated to producing CH4 with superior activity and selectivity, showing a Faradaic efficiency of CH4 as high as ~80% and a large current density of −203 mA cm−2 at −0.9 V vs. RHE. The further investigation based on theoretical calculations and experimental results indicates the Cu-DBC with oxygen-coordinated Cu sites exhibits higher selectivity and activity over the other two crystalline ECR catalysts with nitrogen-coordinated Cu sites due to the lower energy barriers of Cu-O4 sites during ECR process. This work unravels the strong dependence of ECR selectivity on the Cu site coordination environment in crystalline porous catalysts, and provides a platform for constructing highly selective ECR catalysts.
Publisher
Springer Science and Business Media LLC
Subject
General Physics and Astronomy,General Biochemistry, Genetics and Molecular Biology,General Chemistry
Reference49 articles.
1. Chu, S., Cui, Y. & Liu, N. The path towards sustainable energy. Nat. Mater. 16, 16–22 (2017).
2. Lin, W. Y. & Frei, H. Photochemical CO2 splitting by metal-to-metal charge-transfer excitation in mesoporous ZrCu(I)-MCM-41 silicate sieve. J. Am. Chem. Soc. 127, 1610–1611 (2005).
3. Nakata, K., Ozaki, T., Terashima, C., Fujishima, A. & Einaga, Y. High-yield electrochemical production of formaldehyde from CO2 and seawater. Angew. Chem. Int. Ed. 53, 871–874 (2014).
4. Wang, L. et al. Surface strategies for catalytic CO2 reduction: from two-dimensional materials to nanoclusters to single atoms. Chem. Soc. Rev. 48, 5310–5349 (2019).
5. Long, C. et al. Electrochemical reduction of CO2 over heterogeneous catalysts in aqueous solution: recent progress and perspectives. Small Methods 3, 1800369 (2019).
Cited by
148 articles.
订阅此论文施引文献
订阅此论文施引文献，注册后可以免费订阅5篇论文的施引文献，订阅后可以查看论文全部施引文献