1. Fine tuning dual active sites in modulating cascade electrocatalytic nitrate reduction over covalent organic framework.
- Author
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Zhou, Jing, Zhao, Jiani, Liu, Jiquan, Song, Dengmeng, Xu, Wenhua, Yang, Anjin, Li, Jun, and Wang, Ning
- Subjects
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ELECTROLYTIC reduction , *DENITRIFICATION , *ACTIVATION energy , *COPPER , *ELECTROCHEMICAL experiments , *CARBON dioxide , *CATALYSIS - Abstract
[Display omitted] Conversion of NO 3 − to NH 3 proceeds stepwise in natural system under two different enzymes involving intermediate NO 2 −. Artificial electro-driven NO 3 − reduction also faces the obstacle of low faradaic efficiency due to insufficient utilization of this intermediate. Herein, we demonstrate a bimetallic COF-based electrocatalyst for the cascade catalysis of NO 3 −-to-NO 2 −-to-NH 3 for the first time. TpBpy-Cu 2 Co 4 exhibits a significantly improved performance, with an enhancement factor of 1.4–2 compared to monometallic TpBpy-M. The NH 3 yield rate achieves 25.6 mg h−1 mg cat. −1 at −0.55 V vs RHE over TpBpy-Cu 2 Co 4 , together with excellent faradaic efficiency (93.4 %). This achievement demonstrates cascade catalysis between Co and Cu units, and their distinct roles are investigated through electrochemical experiments and theory calculations. In electrocatalytic process, Cu site facilities *NO 3 -to-*NO 3 H step, while the Co site significantly decreases the energy barrier of *NHOH-to-*NH. The present work provides a valuable inspiration in designing efficient catalysts for cascade reaction. [ABSTRACT FROM AUTHOR]
- Published
- 2024
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