AI Article Synopsis
- - Understanding the microstrain environment around diatomic sites is key to enhancing electrochemical CO reduction (eCOR), but creating this environment precisely is difficult.
- - Researchers developed Ag-CdTMT electrocatalysts with diatomic AgNS-CdNS sites, achieving nearly 100% Faradaic efficiency for CO reduction at high current density (∼200 mA cm in H-cell).
- - The study reveals how engineering microstrain and using adjacent silver atoms can improve electron localization and boost COOH adsorption, which is crucial for optimizing the reduction process.
Article Abstract
Deeply understanding how local microstrain environment around diatomic sites influences their electronic state and adsorption is crucial for improving electrochemical CO reduction (eCOR) reaction; however, precise engineering of the atomic microstrain environment is challenging. Herein, we fabricate Ag-CdTMT electrocatalysts with AgNS-CdNS diatomic sites by anchoring Ag to the nodes of CdTMT (TMT = 2,4,6-trimercaptotriazine anion) coordination polymers. The Ag-CdTMT catalysts achieve approximately 100% Faradaic efficiency for CO reduction with an industrial level current density (∼200 mA cm in H-cell). The embedded Ag atoms induce the formation of Ag-Cd diatomic sites with local microstrain, stretching Cd-N/S bonds, and reinforcing electron localization at Cd sites. The microstrain engineering and adjacent Ag atoms synergistically reduced Cd 4d-C 2p antibonding orbital occupancy for intensifying *COOH adsorption as the rate-determining step. This study provides novel insights into customizing the electronic structure of diatomic sites through strain engineering.
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| http://dx.doi.org/10.1021/acs.nanolett.4c03978 | DOI Listing |
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