1. Single-cluster anchored on PC6 monolayer as high-performance electrocatalyst for carbon dioxide reduction reaction: First principles study.
- Author
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Liu, Zhiyi, Ma, Aling, Wang, Zhenzhen, Li, Chenyin, Ding, Zongpeng, Pang, YuShan, Fan, Guohong, and Xu, Hong
- Subjects
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METAL clusters , *CARBON dioxide reduction , *MONOMOLECULAR films , *DENSITY functional theory , *CARBON dioxide , *COPPER , *BINDING sites - Abstract
[Display omitted] • Triple-atom anchored PC 6 TACs for CO 2 RR investigated. • Mn 3 @PC 6 , Fe 3 @PC 6 , and Co 3 @PC 6 exhibit high activity and selectivity. • High-performance originate from synergistic effect of triple-atom center which breaks *CHO–*CO scaling relationship. • Comparative study of M 2 @PC 6 DACs and M 3 @PC 6 TACs on CO 2 RR performance. • E ads (*CO 2) and ε d can be regarded as descriptors for CO 2 RR performance. Tremendous challenges remain to develop high-efficient catalysts for carbon dioxide reduction reaction (CO 2 RR) owing to the poor activity and low selectivity. However, the activity of catalyst with single active site is limited by the linear scaling relationship between the adsorption energy of intermediates. Motivated by the idea of multiple activity centers, triple metal clusters (M = Cr, Mn, Fe, Co, Ni, Cu, Pd, and Rh) doped PC 6 monolayer (M 3 @PC 6) were constructed in this study to investigate the CO 2 RR catalytic performance via density functional theory calculations. Results shows Mn 3 @PC 6 , Fe 3 @PC 6 , and Co 3 @PC 6 exhibit high activity and selectivity for the reduction of CO 2 to CH 4 with limiting potentials of −0.32, −0.28, and −0.31 V, respectively. Analysis on the high-performance origin shows the more binding sites in M 3 @PC 6 render the triple-atom anchored catalysts (TACs) high ability in regulating the binding strength with intermediates by self-adjusting the charges and conformation, leading to the improved performance of M 3 @PC 6 than dual-atom doped PC 6. This work manifests the huge application of PC 6 based TACs in CO 2 RR, which hope to prove valuable guidance for the application of TACs in a broader range of electrochemical reactions. [ABSTRACT FROM AUTHOR]
- Published
- 2024
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