First-Principles Insights into the Selectivity of CO2 Electroreduction over Heterogeneous Single-Atom Catalysts.
J Phys Chem Lett
; 15(23): 6216-6221, 2024 Jun 13.
Article
in En
| MEDLINE
| ID: mdl-38838259
ABSTRACT
Heterogeneous metal-nitrogen-carbon (M-N-C) single-atom catalysts (SACs) have garnered considerable attention in the two-electron CO2 reduction reaction (2e-CO2RR). Interestingly, almost M-N-C SACs mainly produce CO, while Sb is one of the few SACs reported so far that can produce HCOOH. Nevertheless, the underlying factors for different selectivities on Sb-N-C SAC remain controversial, and the lack of in-depth understanding of limiting factors hampers further regulations. Here, by using constant-potential first-principles calculations, we revealed that the high HCOOH selectivity of Sb-N-C SAC is mainly attributed to their weak charge accumulation ability. Remarkably, considering the highly tunable geometric structure of M-N-C SACs, we provide that Sb-N-C SAC with the SbN3S1 center is a promising candidate for CO production. Our work provides the mechanism insight into 2e-CO2RR selectivity and further paves the way toward electrocatalyst regulation and design.
Full text:
1
Collection:
01-internacional
Database:
MEDLINE
Language:
En
Journal:
J Phys Chem Lett
/
J. phys. chem. lett
/
The journal of physical chemistry letters
Year:
2024
Document type:
Article