Single-Atom Catalysts for CO<sub>2</sub> Reduction to Oxalate: Theoretical Design and Reaction Condition Prediction

Single-Atom Catalysts for CO<sub>2</sub> Reduction to Oxalate: Theoretical Design and Reaction Condition Prediction

The electrochemical conversion of carbon dioxide (CO<sub>2</sub>) into high-value-added products under mild conditions is crucial for achieving carbon neutrality. Oxalate (C<sub>2</sub>O<sub>4</sub><sup>2–</sup>) is one of the most important industrial...

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Bibliographic Details
Main Author: Ying Zhou (25031) (author)
Other Authors: Xuan Wu (126953) (author), Ping Zhu (11521) (author), Wenhua Zhang (317886) (author)
Published: 2025
Subjects:
Science Policy
Environmental Sciences not elsewhere classified
Biological Sciences not elsewhere classified
Chemical Sciences not elsewhere classified
reaction condition prediction
2 –</ sup
varying reaction conditions
offers theoretical guidance
achieving carbon neutrality
ti – n
cr – n
single metal atoms
alongside high selectivity
2 </ sub
c – c
– n
x </
theoretical design
mild conditions
carbon dioxide
widely used
using single
systematically tuning
sub ><
remarkably low
reducing agent
promising catalysts
operating efficiently
mechanistic understanding
highly sensitive
findings demonstrate
energy barrier
electrode potential
determining step
designing high
coordination environment
catalytic performance
catalytic activity
atom catalysts
also deepens
added products
6 v
31 ev
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Summary:The electrochemical conversion of carbon dioxide (CO<sub>2</sub>) into high-value-added products under mild conditions is crucial for achieving carbon neutrality. Oxalate (C<sub>2</sub>O<sub>4</sub><sup>2–</sup>) is one of the most important industrial raw materials and is widely used as a reducing agent in the fields of medicine, dyeing, and plastics yet faces challenges in efficient C–C bond formation under mild conditions. In this study, we investigate the reduction of CO<sub>2</sub> to C<sub>2</sub>O<sub>4</sub><sup>2–</sup> using single-atom catalysts (SACs) with M–N<sub><i>x</i></sub>–C configurations, employing density functional theory (DFT) to assess their catalytic performance under varying reaction conditions. Our findings demonstrate that the catalytic activity of Ti–N<sub>3</sub>–C is highly sensitive to the choice of solvent and electrode potential. Lower solvent dielectric constants and more negative electrode potentials promote oxalate formation with Ti–N<sub>3</sub>–C, exhibiting a remarkably low-energy barrier (0.31 eV) for the rate-determining step at −0.7 V in acetonitrile, alongside high selectivity. By systematically tuning the coordination environment of single metal atoms, we identify Ti–N<sub>2</sub>C–C, Cr–N<sub>2</sub>C–C, and Cr–N<sub>3</sub>–C as promising catalysts, operating efficiently at potentials of −0.7, −0.7, and −0.6 V, respectively. This work not only offers theoretical guidance for designing high-performance SACs for CO<sub>2</sub> conversion but also deepens the mechanistic understanding of the electrochemical CO<sub>2</sub> reduction pathways.

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