Reaction mechanism on Ni-C₂-NS single-atom catalysis for the efficient CO₂reduction reaction

Abstract

Ni-based single-atom catalysis (Ni-SAC) has been experimentally reported with superior performance in reducing CO 2 to CO. However, due to the ambiguities in its structures, the active sites of Ni-SAC that are responsible for superior performance have not yet been resolved. This work investigates the CO 2 reduction reaction (CO 2 RR) mechanism on Ni-SAC by carrying out quantum mechanics (QM) simulation to consider both solvation effects. After exploring multiple possible combinations of N, S, and C, we distinguish a Ni-SAC site with two C, one S, and one N, representing the best performance. The predicted formation energy is closely consistent with experimental onset potential. Our prediction also suggests further improvement by finely tuning the electronics state of metal sites by changing the SAC support.

Descriptors and graphical construction forin silicodesign of efficient and selective single atom catalysts for the eNRR

“…The changes in the free energy steps are very small in the whole free energy profile. Therefore, we can infer that the effect of solvent is not sufficient to change the reaction mechanism, as has also been reported in previous studies [87][88][89] .…”

“…Therefore, we can infer that the effect of solvent is not sufficient to change the reaction mechanism, as has also been reported in previous studies. [87][88][89]…”

Band Gap Regulation with Imino Groups in Graphdiyne: A Promising Photocatalyst for Water-Splitting and CO2 Reduction

“…Moreover, the oxAGDY-full system carrying the most imino groups could also work as a photocatalyst for CO 2 reduction reactions (CO 2 RRs), e.g., the reaction CO 2 + 2H + + 2e – → CO + H 2 O, according to its reduction potential at pH = 7, as indicated in Figure , whereas the reaction at the anode is still the OER with H 2 O molecules. The variations of the Gibbs free energies during the CO 2 RR process at the cathode have also been estimated by following the definitions as reported in the previous work . The step graph containing the free energy information is exhibited in Figure c.…”

“…The variations of the Gibbs free energies during the CO 2 RR process at the cathode have also been estimated by following the definitions as reported in the previous work. 68 The step graph containing the free energy…”

Mechanistic understanding and design of non-noble metal-based single-atom catalysts supported on two-dimensional materials for CO2 electroreduction

“…149 A similar study revealed that Ni-SACs with two C, one N, and one S coordination environment were estimated to be the most efficient catalyst for the CO 2 RR, with a theoretically calculated onset potential of 0.67 eV. 150…”