Abstract

Ni-based single-atom catalysis (Ni-SAC) has been experimentally reported with superior performance in reducing CO₂ 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 CO₂ reduction reaction (CO₂RR) 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.

摘要

Ni 基单原子催化 (Ni-SAC) 在将 CO ₂还原为 CO 方面具有优异的性能。然而，由于其结构的模糊性，Ni-SAC 的活性位点具有优异的性能。尚未解决。这项工作研究了 CO ₂还原反应 (CO ₂RR）机制通过进行量子力学（QM）模拟来考虑两种溶剂化效应。在探索了 N、S 和 C 的多种可能组合后，我们将 Ni-SAC 位点区分为两个 C、一个 S 和一个 N，代表最佳性能。预测的地层能量与实验起始电位密切一致。我们的预测还表明，通过改变 SAC 支持来微调金属位点的电子状态，可以进一步改进。