@article{Tian2023, 
author = {Ling-Chan Tian and Jin-Nian Hu and Yang Meng and Jin-Xia Liang and Chun Zhu and Jun Li},
title = {Ultrastable nickel single-atom catalysts with high activity and selectivity for electrocatalytic CO2 methanation},
year = {2023},
journal = {Nano Research},
volume = {16},
number = {7},
pages = {8987-8995},
keywords = {single atom catalyst, density functional theory, CO2 reduction, metal–organic framework, electrocatalysis},
url = {https://www.sciopen.com/article/10.1007/s12274-023-5640-z},
doi = {10.1007/s12274-023-5640-z},
abstract = {Electrochemical conversion of CO2 into valuable hydrocarbon fuel is one of the key steps in solving carbon emission and energy issue. Herein, we report a non-noble metal catalyst, nickel single-atom catalyst (SAC) of Ni1/UiO-66-NH2, with high stability and selectivity for electrochemical reduction of CO2 to CH4. Based on ab initio molecular dynamics (AIMD) simulations, the CO2 molecule is at first reduced into CO2− when stably adsorbed on a Ni single atom with the bidentate coordination mode. To evaluate its activity and selectivity for electrocatalytic reduction of CO2 to different products (HCOOH, CO, CH3OH, and CH4) on Ni1/UiO-66-NH2, we have used density functional theory (DFT) to study different reaction pathways. The results show that CH4 is generated preferentially on Ni1/UiO-66-NH2 and the calculated limiting potential is as low as −0.24 V. Moreover, the competitive hydrogen evolution reaction is unfavorable at the activation site of Ni1/UiO-66-NH2 owing to the higher limiting potential of −0.56 V. Furthermore, the change of Ni single atom valence state plays an important role in promoting CO2 reduction to CH4. This work provides a theoretical foundation for further experimental studies and practical applications of metal–organic framework (UiO-66)-based SAC electrocatalysts with high activity and selectivity for the CO2 reduction reaction.}
}