近日，课题组硕士生陈增璇论文“Revealing the Joint Contribution of Potential and Water Molecules to the High CO2RR Activity of a Single Nickel Atom Catalyst“被ACS Applied Nano Materials（中科院SCI三区期刊，IF = 5.3）接收！

Nitrogen-doped graphene-supported single-atom catalysts (SACs) with maximum atom utilization have high catalytic activity for CO₂ reduction reaction (CO₂RR). Nevertheless, theoretical exploration of these systems remains immensely insufficient due to the complexity of a realistic microenvironment in CO₂RR. This work, taking the NiN₄ SAC as a probe, systematically investigates the synergistic effect of applied potential and water molecules on CO₂RR performance. Results show that only under relatively higher applied potentials and the H₂O molecule could jointly contribute to chemisorption and activation of CO₂. Two possible proton sources during the CO₂RR process are considered. Under relatively high potentials, H₂O-containing H is the proton source for the initial CO₂ activation. The reaction energies and energy barriers for both *CO₂ → *COOH and *COOH → *CO steps are linearly correlated to applied potentials. This can be attributed to the enhanced spin state enabling stronger interaction of the Ni metal center and *COOH intermediate, which is conducive to facilitating the CO₂RR process. This work not only explains a long-standing puzzle for an important catalyst but also highlights the joint contribution of the applied potential and water molecules, which can guide more rational elucidation of other electrocatalytic mechanisms and more effective catalyst design.

https://doi.org/10.1021/acsanm.5c01569