Tailoring the coordination environment of double-atom catalysts to boost electrocatalytic nitrogen reduction: a first-principles study
Jiarui Wu, Donghai Wu, Haobo Li, Yanhao Song, Wenjing Lv, Xiaohu Yu, Dongwei Ma
Abstract
DACs, exhibiting an ultralow limiting potential of -0.27 V, climb to the peak of the activity volcano. In addition, the experimental feasibility of this DAC system was also identified. Overall, benefiting from the coordination engineering effect, the chemical activity and catalytic performance of the DACs for NRR can be significantly boosted. This phenomena can be understood from the adjusted electronic structure of the TM dimer active center due to the changes of its coordination microenvironment, which significantly affects the binding strength (pattern) of key intermediates and changes the reaction pathways, leading to enhanced NRR activity and selectivity. This work highlights the importance of coordination engineering in developing DACs for the electrocatalytic NRR and other important reactions.