Supplanted by electron-deficient B to form RuN2B-CoN4 moiety as superior catalytic site to further promote urea production

Abstract

The potential significance of electrocatalytic urea synthesis as a promising alternative to traditional manufacture is widely recognized. However, the critical hindrance is lack of its highly efficient and robust electrocatalysts until now. Alongside the exploration of novel urea catalysts, it is equally crucial to explore feasible strategies to boost the performance of the identified active sites. In this work, we proposed and demonstrated a modulatory scheme to further promote urea production in Ru-Co dual-metal sites through the substitution of electron-deficient B atom in RuN3 subunit to form RuN2B-CoN4 moiety in graphene. The B-coordinated Ru active site can effectively decrease charge transfer amount from the Ru atom to the substrate. The enhanced single-atomic similarity to free Ru atom results in more negative adsorption energy for N2 molecule and superior catalytic activity/selectivity for urea generation. More significantly, this study provides a new perspective to promote the catalytic performance of the carbon-based diatomic active sites for urea production.