Synergistic Electrocatalytic Nitrogen Reduction Enabled by Confinement of Nanosized Au Particles onto a Two-Dimensional Ti3C2 Substrate

A N-2 fixation by the electrocatalytic nitrogen reduction reaction from humidified air is regarded to be a critical tool for producing NH3 and reducing the globally accelerating CO, emissions. Notwithstanding great efforts to improve catalyst activity and selectivity, promoting catalyst accessibility to high N-2 concentrations to ensure that active sites fulfill their function should be a promising design direction. Here, Au nanoparticles are firmly anchored through atomic O on the surface of two-dimensional Ti3C2 using an ultrasound reduction process. Akin to the conspicuous role of the web in the predatory process of spiders, N-2 adsorption experiments primarily suggest that a Ti3C2 web is beneficial for extraction of N-2 from air, and embedding high valence-state Au clusters in the Ti3C2 web strengthens the chemical bonding effect toward N-2 molecules. The high energy of N-2 adsorption on the interface between gold clusters and Ti3C2 is the driving force for weakening triple N N bonds, and thereby the activation energy barrier is lowered via effective stabilization of N2H* species and destabilizing NH2NH2* under an alternative pathway. With Au loading content of similar to 0.94%, Au/Ti3C2 exhibits an outstanding average yield of 30.06 mu g h(-1) mg(-1) for NH3 production, with a high Faraday efficiency of 18.34% at -0.2 V.