Computational screening of a single transition metal atom supported on the C2N monolayer for electrochemical ammonia synthesis. Issue 18 (27th April 2018)

• Record Type: Journal Article
• Authors: Wang, Zhongxu; Yu, Zhigang; Zhao, Jingxiang
• Is Part Of: Physical chemistry chemical physics. Volume 20:Issue 18(2018)
• Page Start: 12835
• Page End: 12844
• Publication Date: 2018-04-27
• Subjects: Chemistry, Physical and theoretical -- Periodicals; 541.3
• DOI: 10.1039/c8cp01215f
• Languages: English
• ISSNs: 1463-9076

Abstract

Abstract : The single Mo atom supported by C2 N layer is an effective electrocatalyst for NH3 synthesis from N2 . Abstract : The nitrogen reduction reaction (NRR) under ambient conditions using renewable energy is a green and sustainable strategy for the synthesis of NH3, which is one of the most important chemicals and carbon-free carriers. Thus, the search for low-cost, highly efficient, and stable NRR electrocatalysts is critical to achieve this goal. Herein, using comprehensive density functional theory (DFT) computations, we design a new class of NRR electrocatalysts based on a single transition metal (TM) atom supported on the experimentally feasible two-dimensional C2 N monolayer (TM@C2 N). Based on the computed free energies of each elementary pathway, Mo@C2 N is predicted to exhibit the best catalytic activity among the TM@C2 N, in which the proton-coupled electron transfer of the NH2 * species to NH3 (g) is the potential-determining step. Especially, the computed onset potential of the NRR on Mo@C2 N is −0.17 V, which is even lower than that for the well-established stepped Ru(0001) surface (−0.43 V). Furthermore, the NRR catalytic performance of these TM@C2 N can be well explained by their adsorption strength with N2 H* species. Our findings open a new avenue for optimizing the TM catalytic performance for the NRR with the lowest number of metal atoms on porous low-dimensional materials.