A theoretical study of electrocatalytic ammonia synthesis on single metal atom/Mxene

doi:10.1016/S1872-2067(18)63197-3

Abstract

Abstract:

Electrocatalytic ammonia synthesis under mild conditions is an attractive and challenging process in the earth's nitrogen cycle, which requires efficient and stable catalysts to reduce the overpotential. The N₂ activation and reduction overpotential of different Ti₃C₂O₂-supported transition metal (TM) (Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Mo, Ru, Rh, Pd, Ag, Cd, and Au) single-atom catalysts have been analyzed in terms of the Gibbs free energies calculated using the density functional theory (DFT). The end-on N₂ adsorption was more energetically favorable, and the negative free energies represented good N₂ activation performance, especially in the presence Fe/Ti₃C₂O₂ (-0.75 eV). The overpotentials of Fe/Ti₃C₂O₂, Co/Ti₃C₂O₂, Ru/Ti₃C₂O₂, and Rh/Ti₃C₂O₂ were 0.92, 0.89, 1.16, and 0.84 eV, respectively. The potential required for ammonia synthesis was different for different TMs and ranged from 0.68 to 2.33 eV. Two possible potential-limiting steps may be involved in the process:(i) hydrogenation of N₂ to ^*NNH and (ii) hydrogenation of ^*NH₂ to ammonia. These catalysts can change the reaction pathway and avoid the traditional N-N bond-breaking barrier. It also simplifies the understanding of the relationship between the Gibbs free energy and overpotential, which is a significant factor in the rational designing and large-scale screening of catalysts for the electrocatalytic ammonia synthesis.

Key words: Electrocatalytic ammonia synthesis, Single atom catalyst, MXene, Transition metal, Density functional theory, Overpotential, Gibbs free energy

Yijing Gao, Han Zhuo, Yongyong Cao, Xiang Sun, Guilin Zhuang, Shengwei Deng, Xing Zhong, Zhongzhe Wei, Jianguo Wang. A theoretical study of electrocatalytic ammonia synthesis on single metal atom/Mxene[J]. Chinese Journal of Catalysis, 2019, 40(2): 152-159.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(18)63197-3

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