ZrN6-Doped Graphene for Ammonia Synthesis: A Density Functional Theory Study |
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Authors: | Jing Wu Lei Yang Dr. Xin Liu Ze Zhang Shanping Liu Dr. Beibei Xiao |
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Affiliation: | 1. School of Energy and Power Engineering, Jiangsu University of Science and Technology, 212003 Zhenjiang, Jiangsu, China;2. ICGM, University of Montpellier, CNRS, ENSCM, Montpellier, France |
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Abstract: | Considering the pivotal role of ammonia in the modern chemical industry, designing effective catalysts for the N2-to-NH3 conversion stimulates great research enthusiasms. In this work, by means of density functional theory calculations, we systematically investigated the electrocatalysis of six-coordinated transition metal atom anchored graphene for nitrogen fixation. The free energy analysis shows that the ZrN6 configuration has a good activity toward ammonia synthesis under overpotential of 0.51 V. According to the electron transfer analysis, ZrN6 site plays a bridging role in charge transfer between the functional graphene and the reactant. Furthermore, the presence of N6 coordination increases the electron accumulation on the NNHx intermediates, which weakens the intermolecular N−N bond, reducing the thermodynamic barrier of protonation process. This work provides a basic understanding of the interaction between transition metal and the adjacent coordination in tuning the reactivity. |
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Keywords: | nitrogen reduction reaction density functional theory graphene thermodynamics electrocatalysts |
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