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Anchor single atom in h-BN assist NO synthesis NH3: a computational view

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Abstract

Synthesis of ammonia gas through environmental protection and low-cost electrocatalysis is one of the ways to solve the current human energy problems. Herein, through the study of density functional theory (DFT), a series of transition metal single atoms are embedded in the defect-containing h-BN to construct a TM@B2N2 (TM = Ti–Zn, Nb–Ag) two-dimensional nanostructure. The activation effect of these single-atom catalysts on NO molecules and the electrochemical performance of catalyzing NO reduction reaction (NORR) were explored. All reaction pathways are studied in detail, and competition between hydrogen proton and ammonia (NH3) oxidation with NORRs is also explored. Among the 16 transition metal atoms we studied, the intercalation of Pb atom into h-BN has the best catalytic activity. The reaction rate-limiting potential of NORR is only 0.55 eV, and the surface HER reaction and ammonia oxidation can be effectively inhibited. It is hoped that our research can further promote the application of h-BN in the field of catalysis and provide some guidance for experimental workers in the field of ammonia synthesis.

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摘要

通过环保、低成本的电催化合成氨是解决当前人类能源问题的途径之一。在本研究中，通过 密度泛函理论的研究，将一系列过渡金属单原子嵌入到含有缺陷的h-BN 中，构建了 TM@B2N2（TM=Ti‒Zn，Nb‒Ag）二维纳米结构。研究了这些单原子催化剂对NO 分子的活 化作用以及催化NO 还原反应（NORR）的电化学性能。详细研究了所有反应途径，探讨了 氢质子和氨(NH3)氧化与 NORR 反应之间的竞争。在我们研究的16 个过渡金属原子中， Pb 原子嵌入h-BN 的催化活性最好。NORR 的反应限速电位仅为0.55 eV，同时可有效抑 制表面HER 反应和氨氧化。希望我们的研究能够进一步推动h-BN 在催化领域的应用，为 合成氨领域的实验工作者提供一些指导。

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Acknowledgements

This study was financially supported by the Natural Science Foundation of China (No. 21603109), Henan Joint Fund of the National Natural Science Foundation of China (No. U1404216), and the Scientific Research Program Funded by Shaanxi Provincial Education Department (No. 20JK0676).

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  1. Institute of Environment and Energy Catalysis, Shaanxi Key Laboratory of Optoelectronic Functional Materials and Devices, School of Materials Science and Chemical Engineering, Xi’an Technological University, Xi’an, 710021, China

    Chao-Zheng He, Ya-Xing Zhang & Jia Wang

  2. College of Resources and Environmental Engineering, Tianshui Normal University, Tianshui, 741001, China

    Ling Fu

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He, CZ., Zhang, YX., Wang, J. et al. Anchor single atom in h-BN assist NO synthesis NH3: a computational view. Rare Met. 41, 3456–3465 (2022). https://doi.org/10.1007/s12598-022-02059-1

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