Ammonia synthesis from nitrate reduction by the modulation of a built-in electric field and external stimuli

EES catalysis Pub Date : 2025-01-07 DOI:10.1039/D4EY00245H
Shaoce Zhang, Rong Zhang, Ying Guo and Chunyi Zhi
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Abstract

Ammonia (NH3) is a vital chemical feedstock and a carbon-free energy source. The reduction of nitrate (NO3) from environmental pollutants is a sustainable method for NH3 production compared with the industrially intensive Haber–Bosch method, which can mitigate energy and environmental concerns. However, due to the involvement of multi-electron transfer-proton coupling processes, the NO3 reduction reaction (NO3RR) exhibits sluggish kinetics and significant side reactions. This review provides a comprehensive summary of recent research progress in facilitating NO3RRs using a built-in electric field and external stimuli. The paper commences by introducing the mechanisms and challenges of the NO3RR, subsequently focusing on strategies for built-in electric field/external stimuli-assisted catalytic reactions. The internal electric field can be triggered by constructing a Mott–Schottky heterojunction and a semiconductor–semiconductor heterojunction, adjusting the coordination environment of active sites, and regulating the electrical double layer, while the external stimuli include optical, stress, and thermal stimuli. This review focuses on the activation and adsorption processes of reactants and intermediates by a built-in electric field/external stimuli, and their influence on the thermodynamics and kinetics of reactions. Finally, we summarize the strategies for built-in electric field/external stimuli-assisted NO3RRs, highlight the challenges of achieving high activity and selectivity in NH3 production, and provide clear guidance for future research.

Abstract Image

由内建电场和外部刺激调制的硝酸还原合成氨
氨(NH3)是一种重要的化工原料和无碳能源。与工业密集型的Haber-Bosch方法相比,从环境污染物中还原硝酸盐(NO3−)是一种可持续的NH3生产方法,可以减轻能源和环境问题。然而,由于多电子转移-质子耦合过程的参与,NO3−还原反应(NO3RR)表现出缓慢的动力学和明显的副反应。本文综述了利用内置电场和外部刺激促进NO3RRs的最新研究进展。本文首先介绍了NO3RR的机理和挑战,然后重点介绍了内置电场/外部刺激辅助催化反应的策略。内部电场可以通过构建Mott-Schottky异质结和半导体-半导体异质结、调节活性位点的配位环境和调节双电层来触发,而外部刺激包括光学、应力和热刺激。本文综述了内建电场/外部刺激对反应物和中间体的活化和吸附过程及其对反应热力学和动力学的影响。最后,我们总结了内建电场/外部刺激辅助no3rs的策略,强调了在NH3生产中实现高活性和选择性的挑战,并为未来的研究提供了明确的指导。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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