Han Bo, Liu Jiawei, Lee Carmen, Lv Chade, Yan Qingyu
SCARCE Laboratory, Energy Research Institute @ NTU (ERI@N), Nanyang Technological University, Singapore, 637459, Singapore.
School of Materials Science and Engineering, Nanyang Technological University, Singapore, 639798, Singapore.
Small Methods. 2023 Sep;7(9):e2300277. doi: 10.1002/smtd.202300277. Epub 2023 May 18.
The production of ammonia under moderate conditions is of environmental and sustainable importance. The electrochemical nitrogen reduction reaction (E-NRR) method has been intensively investigated in the recent decades. Nowadays, the further development of E-NRR is largely hindered by the lack of competent electrocatalysts. Metal-organic frameworks (MOFs) are considered as the next-generation catalysts for E-NRR, featuring their tailorable structures, abundant active sites and favorable porosity. To present a comprehensive review on both the fundamental and advanced development in MOFs catalyst-based E-NRR field, this paper first introduces the basic principles of E-NRR, including the reaction mechanism, major apparatus components, performance criteria, and ammonia detection protocols. Next, the synthesis and characterization methods for MOFs and their derivatives are discussed. In addition, a reaction mechanism study via density functional theory calculations is also presented. After that, the recent advancement of MOF-based catalysts in the E-NRR field as well as the modification approaches on MOFs for E-NRR optimization is elaborated. Finally, the current challenges and outlook of MOF catalyst-based E-NRR field are emphasized.
在温和条件下生产氨具有环境和可持续发展的重要意义。近几十年来，电化学氮还原反应（E-NRR）方法受到了广泛研究。如今，E-NRR的进一步发展在很大程度上受到缺乏有效电催化剂的阻碍。金属有机框架（MOF）因其可定制的结构、丰富的活性位点和良好的孔隙率而被视为E-NRR的下一代催化剂。为了全面综述基于MOF催化剂的E-NRR领域的基础和前沿发展，本文首先介绍了E-NRR的基本原理，包括反应机理、主要仪器部件、性能标准和氨检测方法。接下来，讨论了MOF及其衍生物的合成和表征方法。此外，还介绍了通过密度泛函理论计算进行的反应机理研究。之后，阐述了基于MOF的催化剂在E-NRR领域的最新进展以及对MOF进行E-NRR优化的改性方法。最后，强调了基于MOF催化剂的E-NRR领域当前面临的挑战和前景。
