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从氮分子进行电合成氨:进展、挑战与未来展望。

NH Electrosynthesis from N Molecules: Progresses, Challenges, and Future Perspectives.

作者信息

Ren Yongwen, Li Shaofeng, Yu Chang, Zheng Yihan, Wang Cheng, Qian Bingzhi, Wang Linshan, Fang Wenhui, Sun Ying, Qiu Jieshan

机构信息

State Key Laboratory of Fine Chemicals, Liaoning Key Lab for Energy Materials and Chemical Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China.

Department of Physics, Technical University of Denmark, Kongens Lyngby 2800, Denmark.

出版信息

J Am Chem Soc. 2024 Mar 13;146(10):6409-6421. doi: 10.1021/jacs.3c11676. Epub 2024 Feb 27.

Abstract

Green ammonia (NH), made by using renewable electricity to split nearly limitless nitrogen (N) molecules, is a vital platform molecule and an ideal fuel to drive the sustainable development of human society without carbon dioxide emission. The NH electrosynthesis field currently faces the dilemma of low yield rate and efficiency; however, decoupling the overlapping issues of this area and providing guidelines for its development directions are not trivial because it involves complex reaction process and multidisciplinary entries (for example, electrochemistry, catalysis, interfaces, processes, etc.). In this Perspective, we introduce a classification scheme for NH electrosynthesis based on the reaction process, namely, direct (N reduction reaction) and indirect electrosynthesis (Li-mediated/plasma-enabled NH electrosynthesis). This categorization allows us to finely decouple the complicated reaction pathways and identify the specific rate-determining steps/bottleneck issues for each synthesis approach such as N activation, H evolution side reaction, solid-electrolyte interphase engineering, plasma process, etc. We then present a detailed overview of the latest progresses on solving these core issues in terms of the whole electrochemical system covering the electrocatalysts, electrodes, electrolytes, electrolyzers, etc. Finally, we discuss the research focuses and the promising strategies for the development of NH electrosynthesis in the future with a multiscale perspective of atomistic mechanisms, nanoscale electrocatalysts, microscale electrodes/interfaces, and macroscale electrolyzers/processes. It is expected that this Perspective will provide the readers with an in-depth understanding of the bottleneck issues and insightful guidance on designing the efficient NH electrosynthesis systems.

摘要

绿色氨(NH₃)通过利用可再生电力分解几乎无穷无尽的氮(N)分子制得,它是一种至关重要的平台分子,也是推动人类社会可持续发展且无二氧化碳排放的理想燃料。目前,氨电合成领域面临着产率和效率低下的困境;然而,厘清该领域重叠的问题并为其发展方向提供指导并非易事,因为这涉及复杂的反应过程和多学科领域(例如,电化学、催化、界面、工艺等)。在这篇观点文章中,我们基于反应过程介绍了一种氨电合成的分类方案,即直接(氮还原反应)和间接电合成(锂介导/等离子体辅助氨电合成)。这种分类使我们能够精细地拆解复杂的反应路径,并确定每种合成方法的特定速率决定步骤/瓶颈问题,如氮活化、析氢副反应、固体电解质界面工程、等离子体过程等。然后,我们从涵盖电催化剂、电极、电解质、电解槽等的整个电化学系统角度,详细概述了解决这些核心问题的最新进展。最后,我们从原子机制、纳米级电催化剂、微米级电极/界面和宏观级电解槽/工艺的多尺度视角,讨论了未来氨电合成发展的研究重点和有前景的策略。期望这篇观点文章能够让读者深入理解瓶颈问题,并为设计高效氨电合成系统提供有见地的指导。

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