水诱导固体电解质界面调控的连续流电化学合成氨

刘鹏博, 翟盛良, 黄继, 张衷硕, 曾杰, 李少锋

doi:10.61558/2993-074X.3605

电化学 >

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DOI: https://doi.org/10.61558/2993-074X.3605

Nitrogen Fixation

水诱导固体电解质界面调控的连续流电化学合成氨

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a. 精准智能化学全国重点实验室, 化学与材料科学学院, 安徽省合肥市，230026, 中华人民共和国;

b. 合肥微尺度物质科学国家研究中心, 中科院强耦合量子材料物理重点实验室, 安徽省高等学校表面与界面化学与能源催化重点实验室, 化学物理系, 中国科学技术大学, 安徽省合肥市, 230026, 中华人民共和国;

c. 化学与化工学院, 安徽工业大学, 安徽省马鞍山市, 243002, 中华人民共和国;

d. 深空探测实验室, 安徽省合肥市, 230088, 中华人民共和国.

网络出版日期: 2026-02-13

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Water-driven Solid Electrolyte Interphase Governs Continuous-flow Ammonia Electrosynthesis

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a. State Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China;

b. Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China;

c. School of Chemistry & Chemical Engineering, Anhui University of Technology, Ma’anshan, Anhui 243002, P. R. China;

d. Deep Space Exploration Laboratory, Hefei 230088, P. R. China.

Online published: 2026-02-13

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摘要

连续流反应器可实现锂介导氮还原反应（Li-NRR）在常温常压下的连续运行，为替代哈伯-博施工艺提供了潜在方案。然而，该体系对电解液中痕量水分高度敏感，水含量的微小波动即会显著改变界面化学过程并影响反应性能。本研究系统考察了电解液初始水含量对连续流Li-NRR性能的影响机制。结果显示，过高的水含量会促进固体电解质界面层（SEI）增厚，阻碍氮气传质与锂离子传导，导致法拉第效率由61%骤降至3%。该机理认识揭示了痕量水在SEI演化中的关键调控作用，强调了精确控水对高效连续流Li-NRR的必要性。

关键词： 水; 固体电解质界面层; 连续流反应器; 锂介导氮还原; 合成氨

本文引用格式

刘鹏博, 翟盛良, 黄继, 张衷硕, 曾杰, 李少锋 . 水诱导固体电解质界面调控的连续流电化学合成氨[J]. 电化学, 0 : 0 -0 . DOI: 10.61558/2993-074X.3605

Abstract

Flow-cell architectures have emerged as a powerful platform for continuous and stable lithium-mediated nitrogen reduction (Li-NRR), enabling ambient-condition electrochemical ammonia synthesis and offering a promising alternative to Haber-Bosch processes. However, Li-NRR is exceptionally sensitive to trace water, and even minor variations in water content can profoundly alter interfacial chemistry. Here, we systematically investigate how initial water concentration affects Li-NRR performance in a continuous-flow cell. Excess water drives the formation of a thick solid electrolyte interphase (SEI) layer, which may impede nitrogen access to metallic lithium and hinder lithium-ion transport. As a result, the ammonia Faradaic efficiency collapses from ~61% to ~3%. These findings reveal the decisive, previously underappreciated role of water in governing SEI evolution and highlight the necessity of precise water control for achieving stable, high-efficiency continuous-flow Li-NRR.

Key words： water; solid electrolyte interphase; continuous-flow cell; lithium-mediated nitrogen reduction; ammonia synthesis

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