水诱导固体电解质界面调控的连续流电化学合成氨OA
Water-Driven Solid Electrolyte Interphase Governs Continuous-Flow Ammonia Electrosynthesis
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.
Flow-cell architectures have emerged as a powerful platform for continuous and stable lithium-mediated nitrogen re-duction(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 con-tent 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.
刘鹏博;翟盛良;黄继;张衷硕;曾杰;李少锋
精准智能化学全国重点实验室,化学与材料科学学院,安徽 合肥 230026,中华人民共和国精准智能化学全国重点实验室,化学与材料科学学院,安徽 合肥 230026,中华人民共和国||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,中国科学技术大学化学物理系,安徽 合肥 230026,中华人民共和国精准智能化学全国重点实验室,化学与材料科学学院,安徽 合肥 230026,中华人民共和国精准智能化学全国重点实验室,化学与材料科学学院,安徽 合肥 230026,中华人民共和国||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,中国科学技术大学化学物理系,安徽 合肥 230026,中华人民共和国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,中国科学技术大学化学物理系,安徽 合肥 230026,中华人民共和国||安徽工业大学化学与化工学院,安徽 马鞍山 243002,中华人民共和国||深空探测实验室,安徽 合肥 230088,中华人民共和国精准智能化学全国重点实验室,化学与材料科学学院,安徽 合肥 230026,中华人民共和国
水固体电解质界面层连续流反应器锂介导氮还原合成氨
WaterSolid electrolyte interphaseContinuous-flow cellLithium-mediated nitrogen reductionAmmonia synthesis
《电化学（中英文）》 2026 (4)
1-11,11
Shao-Feng Li acknowledges the National Natural Science Foundation of China(22579157),the robotic AI-Scientist platform of the Chinese Academy of Sci-ences,the Fundamental Research Funds for the Cen-tral Universities(WK2060250114),the Major Frontier Research Project of the University of Science and Tech-nology of China(LS2060000002).This work was sup-ported by National Key Research and Development Program of China(2021YFA1500500),CAS Project for Young Scientists in Basic Research(YSBR-051),NSFC(22525021,22221003,22250007,22361162655),the Science and Technology Development Fund(FDCT)of Macao S.A.R(0070/2023/AFJ),Fundamental Re-search Funds for the Central Universities,the State Key Laboratory of Catalysis(2024SKL-A-011),and In-ternational Partnership Program of Chinese Academy of Sciences(123GJHZ2022101GC).Jie Zeng acknowl-edges support from the New Cornerstone Science Foundation through the XPLORER PRIZE.This work was partially carried out at the Instruments Center for Physical Science,University of Science and Tech-nology of China.This work was also partially carried out at the USTC Center for Micro and Nanoscale Re-search and Fabrication.We thank Sheng-Quan Fu at Instruments Center for Physical Science,University of Science and Technology of China for provision air-sensitive sample transfer system equipped on CIQTEK Co.,Ltd.,FESEM5000X to complete SEM surface picture and EDS measurements and charac-terizations.Sheng-Liang Zhai acknowledges the Chi-na Postdoctoral Science Foundation(2025M781033).
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