Conjugated phthalocyanine-based framework as artificial SEI for over 400 Wh kg-1 lithium-metal battery

作     者：Ying Zang Peng Peng Fei Pei Run-Han Li Lin Wu Di-Qiu Lu Yi Zhang Kai Huang Yue Shen Yun-Hui Huang Ya-Qian Lan Ying Zang;Peng Peng;Fei Pei;Run-Han Li;Lin Wu;Di-Qiu Lu;Yi Zhang;Kai Huang;Yue Shen;Yun-Hui Huang;Ya-Qian Lan

作者机构：School of ChemistrySouth China Normal University Henan Key Laboratory of Crystalline Molecular Functional MaterialsHenan International Joint Laboratory of Tumor Theranostical Cluster MaterialsGreen Catalysis Center College of Chemistry Zhengzhou University State Key Laboratory of Materials Processing and Die&Mould TechnologySchool of Materials Science and EngineeringHuazhong University of Science and Technology 

出 版 物：《National Science Review》 (国家科学评论(英文版))

年 卷 期：2025年第12卷第2期

页      面：155-164页

核心收录：

学科分类：0808[工学-电气工程] 081704[工学-应用化学] 08[工学] 0817[工学-化学工程与技术] 

基　　金：supported by the National Key R&D Program of China (2023YFA1507204) the National Natural Science Foundation of China (22225109, 22201084 and 52202236) China Postdoctoral Science Foundation (2022M711232,2023M731155, 2023T160236 and 2024T170300) 

主　　题：conjugated phthalocyanine artificial SEI high energy density lithium-metal battery 

摘      要：High-voltage lithium-metal batteries（HVLMBs） are appealing candidates for next-generation high-energy rechargeable batteries, but their practical applications are still limited by the severe capacity degradation,attributed to the poor interfacial stability and compatibility between the electrode and the electrolyte. In this work, a 2D conjugated phthalocyanine framework（CPF） containing single atoms（SAs） of cobalt（CoSAs-CPF） is developed as a novel artificial solid–electrolyte interphase（SEI） in which a large amount of charge is transferred to the CPF skeleton due to the Lewis acid activity of the Co metal sites and the strong electron-absorbing property of the cyano group（-CN）, greatly enhancing the adsorption of the Li+and regulating the Li+distribution toward dendrite-free LMBs, which are superior to most of the reported SEI membranes. As a result, the Li||Li symmetrical cell with CoSAs-CPF-modified Li anodes（CoSAs-CPF@Li） exhibits a low polarization with an area capacity of 1.0 mAh cm-2over 3500 h. The LiFePO4（LFP） ||CoSAs-CPF@Li(LFP: 20 mg cm-2) delivers an ultra-long cycling life of ≤1000 cycles with a high capacity retention of 98.6%. Remarkably, the high-voltage LiNi0.8Co0.1Mn0.1O2||Li@CoSAs-CPF(NCM811: 10 mg cm-2) demonstrates a long cycling life of 800 cycles with a high capacity retention of 80%. Meanwhile, in situ ultrasonic transmission technology confirms the admirable ability of artificial CoSAs-CPF SEI to stabilize the Li-anode interface in pouch cells during cycling. Remarkably, the NCM811||Li@CoSAs-CPF pouch cell exhibits an energy density of 421 Wh kg-1and keeps 130 cycles with a low electrolyte/capacity ratio of 2.5 g Ah-1. The strategy of constructing the CoSAs-CPF-reinforced Li anode provides a promising direction for high-energy-density HVLMBs with long cycling stability.