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 

机构地区：[1]School of Chemistry,South China Normal University,Guangzhou 510006,China [2]Henan Key Laboratory of Crystalline Molecular Functional Materials,Henan International Joint Laboratory of Tumor Theranostical Cluster Materials,Green Catalysis Center,College of Chemistry,Zhengzhou University,Zhengzhou 450001,China [3]State Key Laboratory of Materials Processing and Die&Mould Technology,School of Materials Science and Engineering,Huazhong University of Science and Technology,Wuhan 430074,China

出　　处：《National Science Review》2025年第2期149-158,共10页国家科学评论(英文版)

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).

摘　　要：High-voltage lithium-metal batteries(HVLMBs)are appealing candidates for next-generation high-energy rechargeable batteries,but their practical applications are stilllimited 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^(−2) over 3500 h.The LiFePO_(4)(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 LiNi_(0.8) Co_(0.1) Mn_(0.1) O_(2)||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^(−1) and 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.

关 键 词：conjugated phthalocyanine artificial SEI high energy density lithium-metal battery 

分 类 号：TM9[电气工程—电力电子与电力传动]