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Advanced MaterialsVolume 34, Issue 44 2203417 Research Article “Tree-Trunk” Design for Flexible Quasi-Solid-State Electrolytes with Hierarchical Ion-Channels Enabling Ultralong-Life Lithium-Metal Batteries Yun Zheng, Yun Zheng Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1 CanadaSearch for more papers by this authorNa Yang, Na Yang South China Academy of Advanced Optoelectronics, School of Information and Optoelectronic Science and Engineering, International Academy of Optoelectronics at Zhaoqing, South China Normal University, Guangzhou, 510006 ChinaSearch for more papers by this authorRui Gao, Rui Gao Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1 CanadaSearch for more papers by this authorZhaoqiang Li, Zhaoqiang Li Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1 CanadaSearch for more papers by this authorHaozhen Dou, Haozhen Dou Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1 Canada South China Academy of Advanced Optoelectronics, School of Information and Optoelectronic Science and Engineering, International Academy of Optoelectronics at Zhaoqing, South China Normal University, Guangzhou, 510006 ChinaSearch for more papers by this authorGaoran Li, Gaoran Li Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1 CanadaSearch for more papers by this authorLanting Qian, Lanting Qian Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1 CanadaSearch for more papers by this authorYaping Deng, Yaping Deng Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1 CanadaSearch for more papers by this authorJiequan Liang, Jiequan Liang South China Academy of Advanced Optoelectronics, School of Information and Optoelectronic Science and Engineering, International Academy of Optoelectronics at Zhaoqing, South China Normal University, Guangzhou, 510006 ChinaSearch for more papers by this authorLeixin Yang, Leixin Yang South China Academy of Advanced Optoelectronics, School of Information and Optoelectronic Science and Engineering, International Academy of Optoelectronics at Zhaoqing, South China Normal University, Guangzhou, 510006 ChinaSearch for more papers by this authorYizhou Liu, Yizhou Liu South China Academy of Advanced Optoelectronics, School of Information and Optoelectronic Science and Engineering, International Academy of Optoelectronics at Zhaoqing, South China Normal University, Guangzhou, 510006 ChinaSearch for more papers by this authorQianyi Ma, Qianyi Ma Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1 CanadaSearch for more papers by this authorDan Luo, Dan Luo South China Academy of Advanced Optoelectronics, School of Information and Optoelectronic Science and Engineering, International Academy of Optoelectronics at Zhaoqing, South China Normal University, Guangzhou, 510006 ChinaSearch for more papers by this authorNing Zhu, Ning Zhu Canadian Light Source, 44 Innovation Blvd, Saskatoon, SK, S7N 2V3 CanadaSearch for more papers by this authorKecheng Li, Kecheng Li Department of Chemical and Paper Engineering, Western Michigan University, 1903 W Michigan Ave, Kalamazoo, MI, 49008-5462 USASearch for more papers by this authorXin Wang, Corresponding Author Xin Wang [email protected] South China Academy of Advanced Optoelectronics, School of Information and Optoelectronic Science and Engineering, International Academy of Optoelectronics at Zhaoqing, South China Normal University, Guangzhou, 510006 China E-mail: [email protected]; [email protected]Search for more papers by this authorZhongwei Chen, Corresponding Author Zhongwei Chen [email protected] orcid.org/0000-0003-3463-5509 Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1 Canada E-mail: [email protected]; [email protected]Search for more papers by this author Yun Zheng, Yun Zheng Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1 CanadaSearch for more papers by this authorNa Yang, Na Yang South China Academy of Advanced Optoelectronics, School of Information and Optoelectronic Science and Engineering, International Academy of Optoelectronics at Zhaoqing, South China Normal University, Guangzhou, 510006 ChinaSearch for more papers by this authorRui Gao, Rui Gao Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1 CanadaSearch for more papers by this authorZhaoqiang Li, Zhaoqiang Li Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1 CanadaSearch for more papers by this authorHaozhen Dou, Haozhen Dou Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1 Canada South China Academy of Advanced Optoelectronics, School of Information and Optoelectronic Science and Engineering, International Academy of Optoelectronics at Zhaoqing, South China Normal University, Guangzhou, 510006 ChinaSearch for more papers by this authorGaoran Li, Gaoran Li Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1 CanadaSearch for more papers by this authorLanting Qian, Lanting Qian Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1 CanadaSearch for more papers by this authorYaping Deng, Yaping Deng Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1 CanadaSearch for more papers by this authorJiequan Liang, Jiequan Liang South China Academy of Advanced Optoelectronics, School of Information and Optoelectronic Science and Engineering, International Academy of Optoelectronics at Zhaoqing, South China Normal University, Guangzhou, 510006 ChinaSearch for more papers by this authorLeixin Yang, Leixin Yang South China Academy of Advanced Optoelectronics, School of Information and Optoelectronic Science and Engineering, International Academy of Optoelectronics at Zhaoqing, South China Normal University, Guangzhou, 510006 ChinaSearch for more papers by this authorYizhou Liu, Yizhou Liu South China Academy of Advanced Optoelectronics, School of Information and Optoelectronic Science and Engineering, International Academy of Optoelectronics at Zhaoqing, South China Normal University, Guangzhou, 510006 ChinaSearch for more papers by this authorQianyi Ma, Qianyi Ma Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1 CanadaSearch for more papers by this authorDan Luo, Dan Luo South China Academy of Advanced Optoelectronics, School of Information and Optoelectronic Science and Engineering, International Academy of Optoelectronics at Zhaoqing, South China Normal University, Guangzhou, 510006 ChinaSearch for more papers by this authorNing Zhu, Ning Zhu Canadian Light Source, 44 Innovation Blvd, Saskatoon, SK, S7N 2V3 CanadaSearch for more papers by this authorKecheng Li, Kecheng Li Department of Chemical and Paper Engineering, Western Michigan University, 1903 W Michigan Ave, Kalamazoo, MI, 49008-5462 USASearch for more papers by this authorXin Wang, Corresponding Author Xin Wang [email protected] South China Academy of Advanced Optoelectronics, School of Information and Optoelectronic Science and Engineering, International Academy of Optoelectronics at Zhaoqing, South China Normal University, Guangzhou, 510006 China E-mail: [email protected]; [email protected]Search for more papers by this authorZhongwei Chen, Corresponding Author Zhongwei Chen [email protected] orcid.org/0000-0003-3463-5509 Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1 Canada E-mail: [email protected]; [email protected]Search for more papers by this author First published: 28 July 2022 https://doi.org/10.1002/adma.202203417Citations: 8Read the full textAboutPDF ToolsRequest permissionExport citationAdd to favoritesTrack citation ShareShare Give accessShare full text accessShare full-text accessPlease review our Terms and Conditions of Use and check box below to share full-text version of article.I have read and accept the Wiley Online Library Terms and Conditions of UseShareable LinkUse the link below to share a full-text version of this article with your friends and colleagues. Learn more.Copy URL Abstract The construction of robust (quasi)-solid-state electrolyte (SSE) for flexible lithium-metal batteries is desirable but extremely challenging. Herein, a novel, flexible, and robust quasi-solid-state electrolyte (QSSE) with a “tree-trunk” design is reported for ultralong-life lithium-metal batteries (LMBs). An in-situ-grown metal–organic framework (MOF) layer covers the cellulose-based framework to form hierarchical ion-channels, enabling rapid ionic transfer kinetics and excellent durability. A conductivity of 1.36 × 10−3 S cm−1, a transference number of 0.72, an electrochemical window of 5.26 V, and a good rate performance are achieved. The flexible LMBs fabricated with as-designed QSSEs deliver areal capacity of up to 3.1 mAh cm−2 at the initial cycle with high mass loading of 14.8 mg cm−2 in Li-NCM811 cells and can retain ≈80% capacity retention after 300 cycles. An ultralong-life of 3000 cycles (6000 h) is also achieved in Li-LiFePO4 cells. 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Citing Literature Supporting Information Filename Description adma202203417-sup-0001-SuppMat.pdf2.2 MB Supporting Information Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article. Volume34, Issue44November 3, 20222203417 ReferencesRelatedInformation