Driving inward growth of lithium metal in hollow microcapsule hosts by heteroatom-controlled nucleation
作者机构：Hanyang Univ Div Mat Sci & Engn 222 Wangsimni Ro Seoul 04763 South Korea Daegu Gyeongbuk Inst Sci & Technol DGIST Dept Energy Sci & Engn Daegu South Korea Sungkyunkwan Univ Dept Energy Sci 2066 Seobu Ro Suwon 16419 South Korea Kyung Hee Univ Dept Adv Mat Engn Informat & Elect Integrated Educ Frontier Sci & Technol BK21 Four 1732 Deogyeong Daero Yongin 17104 South Korea
出 版 物：《CARBON ENERGY》 (碳能源（英文）)
年 卷 期：2024年第6卷第8期
页 面：262-272页
核心收录：
学科分类：0820[工学-石油与天然气工程] 08[工学] 0805[工学-材料科学与工程（可授工学、理学学位）] 080502[工学-材料学] 0703[理学-化学]
基 金：National Research Foundation [NRF-2018R1A5A1025594 NRF-2022M3J1A106264]
主 题：hollow carbon hosts lithium metal batteries lithium plating metal-organic frameworks nucleation CARBON NANOSTRUCTURES SPECTRA ROUTE XPS
摘 要：The application of Li metal anodes in rechargeable batteries is impeded by safety issues arising from the severe volume changes and formation of dendritic Li deposits. Three-dimensional hollow carbon is receiving increasing attention as a host material capable of accommodating Li metal inside its cavity; however, uncontrollable and nonuniform deposition of Li remains a challenge. In this study, we synthesize metal-organic framework-derived carbon microcapsules with heteroatom clusters (Zn and Ag) on the capsule walls and it is demonstrated that Ag-assisted nucleation of Li metal alters the outward-to-inward growth in the microcapsule host. Zn-incorporated microcapsules are prepared via chemical etching of zeolitic imidazole framework-8 polyhedra and are subsequently decorated with Ag by a galvanic displacement reaction between Ag+ and metallic Zn. Galvanically introduced Ag significantly reduces the energy barrier and increases the reaction rate for Li nucleation in the microcapsule host upon Li plating. Through combined electrochemical, microstructural, and computational studies, we verify the beneficial role of Ag-assisted Li nucleation in facilitating inward growth inside the cavity of the microcapsule host and, in turn, enhancing electrochemical performance. This study provides new insights into the design of reversible host materials for practical Li metal batteries. A metal-organic framework-derived hollow carbon microcapsule host with lithiophilic heteroatom for Li metal anodes is designed and synthesized using a combination of chemical etching, pyrolysis, and galvanic displacement reaction. Benefiting from the spacious hollow cavity and lithiophilic properties on the inner surface of the carbon shell, the inward growth of Li is prompted, facilitating reversible Li storage. image
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