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Bidirectionally Compatible Buffering Layer Enables Highly Stable and Conductive Interface for 4.5 V Sulfide‐Based All‐Solid‐State Lithium Batteries
Author(s) -
Wang Longlong,
Sun Xingwei,
Ma Jun,
Chen Bingbing,
Li Chao,
Li Jiedong,
Chang Liang,
Yu Xinrun,
Chan TingShan,
Hu Zhiwei,
Noked Malachi,
Cui Guanglei
Publication year - 2021
Publication title -
advanced energy materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.08
H-Index - 220
eISSN - 1614-6840
pISSN - 1614-6832
DOI - 10.1002/aenm.202100881
Subject(s) - materials science , sulfide , interphase , electrochemistry , electrolyte , fast ion conductor , compatibility (geochemistry) , lithium (medication) , solid state , chemical engineering , electrode , nanotechnology , chemistry , composite material , medicine , genetics , engineering , metallurgy , biology , endocrinology
High‐voltage all‐solid‐state lithium batteries (HVASSLBs) are considered attractive systems for portable electronics and electric vehicles, due to their theoretically high energy density and safety. However, realization of HVASSLBs with sulfide solid electrolytes (SEs) is hindered by their limited electrochemical stability, resulting in sluggish interphase dynamics. Here, a bidirectionally compatible buffering layer design scheme is proposed to overcome the interfacial challenges of sulfide‐based HVASSLBs. As a proof of concept, it is found that NASICON‐type Li x Zr 2 (PO 4 ) 3 surprisingly exhibit great compatibility with both 4.5 V LiCoO 2 and Li 6 PS 5 Cl, based on the results of first‐principles calculations and various in situ/ex situ characterizations. This compatibility significantly restrains the interface reactivity and boosts interfacial Li‐ion transport. Therefore, 4.5 V sulfide‐based HVASSLBs can exhibit remarkably enhanced initial discharge capacity (143.3 vs 125.9 mAh·g −1 at 0.2C), capacity retention (95.53% vs 74.74% after 100 cycles), and rate performance (97 vs 45 mAh·g −1 at 2C). This work sheds light on the great prospects of sulfide‐based HVASSLBs with high‐rate characteristics, and constitutes a crucial step toward the rational design of interface and interphase chemistry for high‐performance sulfide‐based HVASSLBs.