Asymmetric quasi-solid-state composite electrolytes via selfassembly of molecular brushes and hairy nanoparticles for dendrite-free lithium metal batteriesOA
The practical application of lithium metal batteries is severely hindered by flammable liquid electrolytes and uncontrollable lithium dendrite growth.In this study,we propose a novel asymmetric quasi-solid-state composite electrolyte(denoted as QSCE-BPL/LPE/PDL)designed to overcome these challenges.QSCE-BPL/LPE/PDL is fabricated by evaporation-induced self-assembly of one-dimensional molecular brush BC-g-PLiSTFSI[BC=bacterial cellulose,PLiSTFSI=poly(lithium 4-styrenesulfonyl-(trifluoromethylsulfonyl)imide)]and zero-dimensional hairy nanoparticle LL-g-PEGMA[LL=Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12),PEGMA=poly(oligo(ethylene glycol)methyl ether methacrylate)],followed by in situ cationic ring-opening polymerization of 1,3-dioxolane.The resulting ultrathin QSCE-BPL/LPE/PDL(19μm)possesses a unique asym-metric architecture comprising a rigid layer of hairy nanoparticles to suppress dendrite penetration and a composite layer to ensure good interfacial contact with the cathode.The grafted PLiSTFSI side chains enable single Li+conduction to reduce concentration polarization,and the PEGMA side chains promote lithium salt dissociation to accelerate Li+trans-port.This design yields a three-dimensional porous network that provides continuous and fast Li+transport pathways.The optimized electrolyte achieves a high ionic conductivity of 5.44×10^(−4) S cm^(−1) and a Li+transference number of 0.67 at room temperature.Consequently,Li/LiFePO_(4) cells with QSCE-BPL/LPE/PDL can operate stably for 200 cycles with a high-capacity retention of 94%at 0.5 C.This study provides a feasible molecular engineering strategy for developing high-performance and safe lithium metal batteries.
Shenghao Lin;Yin Cui;Guofang Yu;Dongtian Miao;Ruliang Liu;Dingcai Wu
PCFM Lab and GDHPRC Lab,School of Chemistry,Sun Yat-sen University,Guangzhou 510006,ChinaPCFM Lab and GDHPRC Lab,School of Chemistry,Sun Yat-sen University,Guangzhou 510006,ChinaPCFM Lab and GDHPRC Lab,School of Chemistry,Sun Yat-sen University,Guangzhou 510006,ChinaPCFM Lab and GDHPRC Lab,School of Chemistry,Sun Yat-sen University,Guangzhou 510006,ChinaSchool of Chemistry and Materials Science,Guangdong University of Education,Guangzhou 510303,ChinaPCFM Lab and GDHPRC Lab,School of Chemistry,Sun Yat-sen University,Guangzhou 510006,China
信息技术与安全科学
quasi-solid-state composite electrolytemolecular brushhairy nanoparticlelithium metal battery
《Energy Materials and Devices》 2026 (2)
P.43-52,10
supported by the National Key Research and Development Program of China(Grant No.2021YFF0500600)the National Natural Science Foundation of China(Grant No.52533009)the Guangdong Major Project of Basic and Applied Basic Research(Grant No.2023B0303000025)the Natural Science Foundation of Guangdong(Grant Nos.2024B1515020023 and 2023A1515030160)the Fundamental Research Funds for the Central Universities,Sun Yat-sen University(Grant Nos.23yxqntd002 and 23lgbj004)the Science and Technology Program of Guangzhou(Grant No.2024A04J10003)the Guangdong Basic Research Center of Excellence for Functional Molecular Engineering.The authors thank the Instrumental Analysis&Research Center,Sun Yat-sen University.
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