首页|Constructing high-toughness polyimide binder with robust polarity and ion-conductive mechanisms ensuring long-term operational stability of silicon-based anodes

Constructing high-toughness polyimide binder with robust polarity and ion-conductive mechanisms ensuring long-term operational stability of silicon-based anodes

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Silicon-based materials have demonstrated remarkable potential in high-energy-density batteries owing to their high theoretical capacity.However,the significant volume expansion of silicon seriously hinders its utilization as a lithium-ion anode.Herein,a functionalized high-toughness polyimide(PDMI)is syn-thesized by copolymerizing the 4,4'-Oxydiphthalic anhydride(ODPA)with 4,4'-oxydianiline(ODA),2,3-diaminobenzoic acid(DABA),and 1,3-bis(3-aminopropyl)-tetramethyl disiloxane(DMS).The combi-nation of rigid benzene rings and flexible oxygen groups(-O-)in the PDMI molecular chain via a rigidness/softness coupling mechanism contributes to high toughness.The plentiful polar carboxyl(-COOH)groups establish robust bonding strength.Rapid ionic transport is achieved by incorporating the flexible siloxane segment(Si-O-Si),which imparts high molecular chain motility and augments free volume holes to facilitate lithium-ion transport(9.8×10-10 cm2 s-1 vs.16×10-10 cm2 s-1).As expected,the SiOx@PDMI-1.5 electrode delivers brilliant long-term cycle performance with a remarkable capacity retention of 85%over 500 cycles at 1.3 A g-1.The well-designed functionalized polyimide also signifi-cantly enhances the electrochemical properties of Si nanoparticles electrode.Meanwhile,the assembled SiOx@PDMI-1.5/NCM811 full cell delivers a high retention of 80%after 100 cycles.The perspective of the binder design strategy based on polyimide modification delivers a novel path toward high-capacity elec-trodes for high-energy-density batteries.

Polyimide binderHigh toughnessRobust ionic transportSilicon-based anodesLithium-ion batteries

Yongjun Kang、Nanxi Dong、Fangzhou Liu、Daolei Lin、Bingxue Liu、Guofeng Tian、Shengli Qi、Dezhen Wu

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State Key Laboratory of Chemical Resource Engineering,Beijing University of Chemical Technology,Beijing 100029,China

ENFI R&D Institute,China ENFI Engineering Corporation,Beijing 100038,China

China Automotive Battery Research Institute Co.,Ltd.,Beijing 101407,China

Changzhou Institute of Advanced Materials,Beijing University of Chemical Technology,Changzhou 213164,Jiangsu,China

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National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaFundamental Research Funds for the Central UniversitiesNatural Science Foundation of Jiangsu Province

5167301721404005XK1802-2BK20150273

2024

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子:0.654
ISSN:2095-4956
年,卷(期):2024.93(6)
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