Nanocrystals with Aggregate Anionic Structure Enable Ion Transport Decoupling of Chain Segment Movement in Poly(ethylene oxide) Electrolytes
Jinze Hou
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorDr. Weiwei Xie
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorLong Shang
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorShuang Wu
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorYuewei Cui
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorDr. Yixin Li
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorProf. Zhenhua Yan
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorProf. Kai Zhang
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorCorresponding Author
Prof. Yong Lu
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorCorresponding Author
Prof. Jun Chen
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorJinze Hou
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorDr. Weiwei Xie
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorLong Shang
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorShuang Wu
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorYuewei Cui
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorDr. Yixin Li
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorProf. Zhenhua Yan
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorProf. Kai Zhang
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorCorresponding Author
Prof. Yong Lu
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorCorresponding Author
Prof. Jun Chen
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 China
Search for more papers by this authorAbstract
All-solid-state polymer electrolytes are promising for lithium batteries, but Li+ transport in these electrolytes relies on amorphous chain segment movement, leading to low Li+ mobility and poor mechanical strength. Here we propose a novel Li+ transport mechanism mediated by PEO3:LiBF4 nanocrystals (NCPB) with the aggregate (AGG) anionic structure, which enables a change from amorphous to crystalline phase dominated ion transport in all-solid-state PEO/LiBF4 electrolyte. Experiments and simulations reveal that the interaction between Li+ and F in NCPB with AGG anionic structure simultaneously restricts anion transport and reorients anions within the free volume of NCPB, resulting in a three-coordination intermediate to facilitate Li+ transport. The unique Li+ transport mechanism through NCPB makes the PEO/LiBF4 electrolyte with a high Li+ transference number (0.73) and remarkably increased mechanical strength (storage modulus >100 MPa) at 45 °C. As a result, the Li|LiFePO4 batteries with the ultrathin self-supported PEO/LiBF4 electrolyte (10 μm) exhibit significantly improved cycle life (97 % @ 468 cycles) compared to those with PEO/LiTFSI electrolyte (failed @ 68 cycles). This work demonstrates a novel ion transport mechanism for achieving selective and rapid Li+ transport.
Conflict of Interests
The authors declare no conflict of interest.
Open Research
Data Availability Statement
The data that support the findings of this study are available from the corresponding author upon reasonable request.
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