Data-driven exploration of weak coordination microenvironment in solid-state electrolyte for safe and energy-dense batteries
Abstract The unsatisfactory ionic conductivity of solid polymer electrolytes hinders their practical use as substitutes for liquid electrolytes to address safety concerns. Although various plasticizers have been introduced to improve lithium-ion conduction kinetics, the lack of microenvironment unde...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-55633-9 |
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| author | Zhoujie Lao Kehao Tao Xiao Xiao Haotian Qu Xinru Wu Zhiyuan Han Runhua Gao Jian Wang Xian Wu An Chen Lei Shi Chengshuai Chang Yanze Song Xiangyu Wang Jinjin Li Yanfei Zhu Guangmin Zhou |
| author_facet | Zhoujie Lao Kehao Tao Xiao Xiao Haotian Qu Xinru Wu Zhiyuan Han Runhua Gao Jian Wang Xian Wu An Chen Lei Shi Chengshuai Chang Yanze Song Xiangyu Wang Jinjin Li Yanfei Zhu Guangmin Zhou |
| author_sort | Zhoujie Lao |
| collection | DOAJ |
| description | Abstract The unsatisfactory ionic conductivity of solid polymer electrolytes hinders their practical use as substitutes for liquid electrolytes to address safety concerns. Although various plasticizers have been introduced to improve lithium-ion conduction kinetics, the lack of microenvironment understanding impedes the rational design of high-performance polymer electrolytes. Here, we design a class of Hofmann complexes that offer continuous two-dimensional lithium-ion conduction channels with functional ligands, creating highly conductive electrolytes. Assisting with unsupervised learning, we use Climbing Image-Nudged Elastic Band simulations to screen lithium-ion conductors and screen out five potential candidates that elucidate the impact of lithium coordination environment on conduction behavior. By adjusting the covalency competition between Metal−O and Li−O bonds within Hofmann complexes, we can manipulate weak coordination environment of lithium-ion for rapid conduction kinetics. Li | |sulfurized polyacrylonitrile (SPAN) cell using solid-state polymer electrolytes with predicted Co(dimethylformamide)2Ni(CN)4 delivers an initial discharge capacity of 1264 mAh g−1 with a capacity retention of 65% after 500 cycles at 0.2 C (335 mA g−1), at 30 °C ± 3 °C. The assembled 0.6 Ah Li | |SPAN pouch cell delivers an areal discharge capacity of 3.8 mAh cm−2 at the second cycle with a solid electrolyte areal mass loading of 18.6 mg cm−2 (mass-to-capacity ratio of 4.9). |
| format | Article |
| id | doaj-art-8337e0a04fce4eb285a3aad47c16a6cb |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-8337e0a04fce4eb285a3aad47c16a6cb2025-02-02T12:31:31ZengNature PortfolioNature Communications2041-17232025-01-0116111310.1038/s41467-024-55633-9Data-driven exploration of weak coordination microenvironment in solid-state electrolyte for safe and energy-dense batteriesZhoujie Lao0Kehao Tao1Xiao Xiao2Haotian Qu3Xinru Wu4Zhiyuan Han5Runhua Gao6Jian Wang7Xian Wu8An Chen9Lei Shi10Chengshuai Chang11Yanze Song12Xiangyu Wang13Jinjin Li14Yanfei Zhu15Guangmin Zhou16Shenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School, Tsinghua UniversityNational Key Laboratory of Advanced Micro and Nano Manufacture Technology, Shanghai Jiao Tong UniversityShenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School, Tsinghua UniversityShenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School, Tsinghua UniversityShenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School, Tsinghua UniversityShenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School, Tsinghua UniversityShenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School, Tsinghua UniversityCanadian Light SourceShenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School, Tsinghua UniversityNational Key Laboratory of Advanced Micro and Nano Manufacture Technology, Shanghai Jiao Tong UniversityNational Key Laboratory of Advanced Micro and Nano Manufacture Technology, Shanghai Jiao Tong UniversityShenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School, Tsinghua UniversityShenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School, Tsinghua UniversityNational Key Laboratory of Advanced Micro and Nano Manufacture Technology, Shanghai Jiao Tong UniversityNational Key Laboratory of Advanced Micro and Nano Manufacture Technology, Shanghai Jiao Tong UniversityShenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School, Tsinghua UniversityShenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School, Tsinghua UniversityAbstract The unsatisfactory ionic conductivity of solid polymer electrolytes hinders their practical use as substitutes for liquid electrolytes to address safety concerns. Although various plasticizers have been introduced to improve lithium-ion conduction kinetics, the lack of microenvironment understanding impedes the rational design of high-performance polymer electrolytes. Here, we design a class of Hofmann complexes that offer continuous two-dimensional lithium-ion conduction channels with functional ligands, creating highly conductive electrolytes. Assisting with unsupervised learning, we use Climbing Image-Nudged Elastic Band simulations to screen lithium-ion conductors and screen out five potential candidates that elucidate the impact of lithium coordination environment on conduction behavior. By adjusting the covalency competition between Metal−O and Li−O bonds within Hofmann complexes, we can manipulate weak coordination environment of lithium-ion for rapid conduction kinetics. Li | |sulfurized polyacrylonitrile (SPAN) cell using solid-state polymer electrolytes with predicted Co(dimethylformamide)2Ni(CN)4 delivers an initial discharge capacity of 1264 mAh g−1 with a capacity retention of 65% after 500 cycles at 0.2 C (335 mA g−1), at 30 °C ± 3 °C. The assembled 0.6 Ah Li | |SPAN pouch cell delivers an areal discharge capacity of 3.8 mAh cm−2 at the second cycle with a solid electrolyte areal mass loading of 18.6 mg cm−2 (mass-to-capacity ratio of 4.9).https://doi.org/10.1038/s41467-024-55633-9 |
| spellingShingle | Zhoujie Lao Kehao Tao Xiao Xiao Haotian Qu Xinru Wu Zhiyuan Han Runhua Gao Jian Wang Xian Wu An Chen Lei Shi Chengshuai Chang Yanze Song Xiangyu Wang Jinjin Li Yanfei Zhu Guangmin Zhou Data-driven exploration of weak coordination microenvironment in solid-state electrolyte for safe and energy-dense batteries Nature Communications |
| title | Data-driven exploration of weak coordination microenvironment in solid-state electrolyte for safe and energy-dense batteries |
| title_full | Data-driven exploration of weak coordination microenvironment in solid-state electrolyte for safe and energy-dense batteries |
| title_fullStr | Data-driven exploration of weak coordination microenvironment in solid-state electrolyte for safe and energy-dense batteries |
| title_full_unstemmed | Data-driven exploration of weak coordination microenvironment in solid-state electrolyte for safe and energy-dense batteries |
| title_short | Data-driven exploration of weak coordination microenvironment in solid-state electrolyte for safe and energy-dense batteries |
| title_sort | data driven exploration of weak coordination microenvironment in solid state electrolyte for safe and energy dense batteries |
| url | https://doi.org/10.1038/s41467-024-55633-9 |
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