Commercially Viable Hybrid Li-Ion/Metal Batteries with High Energy Density Realized by Symbiotic Anode and Prelithiated Cathode

Abstract The energy density of commercial lithium (Li) ion batteries with graphite anode is reaching the limit. It is believed that directly utilizing Li metal as anode without a host could enhance the battery’s energy density to the maximum extent. However, the poor reversibility and infinite volum...

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Main Authors: Kui Lin, Xiaofu Xu, Xianying Qin, Ming Liu, Liang Zhao, Zijin Yang, Qi Liu, Yonghuang Ye, Guohua Chen, Feiyu Kang, Baohua Li
Format: Article
Language:English
Published: SpringerOpen 2022-07-01
Series:Nano-Micro Letters
Subjects:
Online Access:https://doi.org/10.1007/s40820-022-00899-1
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author Kui Lin
Xiaofu Xu
Xianying Qin
Ming Liu
Liang Zhao
Zijin Yang
Qi Liu
Yonghuang Ye
Guohua Chen
Feiyu Kang
Baohua Li
author_facet Kui Lin
Xiaofu Xu
Xianying Qin
Ming Liu
Liang Zhao
Zijin Yang
Qi Liu
Yonghuang Ye
Guohua Chen
Feiyu Kang
Baohua Li
author_sort Kui Lin
collection DOAJ
description Abstract The energy density of commercial lithium (Li) ion batteries with graphite anode is reaching the limit. It is believed that directly utilizing Li metal as anode without a host could enhance the battery’s energy density to the maximum extent. However, the poor reversibility and infinite volume change of Li metal hinder the realistic implementation of Li metal in battery community. Herein, a commercially viable hybrid Li-ion/metal battery is realized by a coordinated strategy of symbiotic anode and prelithiated cathode. To be specific, a scalable template-removal method is developed to fabricate the porous graphite layer (PGL), which acts as a symbiotic host for Li ion intercalation and subsequent Li metal deposition due to the enhanced lithiophilicity and sufficient ion-conducting pathways. A continuous dissolution-deintercalation mechanism during delithiation process further ensures the elimination of dead Li. As a result, when the excess plating Li reaches 30%, the PGL could deliver an ultrahigh average Coulombic efficiency of 99.5% for 180 cycles with a capacity of 2.48 mAh cm−2 in traditional carbonate electrolyte. Meanwhile, an air-stable recrystallized lithium oxalate with high specific capacity (514.3 mAh g−1) and moderate operating potential (4.7–5.0 V) is introduced as a sacrificial cathode to compensate the initial loss and provide Li source for subsequent cycles. Based on the prelithiated cathode and initial Li-free symbiotic anode, under a practical-level 3 mAh capacity, the assembled hybrid Li-ion/metal full cell with a P/N ratio (capacity ratio of LiNi0.8Co0.1Mn0.1O2 to graphite) of 1.3 exhibits significantly improved capacity retention after 300 cycles, indicating its great potential for high-energy-density Li batteries.
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spelling doaj.art-148b0395bd294e19bc1ecaf6ca742d4f2022-12-22T03:04:46ZengSpringerOpenNano-Micro Letters2311-67062150-55512022-07-0114111310.1007/s40820-022-00899-1Commercially Viable Hybrid Li-Ion/Metal Batteries with High Energy Density Realized by Symbiotic Anode and Prelithiated CathodeKui Lin0Xiaofu Xu1Xianying Qin2Ming Liu3Liang Zhao4Zijin Yang5Qi Liu6Yonghuang Ye7Guohua Chen8Feiyu Kang9Baohua Li10Shenzhen Key Laboratory on Power Battery Safety Research and Shenzhen Geim Graphene Center, Tsinghua Shenzhen International Graduate SchoolContemporary Amperex Technology Co. Ltd.Shenzhen Key Laboratory on Power Battery Safety Research and Shenzhen Geim Graphene Center, Tsinghua Shenzhen International Graduate SchoolShenzhen Key Laboratory on Power Battery Safety Research and Shenzhen Geim Graphene Center, Tsinghua Shenzhen International Graduate SchoolShenzhen Key Laboratory on Power Battery Safety Research and Shenzhen Geim Graphene Center, Tsinghua Shenzhen International Graduate SchoolShenzhen Key Laboratory on Power Battery Safety Research and Shenzhen Geim Graphene Center, Tsinghua Shenzhen International Graduate SchoolCollege of Materials Science and Engineering, Hunan UniversityContemporary Amperex Technology Co. Ltd.Department of Mechanical Engineering, The Hong Kong Polytechnic UniversityShenzhen Key Laboratory on Power Battery Safety Research and Shenzhen Geim Graphene Center, Tsinghua Shenzhen International Graduate SchoolShenzhen Key Laboratory on Power Battery Safety Research and Shenzhen Geim Graphene Center, Tsinghua Shenzhen International Graduate SchoolAbstract The energy density of commercial lithium (Li) ion batteries with graphite anode is reaching the limit. It is believed that directly utilizing Li metal as anode without a host could enhance the battery’s energy density to the maximum extent. However, the poor reversibility and infinite volume change of Li metal hinder the realistic implementation of Li metal in battery community. Herein, a commercially viable hybrid Li-ion/metal battery is realized by a coordinated strategy of symbiotic anode and prelithiated cathode. To be specific, a scalable template-removal method is developed to fabricate the porous graphite layer (PGL), which acts as a symbiotic host for Li ion intercalation and subsequent Li metal deposition due to the enhanced lithiophilicity and sufficient ion-conducting pathways. A continuous dissolution-deintercalation mechanism during delithiation process further ensures the elimination of dead Li. As a result, when the excess plating Li reaches 30%, the PGL could deliver an ultrahigh average Coulombic efficiency of 99.5% for 180 cycles with a capacity of 2.48 mAh cm−2 in traditional carbonate electrolyte. Meanwhile, an air-stable recrystallized lithium oxalate with high specific capacity (514.3 mAh g−1) and moderate operating potential (4.7–5.0 V) is introduced as a sacrificial cathode to compensate the initial loss and provide Li source for subsequent cycles. Based on the prelithiated cathode and initial Li-free symbiotic anode, under a practical-level 3 mAh capacity, the assembled hybrid Li-ion/metal full cell with a P/N ratio (capacity ratio of LiNi0.8Co0.1Mn0.1O2 to graphite) of 1.3 exhibits significantly improved capacity retention after 300 cycles, indicating its great potential for high-energy-density Li batteries.https://doi.org/10.1007/s40820-022-00899-1Hybrid lithium-ion/metal batterySymbiotic anodePorous graphite layerCathode prelithiationLithium oxalate
spellingShingle Kui Lin
Xiaofu Xu
Xianying Qin
Ming Liu
Liang Zhao
Zijin Yang
Qi Liu
Yonghuang Ye
Guohua Chen
Feiyu Kang
Baohua Li
Commercially Viable Hybrid Li-Ion/Metal Batteries with High Energy Density Realized by Symbiotic Anode and Prelithiated Cathode
Nano-Micro Letters
Hybrid lithium-ion/metal battery
Symbiotic anode
Porous graphite layer
Cathode prelithiation
Lithium oxalate
title Commercially Viable Hybrid Li-Ion/Metal Batteries with High Energy Density Realized by Symbiotic Anode and Prelithiated Cathode
title_full Commercially Viable Hybrid Li-Ion/Metal Batteries with High Energy Density Realized by Symbiotic Anode and Prelithiated Cathode
title_fullStr Commercially Viable Hybrid Li-Ion/Metal Batteries with High Energy Density Realized by Symbiotic Anode and Prelithiated Cathode
title_full_unstemmed Commercially Viable Hybrid Li-Ion/Metal Batteries with High Energy Density Realized by Symbiotic Anode and Prelithiated Cathode
title_short Commercially Viable Hybrid Li-Ion/Metal Batteries with High Energy Density Realized by Symbiotic Anode and Prelithiated Cathode
title_sort commercially viable hybrid li ion metal batteries with high energy density realized by symbiotic anode and prelithiated cathode
topic Hybrid lithium-ion/metal battery
Symbiotic anode
Porous graphite layer
Cathode prelithiation
Lithium oxalate
url https://doi.org/10.1007/s40820-022-00899-1
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