Regulating lithium affinity of hosts for reversible lithium metal batteries
Abstract Lithium (Li) metal batteries are regarded as the “holy grail” of next‐generation rechargeable batteries, but the poor redox reversibility of Li anode hinders its practical applications. While extensive studies have been carried out to design lithiophilic substrates for facile Li plating, th...
| Main Authors: | , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
| Published: |
Wiley
2024-03-01
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| Series: | Interdisciplinary Materials |
| Subjects: | |
| Online Access: | https://doi.org/10.1002/idm2.12153 |
| _version_ | 1797236833135886336 |
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| author | Hao Liu Yuchen Ji Yang Li Shisheng Zheng Zihang Dong Kai Yang Aimin Cao Yuxiang Huang Yinchao Wang Haifeng Shen Shao‐jian Zhang Feng Pan Luyi Yang |
| author_facet | Hao Liu Yuchen Ji Yang Li Shisheng Zheng Zihang Dong Kai Yang Aimin Cao Yuxiang Huang Yinchao Wang Haifeng Shen Shao‐jian Zhang Feng Pan Luyi Yang |
| author_sort | Hao Liu |
| collection | DOAJ |
| description | Abstract Lithium (Li) metal batteries are regarded as the “holy grail” of next‐generation rechargeable batteries, but the poor redox reversibility of Li anode hinders its practical applications. While extensive studies have been carried out to design lithiophilic substrates for facile Li plating, their effects on Li stripping are often neglected. In this study, by homogeneously loading indium (In) single atoms on N‐doped graphene via In‐N bonds, the affinity between Li and hosting substrates is regulated. In situ observation of Li deposition/stripping processes shows that compared with the N‐doped graphene substrate, the introduction of In effectively promotes its reversibility of Li redox, achieving a dendrite‐free Li anode with much‐improved coulombic efficiency. Interestingly, theoretical calculations demonstrate that In atoms have actually made the substrate less lithophilic via passivating the N sites to avoid the formation of irreversible Li–N bonding. Therefore, a “volcano curve” for reversible Li redox processes is proposed: the affinity of substrates toward Li should be optimized to a moderate value, where the balance for both Li plating and Li stripping processes could be reached. By demonstrating a crucial design principle for Li metal hosting substrates, our finding could trigger the rapid development of related research. |
| first_indexed | 2024-04-24T17:10:08Z |
| format | Article |
| id | doaj.art-096fa15b638b459fbacfa3979b938bb2 |
| institution | Directory Open Access Journal |
| issn | 2767-441X |
| language | English |
| last_indexed | 2024-04-24T17:10:08Z |
| publishDate | 2024-03-01 |
| publisher | Wiley |
| record_format | Article |
| series | Interdisciplinary Materials |
| spelling | doaj.art-096fa15b638b459fbacfa3979b938bb22024-03-28T12:50:13ZengWileyInterdisciplinary Materials2767-441X2024-03-013229730510.1002/idm2.12153Regulating lithium affinity of hosts for reversible lithium metal batteriesHao Liu0Yuchen Ji1Yang Li2Shisheng Zheng3Zihang Dong4Kai Yang5Aimin Cao6Yuxiang Huang7Yinchao Wang8Haifeng Shen9Shao‐jian Zhang10Feng Pan11Luyi Yang12School of Advanced Materials Peking University Shenzhen Graduate School Shenzhen Guangdong ChinaSchool of Advanced Materials Peking University Shenzhen Graduate School Shenzhen Guangdong ChinaInstitute of Process Equipment, College of Energy Engineering Zhejiang University Hangzhou Zhejiang ChinaSchool of Advanced Materials Peking University Shenzhen Graduate School Shenzhen Guangdong ChinaSchool of Environment and Energy Peking University Shenzhen Graduate School Shenzhen Guangdong ChinaAdvanced Technology Institute, Department of Electrical and Electronic Engineering University of Surrey Guildford Surrey UKSchool of Advanced Materials Peking University Shenzhen Graduate School Shenzhen Guangdong ChinaSchool of Advanced Materials Peking University Shenzhen Graduate School Shenzhen Guangdong ChinaSchool of Advanced Materials Peking University Shenzhen Graduate School Shenzhen Guangdong ChinaSchool of Chemical Engineering The University of Adelaide Adelaide South Australia AustraliaSchool of Chemical Engineering The University of Adelaide Adelaide South Australia AustraliaSchool of Advanced Materials Peking University Shenzhen Graduate School Shenzhen Guangdong ChinaSchool of Advanced Materials Peking University Shenzhen Graduate School Shenzhen Guangdong ChinaAbstract Lithium (Li) metal batteries are regarded as the “holy grail” of next‐generation rechargeable batteries, but the poor redox reversibility of Li anode hinders its practical applications. While extensive studies have been carried out to design lithiophilic substrates for facile Li plating, their effects on Li stripping are often neglected. In this study, by homogeneously loading indium (In) single atoms on N‐doped graphene via In‐N bonds, the affinity between Li and hosting substrates is regulated. In situ observation of Li deposition/stripping processes shows that compared with the N‐doped graphene substrate, the introduction of In effectively promotes its reversibility of Li redox, achieving a dendrite‐free Li anode with much‐improved coulombic efficiency. Interestingly, theoretical calculations demonstrate that In atoms have actually made the substrate less lithophilic via passivating the N sites to avoid the formation of irreversible Li–N bonding. Therefore, a “volcano curve” for reversible Li redox processes is proposed: the affinity of substrates toward Li should be optimized to a moderate value, where the balance for both Li plating and Li stripping processes could be reached. By demonstrating a crucial design principle for Li metal hosting substrates, our finding could trigger the rapid development of related research.https://doi.org/10.1002/idm2.12153in situ AFMLi metal anodelithiophilic sitessingle atomsvolcano plot |
| spellingShingle | Hao Liu Yuchen Ji Yang Li Shisheng Zheng Zihang Dong Kai Yang Aimin Cao Yuxiang Huang Yinchao Wang Haifeng Shen Shao‐jian Zhang Feng Pan Luyi Yang Regulating lithium affinity of hosts for reversible lithium metal batteries Interdisciplinary Materials in situ AFM Li metal anode lithiophilic sites single atoms volcano plot |
| title | Regulating lithium affinity of hosts for reversible lithium metal batteries |
| title_full | Regulating lithium affinity of hosts for reversible lithium metal batteries |
| title_fullStr | Regulating lithium affinity of hosts for reversible lithium metal batteries |
| title_full_unstemmed | Regulating lithium affinity of hosts for reversible lithium metal batteries |
| title_short | Regulating lithium affinity of hosts for reversible lithium metal batteries |
| title_sort | regulating lithium affinity of hosts for reversible lithium metal batteries |
| topic | in situ AFM Li metal anode lithiophilic sites single atoms volcano plot |
| url | https://doi.org/10.1002/idm2.12153 |
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