Xin-Yue Qiu, Shi-Cong Mo, Jing Nie, Guang-Ye Li, Pei-Yi Liang, Jun-Xi Li, Chudong Xu* and Shi-Zhang Chen*,
{"title":"设计二维石墨烯C36作为高性能锂离子电池负极材料:第一性原理研究","authors":"Xin-Yue Qiu, Shi-Cong Mo, Jing Nie, Guang-Ye Li, Pei-Yi Liang, Jun-Xi Li, Chudong Xu* and Shi-Zhang Chen*, ","doi":"10.1021/acsaem.4c0332210.1021/acsaem.4c03322","DOIUrl":null,"url":null,"abstract":"<p >Two-dimensional (2D) structures hold promise as advanced lithium-ion battery (LIB) anode materials. Recently synthesized 2D graphullerene faces challenges due to its large electronic insulating band gap. In this study, we construct a quasi-tetragonal graphullerene, C<sub>36</sub>, denoted as GrF-C<sub>36</sub>, using C<sub>36</sub> fullerenes with <i>D</i><sub>6<i>h</i></sub> symmetry as the structural unit. First-principles calculations revealed that the delocalized p<sub><i>z</i></sub> orbitals lead to metallicity, combined with intrinsic porosity, resulting in a large theoretical capacity of 496 mAh/g when they are used as LIB anode material. However, the structure exhibits a large migration barrier for lithium ions (Li<sup>+</sup>), limiting its rate performance. To address this, we further adopt the strategy for constructing long-range-ordered carbon by “removing” the [2 + 2] cycloaddition bonds to form intrinsic one-dimensional channels in the structure, denoted as LOPC-C<sub>32</sub>. Calculations showed that LOPC-C<sub>32</sub> maintains metallicity and enhances the structural stability while achieving a Li capacity of 906 mAh/g. The migration barrier for Li<sup>+</sup> within these channels is only 0.12 eV, significantly improving the rate performance. Coupled with an average open-circuit voltage of 0.43 V and a structural deformation of only 5% at a maximum Li capacity, LOPC-C<sub>32</sub> emerges as an excellent anode material. Our work provides a design strategy for the application of graphullerenes in LIBs.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3698–3706 3698–3706"},"PeriodicalIF":5.5000,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Designing Two-Dimensional Graphullerene C36 as High-Performance Anode Materials for Li-Ion Batteries: A First-Principles Study\",\"authors\":\"Xin-Yue Qiu, Shi-Cong Mo, Jing Nie, Guang-Ye Li, Pei-Yi Liang, Jun-Xi Li, Chudong Xu* and Shi-Zhang Chen*, \",\"doi\":\"10.1021/acsaem.4c0332210.1021/acsaem.4c03322\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Two-dimensional (2D) structures hold promise as advanced lithium-ion battery (LIB) anode materials. Recently synthesized 2D graphullerene faces challenges due to its large electronic insulating band gap. In this study, we construct a quasi-tetragonal graphullerene, C<sub>36</sub>, denoted as GrF-C<sub>36</sub>, using C<sub>36</sub> fullerenes with <i>D</i><sub>6<i>h</i></sub> symmetry as the structural unit. First-principles calculations revealed that the delocalized p<sub><i>z</i></sub> orbitals lead to metallicity, combined with intrinsic porosity, resulting in a large theoretical capacity of 496 mAh/g when they are used as LIB anode material. However, the structure exhibits a large migration barrier for lithium ions (Li<sup>+</sup>), limiting its rate performance. To address this, we further adopt the strategy for constructing long-range-ordered carbon by “removing” the [2 + 2] cycloaddition bonds to form intrinsic one-dimensional channels in the structure, denoted as LOPC-C<sub>32</sub>. Calculations showed that LOPC-C<sub>32</sub> maintains metallicity and enhances the structural stability while achieving a Li capacity of 906 mAh/g. The migration barrier for Li<sup>+</sup> within these channels is only 0.12 eV, significantly improving the rate performance. Coupled with an average open-circuit voltage of 0.43 V and a structural deformation of only 5% at a maximum Li capacity, LOPC-C<sub>32</sub> emerges as an excellent anode material. 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Designing Two-Dimensional Graphullerene C36 as High-Performance Anode Materials for Li-Ion Batteries: A First-Principles Study
Two-dimensional (2D) structures hold promise as advanced lithium-ion battery (LIB) anode materials. Recently synthesized 2D graphullerene faces challenges due to its large electronic insulating band gap. In this study, we construct a quasi-tetragonal graphullerene, C36, denoted as GrF-C36, using C36 fullerenes with D6h symmetry as the structural unit. First-principles calculations revealed that the delocalized pz orbitals lead to metallicity, combined with intrinsic porosity, resulting in a large theoretical capacity of 496 mAh/g when they are used as LIB anode material. However, the structure exhibits a large migration barrier for lithium ions (Li+), limiting its rate performance. To address this, we further adopt the strategy for constructing long-range-ordered carbon by “removing” the [2 + 2] cycloaddition bonds to form intrinsic one-dimensional channels in the structure, denoted as LOPC-C32. Calculations showed that LOPC-C32 maintains metallicity and enhances the structural stability while achieving a Li capacity of 906 mAh/g. The migration barrier for Li+ within these channels is only 0.12 eV, significantly improving the rate performance. Coupled with an average open-circuit voltage of 0.43 V and a structural deformation of only 5% at a maximum Li capacity, LOPC-C32 emerges as an excellent anode material. Our work provides a design strategy for the application of graphullerenes in LIBs.
期刊介绍:
ACS Applied Energy Materials is an interdisciplinary journal publishing original research covering all aspects of materials, engineering, chemistry, physics and biology relevant to energy conversion and storage. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important energy applications.