Extra storage capacity in transition metal oxide lithium-ion batteries revealed by in situ magnetometry
In lithium-ion batteries (LIBs), many promising electrodes that are based on transition metal oxides exhibit anomalously high storage capacities beyond their theoretical values. Although this phenomenon has been widely reported, the underlying physicochemical mechanism in such materials remains elus...
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| Published in | Nature materials Vol. 20; no. 1; pp. 76 - 83 |
|---|---|
| Main Authors | , , , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
London
Nature Publishing Group UK
01.01.2021
Nature Publishing Group |
| Subjects | |
| Online Access | Get full text |
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| Abstract | In lithium-ion batteries (LIBs), many promising electrodes that are based on transition metal oxides exhibit anomalously high storage capacities beyond their theoretical values. Although this phenomenon has been widely reported, the underlying physicochemical mechanism in such materials remains elusive and is still a matter of debate. In this work, we use in situ magnetometry to demonstrate the existence of strong surface capacitance on metal nanoparticles, and to show that a large number of spin-polarized electrons can be stored in the already-reduced metallic nanoparticles (that are formed during discharge at low potentials in transition metal oxide LIBs), which is consistent with a space charge mechanism. Through quantification of the surface capacitance by the variation in magnetism, we further show that this charge capacity of the surface is the dominant source of the extra capacity in the Fe
3
O
4
/Li model system, and that it also exists in CoO, NiO, FeF
2
and Fe
2
N systems. The space charge mechanism revealed by in situ magnetometry can therefore be generalized to a broad range of transition metal compounds for which a large electron density of states is accessible, and provides pivotal guidance for creating advanced energy storage systems.
Although some transition metal oxide-based electrodes exhibit high storage capacities beyond theoretical values, the underlying physicochemical mechanism remains elusive. Surface capacitance on metal nanoparticles involving spin-polarized electrons is now shown to be consistent with a space charge mechanism. |
|---|---|
| AbstractList | In lithium-ion batteries (LIBs), many promising electrodes that are based on transition metal oxides exhibit anomalously high storage capacities beyond their theoretical values. Although this phenomenon has been widely reported, the underlying physicochemical mechanism in such materials remains elusive and is still a matter of debate. In this work, we use in situ magnetometry to demonstrate the existence of strong surface capacitance on metal nanoparticles, and to show that a large number of spin-polarized electrons can be stored in the already-reduced metallic nanoparticles (that are formed during discharge at low potentials in transition metal oxide LIBs), which is consistent with a space charge mechanism. Through quantification of the surface capacitance by the variation in magnetism, we further show that this charge capacity of the surface is the dominant source of the extra capacity in the Fe
3
O
4
/Li model system, and that it also exists in CoO, NiO, FeF
2
and Fe
2
N systems. The space charge mechanism revealed by in situ magnetometry can therefore be generalized to a broad range of transition metal compounds for which a large electron density of states is accessible, and provides pivotal guidance for creating advanced energy storage systems.
Although some transition metal oxide-based electrodes exhibit high storage capacities beyond theoretical values, the underlying physicochemical mechanism remains elusive. Surface capacitance on metal nanoparticles involving spin-polarized electrons is now shown to be consistent with a space charge mechanism. In lithium-ion batteries (LIBs), many promising electrodes that are based on transition metal oxides exhibit anomalously high storage capacities beyond their theoretical values. Although this phenomenon has been widely reported, the underlying physicochemical mechanism in such materials remains elusive and is still a matter of debate. In this work, we use in situ magnetometry to demonstrate the existence of strong surface capacitance on metal nanoparticles, and to show that a large number of spin-polarized electrons can be stored in the already-reduced metallic nanoparticles (that are formed during discharge at low potentials in transition metal oxide LIBs), which is consistent with a space charge mechanism. Through quantification of the surface capacitance by the variation in magnetism, we further show that this charge capacity of the surface is the dominant source of the extra capacity in the Fe O /Li model system, and that it also exists in CoO, NiO, FeF and Fe N systems. The space charge mechanism revealed by in situ magnetometry can therefore be generalized to a broad range of transition metal compounds for which a large electron density of states is accessible, and provides pivotal guidance for creating advanced energy storage systems. In lithium-ion batteries (LIBs), many promising electrodes that are based on transition metal oxides exhibit anomalously high storage capacities beyond their theoretical values. Although this phenomenon has been widely reported, the underlying physicochemical mechanism in such materials remains elusive and is still a matter of debate. In this work, we use in situ magnetometry to demonstrate the existence of strong surface capacitance on metal nanoparticles, and to show that a large number of spin-polarized electrons can be stored in the already-reduced metallic nanoparticles (that are formed during discharge at low potentials in transition metal oxide LIBs), which is consistent with a space charge mechanism. Through quantification of the surface capacitance by the variation in magnetism, we further show that this charge capacity of the surface is the dominant source of the extra capacity in the Fe3O4/Li model system, and that it also exists in CoO, NiO, FeF2 and Fe2N systems. The space charge mechanism revealed by in situ magnetometry can therefore be generalized to a broad range of transition metal compounds for which a large electron density of states is accessible, and provides pivotal guidance for creating advanced energy storage systems.In lithium-ion batteries (LIBs), many promising electrodes that are based on transition metal oxides exhibit anomalously high storage capacities beyond their theoretical values. Although this phenomenon has been widely reported, the underlying physicochemical mechanism in such materials remains elusive and is still a matter of debate. In this work, we use in situ magnetometry to demonstrate the existence of strong surface capacitance on metal nanoparticles, and to show that a large number of spin-polarized electrons can be stored in the already-reduced metallic nanoparticles (that are formed during discharge at low potentials in transition metal oxide LIBs), which is consistent with a space charge mechanism. Through quantification of the surface capacitance by the variation in magnetism, we further show that this charge capacity of the surface is the dominant source of the extra capacity in the Fe3O4/Li model system, and that it also exists in CoO, NiO, FeF2 and Fe2N systems. The space charge mechanism revealed by in situ magnetometry can therefore be generalized to a broad range of transition metal compounds for which a large electron density of states is accessible, and provides pivotal guidance for creating advanced energy storage systems. In lithium-ion batteries (LIBs), many promising electrodes that are based on transition metal oxides exhibit anomalously high storage capacities beyond their theoretical values. Although this phenomenon has been widely reported, the underlying physicochemical mechanism in such materials remains elusive and is still a matter of debate. In this work, we use in situ magnetometry to demonstrate the existence of strong surface capacitance on metal nanoparticles, and to show that a large number of spin-polarized electrons can be stored in the already-reduced metallic nanoparticles (that are formed during discharge at low potentials in transition metal oxide LIBs), which is consistent with a space charge mechanism. Through quantification of the surface capacitance by the variation in magnetism, we further show that this charge capacity of the surface is the dominant source of the extra capacity in the Fe3O4/Li model system, and that it also exists in CoO, NiO, FeF2 and Fe2N systems. The space charge mechanism revealed by in situ magnetometry can therefore be generalized to a broad range of transition metal compounds for which a large electron density of states is accessible, and provides pivotal guidance for creating advanced energy storage systems.Although some transition metal oxide-based electrodes exhibit high storage capacities beyond theoretical values, the underlying physicochemical mechanism remains elusive. Surface capacitance on metal nanoparticles involving spin-polarized electrons is now shown to be consistent with a space charge mechanism. |
| Author | Ge, Chen Hu, Zhengqiang Zhang, Qinghua Shang, Xiantao Yan, Shishen Long, Yunze Miao, Guo-Xing Moodera, Jagadeesh S. Li, Qiang Fan, Shuting Gu, Lin Xia, Qingtao Wang, Xiaoxiong Zhu, Yue Li, Hongsen Yu, Guihua |
| Author_xml | – sequence: 1 givenname: Qiang orcidid: 0000-0001-8891-260X surname: Li fullname: Li, Qiang email: liqiang@qdu.edu.cn organization: College of Physics, Center for Marine Observation and Communications, Qingdao University, Department of Electrical and Computer Engineering and Institute for Quantum Computing, University of Waterloo – sequence: 2 givenname: Hongsen orcidid: 0000-0001-6453-2135 surname: Li fullname: Li, Hongsen email: hsli@qdu.edu.cn organization: College of Physics, Center for Marine Observation and Communications, Qingdao University, Materials Science and Engineering Program and Department of Mechanical Engineering, The University of Texas at Austin – sequence: 3 givenname: Qingtao surname: Xia fullname: Xia, Qingtao organization: College of Physics, Center for Marine Observation and Communications, Qingdao University – sequence: 4 givenname: Zhengqiang surname: Hu fullname: Hu, Zhengqiang organization: College of Physics, Center for Marine Observation and Communications, Qingdao University – sequence: 5 givenname: Yue surname: Zhu fullname: Zhu, Yue organization: Materials Science and Engineering Program and Department of Mechanical Engineering, The University of Texas at Austin – sequence: 6 givenname: Shishen orcidid: 0000-0002-7327-9968 surname: Yan fullname: Yan, Shishen organization: School of Physics, State Key Laboratory of Crystal Materials, Shandong University – sequence: 7 givenname: Chen orcidid: 0000-0002-8093-940X surname: Ge fullname: Ge, Chen organization: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences – sequence: 8 givenname: Qinghua surname: Zhang fullname: Zhang, Qinghua organization: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences – sequence: 9 givenname: Xiaoxiong surname: Wang fullname: Wang, Xiaoxiong organization: College of Physics, Center for Marine Observation and Communications, Qingdao University – sequence: 10 givenname: Xiantao surname: Shang fullname: Shang, Xiantao organization: College of Physics, Center for Marine Observation and Communications, Qingdao University – sequence: 11 givenname: Shuting surname: Fan fullname: Fan, Shuting organization: College of Physics, Center for Marine Observation and Communications, Qingdao University – sequence: 12 givenname: Yunze surname: Long fullname: Long, Yunze organization: College of Physics, Center for Marine Observation and Communications, Qingdao University – sequence: 13 givenname: Lin orcidid: 0000-0002-7504-031X surname: Gu fullname: Gu, Lin organization: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences – sequence: 14 givenname: Guo-Xing orcidid: 0000-0002-8735-8077 surname: Miao fullname: Miao, Guo-Xing email: guo-xing.miao@uwaterloo.ca organization: College of Physics, Center for Marine Observation and Communications, Qingdao University, Department of Electrical and Computer Engineering and Institute for Quantum Computing, University of Waterloo, Department of Physics, Plasma Science and Fusion Center and Francis Bitter Magnet Laboratory, Massachusetts Institute of Technology – sequence: 15 givenname: Guihua orcidid: 0000-0002-3253-0749 surname: Yu fullname: Yu, Guihua email: ghyu@austin.utexas.edu organization: Materials Science and Engineering Program and Department of Mechanical Engineering, The University of Texas at Austin – sequence: 16 givenname: Jagadeesh S. surname: Moodera fullname: Moodera, Jagadeesh S. organization: Department of Physics, Plasma Science and Fusion Center and Francis Bitter Magnet Laboratory, Massachusetts Institute of Technology |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/32807921$$D View this record in MEDLINE/PubMed |
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| Snippet | In lithium-ion batteries (LIBs), many promising electrodes that are based on transition metal oxides exhibit anomalously high storage capacities beyond their... |
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| SubjectTerms | 639/301 639/301/299 Biomaterials Capacitance Chemistry and Materials Science Condensed Matter Physics Electrodes Electron density Electron spin Energy storage Iron nitride Iron oxides Lithium Lithium-ion batteries Magnetic measurement Magnetism Materials Science Metal compounds Metal oxides Metals Nanoparticles Nanotechnology Optical and Electronic Materials Rechargeable batteries Space charge Storage batteries Storage capacity Storage systems Transition metal compounds Transition metal oxides |
| Title | Extra storage capacity in transition metal oxide lithium-ion batteries revealed by in situ magnetometry |
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