High-Capacity Micrometer-Sized Li 2 S Particles as Cathode Materials for Advanced Rechargeable Lithium-Ion Batteries

Handle URI:
http://hdl.handle.net/10754/598484
Title:
High-Capacity Micrometer-Sized Li 2 S Particles as Cathode Materials for Advanced Rechargeable Lithium-Ion Batteries
Authors:
Yang, Yuan; Zheng, Guangyuan; Misra, Sumohan; Nelson, Johanna; Toney, Michael F.; Cui, Yi
Abstract:
Li 2S is a high-capacity cathode material for lithium metal-free rechargeable batteries. It has a theoretical capacity of 1166 mAh/g, which is nearly 1 order of magnitude higher than traditional metal oxides/phosphates cathodes. However, Li 2S is usually considered to be electrochemically inactive due to its high electronic resistivity and low lithium-ion diffusivity. In this paper, we discover that a large potential barrier (∼1 V) exists at the beginning of charging for Li 2S. By applying a higher voltage cutoff, this barrier can be overcome and Li 2S becomes active. Moreover, this barrier does not appear again in the following cycling. Subsequent cycling shows that the material behaves similar to common sulfur cathodes with high energy efficiency. The initial discharge capacity is greater than 800 mAh/g for even 10 μm Li 2S particles. Moreover, after 10 cycles, the capacity is stabilized around 500-550 mAh/g with a capacity decay rate of only ∼0.25% per cycle. The origin of the initial barrier is found to be the phase nucleation of polysulfides, but the amplitude of barrier is mainly due to two factors: (a) charge transfer directly between Li 2S and electrolyte without polysulfide and (b) lithium-ion diffusion in Li 2S. These results demonstrate a simple and scalable approach to utilizing Li 2S as the cathode material for rechargeable lithium-ion batteries with high specific energy. © 2012 American Chemical Society.
Citation:
Yang Y, Zheng G, Misra S, Nelson J, Toney MF, et al. (2012) High-Capacity Micrometer-Sized Li 2 S Particles as Cathode Materials for Advanced Rechargeable Lithium-Ion Batteries . Journal of the American Chemical Society 134: 15387–15394. Available: http://dx.doi.org/10.1021/ja3052206.
Publisher:
American Chemical Society (ACS)
Journal:
Journal of the American Chemical Society
KAUST Grant Number:
KUS-l1-001-12
Issue Date:
19-Sep-2012
DOI:
10.1021/ja3052206
PubMed ID:
22909273
Type:
Article
ISSN:
0002-7863; 1520-5126
Sponsors:
A portion of this work was supported by the Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under contract DE-AC02-76SF0051 through the SLAC National Accelerator Laboratory, Laboratory Directed Research and Development funding, under contract DE-AC02-76SF00515 (J.N., M.F.T., Y.C.). Y.C. acknowledges support from a King Abdullah University of Science and Technology (KAUST) Investigator Award (No. KUS-l1-001-12). Y.Y. acknowledges financial support from the Stanford Graduate Fellowship (SGF). G.Z. acknowledges financial support from the Agency for Science, Technology and Research (A*STAR), Singapore. Portions of this research were carried out at the Stanford Synchrotron Radiation Lightsource, a national user facility operated by Stanford University on behalf of the U.S. Department of Energy, Office of Basic Energy Sciences.
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Full metadata record

DC FieldValue Language
dc.contributor.authorYang, Yuanen
dc.contributor.authorZheng, Guangyuanen
dc.contributor.authorMisra, Sumohanen
dc.contributor.authorNelson, Johannaen
dc.contributor.authorToney, Michael F.en
dc.contributor.authorCui, Yien
dc.date.accessioned2016-02-25T13:30:48Zen
dc.date.available2016-02-25T13:30:48Zen
dc.date.issued2012-09-19en
dc.identifier.citationYang Y, Zheng G, Misra S, Nelson J, Toney MF, et al. (2012) High-Capacity Micrometer-Sized Li 2 S Particles as Cathode Materials for Advanced Rechargeable Lithium-Ion Batteries . Journal of the American Chemical Society 134: 15387–15394. Available: http://dx.doi.org/10.1021/ja3052206.en
dc.identifier.issn0002-7863en
dc.identifier.issn1520-5126en
dc.identifier.pmid22909273en
dc.identifier.doi10.1021/ja3052206en
dc.identifier.urihttp://hdl.handle.net/10754/598484en
dc.description.abstractLi 2S is a high-capacity cathode material for lithium metal-free rechargeable batteries. It has a theoretical capacity of 1166 mAh/g, which is nearly 1 order of magnitude higher than traditional metal oxides/phosphates cathodes. However, Li 2S is usually considered to be electrochemically inactive due to its high electronic resistivity and low lithium-ion diffusivity. In this paper, we discover that a large potential barrier (∼1 V) exists at the beginning of charging for Li 2S. By applying a higher voltage cutoff, this barrier can be overcome and Li 2S becomes active. Moreover, this barrier does not appear again in the following cycling. Subsequent cycling shows that the material behaves similar to common sulfur cathodes with high energy efficiency. The initial discharge capacity is greater than 800 mAh/g for even 10 μm Li 2S particles. Moreover, after 10 cycles, the capacity is stabilized around 500-550 mAh/g with a capacity decay rate of only ∼0.25% per cycle. The origin of the initial barrier is found to be the phase nucleation of polysulfides, but the amplitude of barrier is mainly due to two factors: (a) charge transfer directly between Li 2S and electrolyte without polysulfide and (b) lithium-ion diffusion in Li 2S. These results demonstrate a simple and scalable approach to utilizing Li 2S as the cathode material for rechargeable lithium-ion batteries with high specific energy. © 2012 American Chemical Society.en
dc.description.sponsorshipA portion of this work was supported by the Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under contract DE-AC02-76SF0051 through the SLAC National Accelerator Laboratory, Laboratory Directed Research and Development funding, under contract DE-AC02-76SF00515 (J.N., M.F.T., Y.C.). Y.C. acknowledges support from a King Abdullah University of Science and Technology (KAUST) Investigator Award (No. KUS-l1-001-12). Y.Y. acknowledges financial support from the Stanford Graduate Fellowship (SGF). G.Z. acknowledges financial support from the Agency for Science, Technology and Research (A*STAR), Singapore. Portions of this research were carried out at the Stanford Synchrotron Radiation Lightsource, a national user facility operated by Stanford University on behalf of the U.S. Department of Energy, Office of Basic Energy Sciences.en
dc.publisherAmerican Chemical Society (ACS)en
dc.titleHigh-Capacity Micrometer-Sized Li 2 S Particles as Cathode Materials for Advanced Rechargeable Lithium-Ion Batteriesen
dc.typeArticleen
dc.identifier.journalJournal of the American Chemical Societyen
dc.contributor.institutionStanford University, Palo Alto, United Statesen
dc.contributor.institutionStanford Synchrotron Radiation Laboratory, Menlo Park, United Statesen
dc.contributor.institutionStanford Linear Accelerator Center, Menlo Park, United Statesen
kaust.grant.numberKUS-l1-001-12en

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