Multiple Redox Modes in the Reversible Lithiation of High-Capacity, Peierls-Distorted Vanadium Sulfide
Abstract
Vanadium sulfide VS4 in the patronite mineral structure, is a linear chain compound comprising vanadium atoms coordinated by disulfide anions [S2]2–. 51V NMR shows that the material, despite having V formally in the d1 configuration, is diamagnetic, suggesting potential dimerization through metal-metal bonding associated with a Peierls distortion of the linear chains. This is supported by density functional calculations, and is also consistent with the observed alternation in V-V distances of 2.8 Å and 3.2 Å along the chains. Partial lithiation results in reduction of the disulfide ions to sulfide S2–, including via an internal redox process whereby an electron from V4+ is transferred to [S2]2– resulting in oxidation of V4+ to V5+ and reduction of the [S2]2– to S2- to form Li3VS4 containing tetrahedral [VS4]3– anions. On further lithiation this is followed by reduction of the V5+ in Li3VS4 to form Li3+xVS4 (x=0.5-1), a mixed valent V4+/V5+ compound. Eventually reduction to Li2S plus elemental V occurs. Despite the complex redox processes involving both the cation and the anion occurring in this material, the system is found to be partially reversible between 0 and 3 V. In conclusion, the unusual redox processes in this system are elucidated using amore »
- Authors:
-
- Univ. of Cambridge (United Kingdom)
- Univ. of California, Santa Barbara, CA (United States)
- Ulsan National Inst. of Science and Technology (UNIST), Ulsan (Korea)
- Univ. of Oxford (United Kingdom)
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Univ. of California, Santa Barbara, CA (United States). Mitsubishi Chemicals Center for Advanced Materials Research Laboratory
- Ulsan National Inst. of Science and Technology (UNIST), Ulsan (Korea). Interdisciplinary School of Green Energy
- Publication Date:
- Research Org.:
- Univ. of California, Santa Barbara, CA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1254008
- Grant/Contract Number:
- AC02-06CH11357; NSF CNS-0960316; DMR-1121053
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 137; Journal Issue: 26; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; lithium-ion battery; conversion mechanism; peierls distortion
Citation Formats
Britto, Sylvia, Leskes, Michal, Hua, Xiao, Hébert, Claire-Alice, Shin, Hyeon Suk, Clarke, Simon, Borkiewicz, Olaf, Chapman, Karena W., Seshadri, Ram, Cho, Jaephil, and Grey, Clare P. Multiple Redox Modes in the Reversible Lithiation of High-Capacity, Peierls-Distorted Vanadium Sulfide. United States: N. p., 2015.
Web. doi:10.1021/jacs.5b03395.
Britto, Sylvia, Leskes, Michal, Hua, Xiao, Hébert, Claire-Alice, Shin, Hyeon Suk, Clarke, Simon, Borkiewicz, Olaf, Chapman, Karena W., Seshadri, Ram, Cho, Jaephil, & Grey, Clare P. Multiple Redox Modes in the Reversible Lithiation of High-Capacity, Peierls-Distorted Vanadium Sulfide. United States. https://doi.org/10.1021/jacs.5b03395
Britto, Sylvia, Leskes, Michal, Hua, Xiao, Hébert, Claire-Alice, Shin, Hyeon Suk, Clarke, Simon, Borkiewicz, Olaf, Chapman, Karena W., Seshadri, Ram, Cho, Jaephil, and Grey, Clare P. 2015.
"Multiple Redox Modes in the Reversible Lithiation of High-Capacity, Peierls-Distorted Vanadium Sulfide". United States. https://doi.org/10.1021/jacs.5b03395. https://www.osti.gov/servlets/purl/1254008.
@article{osti_1254008,
title = {Multiple Redox Modes in the Reversible Lithiation of High-Capacity, Peierls-Distorted Vanadium Sulfide},
author = {Britto, Sylvia and Leskes, Michal and Hua, Xiao and Hébert, Claire-Alice and Shin, Hyeon Suk and Clarke, Simon and Borkiewicz, Olaf and Chapman, Karena W. and Seshadri, Ram and Cho, Jaephil and Grey, Clare P.},
abstractNote = {Vanadium sulfide VS4 in the patronite mineral structure, is a linear chain compound comprising vanadium atoms coordinated by disulfide anions [S2]2–. 51V NMR shows that the material, despite having V formally in the d1 configuration, is diamagnetic, suggesting potential dimerization through metal-metal bonding associated with a Peierls distortion of the linear chains. This is supported by density functional calculations, and is also consistent with the observed alternation in V-V distances of 2.8 Å and 3.2 Å along the chains. Partial lithiation results in reduction of the disulfide ions to sulfide S2–, including via an internal redox process whereby an electron from V4+ is transferred to [S2]2– resulting in oxidation of V4+ to V5+ and reduction of the [S2]2– to S2- to form Li3VS4 containing tetrahedral [VS4]3– anions. On further lithiation this is followed by reduction of the V5+ in Li3VS4 to form Li3+xVS4 (x=0.5-1), a mixed valent V4+/V5+ compound. Eventually reduction to Li2S plus elemental V occurs. Despite the complex redox processes involving both the cation and the anion occurring in this material, the system is found to be partially reversible between 0 and 3 V. In conclusion, the unusual redox processes in this system are elucidated using a suite of short range characterization tools including 51V Nuclear Magnetic Resonance spectroscopy (NMR), S Kedge X-ray Absorption Near Edge Spectroscopy (XANES) and Pair Distribution Function (PDF) Analysis of X-ray data.},
doi = {10.1021/jacs.5b03395},
url = {https://www.osti.gov/biblio/1254008},
journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 26,
volume = 137,
place = {United States},
year = {Mon Jun 08 00:00:00 EDT 2015},
month = {Mon Jun 08 00:00:00 EDT 2015}
}
Web of Science
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