Explore the Effects of Microstructural Defects on Voltage Fade of Li- and Mn-Rich Cathodes

Hu, E.; Lyu, Y.; Xin, H.; Xin, H. L.; Liu, J.; Han, L.; Bak, S. -M.; Bai, J.; Yu, X.; Li, H.; Yang, X. Q.

doi:10.1021/acs.nanolett.6b01609

Title: Explore the Effects of Microstructural Defects on Voltage Fade of Li- and Mn-Rich Cathodes

Journal Article · Mon Sep 26 00:00:00 EDT 2016 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.6b01609· OSTI ID:1329785

Hu, E. ^[1]; Lyu, Y. ^[2]; Xin, H. ^[1]; Xin, H. L. ^[1]; Liu, J. ^[1]; Han, L. ^[1]; Bak, S. -M. ^[1]; Bai, J. ^[1]; Yu, X. ^[3]; Li, H. ^[4]; Yang, X. Q. ^[1]

Brookhaven National Lab. (BNL), Upton, NY (United States)
Chinese Academy of Sciences (CAS), Beijing (China). Inst. of Physics. Beijing National Lab. for Condensed Matter Physics (BNLCP-CAS); Shanghai Univ. (China)
Brookhaven National Lab. (BNL), Upton, NY (United States); Chinese Academy of Sciences (CAS), Beijing (China). Inst. of Physics. Beijing National Lab. for Condensed Matter Physics (BNLCP-CAS)
Chinese Academy of Sciences (CAS), Beijing (China). Inst. of Physics. Beijing National Lab. for Condensed Matter Physics (BNLCP-CAS)

Li- and Mn-rich (LMR) cathode materials have been considered as promising candidates for energy storage applications due to high energy density. However, these materials suffer from a serious problem of voltage fade. Oxygen loss and the layer to spinel phase transition are two major contributors of such voltage fade. In this paper, using a combination of x-ray diffraction (XRD), pair distribution function (PDF), x-ray absorption (XAS) techniques and aberration-corrected scanning transmission electron microscopy (STEM), we studied the effects of micro structural defects, especially the grain boundaries on the oxygen loss and layered-to-spinel phase transition through prelithiation of a model compound Li2Ru0.5Mn0.5O3. It is found that the nano-sized micro structural defects, especially the large amount of grain boundaries created by the prelithiation can greatly accelerate the oxygen loss and voltage fade. Defects (such as nano-sized grain boundaries) and oxygen release form a positive feedback loop, promote each other during cycling, and accelerate the two major voltage fade contributors: the transition metal reduction and layered-to-spinel phase transition. These results clearly demonstrate the important relationships among the oxygen loss, microstructural defects and voltage fade. The importance of maintaining good crystallinity and protecting the surface of LMR material are also suggested.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC00112704

OSTI ID:: 1329785

Report Number(s):: BNL-112729-2016-JA

Journal Information:: Nano Letters, Vol. 16, Issue 10; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 62 works

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