ACS applied materials & interfaces, volume 8, issue 12, pages 7843-7853

Insights into the Performance Limits of the Li7P3S11 Superionic Conductor: A Combined First-Principles and Experimental Study.

Iek-Heng Chu ¹

Han Nguyen ¹

Sunny Hy ¹

Yuh-Chieh Lin ¹

Zhenbin Wang ¹

Zihan Xu ¹

Zhi Deng ¹

Ying Meng ¹

Shyue Ping Ong ¹

Hide authors affiliations Show authors affiliations: 1 affiliation

Department of NanoEngineering, University of California, San Diego, 9500 Gilman Drive, Mail Code 0448, La Jolla, California 92093, United States |

Publication type: Journal Article

Publication date: 2016-03-17

American Chemical Society (ACS)

Journal: ACS applied materials & interfaces

Quartile SCImago

Quartile WOS

Impact factor: 9.5

ISSN: 19448244, 19448252

DOI: 10.1021/acsami.6b00833

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General Materials Science

Abstract

The Li7P3S11 glass-ceramic is a promising superionic conductor electrolyte (SCE) with an extremely high Li(+) conductivity that exceeds that of even traditional organic electrolytes. In this work, we present a combined computational and experimental investigation of the material performance limitations in terms of its phase and electrochemical stability, and Li(+) conductivity. We find that Li7P3S11 is metastable at 0 K but becomes stable at above 630 K (∼360 °C) when vibrational entropy contributions are accounted for, in agreement with differential scanning calorimetry measurements. Both scanning electron microscopy and the calculated Wulff shape show that Li7P3S11 tends to form relatively isotropic crystals. In terms of electrochemical stability, first-principles calculations predict that, unlike the LiCoO2 cathode, the olivine LiFePO4 and spinel LiMn2O4 cathodes are likely to form stable passivation interfaces with the Li7P3S11 SCE. This finding underscores the importance of considering multicomponent integration in developing an all-solid-state architecture. To probe the fundamental limit of its bulk Li(+) conductivity, a comparison of conventional cold-press sintered versus spark-plasma sintering (SPS) Li7P3S11 was done in conjunction with ab initio molecular dynamics (AIMD) simulations. Though the measured diffusion activation barriers are in excellent agreement, the AIMD-predicted room-temperature Li(+) conductivity of 57 mS cm(-1) is much higher than the experimental values. The optimized SPS sample exhibits a room-temperature Li(+) conductivity of 11.6 mS cm(-1), significantly higher than that of the cold-pressed sample (1.3 mS cm(-1)) due to the reduction of grain boundary resistance by densification. We conclude that grain boundary conductivity is limiting the overall Li(+) conductivity in Li7P3S11, and further optimization of overall conductivities should be possible. Finally, we show that Li(+) motions in this material are highly collective, and the flexing of the P2S7 ditetrahedra facilitates fast Li(+) diffusion.

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APL Materials	APL Materials, 1, 0.56% APL Materials 1 publication, 0.56%
AIP Advances	AIP Advances, 1, 0.56% AIP Advances 1 publication, 0.56%
Physical Review B	Physical Review B, 1, 0.56% Physical Review B 1 publication, 0.56%
Journal of Vacuum Science and Technology A: Vacuum, Surfaces and Films	Journal of Vacuum Science and Technology A: Vacuum, Surfaces and Films, 1, 0.56% Journal of Vacuum Science and Technology A: Vacuum, Surfaces and Films 1 publication, 0.56%
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Citations by publishers

	10 20 30 40 50 60
American Chemical Society (ACS)	American Chemical Society (ACS), 55, 31.07% American Chemical Society (ACS) 55 publications, 31.07%
Elsevier	Elsevier, 41, 23.16% Elsevier 41 publications, 23.16%
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American Vacuum Society	American Vacuum Society, 1, 0.56% American Vacuum Society 1 publication, 0.56%
World Scientific	World Scientific, 1, 0.56% World Scientific 1 publication, 0.56%
The Electrochemical Society	The Electrochemical Society, 1, 0.56% The Electrochemical Society 1 publication, 0.56%
Nonferrous Metals Society of China	Nonferrous Metals Society of China, 1, 0.56% Nonferrous Metals Society of China 1 publication, 0.56%
Cambridge University Press	Cambridge University Press, 1, 0.56% Cambridge University Press 1 publication, 0.56%
Chinese Ceramic Society	Chinese Ceramic Society, 1, 0.56% Chinese Ceramic Society 1 publication, 0.56%
Taiwan Institute of Chemical Engineers	Taiwan Institute of Chemical Engineers, 1, 0.56% Taiwan Institute of Chemical Engineers 1 publication, 0.56%
Chemical Industry Press	Chemical Industry Press, 1, 0.56% Chemical Industry Press 1 publication, 0.56%
American Association for the Advancement of Science (AAAS)	American Association for the Advancement of Science (AAAS), 1, 0.56% American Association for the Advancement of Science (AAAS) 1 publication, 0.56%
Japan Society of Applied Physics	Japan Society of Applied Physics, 1, 0.56% Japan Society of Applied Physics 1 publication, 0.56%
Walter de Gruyter	Walter de Gruyter, 1, 0.56% Walter de Gruyter 1 publication, 0.56%
Emerald	Emerald, 1, 0.56% Emerald 1 publication, 0.56%
Autonomous Non-profit Organization Editorial Board of the journal Uspekhi Khimii	Autonomous Non-profit Organization Editorial Board of the journal Uspekhi Khimii, 1, 0.56% Autonomous Non-profit Organization Editorial Board of the journal Uspekhi Khimii 1 publication, 0.56%
	10 20 30 40 50 60

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Chu I. et al. Insights into the Performance Limits of the Li7P3S11 Superionic Conductor: A Combined First-Principles and Experimental Study. // ACS applied materials & interfaces. 2016. Vol. 8. No. 12. pp. 7843-7853.

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Chu I., Nguyen H., Hy S., Lin Y., Wang Z., Xu Z., Deng Z., Meng Y., Ong S. P. Insights into the Performance Limits of the Li7P3S11 Superionic Conductor: A Combined First-Principles and Experimental Study. // ACS applied materials & interfaces. 2016. Vol. 8. No. 12. pp. 7843-7853.

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TY - JOUR

DO - 10.1021/acsami.6b00833

UR - https://doi.org/10.1021/acsami.6b00833

TI - Insights into the Performance Limits of the Li7P3S11 Superionic Conductor: A Combined First-Principles and Experimental Study.

T2 - ACS applied materials & interfaces

AU - Nguyen, Han

AU - Hy, Sunny

AU - Chu, Iek-Heng

AU - Lin, Yuh-Chieh

AU - Wang, Zhenbin

AU - Xu, Zihan

AU - Deng, Zhi

AU - Meng, Ying

AU - Ong, Shyue Ping

PY - 2016

DA - 2016/03/17 00:00:00

PB - American Chemical Society (ACS)

SP - 7843-7853

IS - 12

VL - 8

SN - 1944-8244

SN - 1944-8252

ER -

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BibTex Copy

@article{2016_Chu,

author = {Han Nguyen and Sunny Hy and Iek-Heng Chu and Yuh-Chieh Lin and Zhenbin Wang and Zihan Xu and Zhi Deng and Ying Meng and Shyue Ping Ong},

title = {Insights into the Performance Limits of the Li7P3S11 Superionic Conductor: A Combined First-Principles and Experimental Study.},

journal = {ACS applied materials & interfaces},

year = {2016},

volume = {8},

publisher = {American Chemical Society (ACS)},

month = {mar},

url = {https://doi.org/10.1021/acsami.6b00833},

number = {12},

pages = {7843--7853},

doi = {10.1021/acsami.6b00833}

}

MLA

Cite this

MLA Copy

Chu, Iek-Heng, et al. “Insights into the Performance Limits of the Li7P3S11 Superionic Conductor: A Combined First-Principles and Experimental Study..” ACS applied materials & interfaces, vol. 8, no. 12, Mar. 2016, pp. 7843-7853. https://doi.org/10.1021/acsami.6b00833.

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Publisher

American Chemical Society (ACS)

Journal

ACS applied materials & interfaces

Quartile SCImago

Quartile WOS

Impact factor

9.5

ISSN

19448244 (Print)
19448252 (Electronic)