Lithium Argyrodite as Solid Electrolyte and Cathode Precursor for Solid-State Batteries with Long Cycle Life

Shuo WANG; Mingxue TANG; Qinghua ZHANG; Baohua LI; Saneyuki OHNO; Felix WALTHER; Ruijun PAN; Xiaofu XU; Chengzhou XIN; Wenbo ZHANG; Liangliang LI; Yang SHEN; Felix H. RICHTER; Jürgen JANEK; Ce-Wen NAN

doi:10.1002/aenm.202101370

Lithium Argyrodite as Solid Electrolyte and Cathode Precursor for Solid-State Batteries with Long Cycle Life

Shuo WANG, Mingxue TANG, Qinghua ZHANG, Baohua LI, Saneyuki OHNO, Felix WALTHER, Ruijun PAN, Xiaofu XU, Chengzhou XIN, Wenbo ZHANG, Liangliang LI, Yang SHEN, Felix H. RICHTER, Jürgen JANEK, Ce-Wen NAN

Research output: Journal Publications › Journal Article (refereed) › peer-review

78 Citations (Scopus)

Abstract

All-solid-state batteries with conversion-type cathodes promise to exceed the performance of lithium-ion batteries due to their high theoretical specific energy and potential safety. However, the reported performance of solid-state batteries is still unsatisfactory due to poor electronic and ionic conduction in the composite cathodes. Here, in situ formation of active material as well as highly effective ion- and electron-conducting paths via electrochemical decomposition of Li₆PS₅Cl_0.5Br_0.5 (LPSCB)/multiwalled carbon nanotube mixtures during cycling is reported. Effectively, the LPSCB electrolyte forms a multiphase conversion-type cathode by partial decomposition during the first discharge. Comprehensive characterization, especially operando pressure monitoring, reveals a co-redox process of two redox-active elements during cycling. The monolithic LPSCB-based cell shows stable cycling over 1000 cycles with a very high capacity retention of 94% at high current density (0.885 mA cm−2, ≈0.7 C) at room temperature and a high areal capacity of 12.56 mAh cm⁻²is achieved.

Original language	English
Article number	2101370
Journal	Advanced Energy Materials
Volume	11
Issue number	31
Early online date	1 Jul 2021
DOIs	https://doi.org/10.1002/aenm.202101370
Publication status	Published - 19 Aug 2021
Externally published	Yes

Bibliographical note

This work was supported by the Basic Science Center Program of National Natural Science Foundation of China (NSFC) under Grant No. 51788104 and NSFC projects under Grant Nos. 51625202, 51872157, and 21974007. J.J. and F.H.R. acknowledge the financial support from the project 03XP0177A funded by Bundesministerium für Bildung und Forschung (BMBF) within the cluster of competence FESTBATT. S.W. acknowledges the financial support by China Scholarship Council. The authors thank Yuan Liu at Qingdao University for drawing the schematic illustration of the LPSCB‐MWCNTs composite electrode, Jing Li at TESCAN CHINA conducting the FIB‐SEM measurements, and Xiaorui Hao at Tsinghua University for conducting some XPS measurements.

Keywords

all-solid-state batteries
argyrodite
conversion-type cathodes
operando pressure measurements

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1002/aenm.202101370Licence: CC BY-NC-ND

Cite this

@article{da2dff15c4b94200a305b874bc3078cd,

title = "Lithium Argyrodite as Solid Electrolyte and Cathode Precursor for Solid-State Batteries with Long Cycle Life",

abstract = "All-solid-state batteries with conversion-type cathodes promise to exceed the performance of lithium-ion batteries due to their high theoretical specific energy and potential safety. However, the reported performance of solid-state batteries is still unsatisfactory due to poor electronic and ionic conduction in the composite cathodes. Here, in situ formation of active material as well as highly effective ion- and electron-conducting paths via electrochemical decomposition of Li6PS5Cl0.5Br0.5 (LPSCB)/multiwalled carbon nanotube mixtures during cycling is reported. Effectively, the LPSCB electrolyte forms a multiphase conversion-type cathode by partial decomposition during the first discharge. Comprehensive characterization, especially operando pressure monitoring, reveals a co-redox process of two redox-active elements during cycling. The monolithic LPSCB-based cell shows stable cycling over 1000 cycles with a very high capacity retention of 94% at high current density (0.885 mA cm−2, ≈0.7 C) at room temperature and a high areal capacity of 12.56 mAh cm−2 is achieved.",

keywords = "all-solid-state batteries, argyrodite, conversion-type cathodes, operando pressure measurements",

author = "Shuo WANG and Mingxue TANG and Qinghua ZHANG and Baohua LI and Saneyuki OHNO and Felix WALTHER and Ruijun PAN and Xiaofu XU and Chengzhou XIN and Wenbo ZHANG and Liangliang LI and Yang SHEN and RICHTER, {Felix H.} and J{\"u}rgen JANEK and Ce-Wen NAN",

note = "This work was supported by the Basic Science Center Program of National Natural Science Foundation of China (NSFC) under Grant No. 51788104 and NSFC projects under Grant Nos. 51625202, 51872157, and 21974007. J.J. and F.H.R. acknowledge the financial support from the project 03XP0177A funded by Bundesministerium f{\"u}r Bildung und Forschung (BMBF) within the cluster of competence FESTBATT. S.W. acknowledges the financial support by China Scholarship Council. The authors thank Yuan Liu at Qingdao University for drawing the schematic illustration of the LPSCB‐MWCNTs composite electrode, Jing Li at TESCAN CHINA conducting the FIB‐SEM measurements, and Xiaorui Hao at Tsinghua University for conducting some XPS measurements.",

year = "2021",

month = aug,

day = "19",

doi = "10.1002/aenm.202101370",

language = "English",

volume = "11",

journal = "Advanced Energy Materials",

issn = "1614-6832",

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TY - JOUR

T1 - Lithium Argyrodite as Solid Electrolyte and Cathode Precursor for Solid-State Batteries with Long Cycle Life

AU - WANG, Shuo

AU - TANG, Mingxue

AU - ZHANG, Qinghua

AU - LI, Baohua

AU - OHNO, Saneyuki

AU - WALTHER, Felix

AU - PAN, Ruijun

AU - XU, Xiaofu

AU - XIN, Chengzhou

AU - ZHANG, Wenbo

AU - LI, Liangliang

AU - SHEN, Yang

AU - RICHTER, Felix H.

AU - JANEK, Jürgen

AU - NAN, Ce-Wen

N1 - This work was supported by the Basic Science Center Program of National Natural Science Foundation of China (NSFC) under Grant No. 51788104 and NSFC projects under Grant Nos. 51625202, 51872157, and 21974007. J.J. and F.H.R. acknowledge the financial support from the project 03XP0177A funded by Bundesministerium für Bildung und Forschung (BMBF) within the cluster of competence FESTBATT. S.W. acknowledges the financial support by China Scholarship Council. The authors thank Yuan Liu at Qingdao University for drawing the schematic illustration of the LPSCB‐MWCNTs composite electrode, Jing Li at TESCAN CHINA conducting the FIB‐SEM measurements, and Xiaorui Hao at Tsinghua University for conducting some XPS measurements.

PY - 2021/8/19

Y1 - 2021/8/19

N2 - All-solid-state batteries with conversion-type cathodes promise to exceed the performance of lithium-ion batteries due to their high theoretical specific energy and potential safety. However, the reported performance of solid-state batteries is still unsatisfactory due to poor electronic and ionic conduction in the composite cathodes. Here, in situ formation of active material as well as highly effective ion- and electron-conducting paths via electrochemical decomposition of Li6PS5Cl0.5Br0.5 (LPSCB)/multiwalled carbon nanotube mixtures during cycling is reported. Effectively, the LPSCB electrolyte forms a multiphase conversion-type cathode by partial decomposition during the first discharge. Comprehensive characterization, especially operando pressure monitoring, reveals a co-redox process of two redox-active elements during cycling. The monolithic LPSCB-based cell shows stable cycling over 1000 cycles with a very high capacity retention of 94% at high current density (0.885 mA cm−2, ≈0.7 C) at room temperature and a high areal capacity of 12.56 mAh cm−2 is achieved.

AB - All-solid-state batteries with conversion-type cathodes promise to exceed the performance of lithium-ion batteries due to their high theoretical specific energy and potential safety. However, the reported performance of solid-state batteries is still unsatisfactory due to poor electronic and ionic conduction in the composite cathodes. Here, in situ formation of active material as well as highly effective ion- and electron-conducting paths via electrochemical decomposition of Li6PS5Cl0.5Br0.5 (LPSCB)/multiwalled carbon nanotube mixtures during cycling is reported. Effectively, the LPSCB electrolyte forms a multiphase conversion-type cathode by partial decomposition during the first discharge. Comprehensive characterization, especially operando pressure monitoring, reveals a co-redox process of two redox-active elements during cycling. The monolithic LPSCB-based cell shows stable cycling over 1000 cycles with a very high capacity retention of 94% at high current density (0.885 mA cm−2, ≈0.7 C) at room temperature and a high areal capacity of 12.56 mAh cm−2 is achieved.

KW - all-solid-state batteries

KW - argyrodite

KW - conversion-type cathodes

KW - operando pressure measurements

UR - http://www.scopus.com/inward/record.url?scp=85109271873&partnerID=8YFLogxK

U2 - 10.1002/aenm.202101370

DO - 10.1002/aenm.202101370

M3 - Journal Article (refereed)

AN - SCOPUS:85109271873

SN - 1614-6832

VL - 11

JO - Advanced Energy Materials

JF - Advanced Energy Materials

IS - 31

M1 - 2101370

ER -

Lithium Argyrodite as Solid Electrolyte and Cathode Precursor for Solid-State Batteries with Long Cycle Life

Abstract

Bibliographical note

Keywords

UN SDGs

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