Compatibility issues between electrodes and electrolytes in solid-state batteries
Abstract
Remarkable success has been achieved in the discovery of ceramic alkali superionic conductors as electrolytes in solid-state batteries; however, obtaining a stable interface between these electrolytes and electrodes is difficult. Only limited studies on the compatibility between electrodes and solid electrolytes have been reported, partially because of the need for expensive instrumentation and special cell designs. Without simple yet powerful tools, these compatibility issues cannot be systematically investigated, thus hindering the generalization of design rules for the integration of solid-state battery components. Herein, we present a methodology that combines density functional theory calculations and simple experimental techniques such as X-ray diffraction, simultaneous differential scanning calorimetry and thermal gravimetric analysis, and electrochemistry to efficiently screen the compatibility of numerous electrode/electrolyte pairs. We systemically distinguish between the electrochemical stability of the solid-state conductor, which is relevant wherever the electrolyte contacts an electron pathway, and the electrochemical stability of the electrode/electrolyte interfaces. For the solid electrolyte, we are able to computationally derive an absolute thermodynamic stability voltage window, which is small for Na3PS4 and Na3PSe4, and a larger voltage window which can be kinetically stabilized. The experimental stability, when measured with reliable techniques, falls between these thermodynamic and kinetic limits. Employing a Namore »
- Authors:
-
- Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
- Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Samsung Advanced Inst. of Technology (Korea, Republic of)
- OSTI Identifier:
- 1475003
- Grant/Contract Number:
- AC02-05CH11231; ACI-1053575
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Energy & Environmental Science
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 5; Journal ID: ISSN 1754-5692
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE
Citation Formats
Tian, Yaosen, Shi, Tan, Richards, William D., Li, Juchuan, Kim, Jae Chul, Bo, Shou-Hang, and Ceder, Gerbrand. Compatibility issues between electrodes and electrolytes in solid-state batteries. United States: N. p., 2017.
Web. doi:10.1039/c7ee00534b.
Tian, Yaosen, Shi, Tan, Richards, William D., Li, Juchuan, Kim, Jae Chul, Bo, Shou-Hang, & Ceder, Gerbrand. Compatibility issues between electrodes and electrolytes in solid-state batteries. United States. https://doi.org/10.1039/c7ee00534b
Tian, Yaosen, Shi, Tan, Richards, William D., Li, Juchuan, Kim, Jae Chul, Bo, Shou-Hang, and Ceder, Gerbrand. Wed .
"Compatibility issues between electrodes and electrolytes in solid-state batteries". United States. https://doi.org/10.1039/c7ee00534b. https://www.osti.gov/servlets/purl/1475003.
@article{osti_1475003,
title = {Compatibility issues between electrodes and electrolytes in solid-state batteries},
author = {Tian, Yaosen and Shi, Tan and Richards, William D. and Li, Juchuan and Kim, Jae Chul and Bo, Shou-Hang and Ceder, Gerbrand},
abstractNote = {Remarkable success has been achieved in the discovery of ceramic alkali superionic conductors as electrolytes in solid-state batteries; however, obtaining a stable interface between these electrolytes and electrodes is difficult. Only limited studies on the compatibility between electrodes and solid electrolytes have been reported, partially because of the need for expensive instrumentation and special cell designs. Without simple yet powerful tools, these compatibility issues cannot be systematically investigated, thus hindering the generalization of design rules for the integration of solid-state battery components. Herein, we present a methodology that combines density functional theory calculations and simple experimental techniques such as X-ray diffraction, simultaneous differential scanning calorimetry and thermal gravimetric analysis, and electrochemistry to efficiently screen the compatibility of numerous electrode/electrolyte pairs. We systemically distinguish between the electrochemical stability of the solid-state conductor, which is relevant wherever the electrolyte contacts an electron pathway, and the electrochemical stability of the electrode/electrolyte interfaces. For the solid electrolyte, we are able to computationally derive an absolute thermodynamic stability voltage window, which is small for Na3PS4 and Na3PSe4, and a larger voltage window which can be kinetically stabilized. The experimental stability, when measured with reliable techniques, falls between these thermodynamic and kinetic limits. Employing a Na solid-state system as an example, we demonstrate the efficiency of our method by finding the most stable system (NaCrO2|Na3PS4|Na–Sn) within a selected chemical space (more than 20 different combinations of electrodes and electrolytes). Important selection criteria for the cathode, electrolyte, and anode in solid-state batteries are also derived from this study. The current method not only provides an essential guide for integrating all-solid-state battery components but can also significantly accelerate the expansion of the electrolyte/electrode compatibility data.},
doi = {10.1039/c7ee00534b},
journal = {Energy & Environmental Science},
number = 5,
volume = 10,
place = {United States},
year = {Wed Apr 26 00:00:00 EDT 2017},
month = {Wed Apr 26 00:00:00 EDT 2017}
}
Web of Science
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Sulfide‐Compatible Conductive and Adhesive Glue‐Like Interphase Engineering for Sheet‐Type All‐Solid‐State Battery
journal, August 2019
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High magnesium mobility in ternary spinel chalcogenides
journal, November 2017
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Three-dimensional atomic-scale observation of structural evolution of cathode material in a working all-solid-state battery
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Fundamentals of inorganic solid-state electrolytes for batteries
journal, August 2019
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Clarifying the relationship between redox activity and electrochemical stability in solid electrolytes
journal, January 2020
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Understanding interface stability in solid-state batteries
journal, December 2019
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Theoretical tuning of Ruddlesden–Popper type anti-perovskite phases as superb ion conductors and cathodes for solid sodium ion batteries
journal, January 2019
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- Journal of Materials Chemistry A, Vol. 7, Issue 17
The critical role of oxygen-evolution kinetics in the electrochemical stability of oxide superionic conductors
journal, January 2019
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Theoretical formulation of Na 3 AO 4 X (A = S/Se, X = F/Cl) as high-performance solid electrolytes for all-solid-state sodium batteries
journal, January 2019
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Electrochemically Stable Coating Materials for Li, Na, and Mg Metal Anodes in Durable High Energy Batteries
journal, January 2017
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Surface Modification of the LiNi 0.5 Co 0.2 Mn 0.3 O 2 Cathode by a Protective Interface Layer of Li 1.3 Ti 1.7 Al 0.3 (PO 4 ) 3
journal, January 2019
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Predictive modeling and design rules for solid electrolytes
journal, October 2018
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Building Better Batteries in the Solid State: A Review
journal, November 2019
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Tailored Organic Electrode Material Compatible with Sulfide Electrolyte for Stable All-Solid-State Sodium Batteries
journal, February 2018
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Integrated study of first principles calculations and experimental measurements for Li-ionic conductivity in Al-doped solid-state LiGe2(PO4)3 electrolyte
journal, October 2015
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