How Solid-Electrolyte Interphase Forms in Aqueous Electrolytes

Suo, Liumin; Oh, Dahyun; Lin, Yuxiao; Zhuo, Zengqing; Borodin, Oleg; Gao, Tao; Wang, Fei; Kushima, Akihiro; Wang, Ziqiang; Kim, Ho-Cheol; Qi, Yue; Yang, Wanli; Pan, Feng; Li, Ju; Xu, Kang; Wang, Chunsheng

doi:10.1021/jacs.7b10688

Title: How Solid-Electrolyte Interphase Forms in Aqueous Electrolytes

Journal Article · Wed Nov 29 00:00:00 EST 2017 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.7b10688· OSTI ID:1470066

Suo, Liumin ^[1];

^[2]; Lin, Yuxiao ^[3]; Zhuo, Zengqing ^[4];

^[5]; Gao, Tao ^[6]; Wang, Fei ^[7]; Kushima, Akihiro ^[8]; Wang, Ziqiang ^[8]; Kim, Ho-Cheol ^[9];

^[3];

^[10];

^[11];

^[8]; Xu, Kang ^[5];

^[6]

Chinese Academy of Sciences (CAS), Beijing (China). Key Lab. for Renewable Energy, Beijing Key Lab. for New Energy Materials and Devices, Beijing National Lab. for Condensed Matter Physics, Inst. of Physics
San Jose State Univ., CA (United States). Biomedical, Chemical and Materials Engineering Dept.; IBM Almaden Research Center, San Jose, CA (United States)
Michigan State Univ., East Lansing, MI (United States). Dept. of Chemical Engineering and Materials Science
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Peking Univ., Beijing (China). School of Advanced Materials
Army Research Lab., Adelphi, MD (United States). Electrochemistry Branch, Sensor and Electron Devices Directorate
Univ. of Maryland, College Park, MD (United States). Dept. of Chemical and Biomolecular Engineering
Army Research Lab., Adelphi, MD (United States). Electrochemistry Branch, Sensor and Electron Devices Directorate; Univ. of Maryland, College Park, MD (United States). Dept. of Chemical and Biomolecular Engineering
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Nuclear Science and Engineering, Dept. of Materials Science and Engineering
IBM Almaden Research Center, San Jose, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Peking Univ., Beijing (China). School of Advanced Materials

Solid-electrolyte interphase (SEI) is the key component that enables all advanced electrochemical devices, the best representative of which is Li-ion battery (LIB). It kinetically stabilizes electrolytes at potentials far beyond their thermodynamic stability limits, so that cell reactions could proceed reversibly. Its ad hoc chemistry and formation mechanism has been a topic under intensive investigation since the first commercialization of LIB 25 years ago. Traditionally SEI can only be formed in nonaqueous electrolytes. However, recent efforts successfully transplanted this concept into aqueous media, leading to significant expansion in the electrochemical stability window of aqueous electrolytes from 1.23 V to beyond 4.0 V. This not only made it possible to construct a series of high voltage/energy density aqueous LIBs with unprecedented safety, but also brought high flexibility and even “open configurations” that have been hitherto unavailable for any LIB chemistries. While this new class of aqueous electrolytes has been successfully demonstrated to support diversified battery chemistries, the chemistry and formation mechanism of the key component, an aqueous SEI, has remained virtually unknown. In this work, combining various spectroscopic, electrochemical and computational techniques, we rigorously examined this new interphase, and comprehensively characterized its chemical composition, microstructure and stability in battery environment. A dynamic picture obtained reveals how a dense and protective interphase forms on anode surface under competitive decompositions of salt anion, dissolved ambient gases and water molecule. By establishing basic laws governing the successful formation of an aqueous SEI, the in-depth understanding presented in this work will assist the efforts in tailor-designing better interphases that enable more energetic chemistries operating farther away from equilibria in aqueous media.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Nanostructures for Electrical Energy Storage (NEES)

Sponsoring Organization:: USDOE Advanced Research Projects Agency - Energy (ARPA-E)

Grant/Contract Number:: SC0001160

OSTI ID:: 1470066

Journal Information:: Journal of the American Chemical Society, Vol. 139, Issue 51; Related Information: NEES partners with University of Maryland (lead); University of California, Irvine; University of Florida; Los Alamos National Laboratory; Sandia National Laboratories; Yale University; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 289 works

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Title: How Solid-Electrolyte Interphase Forms in Aqueous Electrolytes

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