All-temperature zinc batteries with high-entropy aqueous electrolyte

Yang, Chongyin; Xia, Jiale; Cui, Chunyu; Pollard, Travis P.; Vatamanu, Jenel; Faraone, Antonio; Dura, Joseph A.; Tyagi, Madhusudan; Kattan, Alex; Thimsen, Elijah; Xu, Jijian; Song, Wentao; Hu, Enyuan; Ji, Xiao; Hou, Singyuk; Zhang, Xiyue; Ding, Michael S.; Hwang, Sooyeon; Su, Dong; Ren, Yang; Yang, Xiao-Qing; Wang, Howard; Borodin, Oleg; Wang, Chunsheng

doi:10.1038/s41893-022-01028-x

Title: All-temperature zinc batteries with high-entropy aqueous electrolyte

Journal Article · Mon Jan 09 00:00:00 EST 2023 · Nature Sustainability

DOI:https://doi.org/10.1038/s41893-022-01028-x· OSTI ID:1960271

^[1]; Xia, Jiale ^[2]; Cui, Chunyu ^[2];

^[3];

^[3]; Faraone, Antonio ^[4];

^[4]; Tyagi, Madhusudan ^[5]; Kattan, Alex ^[6]; Thimsen, Elijah ^[6];

^[2];

^[7];

^[8]; Ji, Xiao ^[2];

^[2]; Zhang, Xiyue ^[2]; Ding, Michael S. ^[3]; Hwang, Sooyeon ^[9];

^[9]; Ren, Yang ^[10] more »

Univ. of Maryland, College Park, MD (United States); Dalhousie Univ., Halifax, NS (Canada)
Univ. of Maryland, College Park, MD (United States)
DEVCOM Army Research Lab., Adelphi, MD (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States); Univ. of Maryland, College Park, MD (United States)
Washington Univ., St. Louis, MO (United States)
Dalhousie Univ., Halifax, NS (Canada)
Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Div.
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS); City Univ. of Hong Kong, Kowloon (Hong Kong)

Electrification of transportation and rising demand for grid energy storage continue to build momentum around batteries across the globe. However, the supply chain of Li-ion batteries is exposed to the increasing challenges of resourcing essential and scarce materials. Therefore, incentives to develop more sustainable battery chemistries are growing. Here, in this paper, we show an aqueous ZnCl₂ electrolyte with introduced LiCl as supporting salt. Once the electrolyte is optimized to Li₂ZnCl₄∙9H₂O, the assembled Zn–air battery can sustain stable cycling over the course of 800 hours at a current density of 0.4 mA cm^-2 between -60 °C and +80 °C, with 100% Coulombic efficiency for Zn stripping/plating. Even at -60 °C, >80% of room-temperature power density can be retained. Advanced characterization and theoretical calculations reveal a high-entropy solvation structure that is responsible for the excellent performance. The strong acidity allows ZnCl₂ to accept donated Cl^- ions to form ZnCl₄^2- anions, while water molecules remain within the free solvent network at low salt concentration or coordinate with Li ions. Our work suggests an effective strategy for the rational design of electrolytes that could enable next-generation Zn batteries.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Advanced Research Projects Agency - Energy (ARPA-E); Natural Sciences and Engineering Research Council of Canada (NSERC); US Army Research Laboratory (USARL); Joint Center for Energy Storage Research (JCESR); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704; AR0000389; IAA SN2020957; RGPIN-2021-02426; 1847469; 1508249

OSTI ID:: 1960271

Report Number(s):: BNL-224094-2023-JAAM

Journal Information:: Nature Sustainability, Vol. 6, Issue 3; ISSN 2398-9629

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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Title: All-temperature zinc batteries with high-entropy aqueous electrolyte

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