Enabling Magnesium Anodes by Tuning the Electrode/Electrolyte Interfacial Structure

Wen, Xiaoyu; Yu, Zhou; Zhao, Yifan; Zhang, Jian; Qiao, Rui; Cheng, Lei; Ban, Chunmei; Guo, Juchen

doi:10.1021/acsami.1c10446

Enabling Magnesium Anodes by Tuning the Electrode/Electrolyte Interfacial Structure

Journal Article · Mon Nov 01 00:00:00 EDT 2021 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.1c10446· OSTI ID:1844340

Wen, Xiaoyu ^[1]; ^[2]; Zhao, Yifan ^[1]; ^[1]; ^[3]; ^[2]; ^[4]; ^[1]

Univ. of California, Riverside, CA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research (JCESR)
Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
Univ. of Colorado, Boulder, CO (United States)

Here, a new deposition mechanism is presented in this study to achieve highly reversible plating and stripping of magnesium (Mg) anodes for Mg-ion batteries. It is known that the reduction of electrolyte anions such as bi s (trifluoromethanesulfonyl) imide (TFSI^-) causes Mg surface passivation, resulting in poor electrochemical performance for Mg-ion batteries. We reveal that the addition of sodium cations (Na⁺) in Mg-ion electrolytes can fundamentally alter the interfacial chemistry and structure at the Mg anode surface. The molecular dynamics simulation suggests that Na⁺ cations contribute to a significant population in the interfacial double layer so that TFSI^- anions are excluded from the immediate interface adjacent to the Mg anode. As a result, the TFSI^- decomposition is largely suppressed so does the formation of passivation layers at the Mg surface. This mechanism is supported by our electrochemical, microscopic, and spectroscopic analyses. The resultant Mg deposition demonstrates smooth surface morphology and lowered overpotential compared to the pure Mg(TFSI)₂ electrolyte.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1844340

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 44 Vol. 13; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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