A Garnet-Type Solid-Electrolyte-Based Molten Lithium-Molybdenum-Iron(II) Chloride Battery with Advanced Reaction Mechanism

Jing Xu; Kai Liu; Yang Jin; Bin Sun; Zili Zhang; Yi Chen; Dawei Su; Guoxiu Wang; Hui Wu; Yi Cui

doi:10.1002/adma.202000960

A Garnet-Type Solid-Electrolyte-Based Molten Lithium-Molybdenum-Iron(II) Chloride Battery with Advanced Reaction Mechanism

Adv Mater. 2020 Aug;32(32):e2000960. doi: 10.1002/adma.202000960. Epub 2020 Jun 23.

Authors

Jing Xu¹, Kai Liu², Yang Jin¹, Bin Sun¹, Zili Zhang¹, Yi Chen³, Dawei Su³, Guoxiu Wang³, Hui Wu², Yi Cui^{4

5}

Affiliations

¹ Research Center of Grid Energy Storage and Battery Application, School of Electrical Engineering, Zhengzhou University, Zhengzhou, 450001, China.
² State Key Lab of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China.
³ Centre for Clean Energy Technology, University of Technology Sydney, Sydney, NSW, 2007, Australia.
⁴ Department of Materials Science and Engineering, Stanford University, Stanford, CA, 94305, USA.
⁵ Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA, 94025, USA.

PMID: 32578274
DOI: 10.1002/adma.202000960

Abstract

Solid-electrolyte-based molten-metal batteries have attracted considerable attention for grid-scale energy storage. Although ZEBRA batteries are considered one of the promising candidates, they still have the potential concern of metal particle growth and ion exchange with the β"-Al₂ O₃ electrolyte. Herein, a Li_6.4 La₃ Zr_1.4 Ta_0.6 O₁₂ solid-electrolyte-based molten lithium-molybdenum-iron(II) chloride battery (denoted as Li-Mo-FeCl₂ ) operated at temperature of 250 °C, comprising a mixture of Fe and LiCl cathode materials, a Li anode, a garnet-type Li-ion ceramic electrolyte, and Mo additive, is designed to overcome these obstacles. Different from conventional battery reaction mechanisms, this battery revolutionarily synchronizes the reversible Fe-Mo alloying-dealloying reactions with the delithiation-lithiation processes, meaning that the porous Mo framework derived from Fe-Mo alloy simultaneously suppresses the growth of pure Fe particles. By adopting a Li anode and a Li-ion ceramic electrolyte, the corrosion problem between the cathode and the solid electrolyte is overcome. With similar battery cost ($12 kWh^-1 ), the theoretical energy density of Li-Mo-FeCl₂ battery surpasses that of a Na-FeCl₂ ZEBRA battery over 25%, to 576 Wh kg^-1 and 2216 Wh L^-1 , respectively. Experimental results further prove this cell has excellent cycling performance (472 mAh g_LiCl ^-1 after 300 cycles, 50 mg active material) and strong tolerance against the overcharge-overdischarge (3-1.6 V) and freezing-thawing (25-250 °C) incidents.

Keywords: Fe3Mo alloys; garnet-type solid electrolytes; molten lithium; particle growth.

Abstract

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