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Hao, Hongchang
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Publications (5/5 displayed)
- 2024Alumina - Stabilized SEI and CEI in Potassium Metal Batteries.citations
- 2024Mechanical Milling – Induced Microstructure Changes in Argyrodite LPSCl Solid‐State Electrolyte Critically Affect Electrochemical Stabilitycitations
- 2023Tuned Reactivity at the Lithium Metal–Argyrodite Solid State Electrolyte Interphasecitations
- 2022Stable Anode-Free All-Solid-State Lithium Battery through Tuned Metal Wetting on the Copper Current Collectorcitations
- 2021A Sodium-Antimony-Telluride Intermetallic Allows Sodium-Metal Cycling at 100% Depth of Discharge and as an Anode-Free Metal Batterycitations
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article
Stable Anode-Free All-Solid-State Lithium Battery through Tuned Metal Wetting on the Copper Current Collector
Abstract
A stable anode-free all-solid-state battery (AF-ASSB) with sulfide-based solid-electrolyte (SE) (argyrodite Li6 PS5 Cl) is achieved by tuning wetting of lithium metal on "empty" copper current-collector. Lithiophilic 1 µm Li2 Te is synthesized by exposing the collector to tellurium vapor, followed by in situ Li activation during the first charge. The Li2 Te significantly reduces the electrodeposition/electrodissolution overpotentials and improves Coulombic efficiency (CE). During continuous electrodeposition experiments using half-cells (1 mA cm-2 ), the accumulated thickness of electrodeposited Li on Li2 Te-Cu is more than 70 µm, which is the thickness of the Li foil counter-electrode. Full AF-ASSB with NMC811 cathode delivers an initial CE of 83% at 0.2C, with a cycling CE above 99%. Cryogenic focused ion beam (Cryo-FIB) sectioning demonstrates uniform electrodeposited metal microstructure, with no signs of voids or dendrites at the collector-SE interface. Electrodissolution is uniform and complete, with Li2 Te remaining structurally stable and adherent. By contrast, an unmodified Cu current-collector promotes inhomogeneous Li electrodeposition/electrodissolution, electrochemically inactive "dead metal," dendrites that extend into SE, and thick non-uniform solid electrolyte interphase (SEI) interspersed with pores. Density functional theory (DFT) and mesoscale calculations provide complementary insight regarding nucleation-growth behavior. Unlike conventional liquid-electrolyte metal batteries, the role of current collector/support lithiophilicity has not been explored for emerging AF-ASSBs.