Stable metal anodes enabled by a labile organic molecule bonded to a reduced graphene oxide aerogel

Abstract

Metallic anodes (lithium, sodium, and zinc) are attractive for rechargeable battery technologies but are plagued by an unfavorable metal–electrolyte interface that leads to nonuniform metal deposition and an unstable solid–electrolyte interphase (SEI). Here we report the use of electrochemically labile molecules to regulate the electrochemical interface and guide even lithium deposition and a stable SEI. The molecule, benzenesulfonyl fluoride, was bonded to the surface of a reduced graphene oxide aerogel. During metal deposition, this labile molecule not only generates a metal-coordinating benzenesulfonate anion that guides homogeneous metal deposition but also contributes lithium fluoride to the SEI to improve Li surface passivation. Consequently, high-efficiency lithium deposition with a low nucleation overpotential was achieved at a high current density of 6.0 mA cm−2. A Li|LiCoO2cell had a capacity retention of 85.3% after 400 cycles, and the cell also tolerated low-temperature (−10 °C) operation without additional capacity fading. This strategy was applied to sodium and zinc anodes as well.

Recent advances and future perspectives for aqueous zinc-ion capacitors

“…Third, the design of the zinc electrode structure can improve the electric field distribution, weaken the tip effect of deposition, and induce uniform deposition [96] and the design of the electrode electrolyte interface [97] is aimed at reducing interface impedance, improving interfacial wettability and reducing the overpotential and polarization of the deposition process [98]. For instance, the CC with zeolitic imidazolate framework-8 (ZIF-8) pre-grown was utilized to modify the surface of a zinc anode, which demonstrated a regulation effect on the nucleation, diffusion and deposition behaviors of zinc ions [99].…”

A perspective on energy chemistry of low-temperature lithium metal batteries

“…This robust SEI enables stable operation of LMBs in the temperature ranging from −15 to 70 °C. An all-fluorinated ester electrolyte was constructed to form a fluorine-rich SEI, which provides high capacities of 161, 149, and 133 mAh•g −1 of Li||NCM811 cell operating at −40, −50, and −60 °C [89] .…”

“…The SEI components can be facilely tailored through the employment of different solvents and Li salts [89] . However, the uncertainty and complexity of SEI properties varying with the temperatures make it tough to precisely control the SEI chemistry by simply regulating electrolytes.…”

A Li-based MOF-derived multifunctional PEO polymer solid-state electrolyte for lithium energy storage

“…6–11 Nonetheless, the usage of SSE enables us to construct a battery with high voltage cathodes; for example, Ni-rich layered oxide LiNi 0.8 Co 0.1 Mn 0.1 O 2 and spinel LiNi 0.5 Mn 1.5 O 2 , and high-capacity Li metal anode, thus leading to a high specific capacity (>500 W h kg −1 ). 12–17…”