Metal–Organic Frameworks Derived Electrolytes Build Multiple Wetting Interfaces for Integrated Solid‐State Lithium–Oxygen Battery

Abstract

Solid-state lithium-oxygen (Li-O 2 ) batteries are considered as the next-generation solution for high-safety energy storage systems to overcome the persistent problems associated with liquid battery systems. However, the absence of stable solid-state electrolytes (SSEs) and the design complexity of functional solid-state cathode (SSC) remains a fundamental challenge. Here, a high-performance solid-state Li-O 2 battery is presented with Li-ion-conducted UiO-67 (UiO-67-Li) as SSEs and UiO-67-Li@reduced graphene oxide (rGO) aerogel integrated structure as SSC. The UiO-67-Li SSEs reveal exceptional conductivity (0.64 mS cm −1 at 25 °C) along with high chemical/electrochemical robustness. Furthermore, the prepared UiO-67-Li@rGO aerogel exhibits continuous and abundant Li + /e − transfer and O 2 diffusion channels. Benefiting from the unique chemical properties of the UiO-67-Li SSEs layer, the solid-state Li-O 2 battery achieves suppression of anode dendrite formation, resistance to air-corrosion, and presence of multiple low-impedance wetting interfaces including anode/electrolyte and electrolyte/cathode. This ingenious arrangement endows the solid-state Li-O 2 battery with low overpotential (0.8 V), superior rate capability, and stable cycling life (up to 115 cycles). This novel design and exciting result will open up one avenue for the development of MOF-based SSEs and cathodes for high-performance solid-state Li-O 2 batteries and other solid-state energy-storage devices.

Metal–Organic Framework-Based Mixed Conductors Achieve Highly Stable Photo-assisted Solid-State Lithium–Oxygen Batteries

“…Besides, the EIS results revealed that H 2 O and KO 2 /DMSO treatments have a negligible effect on NH 2 -MIL-125-Li (Figure S26). 18 Advanced comprehensive performance of NH 2 -MIL-125-Li could also be confirmed compared with other different reported MOFs applied in Li-ion batteries (Figure S27 and Table S1). 5b).…”

“…Besides, the EIS results revealed that H 2 O and KO 2 /DMSO treatments have a negligible effect on NH 2 -MIL-125-Li (Figure S26). Advanced comprehensive performance of NH 2 -MIL-125-Li could also be confirmed compared with other different reported MOFs applied in Li-ion batteries (Figure S27 and Table S1). The superior ionic conductivity behavior, electrochemical stability, and chemical stability would guarantee their great potential as SSEs in solid-state Li–O 2 batteries.…”

“…The introduction of photo-assisted Li–O 2 batteries has been demonstrated as an effective strategy to achieve high performance with superior reaction kinetics and low energy barriers, ,− which depend largely on the development of semiconductor photocathodes with the generation capability of highly active electrons and holes by capturing photons. Thus, many research efforts have been devoted to the rational design of semiconductor cathode catalysts to expand the limited utilization of solar energy and the recombination of photoelectron–hole pairs. , However, the severe electrolyte decomposition and Li anode corrosion almost always lead to premature battery failure. , To alleviate these issues, solid-state electrolytes (SSEs) are considered to be an effective strategy benefiting from their inherent safety characteristics and mechanical strength to block dendrites. ,, Furthermore, a solid-state Li–O 2 battery offers a promising direction to reduce irreversible electrolyte decomposition, enhance the safety, and suppress the dendrite growth by replacing liquid electrolytes with SSEs. − However, high-performance solid-state Li–O 2 batteries are restricted by several key factors such as superior multifunctional solid-state cathodes (SSCs), high ionic-conductive SSEs, electrochemical/chemical stability at interfaces, and sustainable recycling. The combination of SSEs with photo-assisted batteries would provide a feasible and efficient direction for the development of high-performance, safe Li–O 2 batteries.…”

Hierarchical porous metal–organic gels and derived materials: from fundamentals to potential applications

“…368,369 MOF-based aerogels recently attracted much attention as promising electrode materials for EES due to their high surface areas and interconnected networks of multimodalities, which provide short diffusion paths and fine dispersion of active sites to maximize the rate of reactions. 370–373 Although the direct use of many MOFs in electrochemical devices is limited due to their poor electrical conductivity and low chemical stability, metal–carbon complex nanostructures have shown potential to deliver desired electrochemical properties. 374–376 This section highlights how such tuneable MOGs derived materials advance the performance of lithium-ion batteries (LIBs) and supercapacitors.…”

Homogeneous Li+flux realized by anin situ-formed Li–B alloy layer enabling the dendrite-free lithium metal anode

“…[8][9][10][11] Recently, several state-of-the-art strategies have been proposed to circumvent the above issues, mainly including constructing an artificial SEI film to stabilize the electrode surface and reduce side reactions between the electrolyte and electrode, 12,13 optimizing electrolyte composition to enhance the stability of the SEI film, [14][15][16][17] and developing solid-state electrolytes with high modulus to protect the separator from dendrites. [18][19][20][21] Although these strategies can effectively suppress the growth of Li dendrites and improve the electrochemical performance to some extent, the SEI-modified LMAs with the "hostless" feature hardly withstand the large volume change during long-term cycling and hinder further development of LMBs. [22][23][24] By contrast, accommodating the deposited Li metal into the three-dimensional (3D) current collectors has the potential to become a more effective strategy to resolve these intractable problems.…”