A High‐Capacity, Long‐Cycling All‐Solid‐State Lithium Battery Enabled by Integrated Cathode/Ultrathin Solid Electrolyte

Abstract

flammable organic liquid electrolytes to solid-state electrolytes not only endows all-solid-state lithium batteries (ASSLBs) with considerable improvements in battery safety, but also potentially allows the use of Li metal anode, which is regarded as the ultimate anode due to its high theoretical specific capacity (3860 mAh g -1 ) and low electrochemical potential (−3.04 V versus standard hydrogen electrode). [3][4][5][6][7] Thus, ASSLBs have been widely exploited as next-generation energy storage technologies with enhanced energy density and safety. [8] However, current ASSLBs are far from competitive with commercial LIBs in terms of battery performance and ease of manufacturing. [9,10] This is because conventional ASSLB assembly requires laborious fabrication of solid electrolyte and electrodes separately, followed by stacking each component together, which inevitably results in poor interfacial contact. [11,12] Radically different from LIBs, solid electrolyte in ASSLBs cannot spontaneously wet the electrodes as liquid electrolyte does, leading to discontinuous ion transport at the cathode/solid electrolyte interfaces and inside the porous cathode, which results in a large interfacial resistance and low active material utilization. [13] As a consequence, the mass loading of most reported ASSLBs is too low (usually <4 mg cm -2 ) to meet the requirement for practical energy-dense batteries. [14] In addition, due to unfavorable mechanical properties, typical solid electrolytes need to be fabricated to be overly thick as a way of ensuring their integrity under unavoidable stress during conventional cell assembly processes. [9,15] For instance, pure ceramic solid electrolytes are generally too brittle to be produced with a thickness less than 100 µm. [16,17] Although blending the ceramics with polymers can endow the composite solid electrolyte with good flexibility, it is still challenging to reduce the thickness to be comparable with that of separators (usually <30 µm) in current LIBs, which, as a result, considerably sacrifices the battery energy density. [15,18] Even worse, the inferior mechanical strength of solid electrolytes renders a poor Li dendrite suppression capability, resulting in poor cyclability of the battery. [19] These limitations of conventional ASSLB manufacturing impose a great penalty on the attainable energy density and cyclability of the battery.To address these issues, several strategies have been developed for ASSLBs. For instance, Hu et al. reported on a dense/ porous bilayer garnet electrolyte, where the porous layer served Current all-solid-state lithium battery (ASSLB) manufacturing typically involves laborious fabrication and assembly of individual electrodes and solid electrolyte, which inevitably result in large interfacial resistances. Moreover, due to the unfavorable mechanical strength, most solid electrolytes are fabricated to be overly thick and are incapable of retarding lithium dendrite formation. These factors limit the attainable energy density and cyclability of ASSLBs. Her...

Progress and perspectives on electrospinning techniques for solid‐state lithium batteries

“…Battery tests verified the enhanced interfacial interaction in reducing the interface charge transfer resistance and the polarization, and a small interfacial charge transfer resistance ( R ct ) of 116.32 Ω was obtained for the LiFePO 4 half coin cell assembled with in situ PVDF‐HFP matrix, while as a contrast, the R ct of the mechanically mounted GPE assembled battery was 207.80 Ω. A similar strategy was reported recently by Lin and coworkers 146 . In such a work, the PVDF nanofibers were electrospun directly on the cathode, serving as the support for PEO/garnet‐type Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 based composite.…”

“…A similar strategy was reported recently by Lin and coworkers. 146 In such a work, the PVDF nanofibers were electrospun directly on the cathode, serving as the support for PEO/garnet-type Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 based composite. Due to the reinforcement of the robust fibrous network, an ultrathin SSE with a thickness of 17 µm is obtained with satisfying mechanical strength to inhibit the Li dendrite growth.…”

A High-Capacity Polyethylene Oxide-Based All-Solid-State Battery Using a Metal–Organic Framework Hosted Silicon Anode

“…The PPG was fabricated by incorporating PEO and garnet-type Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 (LLZTO) into the PVDF fiber skeleton developed in our previous work Figure d shows the SEM image of the PPG from the top view, which indicates that the CPE has a rather smooth surface.…”

“…The overwhelming trend of vehicle electrification worldwide has posed tremendous demands for power batteries with high energy density, long cycle life, and absolute safety. , Although lithium-ion batteries (LIBs) using graphite anodes have been widely used, they have gradually approached their limits on energy, and the flammable organic liquid electrolytes used in the LIBs also bring serious safety concerns. − To tackle the issues, all-solid-state batteries (ASSBs) using solid electrolytes (SEs) are regarded as promising future energy storage devices because they enable the possible use of a Li metal anode with greatly improved security. , …”

Dendrites‐Free Lithium Metal Anode Enabled by Synergistic Surface Structural Engineering

“…Nonetheless, the interfacial resistance between the electrode and solid electrolyte is extremely higher than that of the liquid one, which will deteriorate the electrochemical performance of the cells. [20][21][22][23] The ideal SEI layer with high Li + conductivity, electrical insulation, good chemical stability, high elastic modulus, and suitable thickness is typically prepared using chemical vapor deposition (CVD), [24] atomic layer deposition (ALD), [25] and magnetron sputtering, [26] which is tedious and costly, and cannot be applied to industrial production at a large scale. Generally, the dendrites can be physically confined in the internal pores of either the porous conductive framework (carbon-based materials [27][28][29] and metal-based materials [30][31][32][33][34] ) or hierarchical structure of Li metal with large specific surface area to some extent, and the overpotential of lithium nucleation can be reduced by lowering the local current density.…”