Large-Scale Fabrication of Boron Nitride Nanosheets and Their Utilization in Polymeric Composites with Improved Thermal and Mechanical Properties

Solid-state lithium (Li) metal batteries (SSLMBs) have become a research hotspot in the energy storage field due to the much-enhanced safety and high energy density. However, the SSLMBs suffer from failures including dendrite-induced short circuits and contact-loss-induced high impedance, which are highly related to the Li plating/stripping kinetics and hinder the practical application of SSLMBs. The maximum endurable current density of lithium battery cycling without cell failure in SSLMB is generally defined as critical current density (CCD). Therefore, CCD is an important parameter for the application of SSLMBs, which can help to determine the rate-determining steps of Li kinetics in solid-state batteries. Herein, the theoretical and practical meanings for CCD from the fundamental thermodynamic and kinetic principles, failure mechanisms, CCD identifications, and influence factors for improving CCD performances are systematically reviewed. Based on these fundamental understandings, a series of strategies and outlooks for future researches on SSLMB are presented, endeavoring on increasing CCD for practical SSLMBs.

Critical Current Density in Solid‐State Lithium Metal Batteries: Mechanism, Influences, and Strategies

Rechargeable batteries with lithium metal anodes exhibit higher energy densities than conventional lithium-ion batteries. Solid-state electrolytes (SSEs) provide the opportunity to unlock the full potential of lithium metal anodes and fundamentally eliminate safety concerns caused by flammable liquid electrolytes. Up to now, most studies on SSEs have been focused on enhancing the ionic conductivity and improving the interfacial stability. However, the electrolyte thickness, which has received less attention, also plays an important role in determining the energy density and electrochemical performance of all-solid-state lithium batteries (ASSLBs). Recognizing this, our review evaluates SSE studies beyond traditional factors and focuses on a thickness perspective. We systematically analyze the influence of the electrolyte thickness on the energy densities of ASSLB pouch cells, and highlight the strategies that dramatically reduce the thickness of SSE membranes without sacrificing their mechanical properties. Then, we discuss recent advances and challenges of ASSLBs based on high-voltage and high-capacity cathodes, as well as novel configurations such as bipolar and flexible ASSLBs. Finally, we provide perspectives and suggestions towards high energy-density ASSLBs for future commercialization.

Reducing the thickness of solid-state electrolyte membranes for high-energy lithium batteries

With the low redox potential of -3.04 V (vs SHE) and ultrahigh theoretical capacity of 3862 mAh g-1 , lithium metal has been considered as promising anode material. However, lithium metal battery has ever suffered a trough in the past few decades due to its safety issues. Over the years, the limited energy density of the lithium-ion battery cannot meet the growing demands of the advanced energy storage devices. Therefore, lithium metal anodes receive renewed attention, which have the potential to achieve high-energy batteries. In this review, the history of the lithium anode is reviewed first. Then the failure mechanism of the lithium anode is analyzed, including dendrite, dead lithium, corrosion, and volume expansion of the lithium anode. Further, the strategies to alleviate the lithium anode issues in recent years are discussed emphatically. Eventually, remaining challenges of these strategies and possible research directions of lithium-anode modification are presented to inspire innovation of lithium anode.

Confronting the Challenges in Lithium Anodes for Lithium Metal Batteries.

Garnet Solid Electrolyte for Advanced All-Solid-State Li Batteries

Solid-state lithium metal batteries (SSLMBs) are promising energy storage devices by employing lithium metal anodes and solid-state electrolytes (SSEs) to offer high energy density and high safety. However, their efficiency is limited by Li metal/SSE interface barriers, including insufficient contact area and chemical/electrochemical incompatibility. Herein, a strategy to effectively improve the adhesiveness of Li metal to garnet-type SSE is proposed by adding only a few two-dimensional boron nitride nanosheets (BNNS) (5 wt %) into Li metal by triggering the transition from point contact to complete adhesion between Li metal and ceramic SSE. The interface between the Li-BNNS composite anode and the garnet exhibits a low interfacial resistance of 9 Ω cm2, which is significantly lower than that of bare Li/garnet interface (560 Ω cm2). Furthermore, the enhanced contact and the additional BNNS in the interface act synergistically to offer a high critical current density of 1.5 mA/cm2 and a stable electrochemical plating/striping over 380 h. Moreover, the full cell paired with the Li-BNNS composite anode and the LiFePO4 cathode shows stable cycling performance at room temperature. Our results introduce an appealing composite strategy with two-dimensional materials to overcome the interface challenges, which provide more opportunities for the development of SSLMBs.

Highly Adhesive Li-BN Nanosheet Composite Anode with Excellent Interfacial Compatibility for Solid-State Li Metal Batteries.

Solid-state lithium metal batteries (SSLMBs), using lithium metal as the anode and garnet-structured Li6.5La3Zr1.5Ta0.5O12 (LLZTO) as the electrolyte, are attractive and promising due to their high energy density and safety. However, the interface contact between the lithium metal and LLZTO is a major obstacle to the performance of SSLMBs. Here, we successfully improve the interface wettability by introducing one-dimensional (1D) TiO2 nanofibers into the lithium metal to obtain a Li-lithiated TiO2 composite anode (Li-TiO2). When 10 wt % TiO2 nanofibers are added, the formed composite anode offers a seamless interface contact with LLZTO and enables an interfacial resistance of 27 Ω cm2, which is much smaller than 374 Ω cm2 of pristine lithium metal. Due to the enhanced interface wettability, the symmetric Li-TiO2|LLZTO|Li-TiO2 cell upgrades the critical current density to 2.2 mA cm-2 and endures stable cycling over 550 h. Furthermore, by coupling the Li-TiO2 composite anode with the LiFePO4 cathode, the full cell shows stable cycling performance. This work proves the role of TiO2 nanofibers in enhancing the interface contact between the garnet electrolyte and the lithium metal anode and improving the performance of SSLMBs and provides an effective approach with 1D additives for solving the interface issues.

TiO2 Nanofiber-Modified Lithium Metal Composite Anode for Solid-State Lithium Batteries.

of times higher of cell this new blending can the control cell with the a stable cycling performance in solid-state LiFePO a retention of

Engineering a flexible and mechanically strong composite electrolyte for solid-state lithium batteries

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Highly Adhesive Li-BN Nanosheet Composite Anode with Excellent Interfacial Compatibility for Solid-State Li Metal Batteries.

TiO2 Nanofiber-Modified Lithium Metal Composite Anode for Solid-State Lithium Batteries.

Engineering a flexible and mechanically strong composite electrolyte for solid-state lithium batteries