刘泽宇

Liu, Z.-Y., Huang, W.-Z., Xiao, Y., Zhang, J.-D., Kong, W.-J., Wu, P., Zhao, C.-Z.^*, Chen, A., & Zhang, Q.^* (2024). Nanocomposite Current Collectors for Anode-Free All-Solid-State Lithium Batteries. Acta Physico-Chimica Sinica, 40(3), 2305040. doi:10.3866/PKU.WHXB202305040

The anode-free solid-state lithium battery (AFSSLB) is a type of lithium battery that utilizes an initial charging process to generate lithium metal as the anode. With a 1: 1 anode-to-cathode capacity ratio, it enables any lithiated cathode system to achieve a maximal energy density. Furthermore, the incorporation of inorganic solid electrolytes in the AFSSLB greatly enhances its intrinsic safety. However, the AFSSLB faces challenges related to interfacial issues between the electrolyte and collector. During the cycling process, uneven lithium-ion flux can result in contact loss and dendrite growth, ultimately leading to rapid battery failure. Addressing these interfacial problems is crucial for the successful implementation and performance of AFSSLBs. The absence of initial lithium metal material prevents the battery system from accommodating additional lithium through a modified anode. Instead, it relies on high Coulomb efficiency during cycling. Consequently, ensuring continuous and uniform contact at the anode interface is crucial for maintaining the reversibility of lithium deposition. Herein, a nanocomposite current collector is introduced to enhance the interface between the collector and electrolyte in AFSSLB. In this approach, silver nanoparticles are dispersed within the carbon materials to construct a composite current collector. The incorporation of the silver-carbon nanocomposite layer results in a low interfacial impedance of 10 Ω·cm-2, indicating that the electrolyte-collector interface maintains contact throughout the charging and discharging processes. The focused ion beam (FIB) technology and electron microscopy were employed to analyze the battery cross sections, revealing that lithium metal could be deposited in a thickness of more than 25 μm without short-circuiting using this silver-carbon nanocomposite current collector. The solid-state batteries equipped with nanocomposite current collectors exhibited an enhanced dissolution of silver in the lithium metal, leading to the formation of abundant lithiophilic sites. The nanocomposites facilitate the rapid transfer of Li atoms within the anodes, thus achieving uniform lithium metal deposition. Theoretical analysis using the nucleation equation demonstrates that using nano-silver as a current collector can reduce the nucleation work required for deposition by at least four orders of magnitude. The smaller nucleation force contributes to the uniform and stable deposition of lithium metal during continuous cycling. The solid-state batteries demonstrated improved interfacial contact, resulting in the uniform and stable lithium metal deposition of over 7.0 mAh·cm-2 for more than 200 cycles at 0.25 mA·cm-2. The cycling performances of all-solid-state batteries can be significantly improved through the design of nanocomposite collectors. This presents an effective strategy for advancing the practical implementation of all-solid-state lithium metal batteries, particularly those utilizing an anode-free configuration.

https://www.whxb.pku.edu.cn/EN/10.3866/PKU.WHXB202305040

Huang, W.-Z., Liu, Z.-Y., Xu, P., Kong, W.-J., Huang, X.-Y., Shi, P., Wu, P., Zhao, C.-Z.^*, Yuan, H., Huang, J.-Q., & Zhang, Q.^* (2023). High-areal-capacity anode-free all-solid-state lithium batteries enabled by interconnected carbon-reinforced ionic-electronic composites. Journal of Materials Chemistry A, 11(24), 12713-12718. doi:10.1039/D3TA00121K

Taking energy density and safety into account, the anode-free all-solid-state lithium battery is a strong candidate to surpass the capabilities of routine lithium-ion batteries. However, achieving uniform stable lithium metal plating under high areal capacity is a grand challenge facing practical applications of lithium metal batteries. We report a high-performance anode-free all-solid-state lithium battery with a current collector consisting of carbon-reinforced ionic-electronic composites. When an interconnected carbon paper is compounded with a solid electrolyte, a three-dimensional ionic-electronic conduction network can be achieved, affording a large number of sites and scalable spaces for the nucleation and growth of lithium metal. The composite layer can achieve a long cycle life (>5000 cycles), stable lithium metal plating with a high areal capacity (>8 mAh cm−2), which is significantly better than that of the copper current collectors for routine anode-free configurations. The application of high-areal-capacity (4 mAh cm−2) pouch cell provides an efficient and effective strategy for practical anode-free all-solid-state lithium batteries.

https://pubs.rsc.org/en/content/articlelanding/2023/ta/d3ta00121k

Huang, W.-Z., Zhao, C.-Z.^*, Wu, P., Yuan, H., Feng, W.-E., Liu, Z.-Y., Lu, Y., Sun, S., Fu, Z.-H., Hu, J.-K., Yang, S.-J., Huang, J.-Q., & Zhang, Q.^* (2022). Anode-Free Solid-State Lithium Batteries: A Review. Advanced Energy Materials, 12(26), 2201044. doi:org/10.1002/aenm.202201044

Anode-free solid-state lithium batteries are promising for next-generation energy storage systems, especially the mobile sectors, due to their enhanced energy density, improved safety, and extended calendar life. However, the inefficiency of lithium plating and stripping leads to rapid capacity degradation due to the absence of excess lithium inventory. Therefore, dissecting the difficulties and challenges faced by anode-free solid-state lithium batteries can pave the way to improving the cycle life of many lithium batteries. In this review, the key issues affecting capacity degradation are elaborated step-by-step based on the current understanding of anode-free solid-state lithium batteries. Furthermore, various strategies for optimizing performance are targeted. Finally, future opportunities and possible directions for anode-free solid-state lithium batteries are evaluated, aiming to stimulate the exploration of this emerging field.

https://doi.org/10.1002/aenm.202201044