Journal
ACS APPLIED ENERGY MATERIALS
Volume 4, Issue 7, Pages 6454-6465Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsaem.1c00438
Keywords
lithium metal anode; porous copper; three-dimensional current collector; tortuosity factor; X-ray microscale computed tomography; titration gas chromatography
Funding
- Office of Vehicle Technologies of the U.S. Department of Energy through the Advanced Battery Materials Research (BMR) Program (Battery500 Consortium) [DE-EE0007764]
- Office of Basic Energy Science of the U.S. Department of Energy [DE-SC0014213]
- National Science Foundation [ECCS-1542148]
- European Union through the European Research Council [772873]
- U.S. Department of Energy (DOE) [DE-SC0014213] Funding Source: U.S. Department of Energy (DOE)
- European Research Council (ERC) [772873] Funding Source: European Research Council (ERC)
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This study quantitatively investigated the impact of surface area, tortuosity factor, and surface chemistry on the performance of lithium metal batteries using porous copper networks. The role of tortuosity factor in lithiation was interpreted, and the optimal range of key parameters for porous coppers was identified to predict their performance, achieving high Coulombic efficiencies up to 99.63% and paving the way for effective 3D current collector systems.
Lithium metal has been an attractive candidate as a next-generation anode material. Despite its popularity, stability issues of lithium in the liquid electrolyte and the formation of lithium whiskers have kept it from practical use. Three-dimensional (3D) current collectors have been proposed as an effective method to mitigate whisker growth. Although extensive research has been done, the effects of three key parameters of the 3D current collectors, namely, the surface area, the tortuosity factor, and the surface chemistry, on the performance of lithium metal batteries remain elusive. Herein, we quantitatively studied the role of these three parameters by synthesizing four types of porous copper networks with different sizes of well-structured microchannels. X-ray microscale computed tomography (micro-CT) allowed us to assess the surface area, the pore size, and the tortuosity factor of the porous copper materials. A metallic Zn coating was also applied to study the influence of surface chemistry on the performance of the 3D current collectors. The effects of these parameters on the performance were studied in detail through scanning electron microscopy (SEM) and titration gas chromatography (TGC). Stochastic simulations further allowed us to interpret the role of the tortuosity factor in lithiation. The optimal range of the key parameters is thereby found for the porous coppers and their performance is predicted. Using these parameters to inform the design of porous copper anodes for Li deposition, Coulombic efficiencies (CEs) of up to 99.63% are achieved, thus paving the way for the design of effective 3D current collector systems.
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