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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 whiskers growth. Although extensive research efforts have 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 micro-channels. 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. By understanding these effects, the optimal range of the key parameters is found for the porous copper anodes and their performance is predicted. Using these parameters to inform the design of porous copper anodes for Li deposition, Coulombic efficiencies (CE) of up to 99.56% are achieved, thus paving the way for the design of effective 3D current collector systems.
Lithium metal cells are key towards achieving high specific energy and energy density for electrification of transportation and aviation. Anode-free cells are the limiting case of lithium metal cells involving no excess lithium and the highest possib
Using first principles structure searching with density-functional theory (DFT) we identify a novel $Fmbar{3}m$ phase of Cu$_2$P and two low-lying metastable structures, an $Ibar{4}3d$--Cu$_3$P phase, and a $Cm$--Cu$_3$P$_{11}$ phase. The computed pa
Li-ion rechargeable batteries have enabled the wireless revolution transforming global communication. Future challenges, however, demands distributed energy supply at a level that is not feasible with the current energy-storage technology. New materi
Extensive efforts have been devoted to C-Si compound materials for improving the limited specific capacity of graphite anode and avoiding the huge volume change of Si anode in Li-ion battery, but not much progress has been made during the past decade
Next generation batteries based on lithium (Li) metal anodes have been plagued by the dendritic electrodeposition of Li metal on the anode during cycling, resulting in short circuit and capacity loss. Suppression of dendritic growth through the use o