Lithium (Li) metal is a promising anode material for lithium-ion batteries (LIBs) because of its high theoretical specific capacity of 3860 mAh g −1 and the low potential of −3.04 V versus the standard hydrogen electrode (SHE). However, these anodes rely on repeated plating and stripping of Li, which leads to consumption of Li inventory and the growth of dendrites that can lead to self-discharge and safety issues. To address these issues, as well as problems related to the volume change of these anodes, a number of different porous conductive scaffolds have been reported to create high surface area electrode on which Li can be plated reliably. While impressive results have been reported in literature, current processes typically rely on either expensive or poorly scalable techniques. Herein, we report a scalable fabrication method to create robust 3D Cu anodes using a one-step electrodeposition process. The areal loading, pore structure, and electrode thickness can be tuned by changing the electrodeposition parameters, and we show how standard mechanical calendering provides a way to further optimize electrode volume, capacity, and cycling stability. Optimized electrodes achieve high Coulombic efficiencies (CEs) of 99% during 800 cycles in half cells at a current density of 0.5 mA cm −2 with a total capacity of 0.5 mAh cm −2 . To the best of our knowledge, this is the highest value ever reported for a host for Li-metal anodes using lithium bis(trifluoromethanesulfonyl)imide LITFSI based electrolyte.

The use of emulsions as templates for nanomaterial assembly is a versatile method to create controlled microstructures. However, production rates are often low, particularly where the droplet phase solvent must be removed to achieve consolidation. Here, the emulsion templated fabrication of microparticles from multi‐walled carbon nanotubes (CNTs) is studied. As an exemplar primary nanoparticle for microparticle assembly, CNTs present particular challenges due to their strong inter‐particle interactions and limited dispersion in solvents. Nevertheless, small batches of CNT microparticles have demonstrated promising performances in energy storage, environmental remediation, and sensing due to their controlled structures. Improving CNT microparticle production through emulsion processing is therefore interesting to promote these real‐world applications. In this work, it is shown that the slow rate of CNT microparticle formation from water‐in‐oil emulsions is due to spontaneous emulsification. Then methanol‐in‐oil emulsions are tested, which rapidly form fragile CNT capsules. Using mixtures of methanol and water, a faster rate of solvent loss can be balanced alongside nanoparticle assembly; CNT microparticle formation is up to twice as fast using 40% methanol compared to aqueous dispersions. In addition to facilitating faster CNT microparticle production, these findings offer more broadly applicable insights into the mechanisms of solvent transport in emulsions.