Synergizing Conformal Lithiophilic Granule and Dealloyed Porous Skeleton toward Pragmatic Li Metal Anodes

Abstract

Li metal is regarded as one of the most promising anodes for next‐generation rechargeable batteries. Nonetheless, infinite volume change and severe dendrite growth impede its practicability. To date, unremitting efforts have been devoted to stabilizing Li metal anode via the rational design of 3D current collectors. In this sense, optimizing Li nucleation behavior plays a pivotal role in alleviating the dendrite formation. Herein, a practically viable route is devised by in situ crafting lithiophilic CuSe granules on the dealloyed Cu skeleton (D‐Cu@CuSe). Persuasive electrochemical analysis and systematic theoretical calculation disclose the underlying Li nucleation mechanism on the CuSe overlayer. Impressively, the D‐Cu@CuSe‐Li symmetric cell can sustain a stable plating/stripping operation over 1000 h at a high depth of discharge at 62.5%. More crucially, when paired with high‐loading sulfur cathodes, D‐Cu@CuSe‐Li||S batteries harvest advanced areal capacity and stable cycling performance even under stringent working conditions of low negative‐to‐positive (N/P) (≈2) and electrolyte‐to‐sulfur (8 μL mgs−1) ratios. Overall, a fresh perspective into rationalizing current collector design is afforded, which extends Li utilization and cycling durability in the pursuit of pragmatic Li metal anodes.

Efficient Charge Transfers in Highly Conductive Copper Selenide Quantum Dot-Confined Catalysts for Robust Oxygen Evolution Reaction

“…The high-resolution TEM (HRTEM) image (Figure c) of a representative single-QD demonstrated the high crystallinity of CuSe QDs. The interplanar spacing extracted from Figure c is 0.32 nm, which perfectly matches the crystallographic (102) plane of CuSe . By matching the simulated diffraction pattern produced by JEMS software with the selected area electron diffraction (SAED) pattern (Figure d) of CuSe QD-confined catalysts, it can be deduced that the crystal structure of the CuSe QDs is a hexagonal structure with a space group of P 63/ mmc .…”

Direct-Chemical Vapor Deposition-Enabled Graphene for Emerging Energy Storage: Versatility, Essentiality, and Possibility

“…As for the prevailing metal anodes, pristine current collectors (e.g., Cu, Ni, Al) are prone to exhibit weak interaction with deposited metal. − Even worse, they can barely afford sufficient nucleation sites and homogenize electric field distributions, thereby inducing random metal deposition and severe dendritic growth. In this sense, the surface modification of current collectors is recognized as a promising way to ameliorate the electrochemical behavior of metal nucleation .…”

Revisiting the Role of Physical Confinement and Chemical Regulation of 3D Hosts for Dendrite-Free Li Metal Anode

“…Although these strategies can prevent the Li dendrite growth to some degree, the dramatical electrode volume change generated by "hostless" Li plating/stripping still prevails and will destroy the solid electrolyte interface (SEI), which ineluctably facilitates dendrite growth and exacerbates the depletion of Li metal, especially at high current densities and cycling capacities [25][26][27]. The three-dimensional (3D) framework can reform the traditional nucleation and growth mode at the source, which not only can accommodate the large volume change but also can control the nucleation of Li + to obtain stable Li deposition and growth [28][29][30][31]. The 3D carbon frameworks with lightweight, flexibility, and abundant voids are the better option compared with widely investigated 3D metal foams.…”