Unveiling and regulating heterogeneous Li+ transport in 3D scaffolds: a gradient electrodeposition strategy toward ultralight and stable Li metal anodes
Abstract
Three-dimensional (3D) current collectors are widely explored to suppress lithium dendrite growth in Li metal anodes, particularly under high-current-density operation. Nevertheless, a fundamental mechanistic understanding of Li electrodeposition within such complex 3D architectures remains markedly incomplete. Herein, using a 3D Cu mesh as a model system, we demonstrate that intrinsic heterogeneity in Li+ transport within 3D architectures promotes localized ion-flux amplification, triggering preferential deposition and dendritic nucleation. Guided by this insight, a gradient-descending electrodeposition is proposed to regulate ion flux distribution, enabling dense, uniform, and strongly adherent bulk-like Li deposition. To mitigate the gravimetric penalty associated with conventional metallic scaffolds, an ultralight PET@Cu 3D current collector is further engineered via polymer metallization, achieving an areal mass reduction of 59.2% relative to the Cu mesh while retaining sufficient electrical conductivity and mechanical robustness. When integrated with the gradient deposition strategy, the resulting PET@Cu@G-Li anodes paired with NMC811 cathodes exhibit high-rate capability and exceptional cycling stability, retaining 90.82% of their initial capacity after 600 cycles at 3C. This work elucidates the critical role of mass-transport heterogeneity in Li electrodeposition within 3D frameworks and offers a practical anode design paradigm that reconciles high power density with…
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