Spatially Distributed Lithiophilic Gradient in Low‐Tortuosity 3D Hosts via Capillary Action for High‐Performance Li Metal Anodes

Abstract Regulating lithium deposition/stripping behavior in 3D hosts is critical for the development of stable lithium metal batteries. Herein, a low‐tortuosity wood derived carbon (WDC) with gradient‐distributed lithiophilic sites is rationally constructed via biomimetic capillary action, as an efficient scaffold for lithium deposition/stripping. Due to the merits of excellent spatial controllability, the gradient Ag particles modified WDC (WDC‐GDAg) displays favorable bottom‐up Li plating behavior with high columbic efficiency and long cycling stability. Finite element simulation reveals that gradient‐distributed Ag sites enable high lithium flux distribution at the bottom and homogeneous electric field distribution on the top of the WDC electrode. Moreover, the full cells with a WDC‐GDAg anode and a LiFePO₄ cathode demonstrate high capacity retention of ≈78.9% after 2000 cycles at 10 C and remarkable rate performance even at 40 C, presenting great potential for practical applications.