Robust Siloxane Network‐Driven Electrostatically Heterogeneous 3D Nano‐Assembled Hard Carbon Host toward High Utilization Lithium Metal Anodes
Year: 2025
Type: article
Abstract: Achieving high lithium utilization and long‐term stability in lithium metal batteries (LMB) with 3D host remains a significant challenge. Herein, a robust siloxane network‐driven electrostatically heterogeneous 3D nano‐assembled hard carbon (EH‐NHC) host is introduced. The 3D EH‐NHC host is integrated with a strongly chemical‐bonded siloxane coating layer, imparting a negative surface charge originating from the lithiophilic hydroxyl groups (Si─OH). This host retains its thickness of coating layer, surface charge, and structural integrity even after repeated cycling. The lithiophilic sites promote uniform, bottom‐up lithium deposition within the porous EH‐NHC framework, which accommodates volume changes and enables uniform plating under high areal capacity (5 mAh cm −2 ). The EH‐NHC host exhibits outstanding stability in symmetric cells, maintaining consistent operation for 4000 h at a current density of 6 mA cm −2 and 65% Li utilization. Furthermore, LiFePO₄/EH‐NHC host full cell demonstrates remarkable cycle stability, achieving capacity retention of 81.5% after 500 cycles, even with a high lithium utilization of 50%. In this study, we demonstrate that EH‐NHC is a promising candidate as a practically operable 3D host for next‐generation LMBs, preventing degradation of the lithiophilic sites, thus preserving the functionality of the initially designed hierarchical structure and maximizing the reversible efficiency of active lithium.
Source: Small Methods
Authors: Sumin Ko, Kyungjun Kim, Sang‐Min Lee
Institution: Pohang University of Science and Technology
Language: English
Subfield: Electrical and Electronic Engineering
Field: Engineering
Domain: Physical Sciences
Open Access status: bronze
Awards: G5094049988, G5353228825, G7620315661
OpenAlex ID: W4409622781