Authors
Lei Zhang, Yu Han, Huiling Peng, Yaheng Geng, Xiangxiang Pang, Zichao Yan, Jian Zhu, Zhiqiang Zhu
Published in
Angewandte Chemie (International ed. in English). Pages e6078477. Sep 09, 2026. Epub Sep 09, 2026.
Abstract
Anode-free zinc batteries offer a promising route to maximize energy density, yet their viability is compromised by uncontrolled Zn nucleation and severe parasitic reactions at the anode side. Herein, we address this issue by designing a dual-functional fluorinated interphase on a Cu current collector, which couples high zincophilicity with robust hydrophobicity. This design leverages the electronegative fluorine atoms to enhance the zincophility of the sulfonyl tail group and guide uniform nucleation, while the fluorinated chains establish a compact hydrophobic barrier thermodynamically suppressing water-induced side reactions. As a proof-of-concept, we employ molecularly tunable self-assembled monolayers (SAMs) of benzene-based thiols on Cu. By designing a series of ligands with stepwise increased fluorination (non-fluorinated CPM → mono-fluorosulfonyl MPM → di-fluorosulfonyl DMPM), we demonstrate that higher fluorine content progressively enhances zincophilic site density and hydrophobic shielding. Consequently, the DMPM-modified Cu electrode achieves highly reversible dendrite-free Zn plating/stripping with an average Coulombic efficiency of 99.56% over 1000 cycles. This fluorinated interface exhibits universal robustness across capacitive (graphite), intercalation (ZnxV2O5), and conversion (ZnI2) cathodes, with practical viability demonstrated in a 0.2 Ah pouch cell. This work establishes a molecular-level design paradigm for constructing robust interfaces for high-energy, long-life anode-free batteries.
PMID:
42713814
Bibliographic data and abstract were imported from PubMed on 09 Sep 2026.
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