journal article·2026-01Open access

Electron-funnel mediated anion confinement enables ultra-reversible interphases in solid-state batteries

Yi Chen, Ji Qian, Ke Wang, Tianyang Xue, Zhengqiang Hu, Fengling Zhang, Tong Lian, Xinhui Pan, Teng Zhao, Li Li, Feng Wu, Renjie Chen

eScience· Volume 6· Issue 1

Abstract

Solid-state lithium metal batteries face challenges from irreversible interfacial degradation and sluggish ion transport. We propose an electron-funnel-mediated anion confinement strategy via atomic-level electronic field engineering. Incorporating electron-withdrawing –NO 2 groups into Zr-based frameworks induces a 0.38 eV upward d-band center shift, generating a quantum-confined electrostatic gradient that polarizes TFSI - anions. This reduces TFSI - decomposition energy barrier (ΔG: −0.35 → −1.22 eV), selectively promoting LiF nucleation while suppressing side reactions. Concurrently, Zr 4+ -PEO Lewis interactions disrupt polymer crystallinity, enhancing ionic conductivity and Li + transference number. Cryo-TEM tomography and TOF-SIMS mapping reveal a fractal LiF-rich interphase enabling dendrite-free lithium plating for >11,000 h with polarization <40 mV. LiFePO 4 full cells achieve 86.3% capacity retention after 400 cycles at 1C (1.3 mAh cm −2 ). This work establishes anion confinement as a universal framework synchronizing ion transport and interfacial durability, advancing practical solid-state batteries with exceptional longevity.
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Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Advancements in Battery Materials · Advanced Battery Technologies Research

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