Zero-excess lithium batteries (ZELBs), in which the anode is formed in situ during charging, offer a promising route to overcome the safety and cost limitations of conventional lithium metal batteries. However, non-uniform lithium nucleation on copper current collectors often leads to dendrite formation and rapid degradation. Here, we combine fine-tuned machine-learning interatomic potentials with large-scale molecular dynamics simulations to resolve the atomistic pathways of lithium alloying and crystallization on Cu and interlayer metals (Zn, Mg, and Bi). On Cu, lithium nucleates through metastable disordered, HCP, and FCC phases before stabilizing into BCC lithium, whereas Zn and Mg interlayers promote alloy-mediated crystallization, enhancing lithium diffusion and structural uniformity. Distinctly, Bi forms ordered Li3Bi intermetallics with limited interfacial coherence. Experimental validation through scanning electron microscopy, x-ray diffraction, atomic force microscopy, and time-of-flight elastic recoil detection corroborates the predicted alloying and phase evolution. The results reveal that interlayer-dependent alloying dynamics govern lithium crystallization and morphology, establishing a direct link between interfacial chemistry, diffusion behavior, and deposition uniformity. These insights provide a general atomistic framework for rationally designing metal interlayers that regulate lithium nucleation and enable stable and high-efficiency operation of next-generation zero-excess lithium batteries.
- Atomistic Insights Into Lithium Alloying and Crystallization at Metal Interlayers in Zero-Excess Lithium Batteries
- Neubi F. Xavier Jr (Corresponding Author) - Univ Surrey, Fac Engn & Phys Sci, Sch Chem & Chem Engn, Guildford, EnglandNicolas Rospars - Ctr Suisse Elect & Microtech CSEM, Battery Innovat Hub, Neuchatel, SwitzerlandMohammed Srout (Corresponding Author) - Ctr Suisse Elect & Microtech CSEM, Battery Innovat Hub, Neuchatel, SwitzerlandMatthew K. Sharpe (Author) - University of SurreyPablo Hernandez-Martin - Univ Autonoma Madrid, Condensed Matter Phys Ctr IFIMAC, Madrid, SpainCallum D. McAleese - University of SurreySatheesh Krishnamurthy - Univ Surrey, Adv Technol Inst, Ion Beam Ctr, Guildford, EnglandTao Chen - Univ Surrey, Fac Engn & Phys Sci, Sch Chem & Chem Engn, Guildford, EnglandCelia Polop - Univ Autonoma Madrid, Condensed Matter Phys Ctr IFIMAC, Madrid, SpainAndrea Ingenito - Ctr Suisse Elect & Microtech CSEM, Battery Innovat Hub, Neuchatel, SwitzerlandQiong Cai (Corresponding Author) - Univ Surrey, Fac Engn & Phys Sci, Sch Chem & Chem Engn, Guildford, England
- Advanced energy materials, Vol.16(26), e70973
- Wiley
- 14
- 20/04/2026
- 07/2026
- 10/04/2026
- The authors would like to acknowledge financial support by Horizon Europe through the OPERA consortium (Grant Number 101103834) and under the UKRI Horizon Europe Guarantee Extension (Ref Number 10078555), by the Faraday Institution through the LiSTAR program (Grants FIRG014, FIRG058), and by the Royal Society (IEC∖NSFC∖211200). The UK Materials and Molecular Modelling Hub, which is partially funded by EPSRC (EP/T022213 and EP/W032260), is acknowledged for computational resources. The ToF-ERDA measurements were supported through the Surrey Ion Beam Centre, which is funded by UK EPSRC (EP/X015491/1). The authors thank Vlad Palitsin for help in the ion beam analysis laboratory at the Surrey Ion Beam Centre. The authors acknowledge funding received from the Spanish Ministry of Science, Innovation and Universities and Agencia Estatal de Investigación (PCI2022-132998, PID2021–1246670B and CEX2023-001316-M).
- 991121854002346; WOS:001743694500001
- © 2026 The Author(s).
- School of Chemistry & Chemical Engineering; School of Computer Science & Electronic Engineering
- English
- Journal article
- The data and scripts that support the findings of this study are openly available at https://github.com/neubifx/Dataset_fine_tuning_MLIPs_lithium_interface.