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PreprintCC BYChemRxiv

Selective Operando Visualization of Ultrathin Lithium in Li-Metal Batteries by Neutron Capture Imaging

  • Xiaolong Zhang1
  • Leon Skarjan2
  • Ricardo Carreon1
  • Jongmin Lee1
  • Andreas Borgschulte3,4
  • Thomas J. Schmidt2,5,6
  • Markus Strobl1,7,8
  • Sigita Trabesinger2
  • Pierre Boillat1,2
8 affiliations
  1. 1PSI Center for Neutron and Muon Sciences
  2. 2PSI Center for Energy and Environmental Sciences
  3. 3Empa Swiss Federal Laboratories for Materials Science and Technology
  4. 4Chemical Energy Carriers and Vehicle Systems Laboratory
  5. 5Institute for Molecular Physical Sciences
  6. 6ETH Zurich
  7. 7Niels Bohr Institute
  8. 8University of Copenhagen
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Abstract

Operando visualization of ultrathin lithium is essential for understanding plating and stripping in lithium-metal batteries, but existing neutron imaging techniques lack sufficient sensitivity for ultra-thin lithium layers formed at crucial early stages. Here we introduce neutron capture imaging (NCI), which selectively detects tritons generated by neutron capture in 6 Li. Ex situ measurements of electrochemically plated and thermally evaporated 6 Li demonstrate sensitivity around 10 nm for a 1.5 h acquisition and two-dimensional imaging with around 100 μm lateral resolution. Simulations indicate that the resolution could approach 25 μm through optical optimization. Operando measurements in an asymmetric Cu|| 6 Li cell reveal spatially heterogeneous lithium plating and stripping in agreement with electrochemical data. Our results establish NCI as a high-sensitivity, near-zero-background tool for operando studies of lithium metal batteries, opening new possibilities for resolving early-stage deposition, dead lithium formation, and interfacial dynamics with broad applicability to ultrathin reactive lithium layers in electrochemical systems.

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Cite

BibTeXRIS
BibTeX
@misc{zhang2026selective,
  title = {{Selective Operando Visualization of Ultrathin Lithium in Li-Metal Batteries by Neutron Capture Imaging}},
  author = {Xiaolong Zhang and Leon Skarjan and Ricardo Carreon and Jongmin Lee and Andreas Borgschulte and Thomas J. Schmidt and Markus Strobl and Sigita Trabesinger and Pierre Boillat},
  howpublished = {ChemRxiv},
  year = {2026},
  month = oct,
  doi = {10.26434/chemrxiv.15009867/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009867/v1},
  note = {CC BY},
}
RIS
TY  - UNPB
TI  - Selective Operando Visualization of Ultrathin Lithium in Li-Metal Batteries by Neutron Capture Imaging
AU  - Xiaolong Zhang
AU  - Leon Skarjan
AU  - Ricardo Carreon
AU  - Jongmin Lee
AU  - Andreas Borgschulte
AU  - Thomas J. Schmidt
AU  - Markus Strobl
AU  - Sigita Trabesinger
AU  - Pierre Boillat
PY  - 2026
DA  - 2026/10/05
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15009867/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009867/v1
AB  - Operando visualization of ultrathin lithium is essential for understanding plating and stripping in lithium-metal batteries, but existing neutron imaging techniques lack sufficient sensitivity for ultra-thin lithium layers formed at crucial early stages. Here we introduce neutron capture imaging (NCI), which selectively detects tritons generated by neutron capture in 6 Li. Ex situ measurements of electrochemically plated and thermally evaporated 6 Li demonstrate sensitivity around 10 nm for a 1.5 h acquisition and two-dimensional imaging with around 100 μm lateral resolution. Simulations indicate that the resolution could approach 25 μm through optical optimization. Operando measurements in an asymmetric Cu|| 6 Li cell reveal spatially heterogeneous lithium plating and stripping in agreement with electrochemical data. Our results establish NCI as a high-sensitivity, near-zero-background tool for operando studies of lithium metal batteries, opening new possibilities for resolving early-stage deposition, dead lithium formation, and interfacial dynamics with broad applicability to ultrathin reactive lithium layers in electrochemical systems.
ER  -