Imaging of nitrogen fixation at lithium solid electrolyte interphases via cryo-electron microscopy

Katherine Steinberg, Xintong Yuan, Channing K. Klein, Nikifar Lazouski, Matthew Mecklenburg, Karthish Manthiram () and Yuzhang Li ()
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Katherine Steinberg: Massachusetts Institute of Technology
Xintong Yuan: University of California, Los Angeles
Channing K. Klein: California Institute of Technology
Nikifar Lazouski: Massachusetts Institute of Technology
Matthew Mecklenburg: University of California, Los Angeles
Karthish Manthiram: California Institute of Technology
Yuzhang Li: University of California, Los Angeles

Nature Energy, 2023, vol. 8, issue 2, 138-148

Abstract: Abstract Ammonia is an important industrial chemical and is also being discussed as a potential energy carrier. Electrifying ammonia synthesis could help to decarbonize the chemical industry, as the Haber–Bosch process contributes markedly to global carbon emissions. A lithium-mediated pathway is among the most promising ambient-condition electrochemical ammonia synthesis methods. However, the role of metallic lithium and its passivation layer, the solid electrolyte interphase (SEI), remains unresolved. Here we use cryogenic transmission electron microscopy as part of a multiscale approach to explore lithium reactivity and the SEI, discovering that the proton donor (for example, ethanol) governs lithium reactivity towards nitrogen fixation. Without ethanol, the SEI passivates lithium metal, rendering it inactive for nitrogen reduction. Ethanol disrupts this passivation layer, enabling continuous reactivity at the lithium surface. As a result, metallic lithium is consumed via reactions with nitrogen, proton donor and other electrolyte components. This reactivity across the SEI is vital to device-level performance of lithium-mediated ammonia synthesis.

Date: 2023
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DOI: 10.1038/s41560-022-01177-5

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