Temperature-dependent solid electrolyte interphase reactions drive performance in lithium-mediated nitrogen reduction to ammonia

Benedek, Peter; Cornejo-Carrillo, Yamile E.; O’Rafferty, Alden H.; Niemann, Valerie A.; Lee, Sang-Won; McShane, Eric J.; Cargnello, Matteo; Nielander, Adam C.; Jaramillo, Thomas F.

doi:10.1016/j.joule.2024.101810

Title: Temperature-dependent solid electrolyte interphase reactions drive performance in lithium-mediated nitrogen reduction to ammonia

Journal Article · Thu Jan 23 00:00:00 UTC 2025 · Joule

DOI: https://doi.org/10.1016/j.joule.2024.101810 · OSTI ID:2587303

Benedek, Peter ^[1]; Cornejo-Carrillo, Yamile E. ^[1]; O’Rafferty, Alden H. ^[2]; Niemann, Valerie A. ^[1]; Lee, Sang-Won ^[1]; McShane, Eric J. ^[2]; Cargnello, Matteo ^[1];

^[3];

^[1]

Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis
Stanford Univ., CA (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis

The solid electrolyte interphase (SEI) is a vital component to control mass transport and selectivity in the lithium-mediated reduction of N₂ to NH₃ (Li-N₂R). Finding strategies that generate the optimal SEI, a complex network of organic and inorganic species, can potentially improve Li-N₂R performance. Here, we unravel structure-property relationships of the SEI by correlating its composition with the NH₃ faradaic efficiency (FENH3). By modifying the reaction temperature, we alter electrolyte decomposition reactions and observe changes in the SEI that explain FE_NH3 trends between electrolyte solvents. We quantify a complex reaction environment at elevated temperatures where SEI formation is counteracted by etching reactions. This tradeoff leads to temporal fluctuations of FE_NH3, but the maximal FE_NH3 can reach up to 40%, the highest value reported for batch cells at ambient pressure, thus far. In conclusion, our work underscores the potential of novel electrolytes that steer SEI selectivity and, ultimately, improve Li-N₂R performance.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 2587303

Journal Information:: Joule, Journal Name: Joule Journal Issue: 3 Vol. 9; ISSN 2542-4351

Publisher:: Elsevier BVCopyright Statement

Country of Publication:: United States

Language:: English

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