DOE OSTI · 2587303
Temperature-dependent solid electrolyte interphase reactions drive performance in lithium-mediated nitrogen reduction to ammonia
Abstract
The solid electrolyte interphase (SEI) is a vital component to control mass transport and selectivity in the lithium-mediated reduction of N 2 to NH 3 (Li-N 2 R). Finding strategies that generate the optimal SEI, a complex network of organic and inorganic species, can potentially improve Li-N 2 R performance. Here, we unravel structure-property relationships of the SEI by correlating its composition with the NH 3 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-N 2 R performance.
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Benedek, Peter [Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis], Cornejo-Carrillo, Yamile E. [Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis], O’Rafferty, Alden H. [Stanford Univ., CA (United States)], Niemann, Valerie A. [Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis], Lee, Sang-Won [Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis], McShane, Eric J. [Stanford Univ., CA (United States)], Cargnello, Matteo [Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis], Nielander, Adam C. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis] (ORCID:0000000236392427), Jaramillo, Thomas F. [Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis] (ORCID:0000000199000622). 2025-01-23. Temperature-dependent solid electrolyte interphase reactions drive performance in lithium-mediated nitrogen reduction to ammonia. https://doi.org/10.1016/j.joule.2024.101810
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