A Caltech Library Service

Closed-Loop Electrolyte Design for Lithium-Mediated Ammonia Synthesis

Krishnamurthy, Dilip and Lazouski, Nikifar and Gala, Michal L. and Manthiram, Karthish and Viswanathan, Venkatasubramanian (2021) Closed-Loop Electrolyte Design for Lithium-Mediated Ammonia Synthesis. ACS Central Science, 7 (12). pp. 2073-2082. ISSN 2374-7943. PMCID PMC8704027. doi:10.1021/acscentsci.1c01151.

[img] PDF - Published Version
Creative Commons Attribution Non-commercial No Derivatives.

[img] PDF (Materials, electrolyte preparation, nitrogen reduction experiments, choosing proton carrier concentrations, ammonia qualification, analysis of water content, modeling approach, classification model, deep learning model, sources of uncertainty, Figures ...) - Supplemental Material
Creative Commons Attribution Non-commercial No Derivatives.


Use this Persistent URL to link to this item:


Novel methods for producing ammonia, a large-scale industrial chemical, are necessary for reducing the environmental impact of its production. Lithium-mediated electrochemical nitrogen reduction is one attractive alternative method for producing ammonia. In this work, we experimentally tested several classes of proton donors for activity in the lithium-mediated approach. From these data, an interpretable data-driven classification model is constructed to distinguish between active and inactive proton donors; solvatochromic Kamlet–Taft parameters emerged to be the key descriptors for predicting nitrogen reduction activity. A deep learning model is trained to predict these parameters using experimental data from the literature. The combination of the classification and deep learning models provides a predictive mapping from proton donor structure to activity for nitrogen reduction. We demonstrate that the two-model approach is superior to a purely mechanistic or a data-driven approach in accuracy and experimental data efficiency.

Item Type:Article
Related URLs:
URLURL TypeDescription CentralArticle
Krishnamurthy, Dilip0000-0001-8231-5492
Lazouski, Nikifar0000-0002-4655-2041
Gala, Michal L.0000-0003-0676-5146
Manthiram, Karthish0000-0001-9260-3391
Viswanathan, Venkatasubramanian0000-0003-1060-5495
Additional Information:© 2021 The Authors. Published by American Chemical Society. Attribution-NonCommercial-NoDerivatives 4.0 International (CC BY-NC-ND 4.0). Received 20 September 2021. Published online 2 December 2021. Published in issue 22 December 2021. We thank Matt Wolski of Daramic for providing us with polyporous separator samples. This material is based upon work supported by the National Science Foundation under Grant No. 1944007. Funding for this research was provided by the Abdul Latif Jameel World Water and Food Systems Lab (J-WAFS) at MIT. N.L. acknowledges support by the National Science Foundation Graduate Research Fellowship under Grant No. 1122374. D.K. and V.V. gratefully acknowledge funding support from the National Science Foundation under Award CBET-1554273. D.K. and V.V. thank Dr. Bharath Ramsundar for useful discussions and feedback about the computational models and the deep-learning methodology. V.V. acknowledges support from the Scott Institute for Energy Innovation at Carnegie Mellon University. D.K. acknowledges discussions with Victor Venturi regarding the deep-learning model implementation. Author Contributions. D.K. and N.L. contributed equally. Conceptualization: N.L. and K.M. Methodology - Experimental: N.L. Methodology - Modeling: D.K. and V.V. Investigation: N.L. and M.L.G. Formal analysis: D.K. and V.V. Data curation: D.K. Writing - Original Draft: N.L. and D.K. Writing - Review and Editing: N.L., D.K., K.M., and V.V. Supervision: K.M. and V.V. The authors declare the following competing financial interest(s): D.K., V.V., N.L., and K.M. are inventors on a provisional patent application, 63/066841, related to hydrogen donors for lithium-mediated ammonia synthesis.
Funding AgencyGrant Number
Massachusetts Institute of Technology (MIT)UNSPECIFIED
NSF Graduate Research FellowshipDGE-1122374
Carnegie Mellon UniversityUNSPECIFIED
Subject Keywords:Nitrogen, Molecular modeling, Ammonia, Computational modeling, Lithium
Issue or Number:12
PubMed Central ID:PMC8704027
Record Number:CaltechAUTHORS:20220505-565053000
Persistent URL:
Official Citation:Closed-Loop Electrolyte Design for Lithium-Mediated Ammonia Synthesis Dilip Krishnamurthy, Nikifar Lazouski, Michal L. Gala, Karthish Manthiram, and Venkatasubramanian Viswanathan ACS Central Science 2021 7 (12), 2073-2082 DOI: 10.1021/acscentsci.1c01151
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:114606
Deposited By: George Porter
Deposited On:06 May 2022 16:13
Last Modified:06 May 2022 16:13

Repository Staff Only: item control page