Ammonia Synthesis From N2 And H2O Using A Lithium Cycling ...

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Energy & Environmental Science

Ammonia synthesis from N2 and H2O using a lithium cycling electrification strategy at atmospheric pressure†

Joshua M. McEnaney, a Aayush R. Singh,a Jay A. Schwalbe,a Jakob Kibsgaard,c John C. Lin,a Matteo Cargnello, ab Thomas F. Jaramillo *ab and Jens K. Nørskov*ab Author affiliations

* Corresponding authors

a SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering Stanford University, Shriram Center, 443 Via Ortega, Stanford, CA 94305, USA E-mail: [email protected], [email protected]

b SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA

c Department of Physics, Technical University of Denmark, DK-2800 Kongens Lyngby, Denmark

Abstract

Ammonia production is imperative to providing food for a growing world population. However, the primary method of synthetic ammonia production, the Haber Bosch process, is resource demanding and unsustainable. Here we report a novel ammonia production strategy, exemplified in an electrochemical lithium cycling process, which provides a pathway to sustainable ammonia synthesis via the ability to directly couple to renewable sources of electricity and can facilitate localized production. Whereas traditional aqueous electrochemical approaches are typically dominated by the hydrogen evolution reaction (HER), we are able to circumvent the HER by using a stepwise approach which separates the reduction of N2 from subsequent protonation to NH3, thus our synthesis method is predominantly selective for ammonia production. Density functional theory calculations for thermodynamic and diffusion energy barrier insights suggest that Li-based materials are well suited to carry out this process, though other materials may also be useful. The three steps of the demonstrated process are LiOH electrolysis, direct nitridation of Li, and the exothermic release of ammonia from Li3N, which reproduces the LiOH, completing the cycle. The process uses N2 and H2O at atmospheric pressure and reasonable temperatures, and, while approaching industrial level electrolytic current densities, we report an initial current efficiency of 88.5% toward ammonia production.

• This article is part of the themed collection: 2017 Energy and Environmental Science HOT articles

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Article information

DOI https://doi.org/10.1039/C7EE01126A Article type Paper Submitted 26 Apr 2017 Accepted 27 Jun 2017 First published 27 Jun 2017

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Energy Environ. Sci., 2017,10, 1621-1630 BibTex EndNote MEDLINE ProCite ReferenceManager RefWorks RIS

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Ammonia synthesis from N2 and H2O using a lithium cycling electrification strategy at atmospheric pressure

J. M. McEnaney, A. R. Singh, J. A. Schwalbe, J. Kibsgaard, J. C. Lin, M. Cargnello, T. F. Jaramillo and J. K. Nørskov, Energy Environ. Sci., 2017, 10, 1621 DOI: 10.1039/C7EE01126A

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Joshua M. McEnaney Aayush R. Singh Jay A. Schwalbe Jakob Kibsgaard John C. Lin Matteo Cargnello Thomas F. Jaramillo Jens K. Nørskov

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