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DOI | 10.1039/c7ee01126a |
Ammonia synthesis from N2 and H2O using a lithium cycling electrification strategy at atmospheric pressure | |
McEnaney J.M.; Singh A.R.; Schwalbe J.A.; Kibsgaard J.; Lin J.C.; Cargnello M.; Jaramillo T.F.; Nørskov J.K. | |
发表日期 | 2017 |
ISSN | 17545692 |
起始页码 | 1621 |
结束页码 | 1630 |
卷号 | 10期号:7 |
英文摘要 | 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. © The Royal Society of Chemistry 2017. |
英文关键词 | Atmospheric pressure; Density functional theory; Kinetic theory; Lithium; Ammonia production; Current efficiency; Diffusion energy barriers; Direct nitridation; Electrolytic current densities; Haber-Bosch process; Hydrogen evolution reactions; Stepwise approach; Ammonia; ammonia; atmospheric pressure; electrification; electrochemical method; energy resource; lithium; nitrogen; reduction; temperature; thermodynamics; water |
语种 | 英语 |
来源期刊 | Energy & Environmental Science
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文献类型 | 期刊论文 |
条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/190454 |
作者单位 | SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering Stanford University, Shriram Center, 443 Via Ortega, Stanford, CA 94305, United States; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, United States; Department of Physics, Technical University of Denmark, Kongens Lyngby, DK-2800, Denmark |
推荐引用方式 GB/T 7714 | McEnaney J.M.,Singh A.R.,Schwalbe J.A.,et al. Ammonia synthesis from N2 and H2O using a lithium cycling electrification strategy at atmospheric pressure[J],2017,10(7). |
APA | McEnaney J.M..,Singh A.R..,Schwalbe J.A..,Kibsgaard J..,Lin J.C..,...&Nørskov J.K..(2017).Ammonia synthesis from N2 and H2O using a lithium cycling electrification strategy at atmospheric pressure.Energy & Environmental Science,10(7). |
MLA | McEnaney J.M.,et al."Ammonia synthesis from N2 and H2O using a lithium cycling electrification strategy at atmospheric pressure".Energy & Environmental Science 10.7(2017). |
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