Lithium-mediated ammonia synthesis from water and nitrogen: a membrane-free approach enabled by an immiscible aqueous/organic hybrid electrolyte system

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2019-07-21
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Kim, Kwiyong
Chen, Yifu
Han, Jong-In
Yoon, Hyung Chul
Li, Wenzhen
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Li, Wenzhen
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Ames National Laboratory

Ames National Laboratory is a government-owned, contractor-operated national laboratory of the U.S. Department of Energy (DOE), operated by and located on the campus of Iowa State University in Ames, Iowa.

For more than 70 years, the Ames National Laboratory has successfully partnered with Iowa State University, and is unique among the 17 DOE laboratories in that it is physically located on the campus of a major research university. Many of the scientists and administrators at the Laboratory also hold faculty positions at the University and the Laboratory has access to both undergraduate and graduate student talent.

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Chemical and Biological Engineering

The function of the Department of Chemical and Biological Engineering has been to prepare students for the study and application of chemistry in industry. This focus has included preparation for employment in various industries as well as the development, design, and operation of equipment and processes within industry.Through the CBE Department, Iowa State University is nationally recognized for its initiatives in bioinformatics, biomaterials, bioproducts, metabolic/tissue engineering, multiphase computational fluid dynamics, advanced polymeric materials and nanostructured materials.

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The Department of Chemical Engineering was founded in 1913 under the Department of Physics and Illuminating Engineering. From 1915 to 1931 it was jointly administered by the Divisions of Industrial Science and Engineering, and from 1931 onward it has been under the Division/College of Engineering. In 1928 it merged with Mining Engineering, and from 1973–1979 it merged with Nuclear Engineering. It became Chemical and Biological Engineering in 2005.

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1913 - present

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  • Department of Chemical Engineering (1913–1928)
  • Department of Chemical and Mining Engineering (1928–1957)
  • Department of Chemical Engineering (1957–1973, 1979–2005)
    • Department of Chemical and Biological Engineering (2005–present)

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Abstract

The lithium-mediated pathway provides a promising way for facile and selective dissociation of nitrogen for ammonia synthesis. However, the prevailing electro-deposition of lithium, especially when coupled to the anodic oxygen evolution from water or hydroxide, presents disadvantages including the use of expensive Li-ion conducting ceramics (LISICON) or high temperature operation of molten salts. In this study, a membrane-free approach based on the immiscibility of aqueous/organic electrolytes was adopted for lithium electro-deposition, which could be utilized for subsequent nitridation and ammonia synthesis. We found that a biphasic system of aqueous 1 M LiClO4 and 1 M LiClO4/propylene carbonate reinforced with PMMA (poly(methyl methacrylate)) acts the same as a LISICON-based aqueous/organic hybrid electrolyte system, but without any physical membrane. With a fairly high faradaic efficiency (FE) of 57.2% and a production rate of 1.21 × 10−9 mol cm−2 s−1 for ammonia synthesis, this membrane-free approach and its application to ammonia synthesis provide an innovative way to the advancements in next-generation energy storage technologies.

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This is a manuscript of an article published as Kim, Kwiyong, Yifu Chen, Jong-In Han, Hyung Chul Yoon, and Wenzhen Li. "Lithium-mediated ammonia synthesis from water and nitrogen: a membrane-free approach enabled by an immiscible aqueous/organic hybrid electrolyte system." Green Chemistry 21, no. 14 (2019): 3839-3845. DOI: 10.1039/C9GC01338E. Posted with permission.

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Tue Jan 01 00:00:00 UTC 2019
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