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Title: Electride support boosts nitrogen dissociation over ruthenium catalyst and shifts the bottleneck in ammonia synthesis

Journal Article · · Nature Communications
DOI:https://doi.org/10.1038/ncomms7731· OSTI ID:1260712
 [1];  [2];  [3];  [4];  [5];  [6];  [7];  [8]
  1. Tokyo Inst. of Technology (Japan). Materials Research Center for Element Strategy
  2. Tokyo Inst. of Technology (Japan). Materials and Structures Lab.
  3. Tokyo Inst. of Technology (Japan). Materials and Structures Lab.
  4. Univ. College London (UCL), London (United Kingdom). Dept. of Physics and Astronomy
  5. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); ACCEL, Japan Science and Technology Agency, Kawaguchi (Japan)
  6. Tokyo Inst. of Technology (Japan). Materials Research Center for Element Strategy; ACCEL, Japan Science and Technology Agency, Kawaguchi (Japan)
  7. Tokyo Inst. of Technology (Japan). Materials and Structures Lab.; ACCEL, Japan Science and Technology Agency, Kawaguchi (Japan); Tokyo Inst. of Technology (Japan). Frontier Research Center
  8. Tokyo Inst. of Technology (Japan). Materials Research Center for Element Strategy; Tokyo Inst. of Technology (Japan). Materials and Structures Lab.; ACCEL, Japan Science and Technology Agency, Kawaguchi (Japan); Tokyo Inst. of Technology (Japan). Frontier Research Center

Novel approaches to efficient ammonia synthesis at an ambient pressure are actively sought out so as to reduce the cost of ammonia production and to allow for compact production facilities. It is accepted that the key is the development of a high-performance catalyst that significantly enhances dissociation of the nitrogen–nitrogen triple bond, which is generally considered a rate-determining step. Here we examine kinetics of nitrogen and hydrogen isotope exchange and hydrogen adsorption/desorption reactions for a recently discovered efficient catalyst for ammonia synthesis—ruthenium-loaded 12CaO _ 7Al2O3 electride (Ru/C12A7:e_)—and find that the rate controlling step of ammonia synthesis over Ru/C12A7:e_ is not dissociation of the nitrogen–nitrogen triple bond but the subsequent formation of N–Hn species. A mechanism of ammonia synthesis involving reversible storage and release of hydrogen atoms on the Ru/C12A7:e_ surface is proposed on the basis of observed hydrogen absorption/desorption kinetics.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
EP/ L000202; AC05-76RL01830
OSTI ID:
1260712
Alternate ID(s):
OSTI ID: 1347879
Report Number(s):
PNNL-SA-124228; ncomms7731
Journal Information:
Nature Communications, Vol. 6; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 455 works
Citation information provided by
Web of Science

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