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Cited by 711Ammonia Synthesis and Nitrogen ReductionCatalytic Processes in Materials ScienceHydrogen Storage and Materials

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Breaking scaling relations to achieve low-temperature ammonia synthesis through LiH-mediated nitrogen transfer and hydrogenation

Wang, Peikun, Chang, Fei, Gao, Wenbo, Guo, Jianping, Wu, Guotao, He, Teng, Chen, Ping·2017·Nature Chemistry
DOI 10.1038/nchem.2595
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Abstract

Ammonia synthesis under mild conditions is a goal that has been long sought after. Previous investigations have shown that adsorption and transition-state energies of intermediates in this process on transition metals (TMs) scale with each other. This prevents the independent optimization of these energies that would result in the ideal catalyst: one that activates reactants well, but binds intermediates relatively weakly. Here we demonstrate that these scaling relations can be broken by intervening in the TM-mediated catalysis with a second catalytic site, LiH. The negatively charged hydrogen atoms of LiH act as strong reducing agents, which remove activated nitrogen atoms from the TM or its nitride (TMN), and as an immediate source of hydrogen, which binds nitrogen atoms to form LiNH 2 . LiNH 2 further splits H 2 heterolytically to give off NH 3 and regenerate LiH. This synergy between TM (or TMN) and LiH creates a favourable pathway that allows both early and late 3d TM-LiH composites to exhibit unprecedented lower-temperature catalytic activities.

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Metadata

Authors
Wang, P., Chang, F., Gao, W., Guo, J., Wu, G., He, T., & Chen, P.
Affiliations
Dalian Institute of Chemical Physics (CN)
Corresponding author
  • Guo, Jianping
  • Chen, Ping
ORCID
Venue
Nature Chemistry
Publisher
Springer Science and Business Media LLC
Published
2016-08-22
Volume
9
Issue
1
Pages
64-70
ISSN
  • 1755-4330 (ISSN-L)
  • 1755-4349
DOI
10.1038/nchem.2595
OpenAlex
W2510877666
Cited by
711
References
53
Citations by year
2026: 68 · 2025: 102 · 2024: 100 · 2023: 70 · 2022: 99 · 2021: 84 · 2020: 68 · 2019: 58 · 2018: 44 · 2017: 17
FWCI
13.20
Type
journal article
Language
en
Open access
closed
Licence
www.springer.com/tdm (tdm)
Locations
  • Nature Chemistry (publishedVersion)
  • PubMed (publishedVersion)
  • Dalian Institute of Chemical Physics, CAS Institutional Repository (submittedVersion)
Funders
Collaborative Innovation Center of Chemistry for Energy Materials
Topics
  • Physical Sciences › Chemical Engineering › Catalysis › Ammonia Synthesis and Nitrogen Reduction
  • Physical Sciences › Materials Science › Materials Chemistry › Catalytic Processes in Materials Science
  • Physical Sciences › Materials Science › Materials Chemistry › Hydrogen Storage and Materials
Keywords
ammonia synthesis, low-temperature catalysis, lithium hydride, hydrogenation, nitrogen transfer, transition metal catalysts, scaling laws, adsorption energy, transition metal nitrides, lithium amide, 3d transition metals, bimetallic catalysts

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