Breaking scaling relations to achieve low-temperature ammonia synthesis through LiH-mediated nitrogen transfer and hydrogenation
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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Interfacial spillover offers a promising route to circumvent scaling-relation constraints by spatially separating elementary reaction steps across kinetically optimized components.
“such interfacial spillover offers a promising route to circumvent these constraints by spatially separating elementary reaction steps across kinetically optimized components, thereby enabling each step to proceed under favorable conditions and overcoming activity limitations imposed by scaling relations.21−23”
From High-Entropy Alloy Aerogels with High-Density Solid–Solid Heterointerfaces for Alkaline Hydrogen Evolution (2026) · cites this paper as [23]
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- 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
- Venue
- Nature Chemistry
- Published
- 2016-08-22
- Volume
- 9
- Issue
- 1
- Pages
- 64-70
- ISSN
- 1755-4330 (ISSN-L)
- 1755-4349
- 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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