Hydrogen Spillover to Oxygen Vacancy of TiO2–xHy/Fe: Breaking the Scaling Relationship of Ammonia Synthesis
- 18 September 2020
- journal article
- research article
- Published by American Chemical Society (ACS) in Journal of the American Chemical Society
- Vol. 142 (41), 17403-17412
- https://doi.org/10.1021/jacs.0c06118
Abstract
Optimizing kinetic barriers of ammonia synthesis to reduce the energy intensity has recently attracted significant research interest. The motivation for the research is to discover means by which activation barriers of N2 dissociation and NHz (z = 1-2, surface intermediates) destabilization can be reduced simultaneously, i.e., breaking the “scaling relationship”. However, by far only a single success has been reported in 2016 based on the discovery of a strong-weak N-bonding pair—transition metals (nitrides)-LiH. Described herein is a second example which is counter-intuitively founded upon a strong-strong N-bonding pair unveiled in a bifunctional nanoscale catalyst TiO2-xHy/Fe (where 0.02 ≤ x ≤ 0.03 and 0 < y < 0.03), in which hydrogen spillover (H) from Fe to cascade oxygen vacancies (OV-OV) results in the trapped form of OV-H on the TiO2-xHy component. The Fe component thus enables facile activation of N2 and H2, while the OV-H in TiO2-xHy hydrogenates the NHz to NH3 easily.Keywords
Funding Information
- Ministry of Science and Technology of the People's Republic of China (2016YFA0203002)
- Central China Normal University (2019YBZZ026)
- China Scholarship Council
- Government of Canada
- National Natural Science Foundation of China (21425728, 21872061, 51472100)
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