期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 301, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120766
关键词
Single-atom catalyst; Rare-earth La; Photocatalytic nitrogen fixation; Coordination; MoO3-x
资金
- National Key Research and Development Program of China [2016YFA0203000]
- National Science Foundation of China [U20A20129, 21876058]
- Excellent Doctoral Dissertation Cultivation Grant from Central China Normal University [2017YBZZ018]
The rare-earth La single catalyst, with a well-designed coordination structure, shows excellent catalytic performance in hydrogenation and photocatalysis for nitrogen fixation under visible light, outperforming most reported single atom photocatalysts.
Herein, we demonstrate that the rare-earth La single catalyst with multi-shell characteristic is an excellent choice for this purpose. By merit of its unsaturated orbitals of La, the single La atom strongly bonds with the two-coordinated lattice oxygen on the oxygen-deficient MoO3-x to form O-2c-La-O-2c coordination. This robust metal-support interaction frees single atoms from detachment or aggregation, and prevents catalyst from deactivation. Meanwhile, the occupied 5d orbitals of La back-donate electrons to the 2 pi* molecular orbitals of adsorbed N-2 that substantially activate the inert N equivalent to N bond towards successive hydrogenation. And single La atom could optimize the electron property of the MoO3-x support to promote photocatalytic nitrogen fixation. Without any sacrificial agents, this single atom La catalyst with a well-designed coordination structure delivers an impressive NH3 production rate of 209.0 mu mol h(-1) g(-1) under visible light, outperforming most reported single atom photocatalysts.
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