1. Cent China Normal Univ, Inst Environm Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China
2. Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, Shanghai 200240, Peoples R China
折叠
Abstract
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.
NSTL
Elsevier