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Ca2+ doped metal organic frameworks for enhanced photocatalytic ammonia synthesis.
- Source :
-
Chemical Engineering Journal . Jun2023, Vol. 466, pN.PAG-N.PAG. 1p. - Publication Year :
- 2023
-
Abstract
- [Display omitted] • A metal doping strategy is proposed for N 2 activation. • Ca2+-doped UiO-66 is synthesized. • The Ca2+ doping fortifies the electron transfer from active sites to N 2. • The diamino ligand incorporating fortifies the electron generation and separation. • Photocatalytic NH 3 yield reaches 759.3 μmol h−1 g−1 under full spectrum. Photocatalytic NH 3 synthesis from N 2 is a clean and sustainable approach, however, the efficiency of this process is low due to the difficult activation of N N triple bonds. Herein, we propose a metal-doping strategy to facilitate the interfacial charge transfer for promoting the photocatalytic NH 3 yield. Ca2+ with low electronegativity was doped in UiO-66-NH 2 , a kind of Zr-based MOFs, to increase the electron donor capacity of Zr active sites. The X-ray photoelectron spectroscopy (XPS) spectra and density functional theory (DFT) calculations show that the Ca2+ doping enhances the electron density of Zr active sites. Moreover, the diamino ligand is incorporated to tune the bandgap structure of MOFs to expand its light absorption range. By adjusting the ratio of metals and organic ligands, the optimal photocatalyst UN(Zr-0.30Ca)-4 reaches a high NH 3 evolution rate of 759.3 μmol g−1 h−1 under full spectrum. This study may provide some inspiration for the design of advanced photocatalysts for diverse chemical reduction reactions. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 13858947
- Volume :
- 466
- Database :
- Academic Search Index
- Journal :
- Chemical Engineering Journal
- Publication Type :
- Academic Journal
- Accession number :
- 163845540
- Full Text :
- https://doi.org/10.1016/j.cej.2023.143259