Metal
atoms dispersed on the oxide supports constitute a large
category of single-atom catalysts. In this review, oxide supported
single-atom catalysts are discussed about their synthetic procedures,
characterizations, and reaction mechanism in thermocatalysis, such
as water–gas shift reaction, selective oxidation/hydrogenation,
and coupling reactions. Some typical oxide materials, including ferric
oxide, cerium oxide, titanium dioxide, aluminum oxide, and so on,
are intentionally mentioned for the unique roles as supports in anchoring
metal atoms and taking part in the catalytic reactions. The interactions
between metal atoms and oxide supports are summarized to give a picture
on how to stabilize the atomic metal centers, and rationally tune
the geometric structures and electronic states of single atoms. Furthermore,
several directions in fabricating single-atom catalysts with improved
performance are proposed on the basis of state-of-the-art understanding
in metal-oxide interactions.
The strong metal-support interaction (SMSI) has long been studied in heterogonous catalysis on account of its importance in stabilizing active metals and tuning catalytic performance. As a dynamic process taking place at the metal-support interface, the SMSI is closely related to the metal surface properties which are usually affected by the size of metal nanoparticles (NPs). In this work we report the discovery of a size effect on classical SMSI in Au/TiO2 catalyst where larger Au particles are more prone to be encapsulated than smaller ones. A thermodynamic equilibrium model was established to describe this phenomenon. According to this finding, the catalytic performance of Au/TiO2 catalyst with uneven size distribution can be improved by selectively encapsulating the large Au NPs in a hydrogenation reaction. This work not only brings in-depth understanding of the SMSI phenomenon and its formation mechanism, but also provides an alternative approach to refine catalyst performance.
We propose an efficient method to synthesize large-scale soluble acidified graphitic carbon nitride (g-C3N4). The as-prepared material exhibits the characteristics of a poly-ammonium salt and is soluble in several solvents with good dissolution-recrystallization reversible equilibrium. The pH value- and temperature-dependent solubility of the acidified g-C3N4 facilitates its separation and purification. After dissolution, acidified g-C3N4 forms isolated ultrathin nanosheets, making it an ideal precursor for large quantities of g-C3N4 nanosheets. This study raises the possibility of liquid assembly for g-C3N4 nanosheets based composite materials, expanding the functionalization and application of g-C3N4.
Metal-support interaction predominately determines the electronic structure of metal atoms in single-atom catalysts (SACs), largely affecting their catalytic performance. However, directly tuning the metal-support interaction in oxide supported SACs remains challenging. Here, we report a new strategy to subtly regulate the strong covalent metal-support interaction (CMSI) of Pt/CoFe2O4 SACs by a simple water soaking treatment. Detailed studies reveal that the CMSI is weakened by the bonding of H+, generated from water dissociation, onto the interface of Pt-O-Fe, resulting in reduced charge transfer from metal to support and leading to an increase of C-H bond activation in CH4 combustion by more than 50 folds. This strategy is general and can be extended to other CMSI-existed metal-supported catalysts, providing a powerful tool to modulating the catalytic performance of SACs.
The discoveries and development of the oxidative strong metal–support interaction (OMSI) phenomena in recent years not only promote new and deeper understanding of strong metal–support interaction (SMSI) but also open an alternative way to develop supported heterogeneous catalysts with better performance. In this review, the brief history as well as the definition of OMSI and its difference from classical SMSI are described. The identification of OMSI and the corresponding characterization methods are expounded. Furthermore, the application of OMSI in enhancing catalyst performance, and the influence of OMSI in inspiring discoveries of new types of SMSI are discussed. Finally, a brief summary is presented and some prospects are proposed.
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