文摘
Vanadia redox catalysts, V2O5/SiO2, V2O5/TiO2, and V2O5/TiO2-a href='/search?dc.title=SiO&facet-content-type=ReferenceWorkEntry&sortOrder=relevance' class='reference-link webtrekk-track' gaCategory="Internal link" gaLabel="SiO" gaAction="reference keyword">SiO2 having different structures were prepared by incorporating vanadium oxytripropoxide on granular SiO2, TiO2 nano-particles, and TiO2-grafted-SiO2 pellets, respectively. In order to accelerate the catalyst deactivation, the catalysts were tested for oxidation of 1,2-dichlorobenzene (o-DCB) with temperature elevated from 200 to 550?°C. Using EXAFS and XRPD, the structural changes in the accelerated aging tests were characterized to assess the catalyst stability and the role of the grafted TiO2 in catalysis. The correlation of catalyst structures with catalytic reaction results indicated that: (1) the grafted TiO2 helps anchoring and dispersing vanadia in the catalyst preparation; (2) monomeric vanadia species with umbrella geometry, polymeric VO4, and TiVO4 coexisting with V2O5 clusters were formed on TiO2-a href='/search?dc.title=SiO&facet-content-type=ReferenceWorkEntry&sortOrder=relevance' class='reference-link webtrekk-track' gaCategory="Internal link" gaLabel="SiO" gaAction="reference keyword">SiO2 pellet, granular SiO2, and TiO2 nano-particles, respectively; (3) oxidative destruction of o-DCB induces the aggregation of vanadia species on the supports leading to a decrease of catalytic activity; (4) lower total oxidation selectivity for V2O5/TiO2 as opposed to the other two catalyst samples could be due to the presence of higher Br?nsted-to-Lewis acid sites ratio; (5) a decrease of vanadium-atoms valence charge induced by TiO2–V2O5 interactions alleviates strong adsorption of oxygen-containing intermediates on vanadia sites, thereby increasing the reaction rate; and (6) hydration of vanadia in reaction could lead to aggregation of the vanadia species and catalyst deactivation.