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Metal-support Interactions Of Molybdenum-based Nanostructures For Catalytic Hydrogenation

Posted on:2018-08-08Degree:MasterType:Thesis
Country:ChinaCandidate:Y J ShuFull Text:PDF
GTID:2321330536983208Subject:Chemistry Department Inorganic Chemistry
Abstract/Summary:PDF Full Text Request
Metal-support interactions?MSI?make obvious influence on the properties and catalytic turnover of supported metal catalysts.In the hydrogenation of nitroarenes and ?-? unsaturated aldehydes,MSI plays a key role to accomplish the efficient and selective routes.Herein,our work studied the interactions arising from Mo-based supports,e.g.,carbides and oxides,and the contribution to the chemoselective hydrogenation.Mo2C nanowires were introduced as a versatile support towards highly dispersive Ni owing to the strong MSI on carbide surface,accomplishing the high activity in the hydrogenation of nitrobenzoic acid.A facile carbon coating was further introduced to remarkably enhance the stability,protecting active Ni from corrosive H+ and H2 O.We found that the dispersion of Ni NPs is well improved on Mo2 C support,as compared with CNT and SiO2,as a result of high activity.The as-obtained composites retained the high activity after four consecutive catalytic tests even at corrosive condition?pH 3?,elucidating the promotion associated with the both of carbide support and carbon coating.Hydrogenated MoOx?H-MoOx?supported bimetallic Pt-Sn?Pt-Sn/H-MoOx?was developed to accomplish the selective and efficient hydrogenation of functionalized nitroarenes.The evidenced support interactions form H-MoOx contributed to the efficient turnover on ultrafine nanoparticles,and the atom-rearranged bimetallic Pt-Sn surface promoted the selectivity owing to the preferred nitro adsorption.Furthermore,our PtSn/H-MoOx can be considered in a sense as a universal catalyst for nitroarenes hydrogenation.Employing H-MoOx as the support,the hydrogenation of cinnamaldehyde?CAL?on Pt-M/MoOx?M = Fe?Co?Ni?Cu?Zn?was investigated.The maximum selectivity of cinnamyl alcohol?COL?was accomplished on Pt-Fe/MoOx with 1 MPa H2 at 30 oC,along with the high activity.It's found that the variation of surface structures by MOx is responsible for the improved selectivity and activity in hydrogenation.This work elucidates the efficient MSI of molybdenum-based nanostructures can effectively optimize the activity and selectivity in hydrogenation.Moreover,the further combination with the rational engineering on interface/surface opens up new opportunities for catalyst design.
Keywords/Search Tags:Mo2C, hydrogenated molybdenum oxides, Pt-group metal, metal-support interactions, selective hydrogenation, surface engineering
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