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Tailor Made Catalytic Materials For Selective Oxidation Of Alcohols

Posted on:2018-04-22Degree:MasterType:Thesis
Country:ChinaCandidate:R JiFull Text:PDF
GTID:2321330542460535Subject:Chemical Engineering and Technology
Abstract/Summary:PDF Full Text Request
Selective oxidation of alcohols to corresponding aldehydes or ketones plays a paramount role in dye,perfumery and grochemical-related industries.It is that serious pollution toenvironment,low yield and high-energy consumption for the conventional preparationtechniques.In this paper,owing to Pd NPs have high efficient selective and high catalytic activity for oxidation of alcohols,the preparation of high catalytic activity and strong stability of Pd-base catalyst.Different from those of the preparation of palladium catalysts(1)Without adding complexing agent,equipment simple easy to operate;(2)Owing to the preparation of highly efficient catalyst with enhanced metal-support interaction,the preparation of palladium catalysts higher reliability,higher circulation.the oxidation reaction could be performed smoothly under solvent-and base-free conditions,without chlorine.In the section one,we have prepared the ZrSBA-15,the Zr atoms,incorporated into the framework channels and being as the high charge density sites,not only can improve the hydrothermal stability of pore walls but also can increase the number of lattice defects on the skeleton.The Zr-containing SBA-15 with platelet shortened morphologys seemingly to be a suitable support for palladium nanoparticles(Pd NPs)on account of its easiness in molecular diffusion;namely,the significantly shortened channels offer quicker mass transportation and accordingly higher reaction efficiency.We try to use the NaBH4 as the reducing agent,the palladium ion reduction of Pd NPs.Possibly,by virtue of these features,ZrSBA-15,with increased acidic sites as compared to purely siliceous SBA-15,can favorably enhance the metal-support interactions between Pd NPs and ZrSBA-15.Based on the first study,we have introduced a coating of N-doped carbon layers inside acidic ZrSBA-15 with short pore channels is presented.According to the combinatorial procedures of controllable carbonization of PHEA pre-adsorbed inside ZrSBA-15 and subsequent deposition of active Pd NPs,the temperature is too high to destroy the carrier frame structure.Simultaneously,according to utilizing the synergic effect between the anchoring sites of N-doped carbon layers and the acidic framework of inorganic support ZrSBA-15,which make Pd NPs desirably and firmly disperse inside the pore channels of platelet-like NC-ZS with a low Pd amount.This synthesized composite was used for the aerobic oxidation of BnOH,and excellent conversion of BnOH and selectivity for BzH was gained under testing conditions,without significant loss in activity even after ten times reaction cycles.Validity of the resulting composites was provided by FT-IR?XRD?SEM?TEM?XPS characterization techniques,through which the Pd NPs are dispersed evenly on ZrSBA-15 and NC-ZS has been confirmed.
Keywords/Search Tags:Pd NPs, ZrSBA-15, Selective oxidation, N-doped carbon
PDF Full Text Request
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