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Study On The Controllable Preparation And Catalytic Performance Of Ruthenium-based Nanomaterials

Posted on:2021-08-15Degree:MasterType:Thesis
Country:ChinaCandidate:W KeFull Text:PDF
GTID:2481306527986429Subject:Chemical Engineering and Technology
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As a noble metal element,Ru element contains many empty orbitals and has excellent catalytic performance.However,due to the small content of Ru in nature,it has been restricted from being developed in large quantities to be used as a catalyst.In addition,compared with other non-noble metal element nano-catalysts,Ru nano-catalysts are less stable and tend to aggregate to reduce their catalytic activity.Therefore,in this paper,Ru is the main element.By introducing other non-noble metal elements,a series of Ru-based multimetal nanocatalysts can be controllable preparation,and their catalytic properties have been studied.The specific research contents of this paper are as follows:1.With Ru(acac)3,Ni(acac)2,Cu(acac)2and Fe(acac)3 as metal precursors,by adjusting the amount and type of metal precursors and the reaction temperature,a series of hexagonal Ru-Ni-"M"(M=none,Cu and Fe)alloy NPs can be controllable preparation.Then,using the catalytic degradation of p-NP as a model,according to the efficiency of p-NP degradation,the ratio of Ru-Ni,the reaction temperature and the doping type of the third element are gradually optimized.Finally,Ru44Ni28Fe28 alloy NPs are the strongest catalysts that can completely degrade p-NP,and their speeds are 31 times,29 times and 5 times faster than Ni NPs,Ru NPs and Ru60Ni40 NPs,respectively.In addition,Ru44Ni28Fe28alloy NPs are easy to precipitate,which can be separated from the catalytic system many times.After ten consecutive separations,the dispersibility and morphology of Ru44Ni28Fe28 alloy NPs have not changed significantly,and they still maintain good catalytic activity and selectivity in the catalytic reaction.At the same time,Ru44Ni28Fe28 NPs membrane was prepared at the oil-water(ethyl acetate-water)interface.The membrane is transferred to different solid macro substrates(eg glass,silicon wafers)by evaporating ethyl acetate.The resulting tightly packed Ru44Ni28Fe28NPs membrane is a good Raman substrate.The catalytic performance of Ru44Ni28Fe28NPs membrane was measured by using 4-NTP as a catalytic substrate and Raman probe.In the presence of Na BH4,the membrane can catalyze the complete conversion of 4-NTP to 4-ATP.2.Using Ru(acac)3 and Cu(acac)2 as metal precursors,Ru-Cu alloy nanocatalysts with different structures were synthesized by one-step method.The catalytic performance of Ru-Cu alloy nano-catalyst was measured by catalytic reduction of chromium(Cr6+)as a template.Compared with Ru NPs and Ru-Cu NCs,Ru-Cu solid NPs have better catalytic performance,because the geometry and internal electronic properties of NPs will change due to changes in doping elements or reaction conditions.In the process of catalytic reduction of Cr6+,Ru2Cu2(5 h,p H 8)NPs had excellent catalytic performance.In addition,Ru2Cu2(5 h,p H 8)NPs had excellent stability.After repeated testing,the dispersibility was still good,and the morphology had not changed significantly.3.Taking Ru(acac)3,Co(acac)3,Zn(acac)2,Cu(acac)2 and Fe(acac)3 as metal precursors,by adjusting the types of metal precursors and synthetic system p H value,controllable synthesis of a series of Ru-based two-element alloy NPs.Then,using the catalytic degradation of Cr6+as a template,the catalytic performance of alloy NPs was measured.Within a few tens of minutes,these alloy NPs have significant catalytic degradation performance for Cr6+.According to the time required for the catalytic degradation of Cr6+and the efficiency of degradation,the types of doped elements and the p H value of the synthesized NPs environment system were gradually optimized.Finally,the minimum time required for Ru2Co2 alloy NPs to catalyze the complete degradation of Cr6+.In addition,after many cycles,the dispersion of Ru2Co2 alloy NPs is good,and its morphology has not changed significantly,and it still has good catalytic activity in the catalytic degradation of Cr6+.
Keywords/Search Tags:Ru-based polymetallic nanocatalyst, Controlled synthesis, Catalytic performance, p-NP, Cr6+
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