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Design And Preparation Of Cu-based Nanocatalyst With Dual Photothermal Response And Performance Study On CO2 Hydrogenation Synthesis Fuel

Posted on:2021-01-09Degree:MasterType:Thesis
Country:ChinaCandidate:T ZhangFull Text:PDF
GTID:2381330620976364Subject:Chemistry
Abstract/Summary:PDF Full Text Request
Heterogeneous CO2 hydrogenation catalytic reaction,as a strategy of net CO2emission reduction and green carbon resource recycling,plays an important role in alleviating global warming and energy shortage.However,most of the research on the CO2 hydrogenation synthesis reaction has focused on thermal catalysis,this kind of reaction consumes a lot of energy and therefore induces additional CO2 emissions,which greatly limits its development in industry.Regarding the issue above,this paper proposes a method of coupling thermocatalysis and photocatalysis technology,and designs a series of Cu-based catalysts with photothermal response for thermal/photothermal catalytic CO2 hydrogenation,and the relationship between the physical and chemical properties,catalytic activity,and photothermal catalytic mechanism of the catalyst was also discussed.The results are as follows:?1?By using hydrotalcite?CuCoAl-LDH?as a precursor,a Cu-Co alloy supported catalysts which were highly dispersed on the carrier Al2O3 were obtained through hydrogen reduction.The catalytic performance of methane production via CO2 hydrogenation was investigated under thermal and photothermal conditions.The results demonstrate that the photothermal synergistic catalysis shows a better performance of CO2 hydrogenation to methane than the single thermal catalysis.Under atmospheric pressure?0.1Mpa?and low temperature?280??reaction conditions,the CO2 conversion rate is 41.0%,and the methane selectivity is as high as 96.6%.?2?Two catalysts with different ratios of Cu/ZnMgO?4-3-3?and Cu/ZnMgO?3-2-5?were prepared by hydrothermal synthesis method.This composite material contains metal Cu with surface plasmon resonance?SPR?effect and n-type semiconductor ZnMgO?solid solution?,these components could generate Schottky junction which increases the lifetime of hot electrons generated by the SPR effect of Cu.The catalytic activity of the catalyst to synthesize methanol by CO2hydrogenation under thermal and photothermal conditions was also investigated.The results show that compared with Cu/ZnMgO?4-3-3?catalyst,Cu/ZnMgO?3-2-5?catalyst has better performance in the photothermal co-catalysis of CO2hydrogenation to methanol.Under the reaction conditions of temperature 180?and pressure 2.5Mpa,the CO2 conversion rate is 16.1%,and the selectivity of methanol is as high as 87.0%.Using it as a model catalyst,the catalytic mechanism of photothermal co-catalysis of CO2 hydrogenation to methanol was explored in detail.?3?The sol-gel method was used to prepare Cu/CuFe2O4 catalyst,and the catalytic performance in thermal and photothermal catalytic CO2 hydrogenation reactions was investigated.The results show that at a temperature of 240?and a reaction pressure of 2.5 MPa,the CO2 conversion rate is 33.2%and the hydrocarbon selectivity is 98.0%for the photothermal catalytic reaction.Among them,the selectivity ratio of methane and light alkanes?C2-C4?in hydrocarbons is close to 1:1.From the PXRD of the catalyst after the reaction,it was found that the phase of catalyst had been reconstructed,and a new phase Cu/FeCO3 was generated.
Keywords/Search Tags:photothermal catalysis, CO2 hydrogenation, Cu-based catalyst, SPR effect, Schottky junction, reconstruction phenomenon
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