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Performance Study Of CO-catalyzed SO2 Reduction Over Ir/CeO2 Catalysts

Posted on:2023-05-09Degree:MasterType:Thesis
Country:ChinaCandidate:T R ShaoFull Text:PDF
GTID:2531306797473724Subject:Environmental Engineering
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China is one of the world’s major coal consumers,in the process of coal use produces a large number of SO2,seriously endangering the natural ecological environment and the health of the residents of China.At present,the vast majority of SO2 purification technology is to convert SO2 into sulfate treatment,China’s SO2generation in the steel industry alone in 2020 is about 7.70 million tons,of which more than 80%in the form of sulfate removal,resulting in the waste of sulfur resources and secondary pollution.However,China’s sulfur resources are highly dependent on foreign countries,with a total domestic sulfur consumption of 17.021million tons in 2021,of which 8.535 million tons are imported,with an import dependence of 50.1%.CO is often produced in metal smelting production,and as a reducing agent,CO can reduce SO2 to produce sulfur.While solving CO and SO2pollution,sulfur,a valuable resource,can be obtained,so CO reduction of SO2 to sulfur is a highly promising way to desulfurize.The reaction of CO catalytic reduction of SO2 is difficult to achieve under conventional conditions and usually requires the assistance of catalysts,which are currently immature in design.In this thesis,a series of Ir/CeO2 catalysts were prepared by impregnation method with CO-catalyzed SO2 reduction resourcefulness as the research objective,and the effects of the morphology and preparation conditions of the CeO2 carrier on the catalytic performance of the catalysts were investigated,and the key factors affecting the catalytic performance of the catalysts were deeply explored.Firstly,a series of Ir/CeO2 catalysts were synthesized by impregnation using a hydrothermal method to prepare CeO2 supports with controllable morphology and synthesize rod(R),cubic(C)and polyhedral(P)morphologies.The effect of the change of CeO2 support morphology on the valence state of the active components and the interaction between Ir-O-Ce was investigated.The results of the activity tests showed that the Ir/CeO2 catalyst with a rod-shaped CeO2 support had the best activity at a reaction rate of 10,000 h-1 volumetric air velocity,reaching 60.2%SO2 conversion and nearly 55.8%sulfur yield at 350℃,while the Ir/CeO2 catalyst with cubic-shaped CeO2 carrier had the worst activity,reaching 34.9%SO2 conversion and nearly 33.1%sulfur yield under the same conditions.The sulfur yield was close to 33.1%.The test results showed that the concentration of oxygen vacancies in the catalyst had an influence on the catalytic reaction,and the Ir/CeO2-R catalyst had the highest percentage of Ce3+(22.41%)and Ir0(52.92%)content on the surface,Ir interacted with CeO2-R to the strongest extent,and Ir/CeO2-R catalysts had the highest content of oxygen vacancies and thus showed the best catalytic activity.Secondly,a series of Ir/CeO2 catalysts were synthesized by impregnation method by controlling the catalyst synthesis method and varying the stirring time of the liquid phase mixing of CeO2 precursors to prepare CeO2 carriers with different stirring times(CeO2-0.25,CeO2-3,CeO2-6).The focus is on the effect of structural differences on the catalytic reaction of Ir/CeO2 catalysts caused by CeO2 carriers prepared by different stirring times.The results show that changing the stirring time of the liquid phase mixing of the CeO2 precursors has an effect on the grain size of the Ir/CeO2catalysts.The longer the stirring time,the smaller the grain size of Ir/CeO2 catalysts.The test results showed that the Ir/CeO2 catalysts with smaller grain size had more active oxygen vacancies on the surface.The Ir/CeO2 catalyst with CeO2-6 stirring time of 6 h,for example,exhibited the optimal catalytic performance due to its smallest grain size(12.4 nm)and highest Ir0(59.18%)content percentage on the catalyst surface,thus reaching 98.6%SO2 conversion and 96.7%sulfur yield at375℃,while the Ir/CeO2 catalyst with larger grain size(12.4 nm)exhibited the optimal catalytic performance.CeO2-0.25 catalyst(13.7 nm)with a lower Ir0 content share(53.82%)on the surface and poorer activity,showed a SO2 conversion of 73.9%and sulfur yield of 72.2%at 375℃.In this paper,we investigated the effect of different morphological CeO2 carriers and the interaction between different grain size CeO2 carriers and metal Ir on the CO-catalyzed SO2 reduction reaction.We demonstrated the impact of the interfacial effect between Ir-O-Ce on this catalytic reaction,which is of great value and guidance for the design and application of such catalysts.
Keywords/Search Tags:Support morphology, oxygen vacancy, SO2, Ir/CeO2 catalyst, flue gas resource utilization
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