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Catalytic Decomposition Of Ozone On M/g-?O?C3N4?M=Co,Cu,Mn?

Posted on:2021-05-20Degree:MasterType:Thesis
Country:ChinaCandidate:J Y DingFull Text:PDF
GTID:2381330629487337Subject:Chemical engineering
Abstract/Summary:PDF Full Text Request
O3 is a widely used oxidant and a common by-product in industrial production.O3 in the human environment will harm human health and ecosystems,and will react with organic matter to form secondary pollutants such as aldehydes,acids and ultrafine particles.At present,catalytic decomposition is a method for eliminating O3,which mainly focuses on metal oxide catalysts.Its catalytic action depends on the oxygen vacancies on the surface of the catalyst.When oxygen occupies oxygen vacancies and is difficult to eliminate,the catalyst is deactivated.The regeneration of deactivated catalyst requires the use of hydrogen reduction under high temperature conditions,so it is urgent to develop a catalyst that can overcome the above shortcomings.The two-dimensional material g-C3N4 has a 3-s-triazine ring structure.There are six N atoms in the ring that can coordinate with metal atoms.These coordination bonds can fix metal atoms and efficiently disperse metal atoms.It is stable and uniform for synthesis.The catalyst provides the possibility;metal atoms can be exposed on the surface of g-C3N4,increasing the effective contact between metal atoms and O3;the number and method of coordination between metal atoms and N atoms can be used to affect the catalytic process and regeneration method of decomposing O3.In this study,g-C3N4 supported Co sub-nano clusters,g-C3N4 and O-substituted g-OC3N4supported single-atom Mn and Cu catalysts were prepared by impregnation reduction method.The structure and properties of the catalysts were analyzed by XRD,BET,TEM,XPS,and their performance in decomposing O3 was evaluated.Combined with density functional theory calculation,the stable adsorption structure of sub-nano Cox?x=1-4?clusters on g-C3N4 and the stability of ozone on Cox/g-C3N4?x=1-4?are given.Adsorption configuration;the mechanism of single atom catalyst M/g-?O?C3N4?M=Cu,Mn?for catalytic decomposition of ozone.Studies have shown that g-C3N4 and g-OC3N4 supported metal Co,Mn,Cu catalysts,metal loading methods and carrier doping can significantly affect the catalyst's ozone decomposition activity.Low loading Co/g-C3N4,Co exists as amorphous sub-nano particles,when decomposing O3,Co generates amorphous oxide,does not depend on lattice O vacancy decomposition O3,can be heated by low temperature Regeneration catalyst.Compared with Cu/g-C3N4,single-atom-supported Cu/g-OC3N4,doped O changes the coordination mode of Cu and N in the process of ozone decomposition,and improves the efficiency of the catalyst.Monoatomic Mn/g-C3N4 and Mn/g-OC3N4,by changing the number of Mn-N and Mn-O coordination bonds and coordination mode,to achieve the purpose of efficient decomposition of O3,to avoid dependence on oxygen vacancies.In this experiment,a series quartz tube reactor was used as the catalytic device,and the catalyst was mixed and filled with quartz sand.When the O3 concentration is 40ppm,the relative humidity is1%,and the space velocity is 600L?L-1?h-1,the prepared Mn/g-C3N4and Cu/g-OC3N4 can be operated continuously for 1 day,and the activity still reaches 100%.
Keywords/Search Tags:ozone decomposition, graphitic carbon nitride, oxygen doping, single atom catalysis, transition metals cobalt,copper,manganese
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