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The Study Of Ni-based Catalysts On Amination Of Diethylene Glycol With Tertiarybutylamine

Posted on:2018-06-09Degree:MasterType:Thesis
Country:ChinaCandidate:D D ChengFull Text:PDF
GTID:2311330515976073Subject:Physical chemistry
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Natural gas usually contains CO2,H2 S and organic sulfur compounds,which are commonly referred to as acidic gas.However,H2 S in the storage and transportation process will lead to the corrosion of pipeline equipment,and combustion will pollute the atmosphere seriously.Dimethyaminoethoxyethanol?TBEE?has steric hindrance effect,which makes the amino group show higher chemical activity,and is a very effective solvent for the selective desulfurization.Therefore,TBEE are widely used selective desulfurization in petroleum,natural gas,oil field gas,liquid hydrocarbons and syngas.At present,there are few reports about the synthesis process,the synthesis methods and the corresponding catalyst systems need to be further studied.In this paper,we prepared a series of Ni catalysts for the amination of diethylene glycol with tertiarybutylamine.The catalytic performance of the catalyst was studied in a batch reactor,and the reaction conditions were optimized.At the same time,the structural properties of the catalyst,the active center and the role of the acid-base center in the catalyst reaction system were studied by means of the reaction results and various characterization methods.The influence of preparation conditions for the catalytic performance of the catalysts was also investigated.The main work of this paper is as follows:?1?For the amination reaction of diethylene glycol with tertiarybutylamine,the active contents of the catalyst were screened,and the effects of reaction temperature,pressure,solvent and rotational speed on the catalytic performance were also investigated.The results showed that Ni is the main component of the catalyst,the reaction temperature is 200?,the speed 400r/min,H2 pressure 0.5MPa,the molar ratio of materials TBA:DEG is 2:1,no solvent,and the catalyst has better catalytic performance.?2?We prepared a series of Ni-Al2O3 catalysts by co-precipitation method,the effects of Ni/Al,calcination temperature and reduction temperature on the synthesis of TBEE were investigated.The results showed that the Ni-Al2O3 catalyst prepared by co-precipitation method,Ni/Al was 1:1,the catalyst at 450 ? calcination and reduction at 550? showed higher activity and selectivity.The results also show that the active center of the amination reaction is the metal Ni particles?Ni0?,and the acid-base of the catalyst plays an important role in improving the activity and selectivity of the catalyst.?3?The catalyst preparation conditions have great influence on the structure and catalytic performance of the catalyst.Therefore,preparation conditions of Ni-Al2O3 catalyst system?such as Ni content,precipitation agent,synthesis temperature and precipitation method?were further investigated,and the influence of synthesis conditions and reaction time were also optimized.The results showed that the optimum preparation conditions were as follows: the content of Ni was 20%,Na2CO3 was used as the precipitant,the synthesis temperature was 80?,and the catalyst had good catalytic performance under the optimum reaction conditions for 6h.
Keywords/Search Tags:diethylene glycol, tertiarybutylamine, amination reaction, Ni-based catalyst, dimethyaminoethoxyethanol
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