Reducing the cost of RuO_(2)/TiO_(2)catalysts is still one of the urgent challenges in catalytic HCl oxidation.In the present work,a Ce-doped TiO_(2)supported RuO_(2)catalyst with a low Ru loading was developed,showin...Reducing the cost of RuO_(2)/TiO_(2)catalysts is still one of the urgent challenges in catalytic HCl oxidation.In the present work,a Ce-doped TiO_(2)supported RuO_(2)catalyst with a low Ru loading was developed,showing a high activity in the catalytic oxidation of HCl to Cl_(2).The results on some extensive characterizations of both Ce-doped TiO_(2)carriers and their supported RuO_(2)catalysts show that the doping of Ce into TiO_(2)can effectively change the lattice parameters of TiO_(2)to improve the dispersion of the active RuO_(2)species on the carrier,which facilitates the production of surface Ru species to expose more active sites for boosting the catalytic performance even under some harsh reaction conditions.This work provides some scientific basis and technical support for chlorine recycling.展开更多
Dioxin production is a worldwide concern because of its persistence and carcinogenic,teratogenic, and mutagenic effects. The pyrolysis-chemical looping combustion process of disposing solid waste is an alternative to ...Dioxin production is a worldwide concern because of its persistence and carcinogenic,teratogenic, and mutagenic effects. The pyrolysis-chemical looping combustion process of disposing solid waste is an alternative to traditional solid waste incineration developed to reduce the dioxin production. Based on the equilibrium composition of the Deacon reaction,pyrolysis gas oxidized by seven common oxygen carriers, namely, Cu O, Ni O, Ca SO4, Co O,Fe2O3, Mn3O4, and Fe Ti O3, is studied and compared with the pyrolysis gas directly combusted by air. The result shows that the activity of the Deacon reaction for oxygen carriers is lower than that for air. For four typical oxygen carriers（Cu O, Ni O, Fe2O3, and Fe Ti O3）, the influences of temperature, pressure, gas composition, and tar on the Deacon reaction are discussed in detail. According to these simulation results, the dioxin production in China, Europe, the United States, and Japan is predicted for solid waste disposal by the pyrolysis-chemical looping combustion process. Thermodynamic analysis results in this paper show that chemical looping combustion can reduce dioxin production in the disposal of solid waste.展开更多
Adsorptive reactors(AR),in which an adsorptive functionality is incorporated into the catalytic reactors,offer enhanced performance over their conventional counterparts due to the effective manipulation of concentrati...Adsorptive reactors(AR),in which an adsorptive functionality is incorporated into the catalytic reactors,offer enhanced performance over their conventional counterparts due to the effective manipulation of concentration and temperature profiles.The operation of these attractive reactors is,however,inherently unsteady state,complicating the design and operation of such sorption-enhanced processes.In order to capture,comprehend and capitalize upon the rich dynamic texture of adsorptive reactors,it is necessary to employ cyclic steady state algorithms describing the entire reaction-adsorption/desorption cycle.The stability of this cyclic steady state is of great importance for the design and operation of adsorptive reactors.In this paper,the cyclic steady state of previously proposed novel adsorptive reactor designs has been calculated and then optimized to give maximum space–time yields.The results obtained revealed unambiguously that an improvement potential of up to multifold level could be attained under the optimized cyclic steady state conditions.This additional improvement resulted from the reduction of the regeneration time well below the reaction-adsorption time,which means,in turn,more space–time yield.展开更多
Recently, as a direct consequence of the dwindling world oil reserves and the growing awareness of the environmental problems associated with the use of coal as energy source, there is growing interest in cheaper, abu...Recently, as a direct consequence of the dwindling world oil reserves and the growing awareness of the environmental problems associated with the use of coal as energy source, there is growing interest in cheaper, abundant and cleaner burning methane. The Gas-to-Liquid technology offers perhaps the most attractive routes for the exploitation of the world huge and growing natural gas resources. Using this process the erstwhile stranded gas is converted to premium grade liquid fuels and chemicals that are easily transported. However, a widespread application of the GTL process is being hampered by economical and technical challenges. The high cost of synthesis gas, for instance, weighs heavily on the economics and competitiveness of the process limiting its wider application. This work presented a modified Gas-to-Liquid process that eliminates the costly synthesis gas production step. The proposed process utilized an alternative pathway for methane activation via the production of chloromethane derivatives which are then converted to hydrocarbons. It established that hydrocarbons mainly olefins can be economically produced from di- and tri-chloro- methanes over a typical iron-based Fischer Tropsch catalysts in a moving bed reactor at industrially relevant conditions. Some of the attractions of the proposed process include a) the elimination of the costly air separation plant requirement b) high process selectivity and c) significant reduction of carbon dioxide emissions thereby saving on feedstock loss and the costly CO2 removal and isolation processes.展开更多
基金supported by Zhejiang Provincial Key R&D Project(No.2021C01056)the Programme of Introducing Talents of Discipline to Universities(No.D17008).
文摘Reducing the cost of RuO_(2)/TiO_(2)catalysts is still one of the urgent challenges in catalytic HCl oxidation.In the present work,a Ce-doped TiO_(2)supported RuO_(2)catalyst with a low Ru loading was developed,showing a high activity in the catalytic oxidation of HCl to Cl_(2).The results on some extensive characterizations of both Ce-doped TiO_(2)carriers and their supported RuO_(2)catalysts show that the doping of Ce into TiO_(2)can effectively change the lattice parameters of TiO_(2)to improve the dispersion of the active RuO_(2)species on the carrier,which facilitates the production of surface Ru species to expose more active sites for boosting the catalytic performance even under some harsh reaction conditions.This work provides some scientific basis and technical support for chlorine recycling.
基金supported by the National Basic Research Program of China (973 Program) (No. 2011CB201502)the National Key Technology R&D Program of China (No. 2010BAC66B03)
文摘Dioxin production is a worldwide concern because of its persistence and carcinogenic,teratogenic, and mutagenic effects. The pyrolysis-chemical looping combustion process of disposing solid waste is an alternative to traditional solid waste incineration developed to reduce the dioxin production. Based on the equilibrium composition of the Deacon reaction,pyrolysis gas oxidized by seven common oxygen carriers, namely, Cu O, Ni O, Ca SO4, Co O,Fe2O3, Mn3O4, and Fe Ti O3, is studied and compared with the pyrolysis gas directly combusted by air. The result shows that the activity of the Deacon reaction for oxygen carriers is lower than that for air. For four typical oxygen carriers（Cu O, Ni O, Fe2O3, and Fe Ti O3）, the influences of temperature, pressure, gas composition, and tar on the Deacon reaction are discussed in detail. According to these simulation results, the dioxin production in China, Europe, the United States, and Japan is predicted for solid waste disposal by the pyrolysis-chemical looping combustion process. Thermodynamic analysis results in this paper show that chemical looping combustion can reduce dioxin production in the disposal of solid waste.
基金the German research council(Deutsche Forschungsgemeinschaft) for their financial support to the project:AG 26/18-1
文摘Adsorptive reactors(AR),in which an adsorptive functionality is incorporated into the catalytic reactors,offer enhanced performance over their conventional counterparts due to the effective manipulation of concentration and temperature profiles.The operation of these attractive reactors is,however,inherently unsteady state,complicating the design and operation of such sorption-enhanced processes.In order to capture,comprehend and capitalize upon the rich dynamic texture of adsorptive reactors,it is necessary to employ cyclic steady state algorithms describing the entire reaction-adsorption/desorption cycle.The stability of this cyclic steady state is of great importance for the design and operation of adsorptive reactors.In this paper,the cyclic steady state of previously proposed novel adsorptive reactor designs has been calculated and then optimized to give maximum space–time yields.The results obtained revealed unambiguously that an improvement potential of up to multifold level could be attained under the optimized cyclic steady state conditions.This additional improvement resulted from the reduction of the regeneration time well below the reaction-adsorption time,which means,in turn,more space–time yield.
文摘Recently, as a direct consequence of the dwindling world oil reserves and the growing awareness of the environmental problems associated with the use of coal as energy source, there is growing interest in cheaper, abundant and cleaner burning methane. The Gas-to-Liquid technology offers perhaps the most attractive routes for the exploitation of the world huge and growing natural gas resources. Using this process the erstwhile stranded gas is converted to premium grade liquid fuels and chemicals that are easily transported. However, a widespread application of the GTL process is being hampered by economical and technical challenges. The high cost of synthesis gas, for instance, weighs heavily on the economics and competitiveness of the process limiting its wider application. This work presented a modified Gas-to-Liquid process that eliminates the costly synthesis gas production step. The proposed process utilized an alternative pathway for methane activation via the production of chloromethane derivatives which are then converted to hydrocarbons. It established that hydrocarbons mainly olefins can be economically produced from di- and tri-chloro- methanes over a typical iron-based Fischer Tropsch catalysts in a moving bed reactor at industrially relevant conditions. Some of the attractions of the proposed process include a) the elimination of the costly air separation plant requirement b) high process selectivity and c) significant reduction of carbon dioxide emissions thereby saving on feedstock loss and the costly CO2 removal and isolation processes.
