The continual growth in transportation fuels and more strict environmental legislations have led to immense interest in developing green biomass energy. In this work, a proposed catalytic transformation of oxygenated ...The continual growth in transportation fuels and more strict environmental legislations have led to immense interest in developing green biomass energy. In this work, a proposed catalytic transformation of oxygenated organic compounds (related to bio-oil) into pure hydrogen was desighed, involving the catalytic reforming of oxygenated organic compounds to hydrogen- rich mixture gas followed by the conversion of CO to CO2 via the water gas reaction and the removal of CO2. The optimization of the different reforming catalyst, the reaction conditions as well as various sources of oxygenated organic compounds were investigated in detail. The production of pure hydrogen, with the H2 content up to 99.96% and the conversion of 97.1%, was achieved by the integrated catalytic transformation. The reaction pathways were addressed based on the investigation of decomposition, catalytic reforming, and the water gas reaction.展开更多
Catalytic synthesis of C2 oxygenated compounds from syngas in supercritical cyclohexane was reported in this paper. The effect of the molar ratio of media to feed on the conversion and selectivity was mainly discussed...Catalytic synthesis of C2 oxygenated compounds from syngas in supercritical cyclohexane was reported in this paper. The effect of the molar ratio of media to feed on the conversion and selectivity was mainly discussed. The results showed that the selectivity of C2 oxygenated compounds in supercritical cyclohexane was greatly improved, and the by-products of acetic acid, ace tic ester and alkanes were efficiently suppressed. Although the CO conversion was slightly declined, the space-time yield of C2 oxygenated compounds basically kept the constant at high media/feed ratio.展开更多
The oxygen-containing compounds in Fischer Tropsch synthetic oil greatly affect the downstream deep processing of hydrocarbons,and effective removal is required.Com-pared to traditional removal technologies such as hy...The oxygen-containing compounds in Fischer Tropsch synthetic oil greatly affect the downstream deep processing of hydrocarbons,and effective removal is required.Com-pared to traditional removal technologies such as hydrogenation deoxygenation,solvent extraction,and extraction distillation,adsorption deoxygenation technology has the advantages of low cost,mild operating conditions,easy removal and recovery,and mini-mal impact on oil quality.Therefore,adsorption deoxygenation technology has devel-oped rapidly in various removal processes and has become a research hotspot in the cur-rent Fischer Tropsch oil deoxygenation.Adsorbents are the core of adsorption deoxygen-ation technology.Therefore,this article briefly introduces the adsorption mechanism and summarizes the research progress of adsorbents widely used in recent years,such as silica gel,alumina,molecular sieves,and metal organic frameworks,in adsorbing oxygen-containing compounds in Fischer Tropsch synthetic oils.And provide reference sugges-tions for further adsorption and deoxygenation directions in the future.展开更多
It is reported in this paper a polarographic catalytic double wave of oxygen reduction caused by diphenylamine compounds(diphs).The electrochemical process of the wave includes the polarographic generation of the supe...It is reported in this paper a polarographic catalytic double wave of oxygen reduction caused by diphenylamine compounds(diphs).The electrochemical process of the wave includes the polarographic generation of the superoxide anion O_2^- and the dismutation of O_2^- catalyzed by diphs with redox pseudoreversibility.展开更多
A series of both unsupported and coal‐supported iron–oxygen compounds with gradual changes in microstructure were synthesized by a precipitation‐oxidation process at 20 to 70°C.The relationship between the mic...A series of both unsupported and coal‐supported iron–oxygen compounds with gradual changes in microstructure were synthesized by a precipitation‐oxidation process at 20 to 70°C.The relationship between the microstructures and catalytic activities of these precursors during direct coal liquefaction was studied.The results show that the microstructure could be controlled through adjusting the synthesis temperature during the precipitation‐oxidation procedure,and that compounds synthesized at lower temperatures exhibit higher catalytic activity.As a result of their higher proportions ofγ‐FeOOH orα‐FeOOH crystalline phases,the unsupported iron–oxygen compounds synthesized at 20–30°C,which also had high specific surface areas and moisture levels,generate oil yields 4.5%–4.6%higher than those obtained with precursors synthesized at 70°C.It was also determined that higher oil yields were obtained when the catalytically‐active phase formed by the precursors during liquefaction(pyrrhotite,Fe1-xS)had smaller crystallites.Feed coal added as a carrier was found to efficiently disperse the active precursors,which in turn significantly improved the catalytic activity during coal liquefaction.展开更多
Vapor wall losses can affect the yields of secondary organic aerosol.The effects of surfaceto-volume(S/V)ratio and relative humidity(RH)on the vapor-wall interactions were investigated in this study.The oxygenated vol...Vapor wall losses can affect the yields of secondary organic aerosol.The effects of surfaceto-volume(S/V)ratio and relative humidity(RH)on the vapor-wall interactions were investigated in this study.The oxygenated volatile organic compounds(OVOCs)were generated from toluene-H_(2)O_(2)irradiations.The average gas to wall loss rate constant(k_(gw))of OVOCs in a 400 L reactor(S/V=7.5 m^(-1))is 2.47(2.41 under humid conditions)times higher than that in a 5000 L reactor(S/V=3.6 m-1)under dry conditions.In contrast,the average desorption rate constant(k_(wg))of OVOCs in 400 L reactor is only 1.37(1.20 under humid conditions)times higher than that in 5000 L reactor under dry conditions.It shows that increasing the S/V ratio can promote the wall losses of OVOCs.By contrast,the RH effect on k_(gw)is not prominent.The average k_(gw)value under humid conditions is almost the same as under dry conditions in the 400 L(5000 L)reactor.However,increasing RH can decrease the desorption rates.The average k_(wg)value under dry conditions is 1.45(1.27)times higher than that under humid conditions in the 400 L(5000 L)reactor.The high RH can increase the partitioning equilibrium timescales and enhance the wall losses of OVOCs.展开更多
文摘The continual growth in transportation fuels and more strict environmental legislations have led to immense interest in developing green biomass energy. In this work, a proposed catalytic transformation of oxygenated organic compounds (related to bio-oil) into pure hydrogen was desighed, involving the catalytic reforming of oxygenated organic compounds to hydrogen- rich mixture gas followed by the conversion of CO to CO2 via the water gas reaction and the removal of CO2. The optimization of the different reforming catalyst, the reaction conditions as well as various sources of oxygenated organic compounds were investigated in detail. The production of pure hydrogen, with the H2 content up to 99.96% and the conversion of 97.1%, was achieved by the integrated catalytic transformation. The reaction pathways were addressed based on the investigation of decomposition, catalytic reforming, and the water gas reaction.
基金Project (No. 29873064) supported by the National Natural Science Foundation of China.
文摘Catalytic synthesis of C2 oxygenated compounds from syngas in supercritical cyclohexane was reported in this paper. The effect of the molar ratio of media to feed on the conversion and selectivity was mainly discussed. The results showed that the selectivity of C2 oxygenated compounds in supercritical cyclohexane was greatly improved, and the by-products of acetic acid, ace tic ester and alkanes were efficiently suppressed. Although the CO conversion was slightly declined, the space-time yield of C2 oxygenated compounds basically kept the constant at high media/feed ratio.
文摘The oxygen-containing compounds in Fischer Tropsch synthetic oil greatly affect the downstream deep processing of hydrocarbons,and effective removal is required.Com-pared to traditional removal technologies such as hydrogenation deoxygenation,solvent extraction,and extraction distillation,adsorption deoxygenation technology has the advantages of low cost,mild operating conditions,easy removal and recovery,and mini-mal impact on oil quality.Therefore,adsorption deoxygenation technology has devel-oped rapidly in various removal processes and has become a research hotspot in the cur-rent Fischer Tropsch oil deoxygenation.Adsorbents are the core of adsorption deoxygen-ation technology.Therefore,this article briefly introduces the adsorption mechanism and summarizes the research progress of adsorbents widely used in recent years,such as silica gel,alumina,molecular sieves,and metal organic frameworks,in adsorbing oxygen-containing compounds in Fischer Tropsch synthetic oils.And provide reference sugges-tions for further adsorption and deoxygenation directions in the future.
文摘It is reported in this paper a polarographic catalytic double wave of oxygen reduction caused by diphenylamine compounds(diphs).The electrochemical process of the wave includes the polarographic generation of the superoxide anion O_2^- and the dismutation of O_2^- catalyzed by diphs with redox pseudoreversibility.
文摘A series of both unsupported and coal‐supported iron–oxygen compounds with gradual changes in microstructure were synthesized by a precipitation‐oxidation process at 20 to 70°C.The relationship between the microstructures and catalytic activities of these precursors during direct coal liquefaction was studied.The results show that the microstructure could be controlled through adjusting the synthesis temperature during the precipitation‐oxidation procedure,and that compounds synthesized at lower temperatures exhibit higher catalytic activity.As a result of their higher proportions ofγ‐FeOOH orα‐FeOOH crystalline phases,the unsupported iron–oxygen compounds synthesized at 20–30°C,which also had high specific surface areas and moisture levels,generate oil yields 4.5%–4.6%higher than those obtained with precursors synthesized at 70°C.It was also determined that higher oil yields were obtained when the catalytically‐active phase formed by the precursors during liquefaction(pyrrhotite,Fe1-xS)had smaller crystallites.Feed coal added as a carrier was found to efficiently disperse the active precursors,which in turn significantly improved the catalytic activity during coal liquefaction.
基金supported by the National Key R&D Program of China(No.2017YFC0210005)the National Natural Science Foundation of China(Nos.41875166,41875163 and 41375129)
文摘Vapor wall losses can affect the yields of secondary organic aerosol.The effects of surfaceto-volume(S/V)ratio and relative humidity(RH)on the vapor-wall interactions were investigated in this study.The oxygenated volatile organic compounds(OVOCs)were generated from toluene-H_(2)O_(2)irradiations.The average gas to wall loss rate constant(k_(gw))of OVOCs in a 400 L reactor(S/V=7.5 m^(-1))is 2.47(2.41 under humid conditions)times higher than that in a 5000 L reactor(S/V=3.6 m-1)under dry conditions.In contrast,the average desorption rate constant(k_(wg))of OVOCs in 400 L reactor is only 1.37(1.20 under humid conditions)times higher than that in 5000 L reactor under dry conditions.It shows that increasing the S/V ratio can promote the wall losses of OVOCs.By contrast,the RH effect on k_(gw)is not prominent.The average k_(gw)value under humid conditions is almost the same as under dry conditions in the 400 L(5000 L)reactor.However,increasing RH can decrease the desorption rates.The average k_(wg)value under dry conditions is 1.45(1.27)times higher than that under humid conditions in the 400 L(5000 L)reactor.The high RH can increase the partitioning equilibrium timescales and enhance the wall losses of OVOCs.