Abstract： In order to improve the reactivity of Na2CO3/Al2O3 sorbent with CO2, a new sorbent showing high reactivity was developed by doping Na2CO3/Al2O3 with TiO2 using impregnation. Fourteen multi-cycle carbonation...Abstract： In order to improve the reactivity of Na2CO3/Al2O3 sorbent with CO2, a new sorbent showing high reactivity was developed by doping Na2CO3/Al2O3 with TiO2 using impregnation. Fourteen multi-cycle carbonation/regeneration tests of the sorbent were carried out in a fluidized-bed reactor and the sorbent was characterized by X-ray diffraction and nitrogen adsorption. It is confirmed that TiO2 shows a positive effect on the adsorption process of Na2CO3 and the reaction rate is observed to increase significantly, especially in the first 10 min. Moreover, TiO2 is stable within the temperature range of the process and no other Ti-compounds are detected. The carbonation products are NaHCO3 and Na5H3 （CO3 ）4. The surface area and the pore volume of the sorbent keep stable after 14 cycles. The Fourier transform infrared spectroscopy and the X-ray photoelectron spectroscopy are used to analyze the effect mechanism of TiO2 on CO2 adsorption process of Na2CO3/Al2O3.展开更多
Spinning disk reactor(SDR)has emerged as a novel process intensification photocatalytic reactor,and it has higher mass transfer efficiency and photon utilization for the degradation of toxic organic pollutants by adva...Spinning disk reactor(SDR)has emerged as a novel process intensification photocatalytic reactor,and it has higher mass transfer efficiency and photon utilization for the degradation of toxic organic pollutants by advanced oxidation processes(AOPs).In this study,ZnO—TiO_(2)nanocomposites were prepared by solgel method,and coated on the disk of SDR by impregnation-pull-drying-calcination method.The performance of catalyst was characterized by X-ray diffraction,scanning electron microscope,X-ray photoelectron spectroscopy,photoluminescence and ultraviolet—visible diffuse reflectance spectroscopy.Photocatalytic ozonation in SDR was used to remove phenol,and various factors on degradation effect were studied in detail.The results showed that the rate of degradation and mineralization reached 100%and 83.4%under UV light irradiation after 50 min,compared with photocatalysis and ozonation,the removal rate increased by 69.3%and 34.7%,and mineralization rate increased by 56.7%and 62.9%,which indicated that the coupling of photocatalysis and ozonation had a synergistic effect.The radical capture experiments demonstrated that the active species such as photogenerated holes(h^(+)),hydroxyl radicals(·OH),superoxide radical(·O_(2)-)were responsible for phenol degradation,and·OH played a leading role in the degradation process,while h+and·O_(2)^(-)played a non-leading role.展开更多
A two-stage catalytic membrane reactor(CMR)that couples CO_(2) splitting with methane oxidation reactions was constructed based on an oxygen-permeable perovskite asymmetric membrane.The asymmetric membrane comprises a...A two-stage catalytic membrane reactor(CMR)that couples CO_(2) splitting with methane oxidation reactions was constructed based on an oxygen-permeable perovskite asymmetric membrane.The asymmetric membrane comprises a dense SrFe_(0.9)Ta_(0.1)O_(3-σ)(SFT)separation layer and a porous Sr_(0.9)(Fe_(0.9)Ta_(0.1))_(0.9)Cu_(0.1)O_(3-σ)(SFTC)catalytic layer.In thefirst stage reactor,a CO_(2) splitting reaction(CDS:2CO_(2)→2CO+O_(2))occurs at the SFTC catalytic layer.Subsequently,the O_(2) product is selectively extracted through the SFT separation layer to the permeated side for the methane combustion reaction(MCR),which provides an extremely low oxygen partial pressure to enhance the oxygen extraction.In the second stage,a Sr_(0.9)(Fe_(0.9)Ta_(0.1))_(0.9)Ni_(0.1)O_(3-σ)(SFTN)catalyst is employed to reform the products derived from MCR.The two-stage CMR design results in a remarkable 35.4%CO_(2) conversion for CDS at 900℃.The two-stage CMR was extended to a hollowfiber configuration combining with solar irradiation.The solar-assisted two-stage CMR can operate stably for over 50 h with a high hydrogen yield of 18.1 mL min^(-1) cm^(-2).These results provide a novel strategy for reducing CO_(2) emissions,suggesting potential avenues for the design of the high-performance CMRs and catalysts based on perovskite oxides in the future.展开更多
The development of efficient systems for the catalytic oxidation of 2-nitro-4-methylsulfonyltoluene(NMST)to 2-nitro-4-methylsulfonyl benzoic acid(NMSBA)with atmospheric air or molecular oxygen in alkaline medium prese...The development of efficient systems for the catalytic oxidation of 2-nitro-4-methylsulfonyltoluene(NMST)to 2-nitro-4-methylsulfonyl benzoic acid(NMSBA)with atmospheric air or molecular oxygen in alkaline medium presents a significant challenge for the chemical industry.Here,we report the synthesis of FeOOH/Fe_(3)O_(4)/metal-organic framework(MOF)polygonal mesopores microflower templated from a MIL-88B(Fe)at room temperature,which exposes polygonal mesopores with atomistic edge steps and lattice defects.The obtained FeOOH/Fe_(3)O_(4)/MOF catalyst was adsorbed onto glass beads and then introduced into the microchannel reactor.In the alkaline environment,oxygen was used as oxidant to catalyze the oxidation of NMST to NMSBA,showing impressive performance.This sustainable system utilizes oxygen as a clean oxidant in an inexpensive and environmentally friendly NaOH/methanol mixture.The position and type of substituent critically affect the products.Additionally,this sustainable protocol enabled gram-scale preparation of carboxylic acid and benzyl alcohol derivatives with high chemoselectivities.Finally,the reactions can be conducted in a pressure reactor,which can conserve oxygen and prevent solvent loss.Moreover,compared with the traditional batch reactor,the self-built microchannel reactor can accelerate the reaction rate,shorten the reaction time,and enhance the selectivity of catalytic oxidation reactions.This approach contributes to environmental protection and holds potential for industrial applications.展开更多
The study of scale up for the oxidative coupling of methane （OCM） has been carried out in a 200 ml stainless steel fixed-bed reactor over a 5wt% Na2WO4-1.9wt% Mn/SiO2 （W-Mn/SiO2） catalyst. The effects of reaction ...The study of scale up for the oxidative coupling of methane （OCM） has been carried out in a 200 ml stainless steel fixed-bed reactor over a 5wt% Na2WO4-1.9wt% Mn/SiO2 （W-Mn/SiO2） catalyst. The effects of reaction conditions were investigated in detail. The results showed that, with increasing reaction temperature, the gas-phase reaction was enhanced and a significant amount of methane was converted into COx; with the CH4/O2 molar ratio of 5, the highest C2 （ethylene and ethane） yield of 25% was achieved; the presence of steam （as diluent） had a positive effect on the C2 selectivity and yield. Under lower methane gaseous hourly space velocity （GHSV）, higher selectivity and yield of C2 were obtained as the result of the decrease of released heat energy. In 100 h reaction time, the C2 selectivity of 66%-61% and C2 yield of 24.2%-25.4% were achieved by a single pass without any significant loss in catalytic performance.展开更多
基金The National Natural Science Foundation of China(No.51476030)the Specialized Research Fund for the Doctoral Program of Higher Education(No.20130092110006)
文摘Abstract： In order to improve the reactivity of Na2CO3/Al2O3 sorbent with CO2, a new sorbent showing high reactivity was developed by doping Na2CO3/Al2O3 with TiO2 using impregnation. Fourteen multi-cycle carbonation/regeneration tests of the sorbent were carried out in a fluidized-bed reactor and the sorbent was characterized by X-ray diffraction and nitrogen adsorption. It is confirmed that TiO2 shows a positive effect on the adsorption process of Na2CO3 and the reaction rate is observed to increase significantly, especially in the first 10 min. Moreover, TiO2 is stable within the temperature range of the process and no other Ti-compounds are detected. The carbonation products are NaHCO3 and Na5H3 （CO3 ）4. The surface area and the pore volume of the sorbent keep stable after 14 cycles. The Fourier transform infrared spectroscopy and the X-ray photoelectron spectroscopy are used to analyze the effect mechanism of TiO2 on CO2 adsorption process of Na2CO3/Al2O3.
基金supported by the National Natural Science Foundation of China(22208328)Fundamental Research Program of Shanxi Province(20210302124618,202203021212134)。
文摘Spinning disk reactor(SDR)has emerged as a novel process intensification photocatalytic reactor,and it has higher mass transfer efficiency and photon utilization for the degradation of toxic organic pollutants by advanced oxidation processes(AOPs).In this study,ZnO—TiO_(2)nanocomposites were prepared by solgel method,and coated on the disk of SDR by impregnation-pull-drying-calcination method.The performance of catalyst was characterized by X-ray diffraction,scanning electron microscope,X-ray photoelectron spectroscopy,photoluminescence and ultraviolet—visible diffuse reflectance spectroscopy.Photocatalytic ozonation in SDR was used to remove phenol,and various factors on degradation effect were studied in detail.The results showed that the rate of degradation and mineralization reached 100%and 83.4%under UV light irradiation after 50 min,compared with photocatalysis and ozonation,the removal rate increased by 69.3%and 34.7%,and mineralization rate increased by 56.7%and 62.9%,which indicated that the coupling of photocatalysis and ozonation had a synergistic effect.The radical capture experiments demonstrated that the active species such as photogenerated holes(h^(+)),hydroxyl radicals(·OH),superoxide radical(·O_(2)-)were responsible for phenol degradation,and·OH played a leading role in the degradation process,while h+and·O_(2)^(-)played a non-leading role.
基金supported by the National Key Research and Development Program of China(2022YFE0101600)the National Natural Science Foundation of China(U23A20117)+2 种基金the Natural Science Foundation of Jiangsu Province(BK20220002,BE2022024)the Leading Talents Program of Zhejiang Province(2024C03223)Topnotch Academic Programs Project of Jiangsu Higher Education Institutions(TAPP).
文摘A two-stage catalytic membrane reactor(CMR)that couples CO_(2) splitting with methane oxidation reactions was constructed based on an oxygen-permeable perovskite asymmetric membrane.The asymmetric membrane comprises a dense SrFe_(0.9)Ta_(0.1)O_(3-σ)(SFT)separation layer and a porous Sr_(0.9)(Fe_(0.9)Ta_(0.1))_(0.9)Cu_(0.1)O_(3-σ)(SFTC)catalytic layer.In thefirst stage reactor,a CO_(2) splitting reaction(CDS:2CO_(2)→2CO+O_(2))occurs at the SFTC catalytic layer.Subsequently,the O_(2) product is selectively extracted through the SFT separation layer to the permeated side for the methane combustion reaction(MCR),which provides an extremely low oxygen partial pressure to enhance the oxygen extraction.In the second stage,a Sr_(0.9)(Fe_(0.9)Ta_(0.1))_(0.9)Ni_(0.1)O_(3-σ)(SFTN)catalyst is employed to reform the products derived from MCR.The two-stage CMR design results in a remarkable 35.4%CO_(2) conversion for CDS at 900℃.The two-stage CMR was extended to a hollowfiber configuration combining with solar irradiation.The solar-assisted two-stage CMR can operate stably for over 50 h with a high hydrogen yield of 18.1 mL min^(-1) cm^(-2).These results provide a novel strategy for reducing CO_(2) emissions,suggesting potential avenues for the design of the high-performance CMRs and catalysts based on perovskite oxides in the future.
基金supported by the National Natural Science Foundation of China(22078251)Hubei Province Key Research and Development Program(2023DJC167)the research project of Hubei Provincial Department of Education(D20191504).
文摘The development of efficient systems for the catalytic oxidation of 2-nitro-4-methylsulfonyltoluene(NMST)to 2-nitro-4-methylsulfonyl benzoic acid(NMSBA)with atmospheric air or molecular oxygen in alkaline medium presents a significant challenge for the chemical industry.Here,we report the synthesis of FeOOH/Fe_(3)O_(4)/metal-organic framework(MOF)polygonal mesopores microflower templated from a MIL-88B(Fe)at room temperature,which exposes polygonal mesopores with atomistic edge steps and lattice defects.The obtained FeOOH/Fe_(3)O_(4)/MOF catalyst was adsorbed onto glass beads and then introduced into the microchannel reactor.In the alkaline environment,oxygen was used as oxidant to catalyze the oxidation of NMST to NMSBA,showing impressive performance.This sustainable system utilizes oxygen as a clean oxidant in an inexpensive and environmentally friendly NaOH/methanol mixture.The position and type of substituent critically affect the products.Additionally,this sustainable protocol enabled gram-scale preparation of carboxylic acid and benzyl alcohol derivatives with high chemoselectivities.Finally,the reactions can be conducted in a pressure reactor,which can conserve oxygen and prevent solvent loss.Moreover,compared with the traditional batch reactor,the self-built microchannel reactor can accelerate the reaction rate,shorten the reaction time,and enhance the selectivity of catalytic oxidation reactions.This approach contributes to environmental protection and holds potential for industrial applications.
文摘The study of scale up for the oxidative coupling of methane （OCM） has been carried out in a 200 ml stainless steel fixed-bed reactor over a 5wt% Na2WO4-1.9wt% Mn/SiO2 （W-Mn/SiO2） catalyst. The effects of reaction conditions were investigated in detail. The results showed that, with increasing reaction temperature, the gas-phase reaction was enhanced and a significant amount of methane was converted into COx; with the CH4/O2 molar ratio of 5, the highest C2 （ethylene and ethane） yield of 25% was achieved; the presence of steam （as diluent） had a positive effect on the C2 selectivity and yield. Under lower methane gaseous hourly space velocity （GHSV）, higher selectivity and yield of C2 were obtained as the result of the decrease of released heat energy. In 100 h reaction time, the C2 selectivity of 66%-61% and C2 yield of 24.2%-25.4% were achieved by a single pass without any significant loss in catalytic performance.
