Fe‐based catalysts for the production of light olefins via the Fischer‐Tropsch synthesis were modi‐fied by adding a Zn promoter using both microwave‐hydrothermal and impregnation methods. The physicochemical prope...Fe‐based catalysts for the production of light olefins via the Fischer‐Tropsch synthesis were modi‐fied by adding a Zn promoter using both microwave‐hydrothermal and impregnation methods. The physicochemical properties of the resulting catalysts were determined by scanning electron mi‐croscopy, the Brunauer‐Emmett‐Teller method, X‐ray diffraction, H2 temperature‐programed re‐duction and X‐ray photoelectron spectroscopy. The results demonstrate that the addition of a Zn promoter improves both the light olefin selectivity over the catalyst and the catalyst stability. The catalysts prepared via the impregnation method, which contain greater quantities of surface ZnO, exhibit severe carbon deposition following activity trials. In contrast, those materials synthesized using the microwave‐hydrothermal approach show improved dispersion of Zn and Fe phases and decreased carbon deposition, and so exhibit better CO conversion and stability.展开更多
Co-Cu-based catalysts are widely applied in higher alcohol synthesis (HAS) from synthesis gas. Although the nature of the active sites is still not fully understood, the formation of Co2C under HAS conditions seems to...Co-Cu-based catalysts are widely applied in higher alcohol synthesis (HAS) from synthesis gas. Although the nature of the active sites is still not fully understood, the formation of Co2C under HAS conditions seems to play a major role. A CO pretreatment procedure was developed allowing a systematic investigation of the influence of cobalt carbidization on the structural properties and catalytic performance of the catalysts. By exposing the catalyst to a CO-containing atmosphere prior to HAS, Co enrichment of the catalyst surface occurred followed by carbide formation. This surface modification decreased the formation of hydrocarbons and enhanced the formation of C2+OH. The catalyst pretreated with CO at 20 bar achieved the highest selectivity to ethanol and the lowest hydrocarbon selectivity.展开更多
Solvent-based carbon capture is the most commercially-ready technology for economically and sustainably reaching carbon emission reduction targets in the power sector. Globally, the technology has been deployed to dea...Solvent-based carbon capture is the most commercially-ready technology for economically and sustainably reaching carbon emission reduction targets in the power sector. Globally, the technology has been deployed to deal with flue gases from large scale power plants and different carbon-intensive industries. The success of the technology is due to significant R&D activities on the process development and decades of industrial experience on acid gas removal processes from gaseous mixtures. In this paper, current status of PCC based on chemical absorption--commercial deployment and demonstration projects, analysis of different solvents and process configurations--is reviewed. Although some successes have been recorded in developing this technology, its commercialization has been generally slow as evidenced in the cancellation of high profile projects across the world. This is partly due to the huge cost burden of the technology and unpredictable government policies. Different research directions, namely new process development involving process intensification, new solvent development and a combination of both, are discussed in this paper as possible pathways for reducing the huge cost of the technology.展开更多
Impregnation of isotactic polypropylene (iPP) with nucleating agent (NA21) using supercritical carbon dioxide as the swelling agent at different temperature and pressure and its non-isothermal crystallization kinetics...Impregnation of isotactic polypropylene (iPP) with nucleating agent (NA21) using supercritical carbon dioxide as the swelling agent at different temperature and pressure and its non-isothermal crystallization kinetics were investigated. The results showed that NA21 was dispersed at a nanometer-scale in the PP matrix, resulting in the formation of different typesof crystal phases of iPP and the enhancement of its mechanical properties.展开更多
A series of Zn–Ca–Al oxides with different CaO and ZnO contents have been prepared and evaluated in the synthesis of propylene carbonate(PC) from 1,2-propylene glycol(PG) and urea in a batch reactor. The effect of c...A series of Zn–Ca–Al oxides with different CaO and ZnO contents have been prepared and evaluated in the synthesis of propylene carbonate(PC) from 1,2-propylene glycol(PG) and urea in a batch reactor. The effect of catalyst composition, basicity and reaction process parameters such as temperature, catalyst dose, molar ratio of PG to urea, purge gas flow and reaction time has been studied to find suitable reaction conditions for the PC synthesis. The PC selectivity and yield under the desired conditions could reach 98.4% and 90.8%, respectively. The best performing catalyst also exhibited a good reusability without appreciable loss in the PC selectivity and yield after five consecutive reaction runs. In addition, a stepwise reaction pathway involving a 2-hydroxypropyl carbamate intermediate was proposed for the urea alcoholysis to PC in the presence of Zn–Ca–Al catalysts, according to the time dependences of reaction intermediates and products.展开更多
The idea that single metal atoms dispersed on a solid support can act as an efficient heterogeneous catalyst was raised in2011when single Pt atoms on an FeOx surface were reported to be active for CO oxidation and pre...The idea that single metal atoms dispersed on a solid support can act as an efficient heterogeneous catalyst was raised in2011when single Pt atoms on an FeOx surface were reported to be active for CO oxidation and preferential oxidation of CO in H2.The last six years have witnessed tremendous progress in the field of single‐atom catalysis.Here we introduce the major achievements on this topic in2015and2016.Some particular aspects of single‐atom catalysis are discussed in depth,including new approaches in single‐atom catalyst(SAC)synthesis,stable gold SACs for various reactions,the high selectivity of Pt and Pd SACs in hydrogenation,and the superior performance of non‐noble metal SACs in electrochemistry.These accomplishments will encourage more efforts by researchers to achieve the controllable fabrication of SACs and explore their potential applications.展开更多
Among the current technologies for post-combustion CO2 capture,amine-based chemical absorption appears to be the most technologically mature and commercially viable method.This review highlights the opportunities and ...Among the current technologies for post-combustion CO2 capture,amine-based chemical absorption appears to be the most technologically mature and commercially viable method.This review highlights the opportunities and challenges in post-combustion CO2 capture using amine-based chemical absorption technologies.In addition,this review provides current types and emerging trends for chemical solvents.The issues and performance of amine solvents are reviewed and addressed in terms of thermodynamics,kinetics,mass transfer,regeneration and solvent management.This review also looks at emerging and future trends in post-combustion CO2 capture using chemical solvents in the near to mid-term.展开更多
Pd/LaxPbyMnOz, Pd/C, Pd/molecular sieve and Pd-heteropoly acid catalysts for direct synthesis of diphenyl carbonate (DPC) by heterogeneous catalytic reaction were compared and the results of DPC synthesis indicated th...Pd/LaxPbyMnOz, Pd/C, Pd/molecular sieve and Pd-heteropoly acid catalysts for direct synthesis of diphenyl carbonate (DPC) by heterogeneous catalytic reaction were compared and the results of DPC synthesis indicated that the catalyst Pd/LaxPbyMnOz had higher activity. The Pd/LaxPbyMnOz catalyst and the support was characterized by XRD, SEM and TEM, the main phase was Lao.szPbo.asMnOa and the average diameter could be about 25.4nm. The optimuna conditions for synthesis of DPC with Pd/LasPbyMnOz were determined by orthogonal experiments and the experimental results showed that reaction temperature was the first factor of effect on the selectivity and yield of DPC, and the concentration of O2 in gas phase also had significant effect on selectivity of DPC. The optimum reaction conditions were catalyst/phenol mass ratio l to 50, pressure 4.5MPa, volume concentration of O2 25%, reaction temperature 60℃ and reaction time 4 h. The maximum yield and average selectivity could reach 13% and 97% respectively in the batch operation.展开更多
Catalytic activity of activated carbon supported tungstosilicic acidin synthesizing 2-methyl-2-ethoxycarbonylmethyl- 1,3-dioxolane, 2,4-dimethyl-2-ethoxycarbonylmethyl-1,3-dioxolane, cyclohexanone ethylene ketal, cycl...Catalytic activity of activated carbon supported tungstosilicic acidin synthesizing 2-methyl-2-ethoxycarbonylmethyl- 1,3-dioxolane, 2,4-dimethyl-2-ethoxycarbonylmethyl-1,3-dioxolane, cyclohexanone ethylene ketal, cyclohexanone 1,2-propa- nediol ketal, butanone ethylene ketal, butanone 1,2-propanediol ketal, 2-phenyl-1,3-dioxolane, 4-methyl-2-phenyl-1,3-dioxolane, 2-propyl-1,3-dioxolane, 4-methyl-2-propyl-1,3-dioxolane was reported. It has been demonstrated that activated carbon supported tungstosilicic acid is an excellent catalyst. Various factors involved in these reactions were investigated. The optimum conditions found were: molar ratio of aldehyde/ketone to glycol is 1/1.5, mass ratio of the catalyst used to the reactants is 1.0%, and reaction time is 1.0 h. Under these conditions, the yield of 2-methyl-2-ethoxycarbonylmethyl-1,3-dioxolane is 61.5%, of 2,4-dimethyl- 2-ethoxycarbonylmethyl-1,3-dioxolane is 69.1%, of cyclohexanone ethylene ketal is 74.6%, of cyclohexanone 1,2-propanediol ketal is 80.1%, of butanone ethylene ketal is 69.5%, of butanone 1,2-propanediol ketal is 78.5%, of 2-phenyl-1,3-dioxolane is 56.7%, of 4-methyl-2-phenyl-1,3-dioxolane is 86.2%, of 2-propyl-1,3-dioxolane is 87.5%, of 4-methyl-2-propyl-1,3-dioxolane is 87.9%.展开更多
基金supported by the Key Project of Natural Science Foundation of Ningxia(NZ13010)the National Natural Science Foundation of China(21366025)~~
文摘Fe‐based catalysts for the production of light olefins via the Fischer‐Tropsch synthesis were modi‐fied by adding a Zn promoter using both microwave‐hydrothermal and impregnation methods. The physicochemical properties of the resulting catalysts were determined by scanning electron mi‐croscopy, the Brunauer‐Emmett‐Teller method, X‐ray diffraction, H2 temperature‐programed re‐duction and X‐ray photoelectron spectroscopy. The results demonstrate that the addition of a Zn promoter improves both the light olefin selectivity over the catalyst and the catalyst stability. The catalysts prepared via the impregnation method, which contain greater quantities of surface ZnO, exhibit severe carbon deposition following activity trials. In contrast, those materials synthesized using the microwave‐hydrothermal approach show improved dispersion of Zn and Fe phases and decreased carbon deposition, and so exhibit better CO conversion and stability.
基金funded by the Federal Ministry of Education and Research(Bundesministerium für Bildung und Forschung,BMBF,Verbundvorhaben Carbon2Chem■,FKZ:03EK3041)
文摘Co-Cu-based catalysts are widely applied in higher alcohol synthesis (HAS) from synthesis gas. Although the nature of the active sites is still not fully understood, the formation of Co2C under HAS conditions seems to play a major role. A CO pretreatment procedure was developed allowing a systematic investigation of the influence of cobalt carbidization on the structural properties and catalytic performance of the catalysts. By exposing the catalyst to a CO-containing atmosphere prior to HAS, Co enrichment of the catalyst surface occurred followed by carbide formation. This surface modification decreased the formation of hydrocarbons and enhanced the formation of C2+OH. The catalyst pretreated with CO at 20 bar achieved the highest selectivity to ethanol and the lowest hydrocarbon selectivity.
文摘Solvent-based carbon capture is the most commercially-ready technology for economically and sustainably reaching carbon emission reduction targets in the power sector. Globally, the technology has been deployed to deal with flue gases from large scale power plants and different carbon-intensive industries. The success of the technology is due to significant R&D activities on the process development and decades of industrial experience on acid gas removal processes from gaseous mixtures. In this paper, current status of PCC based on chemical absorption--commercial deployment and demonstration projects, analysis of different solvents and process configurations--is reviewed. Although some successes have been recorded in developing this technology, its commercialization has been generally slow as evidenced in the cancellation of high profile projects across the world. This is partly due to the huge cost burden of the technology and unpredictable government policies. Different research directions, namely new process development involving process intensification, new solvent development and a combination of both, are discussed in this paper as possible pathways for reducing the huge cost of the technology.
基金an International Cooperation Research Program,key project from National Science Foundation of China for multiscale methodology,SINOPEC supported fundamental research project,an Association Franco-Chinoise pour la Recherche Scientifique et Technique(AFCRST) supported project
文摘Impregnation of isotactic polypropylene (iPP) with nucleating agent (NA21) using supercritical carbon dioxide as the swelling agent at different temperature and pressure and its non-isothermal crystallization kinetics were investigated. The results showed that NA21 was dispersed at a nanometer-scale in the PP matrix, resulting in the formation of different typesof crystal phases of iPP and the enhancement of its mechanical properties.
基金Supported by the Changcheng Scholars Program of Beijing(CIT&TCD 20150316)
文摘A series of Zn–Ca–Al oxides with different CaO and ZnO contents have been prepared and evaluated in the synthesis of propylene carbonate(PC) from 1,2-propylene glycol(PG) and urea in a batch reactor. The effect of catalyst composition, basicity and reaction process parameters such as temperature, catalyst dose, molar ratio of PG to urea, purge gas flow and reaction time has been studied to find suitable reaction conditions for the PC synthesis. The PC selectivity and yield under the desired conditions could reach 98.4% and 90.8%, respectively. The best performing catalyst also exhibited a good reusability without appreciable loss in the PC selectivity and yield after five consecutive reaction runs. In addition, a stepwise reaction pathway involving a 2-hydroxypropyl carbamate intermediate was proposed for the urea alcoholysis to PC in the presence of Zn–Ca–Al catalysts, according to the time dependences of reaction intermediates and products.
基金supported by the National Natural Science Foundation of China(21606222,21303184,21573232)China Postdoctoral Science Foundation(2016M601350)+2 种基金Strategic Priority Research Program of the Chinese Academy of Sciences(XDB17020100)National Key Projects for Fundamental Research and Development of China(2016YFA0202801)Department of Science and Technology of Liaoning Province(2015020086-101)~~
文摘The idea that single metal atoms dispersed on a solid support can act as an efficient heterogeneous catalyst was raised in2011when single Pt atoms on an FeOx surface were reported to be active for CO oxidation and preferential oxidation of CO in H2.The last six years have witnessed tremendous progress in the field of single‐atom catalysis.Here we introduce the major achievements on this topic in2015and2016.Some particular aspects of single‐atom catalysis are discussed in depth,including new approaches in single‐atom catalyst(SAC)synthesis,stable gold SACs for various reactions,the high selectivity of Pt and Pd SACs in hydrogenation,and the superior performance of non‐noble metal SACs in electrochemistry.These accomplishments will encourage more efforts by researchers to achieve the controllable fabrication of SACs and explore their potential applications.
基金Supported by the National Natural Science Foundation of China(21276068,U1362112and 21376067,21476064)the National Key Technology R&D Program(2012BAC26B01)+4 种基金Innovative Research Team Development Plan of the Ministry of Education of the People's Republic of China(IRT1238)Specialized Research Fund for the Doctoral Program of Higher Education(20130161110025)Technology Development contract(Shanyan 12-34)Innovative Research Program for Graduate Student of Hunan Province,China(CX2013B158)Key project of international®ional scientific and technological cooperation of Hunan Provincial science and technology plan(2014WK2037)
文摘Among the current technologies for post-combustion CO2 capture,amine-based chemical absorption appears to be the most technologically mature and commercially viable method.This review highlights the opportunities and challenges in post-combustion CO2 capture using amine-based chemical absorption technologies.In addition,this review provides current types and emerging trends for chemical solvents.The issues and performance of amine solvents are reviewed and addressed in terms of thermodynamics,kinetics,mass transfer,regeneration and solvent management.This review also looks at emerging and future trends in post-combustion CO2 capture using chemical solvents in the near to mid-term.
基金National Natural Science Foundation of China(No.20076036Tianjin University C1 National Laboratory Project
文摘Pd/LaxPbyMnOz, Pd/C, Pd/molecular sieve and Pd-heteropoly acid catalysts for direct synthesis of diphenyl carbonate (DPC) by heterogeneous catalytic reaction were compared and the results of DPC synthesis indicated that the catalyst Pd/LaxPbyMnOz had higher activity. The Pd/LaxPbyMnOz catalyst and the support was characterized by XRD, SEM and TEM, the main phase was Lao.szPbo.asMnOa and the average diameter could be about 25.4nm. The optimuna conditions for synthesis of DPC with Pd/LasPbyMnOz were determined by orthogonal experiments and the experimental results showed that reaction temperature was the first factor of effect on the selectivity and yield of DPC, and the concentration of O2 in gas phase also had significant effect on selectivity of DPC. The optimum reaction conditions were catalyst/phenol mass ratio l to 50, pressure 4.5MPa, volume concentration of O2 25%, reaction temperature 60℃ and reaction time 4 h. The maximum yield and average selectivity could reach 13% and 97% respectively in the batch operation.
基金Project supported by the Natural Science Foundation of HubeiProvince Education Committee (No. 2004D007) and the NationalNatural Science Foundation of China (No. 20471044)
文摘Catalytic activity of activated carbon supported tungstosilicic acidin synthesizing 2-methyl-2-ethoxycarbonylmethyl- 1,3-dioxolane, 2,4-dimethyl-2-ethoxycarbonylmethyl-1,3-dioxolane, cyclohexanone ethylene ketal, cyclohexanone 1,2-propa- nediol ketal, butanone ethylene ketal, butanone 1,2-propanediol ketal, 2-phenyl-1,3-dioxolane, 4-methyl-2-phenyl-1,3-dioxolane, 2-propyl-1,3-dioxolane, 4-methyl-2-propyl-1,3-dioxolane was reported. It has been demonstrated that activated carbon supported tungstosilicic acid is an excellent catalyst. Various factors involved in these reactions were investigated. The optimum conditions found were: molar ratio of aldehyde/ketone to glycol is 1/1.5, mass ratio of the catalyst used to the reactants is 1.0%, and reaction time is 1.0 h. Under these conditions, the yield of 2-methyl-2-ethoxycarbonylmethyl-1,3-dioxolane is 61.5%, of 2,4-dimethyl- 2-ethoxycarbonylmethyl-1,3-dioxolane is 69.1%, of cyclohexanone ethylene ketal is 74.6%, of cyclohexanone 1,2-propanediol ketal is 80.1%, of butanone ethylene ketal is 69.5%, of butanone 1,2-propanediol ketal is 78.5%, of 2-phenyl-1,3-dioxolane is 56.7%, of 4-methyl-2-phenyl-1,3-dioxolane is 86.2%, of 2-propyl-1,3-dioxolane is 87.5%, of 4-methyl-2-propyl-1,3-dioxolane is 87.9%.