In this study,a trifunctional strategy was developed to prepare a confined Ni-based catalyst(Ni-CeO_(2)@SiO_(2))for dry reforming of methane(DRM)of two main greenhouse gases-CO_(2)and CH_(4).The Ni-CeO_(2)@SiO_(2)cata...In this study,a trifunctional strategy was developed to prepare a confined Ni-based catalyst(Ni-CeO_(2)@SiO_(2))for dry reforming of methane(DRM)of two main greenhouse gases-CO_(2)and CH_(4).The Ni-CeO_(2)@SiO_(2)catalyst was fabricated by utilizing the confinement effect of the SiO_(2)shell and the synergistic interaction between Ni-Ce and the decoking effect of CeO_(2).The catalysts were systematically characterized via X-ray diffraction,N_(2 )adsorption/desorption,transmission electron microscopy,energy dispersive X-ray spectroscopy,hydrogen temperature reduction and desorption set by program,oxygen temperature program desorption,Raman spectroscopy,thermogravimetric analysis,and in situ diffuse reflectance infrared Fourier transform spectroscopy measurements to reveal their physicochemical properties and reaction mechanism.The Ni-CeO_(2)@SiO_(2)catalyst exhibited higher activity and stability than the catalyst synthesized via the traditional impregnation method.In addition,no carbon deposition was detected over Ni-CeO_(2)@SiO_(2)after a 100 h durability test at 800℃,and the average particle size of Ni nanoparticles(NPs)in the catalyst increased from 5.01 to 5.77 nm.Remarkably,Ni-CeO_(2)@SiO_(2)also exhibited superior low-temperature stability;no coke deposition was observed when the catalyst was reacted at 600℃ for 20 h.The high coking and sintering resistance of this confined Ni-based DRM catalyst can be attributed to its trifunctional effect.The trifunctional strategy developed in this study could be used as a guideline to design other high-performance catalysts for CO_(2)and CH4 dry forming and accelerate their industrialization.展开更多
We report the investigation on the low-temperature oxidation of cyclohexane in a jet-stirred reactor over 500-742 K. Synchrotron vacuum ultraviolet photoionization mass spectrometry （SVUV-PIMS） was used for identify...We report the investigation on the low-temperature oxidation of cyclohexane in a jet-stirred reactor over 500-742 K. Synchrotron vacuum ultraviolet photoionization mass spectrometry （SVUV-PIMS） was used for identifying and quantifying the oxidation species. Major products, cyclic olefins, and oxygenated products including reactive hydroperoxides and high oxygen compounds were detected. Compared with n-alkanes, a narrow low-temperature window （-80 K） was observed in the low-temperature oxidation of cyclohexane. Besides, a kinetic model for cyclohexane oxidation was developed based on the CNRS model [Combust. Flame 160, 2319 （2013）], which can better capture the experimental results than previous models. Based on the modeling analysis, the 1,5-H shift dominates the crucial isomerization steps of the first and second O2 addition products in the low-temperature chain branching process of cyclohexane. The negative temperature coefficient behavior of cyclohexane oxidation results from the reduced chain branching due to the competition from chain inhibition and propagation reactions, i.e. the reaction between cyclohexyl radical and O2 and the de- composition of cyclohexylperoxy radical, both producing cyclohexene and HO2 radical, as well as the decomposition of cyclohexylhydroperoxy radical producing hex-5-en-l-al and OH radical.展开更多
A stable hierarchical porous metal-organic framework PCN-56 with abundant Lewis acid sites(denoted as Defective-PCN-56) was synthesized by the low-temperature synthesis-induced defect formation method.The existence of...A stable hierarchical porous metal-organic framework PCN-56 with abundant Lewis acid sites(denoted as Defective-PCN-56) was synthesized by the low-temperature synthesis-induced defect formation method.The existence of mesopore in structure was confirmed by N2 sorption isotherm and the successful encapsulation of large dye molecules.The Defective-PCN-56 has higher loading capacity toward anti-cancer drug Doxo compared with that of "nearly ideal-crystal"(denoted as Ideal-PCN-56)synthesized at high temperature,showing potential application as drug carrier.The low-temperature synthesis-induced defect formation strategy presented here provides a new and facile way to synthesize stable MOFs with the combination of intrinsic micropore and additional mesopore as well as abundant Lewis acid sites.展开更多
The metallurgical sewage has very complex component and a significant environmental perniciousness and needs high treatment costs. In addition, too much low-temperature waste heat is emitted owing to the lack of suita...The metallurgical sewage has very complex component and a significant environmental perniciousness and needs high treatment costs. In addition, too much low-temperature waste heat is emitted owing to the lack of suitable users. Considering these concerns, a low-temperature-driven pretreatment method via vacuum distillation was proposed to treat the sewage from the metallurgical production. It uses the sensible heat carried by low-temperature exhausted gases to drive the distillation of sewage. The distilled water can be reused into the process as new water supply, while the enriched wastewater is discharged into the sewage treatment center for subsequent treatment. Converter dust removal sewage was chosen to perform an experimental observation. The variations of chemical oxygen demand, ammonia nitrogen, suspended solids, electrical conductivity, and pH of the condensate under different vacuum degrees and evaporation rates were mainly investigated. It can be found that the quality of the condensate gets better under certain conditions, which validates the feasibility of the proposed approach. Furthermore, by comprehensively analyzing the water quality indices and their influencing factors, the optimal vacuum degree was suggested to be controlled between 0.07 and 0.09 MPa, and the best evaporation rate was between 40 and 60%.展开更多
文摘In this study,a trifunctional strategy was developed to prepare a confined Ni-based catalyst(Ni-CeO_(2)@SiO_(2))for dry reforming of methane(DRM)of two main greenhouse gases-CO_(2)and CH_(4).The Ni-CeO_(2)@SiO_(2)catalyst was fabricated by utilizing the confinement effect of the SiO_(2)shell and the synergistic interaction between Ni-Ce and the decoking effect of CeO_(2).The catalysts were systematically characterized via X-ray diffraction,N_(2 )adsorption/desorption,transmission electron microscopy,energy dispersive X-ray spectroscopy,hydrogen temperature reduction and desorption set by program,oxygen temperature program desorption,Raman spectroscopy,thermogravimetric analysis,and in situ diffuse reflectance infrared Fourier transform spectroscopy measurements to reveal their physicochemical properties and reaction mechanism.The Ni-CeO_(2)@SiO_(2)catalyst exhibited higher activity and stability than the catalyst synthesized via the traditional impregnation method.In addition,no carbon deposition was detected over Ni-CeO_(2)@SiO_(2)after a 100 h durability test at 800℃,and the average particle size of Ni nanoparticles(NPs)in the catalyst increased from 5.01 to 5.77 nm.Remarkably,Ni-CeO_(2)@SiO_(2)also exhibited superior low-temperature stability;no coke deposition was observed when the catalyst was reacted at 600℃ for 20 h.The high coking and sintering resistance of this confined Ni-based DRM catalyst can be attributed to its trifunctional effect.The trifunctional strategy developed in this study could be used as a guideline to design other high-performance catalysts for CO_(2)and CH4 dry forming and accelerate their industrialization.
基金supported by the National Natural Science Foundation of China(No.91641205,No.51622605,No.91541201)the Shanghai Science and Technology Committee(No.17XD1402000)
文摘We report the investigation on the low-temperature oxidation of cyclohexane in a jet-stirred reactor over 500-742 K. Synchrotron vacuum ultraviolet photoionization mass spectrometry （SVUV-PIMS） was used for identifying and quantifying the oxidation species. Major products, cyclic olefins, and oxygenated products including reactive hydroperoxides and high oxygen compounds were detected. Compared with n-alkanes, a narrow low-temperature window （-80 K） was observed in the low-temperature oxidation of cyclohexane. Besides, a kinetic model for cyclohexane oxidation was developed based on the CNRS model [Combust. Flame 160, 2319 （2013）], which can better capture the experimental results than previous models. Based on the modeling analysis, the 1,5-H shift dominates the crucial isomerization steps of the first and second O2 addition products in the low-temperature chain branching process of cyclohexane. The negative temperature coefficient behavior of cyclohexane oxidation results from the reduced chain branching due to the competition from chain inhibition and propagation reactions, i.e. the reaction between cyclohexyl radical and O2 and the de- composition of cyclohexylperoxy radical, both producing cyclohexene and HO2 radical, as well as the decomposition of cyclohexylhydroperoxy radical producing hex-5-en-l-al and OH radical.
基金financially supported by National Natural Science Foundation of China (NSFC,No.21871267)the Science and Technology Research Program of Chongqing Municipal Education Commission (No.KJQN201801602)+1 种基金the Key Laboratory for Green Chemical Technology of Chongqing University of Education (No.2016xjpt08)the Young Teachers’ Growth Plan of Chongqing University of Education (No.YX-2019-01)
文摘A stable hierarchical porous metal-organic framework PCN-56 with abundant Lewis acid sites(denoted as Defective-PCN-56) was synthesized by the low-temperature synthesis-induced defect formation method.The existence of mesopore in structure was confirmed by N2 sorption isotherm and the successful encapsulation of large dye molecules.The Defective-PCN-56 has higher loading capacity toward anti-cancer drug Doxo compared with that of "nearly ideal-crystal"(denoted as Ideal-PCN-56)synthesized at high temperature,showing potential application as drug carrier.The low-temperature synthesis-induced defect formation strategy presented here provides a new and facile way to synthesize stable MOFs with the combination of intrinsic micropore and additional mesopore as well as abundant Lewis acid sites.
基金This work was sponsored by the National Natural Science Foundation of China （51734004, 21561122001）, the China Scholarship Council （201702660037） and the Fundamental Research Funds for the China Central Universities （N162504011）.
文摘The metallurgical sewage has very complex component and a significant environmental perniciousness and needs high treatment costs. In addition, too much low-temperature waste heat is emitted owing to the lack of suitable users. Considering these concerns, a low-temperature-driven pretreatment method via vacuum distillation was proposed to treat the sewage from the metallurgical production. It uses the sensible heat carried by low-temperature exhausted gases to drive the distillation of sewage. The distilled water can be reused into the process as new water supply, while the enriched wastewater is discharged into the sewage treatment center for subsequent treatment. Converter dust removal sewage was chosen to perform an experimental observation. The variations of chemical oxygen demand, ammonia nitrogen, suspended solids, electrical conductivity, and pH of the condensate under different vacuum degrees and evaporation rates were mainly investigated. It can be found that the quality of the condensate gets better under certain conditions, which validates the feasibility of the proposed approach. Furthermore, by comprehensively analyzing the water quality indices and their influencing factors, the optimal vacuum degree was suggested to be controlled between 0.07 and 0.09 MPa, and the best evaporation rate was between 40 and 60%.
