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
Environmental awareness and a growing demand for efficient resource utilization encourage the realization of lubricant-free forming processes. A first step in accomplishing dry sheet metal forming is to gain knowledge...Environmental awareness and a growing demand for efficient resource utilization encourage the realization of lubricant-free forming processes. A first step in accomplishing dry sheet metal forming is to gain knowledge about the changing tribological conditions and to identify the relevant influencing parameters. The commonly used flat strip drawing test was selected to investigate the tribological conditions in the flange area of deep drawing processes. The influencing factors of contact pressure and varying drawing velocities were analyzed under dry and lubricated conditions. Additionally,the tool and workpiece surfaces were characterized. Besides lubrication, the contact pressure mainly determines the tribological conditions. In lubricated tests higher normal pressure reduces friction, whereas without lubrication higher pressure results in slightly increasing friction. A changing drawing velocity affects the friction when lubricant is applied. In dry experiments, no influence of velocity was found. Results of surface characterization reveal adhesion as main wear mechanism under dry conditions. Based on the investigated influence of the process parameters, an increase in process understanding for dry forming operations is derived.展开更多
Ni nanocatalysts produced through exsolution have shown strong resistance to particle sintering and carbon coking in a beneficial dry reforming of methane(DRM)reaction utilizing greenhouse gases such as CH_(4)and CO_(...Ni nanocatalysts produced through exsolution have shown strong resistance to particle sintering and carbon coking in a beneficial dry reforming of methane(DRM)reaction utilizing greenhouse gases such as CH_(4)and CO_(2).However,most of the existing oxide supports for exsolution have been limited to perovskite oxide,while studies on fluorite support have been rarely conducted due to the limited solubility despite its excellent redox stability.Here we demonstrate that 3 mol%Ni can be successfully dissolved into the yttria-stabilized zirconia(YSZ)lattice and be further exsolved to the surface in a reducing atmosphere.The YSZ decorated with exsolved Ni nanoparticles shows enhanced catalytic activity for DRM reaction compared to the conventional cermet type of bulk Ni-YSZ.Moreover,the catalytic activity is extremely stable for about 300 h without significant degradation.Overall results suggest that the YSZ-based fluorite structure can be utilized as one of the support oxides for exsolution.展开更多
To reduce the usage of classical lubricants in deep drawing,a new tribological system based on volatile lubricants was developed.Therefore,a volatile medium is injected under high pressure into the interstice between ...To reduce the usage of classical lubricants in deep drawing,a new tribological system based on volatile lubricants was developed.Therefore,a volatile medium is injected under high pressure into the interstice between drawing tool and sheet metal.Depending on temperature and pressure,the temporary lubricant may exist in its gaseous or liquid phase.In this study,a novel high fluid pressure tribometer was designed to investigate the friction and wear of dry steel contacts under comparable conditions like in dry deep drawing.Therefore,a new ball-on-disc tribometer was designed and integrated into a high-pressure vessel.To specifically investigate the effects of different environments(technical air,liquid and gaseous carbon dioxide,nitrogen,argon)at atmospheric and high pressure(0.1 MPa,6 MPa)on tribology,the specimens and all components were operating unlubricated.During the experiments,the friction was measured continuously.Results show that the highest friction occurs in air and the lowest in carbon dioxide environment.Subsequent to the experiments,the wear of the specimens was assessed along with changes in surface chemistry related to tribochemical reactions.Therefore,the tribology of the dry sliding contacts is correlated to changes of the surface chemistry.Also differences as well as similarities regarding the different fluid environments are shown.As the results show,the differences between the media used are most pronounced at elevated pressure.Concluding,this work gives clear indications on the suitability of volatile lubricants in dry friction or rather gas lubrication,especially for dry deep drawing.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the German Research Foundation (DFG) for supporting the present investigations by funding the SPP 1676 project ME 2043/43-1
文摘Environmental awareness and a growing demand for efficient resource utilization encourage the realization of lubricant-free forming processes. A first step in accomplishing dry sheet metal forming is to gain knowledge about the changing tribological conditions and to identify the relevant influencing parameters. The commonly used flat strip drawing test was selected to investigate the tribological conditions in the flange area of deep drawing processes. The influencing factors of contact pressure and varying drawing velocities were analyzed under dry and lubricated conditions. Additionally,the tool and workpiece surfaces were characterized. Besides lubrication, the contact pressure mainly determines the tribological conditions. In lubricated tests higher normal pressure reduces friction, whereas without lubrication higher pressure results in slightly increasing friction. A changing drawing velocity affects the friction when lubricant is applied. In dry experiments, no influence of velocity was found. Results of surface characterization reveal adhesion as main wear mechanism under dry conditions. Based on the investigated influence of the process parameters, an increase in process understanding for dry forming operations is derived.
基金This work was supported by the Korea Institute of Energy Technology Evaluation and Planning(KETEP)and the Ministry of Trade,Industry&Energy(MOTIE)of the Republic of Korea(No.20173020032120)This work also was supported by the Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(NRF-2019R1C1C1005801)Partial support from“CO2 utilization battery for hydrogen production based on fault-tolerance deep learning”(1.200097.01)is also acknowledged.
文摘Ni nanocatalysts produced through exsolution have shown strong resistance to particle sintering and carbon coking in a beneficial dry reforming of methane(DRM)reaction utilizing greenhouse gases such as CH_(4)and CO_(2).However,most of the existing oxide supports for exsolution have been limited to perovskite oxide,while studies on fluorite support have been rarely conducted due to the limited solubility despite its excellent redox stability.Here we demonstrate that 3 mol%Ni can be successfully dissolved into the yttria-stabilized zirconia(YSZ)lattice and be further exsolved to the surface in a reducing atmosphere.The YSZ decorated with exsolved Ni nanoparticles shows enhanced catalytic activity for DRM reaction compared to the conventional cermet type of bulk Ni-YSZ.Moreover,the catalytic activity is extremely stable for about 300 h without significant degradation.Overall results suggest that the YSZ-based fluorite structure can be utilized as one of the support oxides for exsolution.
文摘To reduce the usage of classical lubricants in deep drawing,a new tribological system based on volatile lubricants was developed.Therefore,a volatile medium is injected under high pressure into the interstice between drawing tool and sheet metal.Depending on temperature and pressure,the temporary lubricant may exist in its gaseous or liquid phase.In this study,a novel high fluid pressure tribometer was designed to investigate the friction and wear of dry steel contacts under comparable conditions like in dry deep drawing.Therefore,a new ball-on-disc tribometer was designed and integrated into a high-pressure vessel.To specifically investigate the effects of different environments(technical air,liquid and gaseous carbon dioxide,nitrogen,argon)at atmospheric and high pressure(0.1 MPa,6 MPa)on tribology,the specimens and all components were operating unlubricated.During the experiments,the friction was measured continuously.Results show that the highest friction occurs in air and the lowest in carbon dioxide environment.Subsequent to the experiments,the wear of the specimens was assessed along with changes in surface chemistry related to tribochemical reactions.Therefore,the tribology of the dry sliding contacts is correlated to changes of the surface chemistry.Also differences as well as similarities regarding the different fluid environments are shown.As the results show,the differences between the media used are most pronounced at elevated pressure.Concluding,this work gives clear indications on the suitability of volatile lubricants in dry friction or rather gas lubrication,especially for dry deep drawing.