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
The development of novel porous materials have attracted significant attention owing to its possible application in several fields.In this study,we designed a novel covalent organic framework‐metal‐organic framework...The development of novel porous materials have attracted significant attention owing to its possible application in several fields.In this study,we designed a novel covalent organic framework‐metal‐organic framework(COF‐MOF)material through an in‐situ ligand self‐assembly method.The in‐situ modified ligands not only act as nucleation sites to form Ti‐MOF,but also as a channel to rapidly transfer photogenerated electrons without introducing additional chemical bonds.The photocatalytic hydrogen production rate achieved over B‐CTF‐Ti‐MOF(1:1)was 1975μmol·g^(–1)·h^(–1) with an apparent quantum efficiency of 4.76%,which is 11.8 times higher than that of the pure CTF‐1.In addition,compared with the sample prepared by separating the ligands(CTF‐1/Ti‐MOF),B‐CTF‐Ti‐MOF shows excellent activity and stability.Finally,a reasonable photocatalytic mechanism was proposed using the results of electrochemical tests and spectral analyses.This study provides a universal method for the construction of highly efficient and stable COF/MOF materials with excellent properties.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.
文摘The development of novel porous materials have attracted significant attention owing to its possible application in several fields.In this study,we designed a novel covalent organic framework‐metal‐organic framework(COF‐MOF)material through an in‐situ ligand self‐assembly method.The in‐situ modified ligands not only act as nucleation sites to form Ti‐MOF,but also as a channel to rapidly transfer photogenerated electrons without introducing additional chemical bonds.The photocatalytic hydrogen production rate achieved over B‐CTF‐Ti‐MOF(1:1)was 1975μmol·g^(–1)·h^(–1) with an apparent quantum efficiency of 4.76%,which is 11.8 times higher than that of the pure CTF‐1.In addition,compared with the sample prepared by separating the ligands(CTF‐1/Ti‐MOF),B‐CTF‐Ti‐MOF shows excellent activity and stability.Finally,a reasonable photocatalytic mechanism was proposed using the results of electrochemical tests and spectral analyses.This study provides a universal method for the construction of highly efficient and stable COF/MOF materials with excellent properties.
