Catalysts that can rapidly degrade tetracycline(TC)in water without introducing secondary ion pollution have always been challenging.Herein,a cobalt-based catalyst(CoO_(x)@P-C)is prepared so that CoOx quantum particle...Catalysts that can rapidly degrade tetracycline(TC)in water without introducing secondary ion pollution have always been challenging.Herein,a cobalt-based catalyst(CoO_(x)@P-C)is prepared so that CoOx quantum particles(5e10 nm)are uniformly distributed on a linear substrate,and the outer layer is covered with a shell(P-C).The quantum particles of CoO_(x) provide many active sites for the reaction,which ensures the efficient degradation effect of the catalyst,and 30 mg/L TC can be completely degraded in only 5 min.The shell of the quantum particles'outer layer can effectively reduce ions'extravasation.The combination of the shell-like structure and the linear substrate greatly enhances the catalysis's stability and ensures that the catalyst is prepared into a film for practical application.The high catalytic activity of CoO_(x)@P-C is mainly due to the following factors:(1)Uniformly distributed ultra-small nanoparticles can provide many active sites.(2)The microenvironment formed by the core-shell structure enhances not only catalytic stability but also provides the driving force to improve the reaction rate.(3)The composite of CoO_(x) and P-C core-shell structure can accelerate electron transfer and generate many reactive oxygen species in a short time,which makes TC degrade extremely rapidly.展开更多
In this paper,a series of cobalt catalysts supported on reduced graphene oxide(rGO)nanosheets with the loading of 5,15 and 30 wt-%were provided by the impregnation method.The activity of the prepared catalysts is eval...In this paper,a series of cobalt catalysts supported on reduced graphene oxide(rGO)nanosheets with the loading of 5,15 and 30 wt-%were provided by the impregnation method.The activity of the prepared catalysts is evaluated in the Fischer-Tropsch synthesis(FTS).The prepared catalysts were carefully characterized by nitrogen adsorption-desorption,hydrogen chemisorption,X-ray diffraction,Fourier transform infrared spectroscopy,Raman spectroscopy,temperature programmed reduction,transmission electron microscopy,and field emission scanning electron microscopy techniques to confirm that cobalt particles were greatly dispersed on the rGO nanosheets.The results showed that with increasing the cobalt loading on the rGO support,the carbon defects are increased and as a consequence,the reduction of cobalt is decreased.The FTS activity results showed that the cobalt-time yield and turnover frequency passed from a maximum for catalyst with the Co0 average particle size of 15 nm due to the synergetic effect of cobalt reducibility and particle size.The products selectivity results indicated that the methane selectivity decreases,whereas the C5+selectivity raises with the increasing of the cobalt particle size,which can be explained by chain propagation in the primary chain growth reactions.展开更多
Particle coating is an important method that can be used to expand particle-technology applications. Coated-particle design and preparation for nuclear fuel-element trajectory tracing were focused on in this paper. Pa...Particle coating is an important method that can be used to expand particle-technology applications. Coated-particle design and preparation for nuclear fuel-element trajectory tracing were focused on in this paper. Particles that contain elemental cobalt were selected because of the characteristic gamma ray spectra of 60Co. A novel particle-structure design was proposed by coating particles that contain elemental cobalt with a high-density silicon-carbide (SiC) layer. During the coating process with the high-density SiC layer, cobalt metal was formed and diffused towards the coating, so an inner SiC–CoxSi layer was designed and obtained by fluidized-bed chemical vapor deposition coupled with in-situ chemical reaction. The coating layers were studied by X-ray diffractometry, scanning electron microscopy, and energy dispersive X-ray spectroscopy techniques. The chemical composition was also determined by inductively coupled plasma optical emission spectrometry. The novel particle design can reduce the formation of metallic cobalt and prevent cobalt diffusion in the coating process, which can maintain safety in a nuclear reactor for an extended period. The experimental results also validated that coated particles maintain their structural integrity at extremely high temperatures (~1950 °C), which meets the requirements of next-generation nuclear reactors.展开更多
基金supported by the Joint Funds of the National Natural Science Foundation of China(U22A20140),the Independent Cultivation Program of Innovation Team of Ji'nan City(No.2019GXRC011),the Natural Science Foundation of Shandong Province(Grant No.ZR2021ME143,ZR2021MA073)and National Natural Science Foundation of China(Grant No.51908242)and.All the authors discussed the results and commented on the manuscript.
文摘Catalysts that can rapidly degrade tetracycline(TC)in water without introducing secondary ion pollution have always been challenging.Herein,a cobalt-based catalyst(CoO_(x)@P-C)is prepared so that CoOx quantum particles(5e10 nm)are uniformly distributed on a linear substrate,and the outer layer is covered with a shell(P-C).The quantum particles of CoO_(x) provide many active sites for the reaction,which ensures the efficient degradation effect of the catalyst,and 30 mg/L TC can be completely degraded in only 5 min.The shell of the quantum particles'outer layer can effectively reduce ions'extravasation.The combination of the shell-like structure and the linear substrate greatly enhances the catalysis's stability and ensures that the catalyst is prepared into a film for practical application.The high catalytic activity of CoO_(x)@P-C is mainly due to the following factors:(1)Uniformly distributed ultra-small nanoparticles can provide many active sites.(2)The microenvironment formed by the core-shell structure enhances not only catalytic stability but also provides the driving force to improve the reaction rate.(3)The composite of CoO_(x) and P-C core-shell structure can accelerate electron transfer and generate many reactive oxygen species in a short time,which makes TC degrade extremely rapidly.
基金The authors of this work appreciate the financial support of the Ferdowsi University of Mashhad,Iran(Grant No.3/45803-29/9/96).
文摘In this paper,a series of cobalt catalysts supported on reduced graphene oxide(rGO)nanosheets with the loading of 5,15 and 30 wt-%were provided by the impregnation method.The activity of the prepared catalysts is evaluated in the Fischer-Tropsch synthesis(FTS).The prepared catalysts were carefully characterized by nitrogen adsorption-desorption,hydrogen chemisorption,X-ray diffraction,Fourier transform infrared spectroscopy,Raman spectroscopy,temperature programmed reduction,transmission electron microscopy,and field emission scanning electron microscopy techniques to confirm that cobalt particles were greatly dispersed on the rGO nanosheets.The results showed that with increasing the cobalt loading on the rGO support,the carbon defects are increased and as a consequence,the reduction of cobalt is decreased.The FTS activity results showed that the cobalt-time yield and turnover frequency passed from a maximum for catalyst with the Co0 average particle size of 15 nm due to the synergetic effect of cobalt reducibility and particle size.The products selectivity results indicated that the methane selectivity decreases,whereas the C5+selectivity raises with the increasing of the cobalt particle size,which can be explained by chain propagation in the primary chain growth reactions.
基金This work was supported by the Natural Science Foundation of China (Grant Nos. S1302148, 21306097), the Research Fund for Independent Research Projects of Tsinghua University (Grant Nos. 20131089217, 20121088038), the Specialized Research Fund for the Doctoral Program of Higher Education (Grant No. 20110002120023), and the Higher Education Young Elite Teacher Project of Beijing (Grant No. YETP0155).
文摘Particle coating is an important method that can be used to expand particle-technology applications. Coated-particle design and preparation for nuclear fuel-element trajectory tracing were focused on in this paper. Particles that contain elemental cobalt were selected because of the characteristic gamma ray spectra of 60Co. A novel particle-structure design was proposed by coating particles that contain elemental cobalt with a high-density silicon-carbide (SiC) layer. During the coating process with the high-density SiC layer, cobalt metal was formed and diffused towards the coating, so an inner SiC–CoxSi layer was designed and obtained by fluidized-bed chemical vapor deposition coupled with in-situ chemical reaction. The coating layers were studied by X-ray diffractometry, scanning electron microscopy, and energy dispersive X-ray spectroscopy techniques. The chemical composition was also determined by inductively coupled plasma optical emission spectrometry. The novel particle design can reduce the formation of metallic cobalt and prevent cobalt diffusion in the coating process, which can maintain safety in a nuclear reactor for an extended period. The experimental results also validated that coated particles maintain their structural integrity at extremely high temperatures (~1950 °C), which meets the requirements of next-generation nuclear reactors.