Compared to reforming reactions using hydrocarbons,ethanol steam reforming(ESR)is a sustainable alternative for hydrogen(H_(2))production since ethanol can be produced sustainably using biomass.This work explores the ...Compared to reforming reactions using hydrocarbons,ethanol steam reforming(ESR)is a sustainable alternative for hydrogen(H_(2))production since ethanol can be produced sustainably using biomass.This work explores the catalyst design strategies for preparing the Ni supported on ZSM-5 zeolite catalysts to promote ESR.Specifically,two-dimensional ZSM-5 nanosheet and conventional ZSM-5 crystal were used as the catalyst carriers and two synthesis strategies,i.e.,in situ encapsulation and wet impregnation method,were employed to prepare the catalysts.Based on the comparative characterization of the catalysts and comparative catalytic assessments,it was found that the combination of the in situ encapsulation synthesis and the ZSM-5 nanosheet carrier was the effective strategy to develop catalysts for promoting H_(2) production via ESR due to the improved mass transfer(through the 2-D structure of ZSM-5 nanosheet)and formation of confined small Ni nanoparticles(resulted via the in situ encapsulation synthesis).In addition,the resulting ZSM-5 nanosheet supported Ni catalyst also showed high Ni dispersion and high accessibility to Ni sites by the reactants,being able to improve the activity and stability of catalysts and suppress metal sintering and coking during ESR at high reaction temperatures.Thus,the Ni supported on ZSM-5 nanosheet catalyst prepared by encapsulation showed the stable performance with~88% ethanol conversion and~65% H_(2) yield achieved during a 48-h longevity test at 550-C.展开更多
A series of P/HZSM-5 catalysts prepared by impregnation method were used for ethanol conversion to lower olefins. The catalysts were characterized by X-ray diffraction （XRD）, NH3-temperature-programmed desorption （...A series of P/HZSM-5 catalysts prepared by impregnation method were used for ethanol conversion to lower olefins. The catalysts were characterized by X-ray diffraction （XRD）, NH3-temperature-programmed desorption （NH3-TPD） and N2 adsorption-desorption measurements. It was found that the P/HZSM-5 catalysts showed high activity and selectivity toward light olefins. The selectivities of propylene and butylene can be improved with the introduction of phosphorus （P）. When the content of P reached 3.0 wt%, more than 18.9% propylene in the gaseous products was obtained over the P/HZSM-5 catalyst at 450 ？C. The introduction of P modified the strong Br？nsted acid sites of the original HZSM-5 catalysts and P/HZSM-5 catalysts could resist coke formation and showed good stability.展开更多
The coke deposition on HZSM-5/SAPO-34 composite catalysts has been studied in the conversion of ethanol to propylene. The HZSM-5/SAPO-34 composite catalysts were synthesized by hydrothermal method（ZS-HS） and fully b...The coke deposition on HZSM-5/SAPO-34 composite catalysts has been studied in the conversion of ethanol to propylene. The HZSM-5/SAPO-34 composite catalysts were synthesized by hydrothermal method（ZS-HS） and fully blending（ZS-MM）. The used catalysts were characterized by XRD, N;adsorption–desorption, TGA, TPO, elemental analysis, FTIR and XPS. The coking kinetics on both ZS-HS and ZS-MM has been investigated and their coking rate equations were obtained. The used ZS-MM catalyst had higher amount of coke and lower nC:nHthan the used ZS-HS. 90% of the coke was deposited in the micropores of ZS-HS, while almost 45% of the coke located in the micropores of ZS-MM. The coke deposited on ZS-HS catalyst was mainly graphite-like carbon species, whereas dehydrogenated coke species was the major on ZS-MM. The coking activation energy of ZS-MM was lower than that of ZS-HS, and the coking rate on ZS-MM was faster than on ZS-HS. In addition, the regeneration of ZS-MM catalyst showed that it had a good hydrothermal stability. The differences on coking behaviors on the two catalysts were due to their different acidic properties and textures.展开更多
A series of Fe/HZSM-5 catalysts with different iron loadings were prepared by impregnation method.Characterization was performed by N2 adsorption-desorption,X-ray diffraction（XRD）,NH3 temperature-programmed desorpt...A series of Fe/HZSM-5 catalysts with different iron loadings were prepared by impregnation method.Characterization was performed by N2 adsorption-desorption,X-ray diffraction（XRD）,NH3 temperature-programmed desorption（NH3-TPD）,temperature-programmed reduction （TPR）,temperature-programmed oxidation（TPO）and thermogravimetry（TG）analysis.Iron content in the synthesized samples varied from 1.1 wt%to 20 wt%.The obtained samples have been used for ethanol conversion into light olefins.It was found that the amount of strong acidity at 300 -5 50-C on Fe-modified samples was decreased,going with another new acid site appearance at 550- 600-C and that Fe/HZSM-5 catalysts were highly selective towards light olefins,especially the 9FZ sample.In addition,Fe-modified catalysts suppressed the conversion of ethanol to aromatics and paraffins and enhanced their anti-carbon deposit ability.展开更多
基金funding from the European Union's Horizon 2020 Research and Innovation Program(872102)P.S.thanks the Science Achievement Scholarship of Thailand(SAST)for her research secondment at The University of Manchester.Y.J.thanks the National Natural Science Foundation of China(22378407)for funding.
文摘Compared to reforming reactions using hydrocarbons,ethanol steam reforming(ESR)is a sustainable alternative for hydrogen(H_(2))production since ethanol can be produced sustainably using biomass.This work explores the catalyst design strategies for preparing the Ni supported on ZSM-5 zeolite catalysts to promote ESR.Specifically,two-dimensional ZSM-5 nanosheet and conventional ZSM-5 crystal were used as the catalyst carriers and two synthesis strategies,i.e.,in situ encapsulation and wet impregnation method,were employed to prepare the catalysts.Based on the comparative characterization of the catalysts and comparative catalytic assessments,it was found that the combination of the in situ encapsulation synthesis and the ZSM-5 nanosheet carrier was the effective strategy to develop catalysts for promoting H_(2) production via ESR due to the improved mass transfer(through the 2-D structure of ZSM-5 nanosheet)and formation of confined small Ni nanoparticles(resulted via the in situ encapsulation synthesis).In addition,the resulting ZSM-5 nanosheet supported Ni catalyst also showed high Ni dispersion and high accessibility to Ni sites by the reactants,being able to improve the activity and stability of catalysts and suppress metal sintering and coking during ESR at high reaction temperatures.Thus,the Ni supported on ZSM-5 nanosheet catalyst prepared by encapsulation showed the stable performance with~88% ethanol conversion and~65% H_(2) yield achieved during a 48-h longevity test at 550-C.
基金supported by the Doctor Fund of Science Research of Xinjiang University (Grant No. BS060101)the National Natural ScienceFoundation of China (Grant No. 20963010)
文摘A series of P/HZSM-5 catalysts prepared by impregnation method were used for ethanol conversion to lower olefins. The catalysts were characterized by X-ray diffraction （XRD）, NH3-temperature-programmed desorption （NH3-TPD） and N2 adsorption-desorption measurements. It was found that the P/HZSM-5 catalysts showed high activity and selectivity toward light olefins. The selectivities of propylene and butylene can be improved with the introduction of phosphorus （P）. When the content of P reached 3.0 wt%, more than 18.9% propylene in the gaseous products was obtained over the P/HZSM-5 catalyst at 450 ？C. The introduction of P modified the strong Br？nsted acid sites of the original HZSM-5 catalysts and P/HZSM-5 catalysts could resist coke formation and showed good stability.
基金support for this work from National Ministry of Education(No.NCET-10-878)Shaanxi Province(No.2011ZKC4-08,2009ZDKG-70)Northwest University(10YSY08)
文摘The coke deposition on HZSM-5/SAPO-34 composite catalysts has been studied in the conversion of ethanol to propylene. The HZSM-5/SAPO-34 composite catalysts were synthesized by hydrothermal method（ZS-HS） and fully blending（ZS-MM）. The used catalysts were characterized by XRD, N;adsorption–desorption, TGA, TPO, elemental analysis, FTIR and XPS. The coking kinetics on both ZS-HS and ZS-MM has been investigated and their coking rate equations were obtained. The used ZS-MM catalyst had higher amount of coke and lower nC:nHthan the used ZS-HS. 90% of the coke was deposited in the micropores of ZS-HS, while almost 45% of the coke located in the micropores of ZS-MM. The coke deposited on ZS-HS catalyst was mainly graphite-like carbon species, whereas dehydrogenated coke species was the major on ZS-MM. The coking activation energy of ZS-MM was lower than that of ZS-HS, and the coking rate on ZS-MM was faster than on ZS-HS. In addition, the regeneration of ZS-MM catalyst showed that it had a good hydrothermal stability. The differences on coking behaviors on the two catalysts were due to their different acidic properties and textures.
基金supported by the National Natural Science Foundation of China(No.20963010)the Doctor Fund of Science Research(No.070267)
文摘A series of Fe/HZSM-5 catalysts with different iron loadings were prepared by impregnation method.Characterization was performed by N2 adsorption-desorption,X-ray diffraction（XRD）,NH3 temperature-programmed desorption（NH3-TPD）,temperature-programmed reduction （TPR）,temperature-programmed oxidation（TPO）and thermogravimetry（TG）analysis.Iron content in the synthesized samples varied from 1.1 wt%to 20 wt%.The obtained samples have been used for ethanol conversion into light olefins.It was found that the amount of strong acidity at 300 -5 50-C on Fe-modified samples was decreased,going with another new acid site appearance at 550- 600-C and that Fe/HZSM-5 catalysts were highly selective towards light olefins,especially the 9FZ sample.In addition,Fe-modified catalysts suppressed the conversion of ethanol to aromatics and paraffins and enhanced their anti-carbon deposit ability.
