This article reports the production of COx free hydrogen and carbon nanofibers by the catalytic decomposition of methane over Ni-Al2O3-SiO2 catalysts. The influence of reaction temperature, pretreatment temperature, a...This article reports the production of COx free hydrogen and carbon nanofibers by the catalytic decomposition of methane over Ni-Al2O3-SiO2 catalysts. The influence of reaction temperature, pretreatment temperature, and effect of reductive pretreatment on the decomposition of methane activity is investigated. The physico-chemical characteristics of fresh and deactivated samples were characterized using BET-SA, XRD, TPR, SEM/TEM, CHNS analyses and correlated with the methane decomposition results obtained. The Ni-Al-Si （4 ： 0.5 ： 1.5） catalyst reduced with hydrazine hydrate produced better H2 yields of ca. 1815 mol H2/mol Ni than the catalyst reduced with 5% H2/N2.展开更多
The reduction of carbon emissions in the steel industry is a significant challenge,and utilizing CO_(2) from carbon intensive steel industry off-gases for methanol production is a promising strategy for decarbonizatio...The reduction of carbon emissions in the steel industry is a significant challenge,and utilizing CO_(2) from carbon intensive steel industry off-gases for methanol production is a promising strategy for decarbonization.However,steelwork off-gases typically contain various impurities,including H_(2)S,which can deactivate commercial methanol synthesis catalysts,Cu/ZnO/Al_(2)O_(3)(CZA).Reverse water-gas shift(RWGS)reaction is the predominant side reaction in CO_(2) hydrogenation to methanol which can occur at ambient pressure,enabling the decouple of RWGS from methanol production at high pressure.Then,a series of activated CZA catalysts has been in-situ pretreated in 400 ppm H_(2)S/Ar at 250℃and tested for both RWGS reaction at ambient pressure and CO_(2) hydrogenation to methanol at high pressure.An innovative decoupling strategy was employed to isolate the RWGS reaction from the methanol synthesis process,enabling the investigation of the evolution of active site structures and the poisoning mechanism through elemental analysis,X-ray Diffraction,X-ray Photoelectron Spectroscopy,Fourier Transform Infrared Spectroscopy,Temperature Programmed Reduction and CO_(2) Temperature Programmed Desorption.The results indicate that there are different dynamic migration behaviors of ZnO_(x) in the two reaction systems,leading to different poisoning mechanisms.These interesting findings are beneficial to develop sulfur resistant and durable highly efficient catalysts for CO_(2) hydrogenation to methanol,promoting the carbon emission reduction in steel industry.展开更多
A series of catalysts were prepared by doping different loadings of CeO2 over TiO2-SiO2-WO3 and used for the selective catalytic reduction of NOx by NH3. The experimental results showed that the selective catalytic re...A series of catalysts were prepared by doping different loadings of CeO2 over TiO2-SiO2-WO3 and used for the selective catalytic reduction of NOx by NH3. The experimental results showed that the selective catalytic reduction（SCR） performance and SO2-resistant ability of TiO2-SiO2-WO3 were greatly enhanced by the introduction of cerium. The catalyst containing 10% CeO2 showed the highest NO conversion in a wide temperature range and good N2 selectivity with broad operation temperature window at the gas hourly space velocity（GHSV） of 30000 h–1, which was a very promising catalyst for NOx abatement from diesel engine exhaust. The catalysts were characterized by X-ray diffraction（XRD）, scanning electron microscopy with energy dispersive X-ray spectroscopy（SEM-EDS）, N2 adsorption-desorption（BET） and X-ray photoelectron spectroscopy（XPS）. The characterization results showed that the bigger pore radius, higher surface atomic concentration and dispersion of Ce and the abundant adsorbed oxygen on the surface of catalyst contributed to the best NH3-SCR performance of CeO2/TiO2-SiO2-WO3 catalyst containing 10% CeO2.展开更多
Ni/Al_2O_3-SiO_2 catalysts were synthesized via one-step method employing SiO_2 as an additive for the selective hydrogenation of butyne-1,4-diol(B_3D) to butane-1,4-diol(B1D). The prepared catalysts were evaluated by...Ni/Al_2O_3-SiO_2 catalysts were synthesized via one-step method employing SiO_2 as an additive for the selective hydrogenation of butyne-1,4-diol(B_3D) to butane-1,4-diol(B1D). The prepared catalysts were evaluated by a series of characterization techniques including BET, XRD, SEM, EDX-mapping, TEM, H_2-TPR, XPS, NH_3-TPD and Py-FTIR. Compared to Ni/Al_2O_3 catalyst, the SiO_2-doped samples exhibited better B_3D conversion. SiO_2 could help to form a strong interaction between NiO with the support, which inhibited Ni agglomeration at high temperature, improved the Ni dispersion, and enhanced the hydrogenation activity. B_1D selectivity was mainly influenced by the quantity of Lewis acid sites in addition to the Ni dispersion. The catalyst with a silica loading of 6.4% demonstrated an excellent selectivity of 75.18%(by 13% higher than the contrastive Ni/Al_2O_3 catalyst), which was attributed to the larger amount of Lewis acid sites and the moderate interaction between NiO with the support, which could facilitate the nickel dispersion on a preferable surface area of 176.3 m^2/g of support.展开更多
The Ni-Al2O3 catalyst was prepared by the mechanochemical method in combination with a planetary ballmilling machine.Effect of milling time on the crystal structure,the reduction characteristics and the catalytic perf...The Ni-Al2O3 catalyst was prepared by the mechanochemical method in combination with a planetary ballmilling machine.Effect of milling time on the crystal structure,the reduction characteristics and the catalytic performance of Ni-Al2O3 catalyst for hydrogenation of 1,4-butynediol to produce 1,4-butenediol were investigated.The catalysts were characterized by PSD,EDX,XRD,H2-TPR,BET,TEM,and NH3-TPD methods.Results showed that the MCt2.5 catalyst treated at a ball milling time of 2.5 h could form a smallest particle size of 191.0 nm.The evaluation experiments revealed that the activity of the prepared catalyst increased at first and then reached a constant value with the extension of ballmilling time.The BYD conversion,BED selectivity and yield on the MCt2.5 catalyst reached 35.63%,33.48%and 32.46%,respectively,which were higher than those obtained by other samples.The excellent performance of MCt2.5 sample is mainly related to the following three reasons from characterization results.Firstly,it has a smallest particle size of 191.0 nm;and then,the surface acidity(in terms of strong acids)of the catalyst was weaker than other catalysts;and eventually,the loading amount(23.84%)of the active component Ni exceeded the theoretical value(20%).展开更多
The crystallization behavior and kinetics of CaO-MgO-Al2O3 SiO2（CMAS） glass with the Fe2O3 content ranging from zero to 5%were investigated by differential scanning calorimetry（DSC）.The structure and phase analyse...The crystallization behavior and kinetics of CaO-MgO-Al2O3 SiO2（CMAS） glass with the Fe2O3 content ranging from zero to 5%were investigated by differential scanning calorimetry（DSC）.The structure and phase analyses were made by Fourier transform infrared spectroscopy（FT-IR） and X-ray diffraction（XRD）.The experiment results show that the endothermic peak temperature about 760℃ is associated with transition and the exothermic peak temperature about 1000℃ is associated with crystallization.The crystallization peak temperature decreases with increasing the Fe203 content.The crystallization mechanism is changed from two-dimensional crystallization to one-dimensional growth,and the intensity of diopside peaks becomes stronger gradually.There is a saltation for the crystallization temperature with the addition of 0.5%Fe2O3 due to the decomposition of Fe2O3.Si-O-Si,O-Si-O and T-O-T（T=Si,Fe,Al） linkages are observed in Fe2O3-CaO-MgO-Al2O3-SiO2 glass.展开更多
文摘This article reports the production of COx free hydrogen and carbon nanofibers by the catalytic decomposition of methane over Ni-Al2O3-SiO2 catalysts. The influence of reaction temperature, pretreatment temperature, and effect of reductive pretreatment on the decomposition of methane activity is investigated. The physico-chemical characteristics of fresh and deactivated samples were characterized using BET-SA, XRD, TPR, SEM/TEM, CHNS analyses and correlated with the methane decomposition results obtained. The Ni-Al-Si （4 ： 0.5 ： 1.5） catalyst reduced with hydrazine hydrate produced better H2 yields of ca. 1815 mol H2/mol Ni than the catalyst reduced with 5% H2/N2.
基金supported by the National Natural Science Foundation of China(Nos.22276060 and 21976059)Guangdong Basic and Applied Basic Research Foundation(No.2024A1515012636)China Scholarship Council Scholarship(No.201906155006)。
文摘The reduction of carbon emissions in the steel industry is a significant challenge,and utilizing CO_(2) from carbon intensive steel industry off-gases for methanol production is a promising strategy for decarbonization.However,steelwork off-gases typically contain various impurities,including H_(2)S,which can deactivate commercial methanol synthesis catalysts,Cu/ZnO/Al_(2)O_(3)(CZA).Reverse water-gas shift(RWGS)reaction is the predominant side reaction in CO_(2) hydrogenation to methanol which can occur at ambient pressure,enabling the decouple of RWGS from methanol production at high pressure.Then,a series of activated CZA catalysts has been in-situ pretreated in 400 ppm H_(2)S/Ar at 250℃and tested for both RWGS reaction at ambient pressure and CO_(2) hydrogenation to methanol at high pressure.An innovative decoupling strategy was employed to isolate the RWGS reaction from the methanol synthesis process,enabling the investigation of the evolution of active site structures and the poisoning mechanism through elemental analysis,X-ray Diffraction,X-ray Photoelectron Spectroscopy,Fourier Transform Infrared Spectroscopy,Temperature Programmed Reduction and CO_(2) Temperature Programmed Desorption.The results indicate that there are different dynamic migration behaviors of ZnO_(x) in the two reaction systems,leading to different poisoning mechanisms.These interesting findings are beneficial to develop sulfur resistant and durable highly efficient catalysts for CO_(2) hydrogenation to methanol,promoting the carbon emission reduction in steel industry.
基金supported by the National Natural Science Foundation of China(21173153)the National High Technology Research and Development Program of China(863 project)(2013AA065304)
文摘A series of catalysts were prepared by doping different loadings of CeO2 over TiO2-SiO2-WO3 and used for the selective catalytic reduction of NOx by NH3. The experimental results showed that the selective catalytic reduction（SCR） performance and SO2-resistant ability of TiO2-SiO2-WO3 were greatly enhanced by the introduction of cerium. The catalyst containing 10% CeO2 showed the highest NO conversion in a wide temperature range and good N2 selectivity with broad operation temperature window at the gas hourly space velocity（GHSV） of 30000 h–1, which was a very promising catalyst for NOx abatement from diesel engine exhaust. The catalysts were characterized by X-ray diffraction（XRD）, scanning electron microscopy with energy dispersive X-ray spectroscopy（SEM-EDS）, N2 adsorption-desorption（BET） and X-ray photoelectron spectroscopy（XPS）. The characterization results showed that the bigger pore radius, higher surface atomic concentration and dispersion of Ce and the abundant adsorbed oxygen on the surface of catalyst contributed to the best NH3-SCR performance of CeO2/TiO2-SiO2-WO3 catalyst containing 10% CeO2.
基金Financial support from the National Natural Science Foundation of China (21163019) is gratefully acknowledged
文摘Ni/Al_2O_3-SiO_2 catalysts were synthesized via one-step method employing SiO_2 as an additive for the selective hydrogenation of butyne-1,4-diol(B_3D) to butane-1,4-diol(B1D). The prepared catalysts were evaluated by a series of characterization techniques including BET, XRD, SEM, EDX-mapping, TEM, H_2-TPR, XPS, NH_3-TPD and Py-FTIR. Compared to Ni/Al_2O_3 catalyst, the SiO_2-doped samples exhibited better B_3D conversion. SiO_2 could help to form a strong interaction between NiO with the support, which inhibited Ni agglomeration at high temperature, improved the Ni dispersion, and enhanced the hydrogenation activity. B_1D selectivity was mainly influenced by the quantity of Lewis acid sites in addition to the Ni dispersion. The catalyst with a silica loading of 6.4% demonstrated an excellent selectivity of 75.18%(by 13% higher than the contrastive Ni/Al_2O_3 catalyst), which was attributed to the larger amount of Lewis acid sites and the moderate interaction between NiO with the support, which could facilitate the nickel dispersion on a preferable surface area of 176.3 m^2/g of support.
基金This work has been supported by the Xinjiang Uygur Autonomous Region Key R&D Program(2017B02012)the Xinjiang University Natural Science Foundation Project(BS160221).
文摘The Ni-Al2O3 catalyst was prepared by the mechanochemical method in combination with a planetary ballmilling machine.Effect of milling time on the crystal structure,the reduction characteristics and the catalytic performance of Ni-Al2O3 catalyst for hydrogenation of 1,4-butynediol to produce 1,4-butenediol were investigated.The catalysts were characterized by PSD,EDX,XRD,H2-TPR,BET,TEM,and NH3-TPD methods.Results showed that the MCt2.5 catalyst treated at a ball milling time of 2.5 h could form a smallest particle size of 191.0 nm.The evaluation experiments revealed that the activity of the prepared catalyst increased at first and then reached a constant value with the extension of ballmilling time.The BYD conversion,BED selectivity and yield on the MCt2.5 catalyst reached 35.63%,33.48%and 32.46%,respectively,which were higher than those obtained by other samples.The excellent performance of MCt2.5 sample is mainly related to the following three reasons from characterization results.Firstly,it has a smallest particle size of 191.0 nm;and then,the surface acidity(in terms of strong acids)of the catalyst was weaker than other catalysts;and eventually,the loading amount(23.84%)of the active component Ni exceeded the theoretical value(20%).
基金Projects(51264023,51364020,U1202271)supported by the National Natural Science Foundation of ChinaProject(IRT1250)supported by the Program for Innovative Research Team in University of Ministry of Education of ChinaProject(2014HA003)supported by the Science and Technology Leading Talent of Yunnan Province,China
文摘The crystallization behavior and kinetics of CaO-MgO-Al2O3 SiO2（CMAS） glass with the Fe2O3 content ranging from zero to 5%were investigated by differential scanning calorimetry（DSC）.The structure and phase analyses were made by Fourier transform infrared spectroscopy（FT-IR） and X-ray diffraction（XRD）.The experiment results show that the endothermic peak temperature about 760℃ is associated with transition and the exothermic peak temperature about 1000℃ is associated with crystallization.The crystallization peak temperature decreases with increasing the Fe203 content.The crystallization mechanism is changed from two-dimensional crystallization to one-dimensional growth,and the intensity of diopside peaks becomes stronger gradually.There is a saltation for the crystallization temperature with the addition of 0.5%Fe2O3 due to the decomposition of Fe2O3.Si-O-Si,O-Si-O and T-O-T（T=Si,Fe,Al） linkages are observed in Fe2O3-CaO-MgO-Al2O3-SiO2 glass.
