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
The isothermal phase diagram of the Cu2O-Al2O3-SiO2 ternary system at 1150℃ was reported for the samples which were prepared from sol-gel method and quenched by water after being heated at 1150℃ for 12 h. Based on t...The isothermal phase diagram of the Cu2O-Al2O3-SiO2 ternary system at 1150℃ was reported for the samples which were prepared from sol-gel method and quenched by water after being heated at 1150℃ for 12 h. Based on the conventional X-ray powder diffraction （XRD） and in situ high-temperature XRD quantitative analysis,in addition to scanning electron microscopy measurement,the phase identification was achieved. Combining the deduction from the component phase diagrams of the binary systems using the phase equilibrium theorem,the primary isothermal phase diagram was plotted over the composition area Cu2O-mullite-SiO2. In this area,the approximate composition areas of two two-phase regions and one three-phase region,（L2＋Cr）,（L2＋M）,and （L1＋L2＋Tr）,were determined. Moreover,the precise composition areas of both of the three-phase regions （L2＋Cr＋M） and （L2＋M＋A） were determined according to the results of conventional and in situ high-temperature XRD quantitative analysis by Rietveld method.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
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the National Natural Science Foundation of China (No. 20471010)the Scien-tific Research Fund of Hunan Provincial Education Department (No. 05c173).
文摘The isothermal phase diagram of the Cu2O-Al2O3-SiO2 ternary system at 1150℃ was reported for the samples which were prepared from sol-gel method and quenched by water after being heated at 1150℃ for 12 h. Based on the conventional X-ray powder diffraction （XRD） and in situ high-temperature XRD quantitative analysis,in addition to scanning electron microscopy measurement,the phase identification was achieved. Combining the deduction from the component phase diagrams of the binary systems using the phase equilibrium theorem,the primary isothermal phase diagram was plotted over the composition area Cu2O-mullite-SiO2. In this area,the approximate composition areas of two two-phase regions and one three-phase region,（L2＋Cr）,（L2＋M）,and （L1＋L2＋Tr）,were determined. Moreover,the precise composition areas of both of the three-phase regions （L2＋Cr＋M） and （L2＋M＋A） were determined according to the results of conventional and in situ high-temperature XRD quantitative analysis by Rietveld method.
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.
