Methanol synthesis from hydrogenation of CO2 is investigated over Cu/ZnO/Al2O3 catalysts prepared by decomposition of M（Cu,Zn）-ammonia complexes （DMAC） at various temperatures.The catalysts were characterized in d...Methanol synthesis from hydrogenation of CO2 is investigated over Cu/ZnO/Al2O3 catalysts prepared by decomposition of M（Cu,Zn）-ammonia complexes （DMAC） at various temperatures.The catalysts were characterized in detail,including X-ray diffraction,N2 adsorption-desorption,N2O chemisorption,temperature-programmed reduction and evolved gas analyses.The influences of DMAC temperature,reaction temperature and specific Cu surface area on catalytic performance are investigated.It is considered that the aurichalcite phase in the precursor plays a key role in improving the physiochemical properties and activities of the final catalysts.The catalyst from rich-aurichalcite precursor exhibits large specific Cu surface area and high space time yield of methanol （212 g/（Lcat·h）;T=513 K,p=3MPa,SV=12000 h-1）.展开更多
A number of nanostructured carbon materials were proposed as new effective promoters for preparing modified Cu/ZnO/Al 2O 3 catalyst system for efficient hydrogen production from methanol steam reforming. Compared to t...A number of nanostructured carbon materials were proposed as new effective promoters for preparing modified Cu/ZnO/Al 2O 3 catalyst system for efficient hydrogen production from methanol steam reforming. Compared to the catalysts modified by other type of carbon materials, the ACF-promoted catalyst prepared via carbonate-coprecipitation method exhibit the highest performance in the low-temperature steam reforming of methanol. It was suggested that the intrinsic high surface area nature of ACF material may favor the generation of modified catalysts with a high surface area and improved component dispersion, thus leading to improved performance for methanol steam reforming.展开更多
The synthesis of methanol and dimethyl ether(DME) from CO hydrogenation has been investigated on Cu-based catalysts.A series of Cu/ZnO/Al2O3 catalysts were prepared using a solvent-free routine which involved a direct...The synthesis of methanol and dimethyl ether(DME) from CO hydrogenation has been investigated on Cu-based catalysts.A series of Cu/ZnO/Al2O3 catalysts were prepared using a solvent-free routine which involved a direct blend of copper/zinc/aluminum salts and citric acid,followed by calcination at 450 °C.The calcination processes were monitored using thermogravimetry differential scanning calorimetry(TG-DSC).Catalysts were further characterized using N2 adsorption,scanning electronic microscopy(SEM),X-ray diffraction(XRD),N2O oxidation followed by H2 titration,and temperature-programmed reduction with H2(H2-TPR).The reduction processes were also monitored with in-situ XRD.The physicochemical properties of catalysts depended strongly on the types of precursor salts,and catalysts prepared using Al acetate and Cu nitrate as starting materials had a larger surface area,larger exposed metallic copper surface area,and lower reduction temperature.The CO hydrogenation performances of these catalysts were compared and discussed in terms of their structures.Catalysts prepared with copper nitrate,zinc and aluminum acetates exhibited the highest catalytic activity.展开更多
The induction behavior in CO2 hydrogenation was studied by varying the reaction temperature to investigate the adaptation of the Cu/ZnO/Al2O3 catalyst to the temperature change. The results indicated that a used catal...The induction behavior in CO2 hydrogenation was studied by varying the reaction temperature to investigate the adaptation of the Cu/ZnO/Al2O3 catalyst to the temperature change. The results indicated that a used catalyst had a tendency to keep the last running state in new reaction conditions for MeOH formation, and that this tendency was related to the difference in Cu/Cun+ ratio caused by CO2 and CO produced at different reaction temperatures. However, the reverse water-gas shift reaction (RWGS) induced at four temperatures was completely different from that of methanol synthesis. It implied that the two so-called competitive reactions in CO2+H2, RWGS and methanol synthesis, have different active centers.展开更多
基金supported by the National Basic Research Program of China (No. 2011CB201404)the financial support of the State Key Laboratory for Oxo Synthesis and Selective Oxidation (OSSO) of China
文摘Methanol synthesis from hydrogenation of CO2 is investigated over Cu/ZnO/Al2O3 catalysts prepared by decomposition of M（Cu,Zn）-ammonia complexes （DMAC） at various temperatures.The catalysts were characterized in detail,including X-ray diffraction,N2 adsorption-desorption,N2O chemisorption,temperature-programmed reduction and evolved gas analyses.The influences of DMAC temperature,reaction temperature and specific Cu surface area on catalytic performance are investigated.It is considered that the aurichalcite phase in the precursor plays a key role in improving the physiochemical properties and activities of the final catalysts.The catalyst from rich-aurichalcite precursor exhibits large specific Cu surface area and high space time yield of methanol （212 g/（Lcat·h）;T=513 K,p=3MPa,SV=12000 h-1）.
文摘A number of nanostructured carbon materials were proposed as new effective promoters for preparing modified Cu/ZnO/Al 2O 3 catalyst system for efficient hydrogen production from methanol steam reforming. Compared to the catalysts modified by other type of carbon materials, the ACF-promoted catalyst prepared via carbonate-coprecipitation method exhibit the highest performance in the low-temperature steam reforming of methanol. It was suggested that the intrinsic high surface area nature of ACF material may favor the generation of modified catalysts with a high surface area and improved component dispersion, thus leading to improved performance for methanol steam reforming.
基金supported by the National Natural Science Foundation of China (Nos. 21073159 and 90610002)the National Basic Research Program (973) of China (No. 2007CB210207)the Zhejiang Provincial Natural Science Foundation of China (No. Z406142)
文摘The synthesis of methanol and dimethyl ether(DME) from CO hydrogenation has been investigated on Cu-based catalysts.A series of Cu/ZnO/Al2O3 catalysts were prepared using a solvent-free routine which involved a direct blend of copper/zinc/aluminum salts and citric acid,followed by calcination at 450 °C.The calcination processes were monitored using thermogravimetry differential scanning calorimetry(TG-DSC).Catalysts were further characterized using N2 adsorption,scanning electronic microscopy(SEM),X-ray diffraction(XRD),N2O oxidation followed by H2 titration,and temperature-programmed reduction with H2(H2-TPR).The reduction processes were also monitored with in-situ XRD.The physicochemical properties of catalysts depended strongly on the types of precursor salts,and catalysts prepared using Al acetate and Cu nitrate as starting materials had a larger surface area,larger exposed metallic copper surface area,and lower reduction temperature.The CO hydrogenation performances of these catalysts were compared and discussed in terms of their structures.Catalysts prepared with copper nitrate,zinc and aluminum acetates exhibited the highest catalytic activity.
基金supported by the National Natural Science Foundation of China(50772107)National Key Basic Research Program of China(973)(2007CB210206)National High-Tech Research and Development Program of China(863)(2009AA05Z435)~~
文摘The induction behavior in CO2 hydrogenation was studied by varying the reaction temperature to investigate the adaptation of the Cu/ZnO/Al2O3 catalyst to the temperature change. The results indicated that a used catalyst had a tendency to keep the last running state in new reaction conditions for MeOH formation, and that this tendency was related to the difference in Cu/Cun+ ratio caused by CO2 and CO produced at different reaction temperatures. However, the reverse water-gas shift reaction (RWGS) induced at four temperatures was completely different from that of methanol synthesis. It implied that the two so-called competitive reactions in CO2+H2, RWGS and methanol synthesis, have different active centers.
