A series of modifiedγ-Al_2O_3supported iron-based catalysts(M-Fe/γ-Al_2O_3)was developed to reduce SO_2in actual smelter off-gases using CO–H_2gas mixture as reducing agent for sulfur production.Used as modifiers,t...A series of modifiedγ-Al_2O_3supported iron-based catalysts(M-Fe/γ-Al_2O_3)was developed to reduce SO_2in actual smelter off-gases using CO–H_2gas mixture as reducing agent for sulfur production.Used as modifiers,three metal additives—Ni,Co,and Ce were added to Fe/γ-Al_2O_3catalysts.Changes in catalyst structure and active phase were characterized with X-ray diffraction,XPS,SEM,and EDS.The reduction ability of catalysts was exhibited via CO-TPR.The prepared catalysts only need to be pre-reacted for a period of time,eliminating the need for presulfidation treatment.Reaction conditions were optimized in a fixed bed reactor to achieve high SO_2conversion and sulfur selectivity.XRD characterization was carried out to verify the resulting sulfur products.Combining in situ infrared characterization and catalyst evaluation of support and active component,the reaction mechanism was investigated and proposed.展开更多
The biggest challenging issue in photocatalysis is efficient separation of the photoinduced carriers and the aggregation of photoexcited electrons on photocatalyst’s surface.In this paper,we report that double metall...The biggest challenging issue in photocatalysis is efficient separation of the photoinduced carriers and the aggregation of photoexcited electrons on photocatalyst’s surface.In this paper,we report that double metallic co-catalysts Ti3C2 MXene and metallic octahedral(1T)phase tungsten disulfide(WS2)act pathways transferring photoexcited electrons in assisting the photocatalytic H2 evolution.TiO2 nanosheets were in situ grown on highly conductive Ti3C2 MXenes and 1T-WS2 nanoparticles were then uniformly distributed on TiO2@Ti3C2 composite.Thus,a distinctive 1T-WS2@TiO2@Ti3C2 composite with double metallic co-catalysts was achieved,and the content of 1T phase reaches 73%.The photocatalytic H2 evolution performance of 1T-WS2@TiO2@Ti3C2 composite with an optimized 15 wt%WS2 ratio is nearly 50 times higher than that of TiO2 nanosheets because of conductive Ti3C2 MXene and 1T-WS2 resulting in the increase of electron transfer efficiency.Besides,the 1T-WS2 on the surface of TiO2@Ti3C2 composite enhances the Brunauer–Emmett–Teller surface area and boosts the density of active site.展开更多
CeO2,MnOx and ZnO were used as supports of Cu-based catalysts respectively in this study.The influences of these supports on the catalyst for CO oxidation in H2-rich gases were investigated.The catalysts were characte...CeO2,MnOx and ZnO were used as supports of Cu-based catalysts respectively in this study.The influences of these supports on the catalyst for CO oxidation in H2-rich gases were investigated.The catalysts were characterized by XRD(X-ray diffraction),BET(BET surface area),TPD(Temperature-programmed desorption) and TPR(Temperature-programmed reduction) methods.The results indicate that CuO/CeO2 catalyst has higher catalytic activity,for CO oxidation than CuO/MnO or CuO/ZnO catalyst.The CO conversion of CuO/CeO2 catalyst at 413K and 433K are 85% and 97%,respectively.Comparing with the other two catalysts,CuO/CeO2 catalyst has larger surface area,pore volume,CO adsorption amount and reduction peak area,while lower CO desorption and reduction temperature.Besides there is a stronger metal-support interaction in CuO/CeO2 catalyst than in other catalysts.All these favour the activity of the catalyst.展开更多
Due to coexisting of H2, CO2 and H2O with CO in hydrogen-rich gas produced from methanol reforming, the selective CO oxidation is companied with the side reactions of H2 oxidation, as well as CO or CO2 methanation and...Due to coexisting of H2, CO2 and H2O with CO in hydrogen-rich gas produced from methanol reforming, the selective CO oxidation is companied with the side reactions of H2 oxidation, as well as CO or CO2 methanation and reverse water-gas shift reaction（RWGS）. This paper investigated the effects of the above side reactions on the selective CO oxidation over a 0.5% Pt/Al2O3 monolithic catalyst. The results showed that after 50% H2 is added into the reactants, the highest CO conversion is only 98.3% at 180℃ when the feed molar ratio of O2 to CO is 1, and the corresponding outlet CO concentration is 180×10 -6 . Adding 50% H2 into the reactants accelerate CO oxidation at low temperatures; the catalyst active reaction temperature window shifts down about 40℃ . CO produced from RWGS is 80×10 -6 at 200℃ indicating that the effect of RWGS on selective CO oxidation becomes obvious at temperatures higher than 200℃. On the other side, CO or CO2 methanation does not take place even at 300℃ under current conditions and has little effects on the selective CO oxidation.展开更多
基金Supported by the National Science Fund for Excellent Young Scholars(21422607)Key Program of National Natural Science Foundation of China(91434203)
文摘A series of modifiedγ-Al_2O_3supported iron-based catalysts(M-Fe/γ-Al_2O_3)was developed to reduce SO_2in actual smelter off-gases using CO–H_2gas mixture as reducing agent for sulfur production.Used as modifiers,three metal additives—Ni,Co,and Ce were added to Fe/γ-Al_2O_3catalysts.Changes in catalyst structure and active phase were characterized with X-ray diffraction,XPS,SEM,and EDS.The reduction ability of catalysts was exhibited via CO-TPR.The prepared catalysts only need to be pre-reacted for a period of time,eliminating the need for presulfidation treatment.Reaction conditions were optimized in a fixed bed reactor to achieve high SO_2conversion and sulfur selectivity.XRD characterization was carried out to verify the resulting sulfur products.Combining in situ infrared characterization and catalyst evaluation of support and active component,the reaction mechanism was investigated and proposed.
基金fundings from the National Natural Science Foundation of China (Nos. 51872173 and 51772167)Taishan Scholarship of Young Scholars (No. tsqn201812068)+2 种基金Natural Science Foundation of Shandong Province (No. ZR2017JL020)Taishan Scholarship of Climbing Plan (No. tspd20161006)Key Research and Development Program of Shandong Province (No. 2018GGX102028)
文摘The biggest challenging issue in photocatalysis is efficient separation of the photoinduced carriers and the aggregation of photoexcited electrons on photocatalyst’s surface.In this paper,we report that double metallic co-catalysts Ti3C2 MXene and metallic octahedral(1T)phase tungsten disulfide(WS2)act pathways transferring photoexcited electrons in assisting the photocatalytic H2 evolution.TiO2 nanosheets were in situ grown on highly conductive Ti3C2 MXenes and 1T-WS2 nanoparticles were then uniformly distributed on TiO2@Ti3C2 composite.Thus,a distinctive 1T-WS2@TiO2@Ti3C2 composite with double metallic co-catalysts was achieved,and the content of 1T phase reaches 73%.The photocatalytic H2 evolution performance of 1T-WS2@TiO2@Ti3C2 composite with an optimized 15 wt%WS2 ratio is nearly 50 times higher than that of TiO2 nanosheets because of conductive Ti3C2 MXene and 1T-WS2 resulting in the increase of electron transfer efficiency.Besides,the 1T-WS2 on the surface of TiO2@Ti3C2 composite enhances the Brunauer–Emmett–Teller surface area and boosts the density of active site.
文摘CeO2,MnOx and ZnO were used as supports of Cu-based catalysts respectively in this study.The influences of these supports on the catalyst for CO oxidation in H2-rich gases were investigated.The catalysts were characterized by XRD(X-ray diffraction),BET(BET surface area),TPD(Temperature-programmed desorption) and TPR(Temperature-programmed reduction) methods.The results indicate that CuO/CeO2 catalyst has higher catalytic activity,for CO oxidation than CuO/MnO or CuO/ZnO catalyst.The CO conversion of CuO/CeO2 catalyst at 413K and 433K are 85% and 97%,respectively.Comparing with the other two catalysts,CuO/CeO2 catalyst has larger surface area,pore volume,CO adsorption amount and reduction peak area,while lower CO desorption and reduction temperature.Besides there is a stronger metal-support interaction in CuO/CeO2 catalyst than in other catalysts.All these favour the activity of the catalyst.
文摘Due to coexisting of H2, CO2 and H2O with CO in hydrogen-rich gas produced from methanol reforming, the selective CO oxidation is companied with the side reactions of H2 oxidation, as well as CO or CO2 methanation and reverse water-gas shift reaction（RWGS）. This paper investigated the effects of the above side reactions on the selective CO oxidation over a 0.5% Pt/Al2O3 monolithic catalyst. The results showed that after 50% H2 is added into the reactants, the highest CO conversion is only 98.3% at 180℃ when the feed molar ratio of O2 to CO is 1, and the corresponding outlet CO concentration is 180×10 -6 . Adding 50% H2 into the reactants accelerate CO oxidation at low temperatures; the catalyst active reaction temperature window shifts down about 40℃ . CO produced from RWGS is 80×10 -6 at 200℃ indicating that the effect of RWGS on selective CO oxidation becomes obvious at temperatures higher than 200℃. On the other side, CO or CO2 methanation does not take place even at 300℃ under current conditions and has little effects on the selective CO oxidation.
