A series of Mn-doped K-Co-Mo catalysts were prepared by a sol-gel method. The catalyst structure was well characterized by X-ray diffraction, N2 physisorption, NH3 temperature- programmed adsorption, in situ diffuse r...A series of Mn-doped K-Co-Mo catalysts were prepared by a sol-gel method. The catalyst structure was well characterized by X-ray diffraction, N2 physisorption, NH3 temperature- programmed adsorption, in situ diffuse reflectance infrared Fourier transform spectroscopy, and X-ray absorption fine structure spectroscopy. The catalytic performance for higher alcohol synthesis from syngas was measured. It was found that the Mn-doped catalysts ex- hibited a much higher activity as compared to the unpromoted catalyst, and in particular the C2＋ alcohol selectivity increased significantly. The distribution of alcohol products de- viated from the Anderson-Schulz-Flory law. The portion of methanol in total alcohol was suppressed remarkably and the ethanol became the predominant product. Characterization results indicated that the incorporation of Mn enhanced the interaction of Co and Mo and thus led to the formation of Co-Mo-O species, which was regarded as the active site for the alcohol synthesis. Secondly, the presence of Mn reduced the amount of strong acid sites significantly and meanwhile promoted the formation of weak acid sites, which had a positive effect on the synthesis of alcohol. Furthermore, it was found that the incorporation of Mn can enhance the adsorption of linear- and bridge-type CO significantly, which contributed to the formation of alcohol and growth of carbon chain and thus increased the selectivity to C2＋OH.展开更多
Co(Ⅱ)and Ni(Ⅱ)are two common toxic heavy metals,and may simultaneously exist in contaminated water,soil,and sediment systems in Earth’s surface environment.Under this circumstance,competitive adsorption between the...Co(Ⅱ)and Ni(Ⅱ)are two common toxic heavy metals,and may simultaneously exist in contaminated water,soil,and sediment systems in Earth’s surface environment.Under this circumstance,competitive adsorption between the two metals may influence their migration,toxicity,and bioavailability.In this research,the competitive sorption of Co(Ⅱ)and Ni(Ⅱ)on γ-Al_2O_3was studied using both macroscopic sorption experiments and extended X-ray absorption fine structure(EXAFS)spectroscopy.Results suggest that Ni(Ⅱ)reduced the amount of Co(Ⅱ)sorption in a binary-solute system at pH 6.0.This is because both Co(Ⅱ)and Ni(Ⅱ)form inner-sphere surface complexes during sorption on γ-Al_2O_3and compete for the surface reactive sites.However,Co(Ⅱ)exhibited a negligible influence on sorption amount of Ni(Ⅱ)under the same conditions,which suggests Ni(Ⅱ)has a stronger affinity to alumina surface.At pH 7.5,Co(Ⅱ)and Ni(Ⅱ)sorption density were much higher than that at pH 6.0,but there no mutual competitive effect was observed.EXAFS analysis further revealed that formation of layered double-hydrated precipitates was the dominant sorption mechanism for both Co(Ⅱ)and Ni(Ⅱ)at pH 7.5.Because this type of sorption does not rely on surface reactive sites,there was no competition between Co(Ⅱ)and Ni(Ⅱ).This finding sheds light on risk assessment and remediation of Ni/Co pollution.展开更多
An all optical fiber gas sensor is presented to detect the concentration of NH3 and CO. Based on the spectral absorption, The wideband light source is used to reflect two narrowband spectra by fiber grating of differe...An all optical fiber gas sensor is presented to detect the concentration of NH3 and CO. Based on the spectral absorption, The wideband light source is used to reflect two narrowband spectra by fiber grating of different duty. and piezoelectric ceramics to obtain narrowband output light. The high sensitivity detection can be measured from the second harmonic signal. The two narrowband spectra are corresponding to the absorption spectra of NH3 and CO. Concentration detection are realized by the detection of variety of light intensity. Sensitivity is proved and cost is reduced.展开更多
The oxidation of carbon monoxide is widely investigated for realistic and potential uses in energy production and environmental processes.As a probe reaction to the surface properties,it gives an insight into the rela...The oxidation of carbon monoxide is widely investigated for realistic and potential uses in energy production and environmental processes.As a probe reaction to the surface properties,it gives an insight into the relationship between the structure of active phase and catalytic performance.Noble metals alloyed with certain transition metals in the form of a nanoalloy exhibit enhanced catalytic activity for various reactions,especially when simultaneous activation of oxygen and CO is involved.This article highlights some of these insights into nanoalloy catalysts in which platinum group metal(PGM)is alloyed with a second and/or third transition metal(M/M′=Co,Fe,V,Ni,Ir,etc.),for catalytic oxidation of carbon monoxide in a gas phase.Recent studies have provided important insights into how the atomic-scale structures of the nanoalloy catalysts operate synergistically in activating oxygen and maneuvering surface oxygenated species.The exploration of atomic-scale chemical/structural ordering and coordination in correlation with the catalytic oxidation properties based on findings from ex-and in-situ synchrotron X-ray techniques is emphasized;for example,high-energy X-ray diffraction coupled to atomic-pair distribution function and X-ray absorption fine-structure spectroscopic analysis.The understanding of the detailed active sites of the nanoalloys has significant implications for the design of low-cost,active,and durable catalysts for sustainable energy production and environmental processes.展开更多
文摘A series of Mn-doped K-Co-Mo catalysts were prepared by a sol-gel method. The catalyst structure was well characterized by X-ray diffraction, N2 physisorption, NH3 temperature- programmed adsorption, in situ diffuse reflectance infrared Fourier transform spectroscopy, and X-ray absorption fine structure spectroscopy. The catalytic performance for higher alcohol synthesis from syngas was measured. It was found that the Mn-doped catalysts ex- hibited a much higher activity as compared to the unpromoted catalyst, and in particular the C2＋ alcohol selectivity increased significantly. The distribution of alcohol products de- viated from the Anderson-Schulz-Flory law. The portion of methanol in total alcohol was suppressed remarkably and the ethanol became the predominant product. Characterization results indicated that the incorporation of Mn enhanced the interaction of Co and Mo and thus led to the formation of Co-Mo-O species, which was regarded as the active site for the alcohol synthesis. Secondly, the presence of Mn reduced the amount of strong acid sites significantly and meanwhile promoted the formation of weak acid sites, which had a positive effect on the synthesis of alcohol. Furthermore, it was found that the incorporation of Mn can enhance the adsorption of linear- and bridge-type CO significantly, which contributed to the formation of alcohol and growth of carbon chain and thus increased the selectivity to C2＋OH.
基金co-funded by the National Natural Science Foundation of China(No.41473084)the Project of China Geological Survey(No.12120114092001)the 1000 Youth Talent program
文摘Co(Ⅱ)and Ni(Ⅱ)are two common toxic heavy metals,and may simultaneously exist in contaminated water,soil,and sediment systems in Earth’s surface environment.Under this circumstance,competitive adsorption between the two metals may influence their migration,toxicity,and bioavailability.In this research,the competitive sorption of Co(Ⅱ)and Ni(Ⅱ)on γ-Al_2O_3was studied using both macroscopic sorption experiments and extended X-ray absorption fine structure(EXAFS)spectroscopy.Results suggest that Ni(Ⅱ)reduced the amount of Co(Ⅱ)sorption in a binary-solute system at pH 6.0.This is because both Co(Ⅱ)and Ni(Ⅱ)form inner-sphere surface complexes during sorption on γ-Al_2O_3and compete for the surface reactive sites.However,Co(Ⅱ)exhibited a negligible influence on sorption amount of Ni(Ⅱ)under the same conditions,which suggests Ni(Ⅱ)has a stronger affinity to alumina surface.At pH 7.5,Co(Ⅱ)and Ni(Ⅱ)sorption density were much higher than that at pH 6.0,but there no mutual competitive effect was observed.EXAFS analysis further revealed that formation of layered double-hydrated precipitates was the dominant sorption mechanism for both Co(Ⅱ)and Ni(Ⅱ)at pH 7.5.Because this type of sorption does not rely on surface reactive sites,there was no competition between Co(Ⅱ)and Ni(Ⅱ).This finding sheds light on risk assessment and remediation of Ni/Co pollution.
文摘An all optical fiber gas sensor is presented to detect the concentration of NH3 and CO. Based on the spectral absorption, The wideband light source is used to reflect two narrowband spectra by fiber grating of different duty. and piezoelectric ceramics to obtain narrowband output light. The high sensitivity detection can be measured from the second harmonic signal. The two narrowband spectra are corresponding to the absorption spectra of NH3 and CO. Concentration detection are realized by the detection of variety of light intensity. Sensitivity is proved and cost is reduced.
基金supported by the National Natural Science Foundation of China(21373171),DOE-BES(DE-SC0006877)the NSF(CBET-0709113,CMMI-1100736),UTC Power,and Honda
文摘The oxidation of carbon monoxide is widely investigated for realistic and potential uses in energy production and environmental processes.As a probe reaction to the surface properties,it gives an insight into the relationship between the structure of active phase and catalytic performance.Noble metals alloyed with certain transition metals in the form of a nanoalloy exhibit enhanced catalytic activity for various reactions,especially when simultaneous activation of oxygen and CO is involved.This article highlights some of these insights into nanoalloy catalysts in which platinum group metal(PGM)is alloyed with a second and/or third transition metal(M/M′=Co,Fe,V,Ni,Ir,etc.),for catalytic oxidation of carbon monoxide in a gas phase.Recent studies have provided important insights into how the atomic-scale structures of the nanoalloy catalysts operate synergistically in activating oxygen and maneuvering surface oxygenated species.The exploration of atomic-scale chemical/structural ordering and coordination in correlation with the catalytic oxidation properties based on findings from ex-and in-situ synchrotron X-ray techniques is emphasized;for example,high-energy X-ray diffraction coupled to atomic-pair distribution function and X-ray absorption fine-structure spectroscopic analysis.The understanding of the detailed active sites of the nanoalloys has significant implications for the design of low-cost,active,and durable catalysts for sustainable energy production and environmental processes.
