Spray pyrolysis method was used to deposit Lutetium Oxide (Lu<sub>2</sub>O<sub>3</sub>) thin films using lutetium (III) chloride as source material and water as oxidizer. Annealing was carried ...Spray pyrolysis method was used to deposit Lutetium Oxide (Lu<sub>2</sub>O<sub>3</sub>) thin films using lutetium (III) chloride as source material and water as oxidizer. Annealing was carried out in argon atmosphere at 450°C for 60 minutes of the films. To investigate the composition and stoichiometry of sprayed as-deposited and annealed Lu<sub>2</sub>O<sub>3</sub> thin films, depth profile studies using X-ray photoelectron spectroscopy (XPS) was done. Nearly stoichiometric was observed for both annealed and as-deposited films in inner and surface layers.展开更多
Ga<sub>2</sub>O<sub>3</sub> thin films were fabricated by spray pyrolysis method using gallium acetylacetonate as source material and water as oxidizer. The films were annealed at 450°C fo...Ga<sub>2</sub>O<sub>3</sub> thin films were fabricated by spray pyrolysis method using gallium acetylacetonate as source material and water as oxidizer. The films were annealed at 450°C for 60 minutes in argon atmosphere. X-ray photoelectron spectroscopy (XPS) depth profile studies were carried out to analyze the stoichiometry and composition of sprayed as-deposited and annealed Ga<sub>2</sub>O<sub>3</sub> thin films. Surface layers and the inner layers of as-deposited and annealed films were found nearly stoichiometric.展开更多
Plasmonic nonmetal semiconductors with localized surface plasmon resonance(LSPR)effects possess extended light-response ranges and can act as highly efficient H2 generation photocatalysts.Herein,an LSPR-enhanced 0D/2D...Plasmonic nonmetal semiconductors with localized surface plasmon resonance(LSPR)effects possess extended light-response ranges and can act as highly efficient H2 generation photocatalysts.Herein,an LSPR-enhanced 0D/2D CdS/MoO3‒x heterojunction has been synthesized by the growth of 0D CdS nanoparticles on 2D plasmonic MoO3‒x elliptical nanosheets via a simple coprecipitation method.Taking advantage of the LSPR effect of the MoO3‒x elliptical nanosheets,the light absorption of the CdS/MoO3‒x heterojunction was extended from 600 nm to the near-infrared region(1400 nm).Furthermore,the introduction of 2D plasmonic MoO3‒x elliptical nanosheets not only provided a platform for the growth of CdS nanoparticles,but also contributed to the construction of an LSPR-enhanced S-scheme structure due to the interface between the MoO3‒x and CdS,accelerating the separation of light-induced electrons and holes.Therefore,the CdS/MoO3‒x heterojunction exhibited higher photocatalytic H2 generation activity than pristine CdS under visible light irradiation,including under 420,450,550,and 650 nm monochromic light,as well as improved photo-corrosion performance.展开更多
A series of heteropoly acid (HPA) based Al2O3 catalysts with three-dimensional ordered (3DOM) structure were synthesized by colloidal crystal template method.Interconnected macropores (250 nm) could be clearly observe...A series of heteropoly acid (HPA) based Al2O3 catalysts with three-dimensional ordered (3DOM) structure were synthesized by colloidal crystal template method.Interconnected macropores (250 nm) could be clearly observed by scanning electron microscope (SEM) and transmission electron microscope (TEM).Mesopores could be detected by N2 adsorption-desorption isotherms which further confirmed the 3DOM structural characteristics of catalyst.Moreover,Keggin-type HPW was highly dispersed in the Al2O3 framework,which suggested by powder X-ray diffraction (XRD) and Fourier transform infrared spectra (FT-IR) results.The oxidation desulfurization (ODS) performance of 3DOM H3PW12O40/Al2O3 of refractory sulphur compounds was evaluated in the presence of hydrogen peroxide.It oxidized 98.5% of dibenzothiophene (DBT) into corresponding sulfone within 3 h,which exhibited superior ODS performance than corresponding mesoporous and microporous H3PW12O40/Al2O3 catalyst.The enhancement of ODS efficiency is related to the improvement of mass transfer of DBT in the pore channel resulting from the interconnected 3DOM structure.Furthermore,the as-prepared catalyst still demonstrates outstanding cycle performance after 6 runs,which could be easily recovered from the model fuel.展开更多
In situ quick X-ray absorption spectroscopy(QXAFS) at the Cu and Zn K-edge under operando conditions has been used to unravel the Cu/Zn interaction and identify possible active site of CuO/ZnO/Al_2O_3 catalyst for met...In situ quick X-ray absorption spectroscopy(QXAFS) at the Cu and Zn K-edge under operando conditions has been used to unravel the Cu/Zn interaction and identify possible active site of CuO/ZnO/Al_2O_3 catalyst for methanol synthesis. In this work, the catalyst, whose activity increases with the reaction temperature and pressure, was studied at calcined, reduced, and reacted conditions. TEM and EDX images for the calcined and reduced catalysts showed that copper was distributed uniformly at both conditions. TPR profile revealed two reduction peaks at 165 and 195 °C for copper species in the calcined catalyst. QXAFS results demonstrated that the calcined form consisted mainly of a mixed Cu O and Zn O, and it was progressively transformed into Cu metal particles and dispersed Zn O species as the reduction treatment. It was demonstrated that activation of the catalyst precursor occurred via a Cu^+intermediate, and the active catalyst predominantly consisted of metallic Cu and Zn O evenunder higher pressures. Structure of the active catalyst did not change with the temperature or pressure, indicating that the role of the Zn was mainly to improve Cu dispersion.This indicates the potential of QXAFS method in studying the structure evolutions of catalysts in methanol synthesis.展开更多
Aiming to improve the reactive adsorption desulfurization（RADS） performances of Ni/Zn O adsorbents,ZnxAly（OH）2（CO3）z·x H2 O precursor is synthesized by coprecipitation of Zn2＋,AlO-2,and CO2-3; the Zn OZn6A...Aiming to improve the reactive adsorption desulfurization（RADS） performances of Ni/Zn O adsorbents,ZnxAly（OH）2（CO3）z·x H2 O precursor is synthesized by coprecipitation of Zn2＋,AlO-2,and CO2-3; the Zn OZn6Al2O9 composite oxides are obtained by the calcination of ZnxAly（OH）2（CO3）z·x H2 O precursor,and the Ni/Zn O-Zn6Al2O9（6.0 wt% Ni O） adsorbents are prepared by wetness impregnation method. The phase,acid strength,acid type and quantity,morphology,and thermal properties were characterized by X-ray diffraction,temperature-programmed desorption of ammonia,pyridine-adsorbed infrared spectrum,high-resolution transmission electron microscopy,and Thermo Gravimetry-Derivative Thermo Gravimetry（TG-DTG）,respectively. The breakthrough sulfur capacities of six adsorbents are between 34.2 and 47.9 mg/gcat. The kinetic studies indicated that the active energy of RADS（49.4 k J/mol） could reach nano-sized Zn O,the particle size of is about 12.0 nm. All the excellent RADS performances can be due to the high SBET. Also,there are some extents of aromatization reactions that occur,which can be contributed to the B？nsted acid rooted in Zn6Al2O9 composite oxide,and the octane number of products can be preserved well.展开更多
文摘Spray pyrolysis method was used to deposit Lutetium Oxide (Lu<sub>2</sub>O<sub>3</sub>) thin films using lutetium (III) chloride as source material and water as oxidizer. Annealing was carried out in argon atmosphere at 450°C for 60 minutes of the films. To investigate the composition and stoichiometry of sprayed as-deposited and annealed Lu<sub>2</sub>O<sub>3</sub> thin films, depth profile studies using X-ray photoelectron spectroscopy (XPS) was done. Nearly stoichiometric was observed for both annealed and as-deposited films in inner and surface layers.
文摘Ga<sub>2</sub>O<sub>3</sub> thin films were fabricated by spray pyrolysis method using gallium acetylacetonate as source material and water as oxidizer. The films were annealed at 450°C for 60 minutes in argon atmosphere. X-ray photoelectron spectroscopy (XPS) depth profile studies were carried out to analyze the stoichiometry and composition of sprayed as-deposited and annealed Ga<sub>2</sub>O<sub>3</sub> thin films. Surface layers and the inner layers of as-deposited and annealed films were found nearly stoichiometric.
文摘Plasmonic nonmetal semiconductors with localized surface plasmon resonance(LSPR)effects possess extended light-response ranges and can act as highly efficient H2 generation photocatalysts.Herein,an LSPR-enhanced 0D/2D CdS/MoO3‒x heterojunction has been synthesized by the growth of 0D CdS nanoparticles on 2D plasmonic MoO3‒x elliptical nanosheets via a simple coprecipitation method.Taking advantage of the LSPR effect of the MoO3‒x elliptical nanosheets,the light absorption of the CdS/MoO3‒x heterojunction was extended from 600 nm to the near-infrared region(1400 nm).Furthermore,the introduction of 2D plasmonic MoO3‒x elliptical nanosheets not only provided a platform for the growth of CdS nanoparticles,but also contributed to the construction of an LSPR-enhanced S-scheme structure due to the interface between the MoO3‒x and CdS,accelerating the separation of light-induced electrons and holes.Therefore,the CdS/MoO3‒x heterojunction exhibited higher photocatalytic H2 generation activity than pristine CdS under visible light irradiation,including under 420,450,550,and 650 nm monochromic light,as well as improved photo-corrosion performance.
基金Funded by the National Natural Science Foundation of China(No.21476177)。
文摘A series of heteropoly acid (HPA) based Al2O3 catalysts with three-dimensional ordered (3DOM) structure were synthesized by colloidal crystal template method.Interconnected macropores (250 nm) could be clearly observed by scanning electron microscope (SEM) and transmission electron microscope (TEM).Mesopores could be detected by N2 adsorption-desorption isotherms which further confirmed the 3DOM structural characteristics of catalyst.Moreover,Keggin-type HPW was highly dispersed in the Al2O3 framework,which suggested by powder X-ray diffraction (XRD) and Fourier transform infrared spectra (FT-IR) results.The oxidation desulfurization (ODS) performance of 3DOM H3PW12O40/Al2O3 of refractory sulphur compounds was evaluated in the presence of hydrogen peroxide.It oxidized 98.5% of dibenzothiophene (DBT) into corresponding sulfone within 3 h,which exhibited superior ODS performance than corresponding mesoporous and microporous H3PW12O40/Al2O3 catalyst.The enhancement of ODS efficiency is related to the improvement of mass transfer of DBT in the pore channel resulting from the interconnected 3DOM structure.Furthermore,the as-prepared catalyst still demonstrates outstanding cycle performance after 6 runs,which could be easily recovered from the model fuel.
基金supported by the National Basic Research Program of China(973 Program,2013CB933104)the National Natural Science Foundation of China(Nos.11275258 and 11135008)
文摘In situ quick X-ray absorption spectroscopy(QXAFS) at the Cu and Zn K-edge under operando conditions has been used to unravel the Cu/Zn interaction and identify possible active site of CuO/ZnO/Al_2O_3 catalyst for methanol synthesis. In this work, the catalyst, whose activity increases with the reaction temperature and pressure, was studied at calcined, reduced, and reacted conditions. TEM and EDX images for the calcined and reduced catalysts showed that copper was distributed uniformly at both conditions. TPR profile revealed two reduction peaks at 165 and 195 °C for copper species in the calcined catalyst. QXAFS results demonstrated that the calcined form consisted mainly of a mixed Cu O and Zn O, and it was progressively transformed into Cu metal particles and dispersed Zn O species as the reduction treatment. It was demonstrated that activation of the catalyst precursor occurred via a Cu^+intermediate, and the active catalyst predominantly consisted of metallic Cu and Zn O evenunder higher pressures. Structure of the active catalyst did not change with the temperature or pressure, indicating that the role of the Zn was mainly to improve Cu dispersion.This indicates the potential of QXAFS method in studying the structure evolutions of catalysts in methanol synthesis.
文摘Aiming to improve the reactive adsorption desulfurization（RADS） performances of Ni/Zn O adsorbents,ZnxAly（OH）2（CO3）z·x H2 O precursor is synthesized by coprecipitation of Zn2＋,AlO-2,and CO2-3; the Zn OZn6Al2O9 composite oxides are obtained by the calcination of ZnxAly（OH）2（CO3）z·x H2 O precursor,and the Ni/Zn O-Zn6Al2O9（6.0 wt% Ni O） adsorbents are prepared by wetness impregnation method. The phase,acid strength,acid type and quantity,morphology,and thermal properties were characterized by X-ray diffraction,temperature-programmed desorption of ammonia,pyridine-adsorbed infrared spectrum,high-resolution transmission electron microscopy,and Thermo Gravimetry-Derivative Thermo Gravimetry（TG-DTG）,respectively. The breakthrough sulfur capacities of six adsorbents are between 34.2 and 47.9 mg/gcat. The kinetic studies indicated that the active energy of RADS（49.4 k J/mol） could reach nano-sized Zn O,the particle size of is about 12.0 nm. All the excellent RADS performances can be due to the high SBET. Also,there are some extents of aromatization reactions that occur,which can be contributed to the B？nsted acid rooted in Zn6Al2O9 composite oxide,and the octane number of products can be preserved well.
