The chemistry of acetaldehyde (CH3CHO) adsorbed on the anatase TiO2(001)-(1×4) surface has been investigated by temperature-programmed desorption (TPD) method. Our experimental results provide the direct evidence...The chemistry of acetaldehyde (CH3CHO) adsorbed on the anatase TiO2(001)-(1×4) surface has been investigated by temperature-programmed desorption (TPD) method. Our experimental results provide the direct evidence that the perfect lattice sites on the anatase TiO2(001)-(1×4) surface are quite inert for the reaction of CH3CHO, but the reduced defect sites on the surface are active for the thermally driven reductive carbon-carbon coupling reactions of CH3CHO to produce 2-butanone and butene. We propose that the coupling reactions of CH3CHO on the anatase TiO2(001)-(1×4) surface should undergo through the adsorption of paired CH3CHO molecules at the reduced defect sites, since the existing reduced Ti pairs provide the suitable adsorption sites.展开更多
A sample of sulfated anatase TiO2 with high‐energy(001)facets(TiO2‐001)was prepared by a simple one‐step hydrothermal route using SO42-as a morphology‐controlling agent.After doping ceria,Ce/TiO2‐001 was used as ...A sample of sulfated anatase TiO2 with high‐energy(001)facets(TiO2‐001)was prepared by a simple one‐step hydrothermal route using SO42-as a morphology‐controlling agent.After doping ceria,Ce/TiO2‐001 was used as the catalyst for selective catalytic reduction(SCR)of NO with NH3.Compared with Ce/P25(Degussa P25 TiO2)and Ce/P25‐S(sulfated P25)catalysts,Ce/TiO2‐001 was more suitable for medium‐and high‐temperature SCR of NO due to the high surface area,sulfation,and the excellent properties of the active‐energy(001)facets.All of these facilitated the generation of abundant acidity,chemisorbed oxygen,and activated NOx‐adsorption species,which were the important factors for the SCR reaction.展开更多
Anatase TiO2 with a variant percentage of exposed （001） facets was prepared under hydrothermal processes by adjusting the volume of HF, and the photocatalytic mechanism was studied from atomic-molecular scale by HRT...Anatase TiO2 with a variant percentage of exposed （001） facets was prepared under hydrothermal processes by adjusting the volume of HF, and the photocatalytic mechanism was studied from atomic-molecular scale by HRTEM and Raman spectroscopy. It was revealed that： 1） From HRTEM observations, the surface of original TiO2 with exposed （001） facets was clean without impurity, and the crystal lattice was clear and completed; however, when mixed with methylene blue （MB） solution, there were many 1 nm molecular absorbed at the surface of TiO2; after the photocatalytic experiment, MB molecules disappeared and the TiO2 lattice image became fuzzy. 2） The broken path of the MB chemical bond was obtained by Raman spectroscopy, i.e., after the irradiation of the light, the vibrational mode of C-N-C disappeared due to the chemical bond breakage, and the groups containing C-N bond and carbon rings were gradually decomposed. Accordingly, we propose that the driving force for breaking the chemical bond and the disappearance of groups is from the surface lattice distortion of TiO2 during photocatalyzation.展开更多
Anatase TiO2with exposed{001}facets has been deepgoingly studied for optimizing its photocatalytic activity.In this study,we synthesized N-doped TiO2 nanocrystals with exposed{001}facets by sol–gel method and solvoth...Anatase TiO2with exposed{001}facets has been deepgoingly studied for optimizing its photocatalytic activity.In this study,we synthesized N-doped TiO2 nanocrystals with exposed{001}facets by sol–gel method and solvothermal method,respectively.The physical and chemical properties of as-synthesized samples,such as morphology,crystal phase,surface elements composition,porous structure,specific surface area,and optical response,were characterized in detail.The photocatalytic performances of all samples were evaluated by photocatalytic decoloration of methylene blue under visible-light irradiation(k[420 nm).The results showed that the as-prepared samples present high visible-light photocatalytic performances,which can be ascribed to the excellent crystallization,the enhancement of absorbance in the visible-light region,and the strong adsorption performance,and calcination treatment is helpful to further improve the visible-light photocatalytic performance of N-doped TiO2 nanocrystals with exposed{001}facets.展开更多
基金supported by the Ministry of Science and Technology of China (No.2016YFA0200603)the National Natural Science Foundation of China (No.91421313 and No.21573207)Anhui Initiative in Quantum Information Technologies (AHY090300)
文摘The chemistry of acetaldehyde (CH3CHO) adsorbed on the anatase TiO2(001)-(1×4) surface has been investigated by temperature-programmed desorption (TPD) method. Our experimental results provide the direct evidence that the perfect lattice sites on the anatase TiO2(001)-(1×4) surface are quite inert for the reaction of CH3CHO, but the reduced defect sites on the surface are active for the thermally driven reductive carbon-carbon coupling reactions of CH3CHO to produce 2-butanone and butene. We propose that the coupling reactions of CH3CHO on the anatase TiO2(001)-(1×4) surface should undergo through the adsorption of paired CH3CHO molecules at the reduced defect sites, since the existing reduced Ti pairs provide the suitable adsorption sites.
基金supported by the National Key R&D Program of China(2016YFC0204100)the Zhejiang Provincial "151" Talents Program+1 种基金the Program for Zhejiang Leading Team of S&T Innovation(2013TD07)the Changjiang Scholar Incentive Program(2009)~~
文摘A sample of sulfated anatase TiO2 with high‐energy(001)facets(TiO2‐001)was prepared by a simple one‐step hydrothermal route using SO42-as a morphology‐controlling agent.After doping ceria,Ce/TiO2‐001 was used as the catalyst for selective catalytic reduction(SCR)of NO with NH3.Compared with Ce/P25(Degussa P25 TiO2)and Ce/P25‐S(sulfated P25)catalysts,Ce/TiO2‐001 was more suitable for medium‐and high‐temperature SCR of NO due to the high surface area,sulfation,and the excellent properties of the active‐energy(001)facets.All of these facilitated the generation of abundant acidity,chemisorbed oxygen,and activated NOx‐adsorption species,which were the important factors for the SCR reaction.
文摘Anatase TiO2 with a variant percentage of exposed （001） facets was prepared under hydrothermal processes by adjusting the volume of HF, and the photocatalytic mechanism was studied from atomic-molecular scale by HRTEM and Raman spectroscopy. It was revealed that： 1） From HRTEM observations, the surface of original TiO2 with exposed （001） facets was clean without impurity, and the crystal lattice was clear and completed; however, when mixed with methylene blue （MB） solution, there were many 1 nm molecular absorbed at the surface of TiO2; after the photocatalytic experiment, MB molecules disappeared and the TiO2 lattice image became fuzzy. 2） The broken path of the MB chemical bond was obtained by Raman spectroscopy, i.e., after the irradiation of the light, the vibrational mode of C-N-C disappeared due to the chemical bond breakage, and the groups containing C-N bond and carbon rings were gradually decomposed. Accordingly, we propose that the driving force for breaking the chemical bond and the disappearance of groups is from the surface lattice distortion of TiO2 during photocatalyzation.
基金supported by the Key Project of Science and Technology Plan of Fujian Province (2012Y0066)the Opening Project of State Key Laboratory of High Performance Ceramics and Superfine Microstructure (SKL201107SIC)+2 种基金the National High Technology Research and Development Program of China (2012AA062606)the International Science & Technology Cooperation Program of China (2011DFB91710)the Xiamen Distinguished Young Scholar Award (3502Z20126011)
文摘Anatase TiO2with exposed{001}facets has been deepgoingly studied for optimizing its photocatalytic activity.In this study,we synthesized N-doped TiO2 nanocrystals with exposed{001}facets by sol–gel method and solvothermal method,respectively.The physical and chemical properties of as-synthesized samples,such as morphology,crystal phase,surface elements composition,porous structure,specific surface area,and optical response,were characterized in detail.The photocatalytic performances of all samples were evaluated by photocatalytic decoloration of methylene blue under visible-light irradiation(k[420 nm).The results showed that the as-prepared samples present high visible-light photocatalytic performances,which can be ascribed to the excellent crystallization,the enhancement of absorbance in the visible-light region,and the strong adsorption performance,and calcination treatment is helpful to further improve the visible-light photocatalytic performance of N-doped TiO2 nanocrystals with exposed{001}facets.
