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
Response surface methodology(RSM)was employed to optimize the control parameters of TiO_(2)/graphene with exposed{001}facets during synthesis,and its enhanced photocatalytic activities were evaluated in the photodegra...Response surface methodology(RSM)was employed to optimize the control parameters of TiO_(2)/graphene with exposed{001}facets during synthesis,and its enhanced photocatalytic activities were evaluated in the photodegradation of toluene.Experimental results were in good agreement with the predicted results obtained using RSM with a correlation coefficient(R^(2))of 0.9345.When 22.06 mg of graphite oxide(GO)and 2.09 mL of hydrofluoric acid(HF)were added and a hydrothermal time of 28 h was used,a maximum efficiency in the degradation of toluene was achieved.X-ray diffraction(XRD),transmission electron microscopy(TEM),and scanning electron microscopy(SEM)were employed to characterize the obtained hybrid photocatalyst.The electron transferred between Ti and C retarded the combination of electron–hole pairs and hastened the transferring of electrons,which enhanced the photocatalytic activity.展开更多
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
This study investigated the positive effect of surface modification with ozone on the photocatalytic performance of anatase TiO2 with dominated(001) facets for toluene degradation.The performance of photocatalyst wa...This study investigated the positive effect of surface modification with ozone on the photocatalytic performance of anatase TiO2 with dominated(001) facets for toluene degradation.The performance of photocatalyst was tested on a home-made volatile organic compounds degradation system. The ozone modification, toluene adsorption and degradation mechanism were established by a combination of various characterization methods, in situ diffuse reflectance infrared fourier transform spectroscopy, and density functional theory calculation.The surface modification with ozone can significantly enhance the photocatalytic degradation performance for toluene. The abundant unsaturated coordinated 5 c-Ti sites on(001)facets act as the adsorption sites for ozone. The formed Ti–O bonds reacted with H2O to generate a large amount of isolated Ti5 c-OH which act as the adsorption sites for toluene,and thus significantly increase the adsorption capacity for toluene. The outstanding photocatalytic performance of ozone-modified TiO2 is due to its high adsorption ability for toluene and the abundant surface hydroxyl groups, which produce very reactive OH·radicals under irradiation. Furthermore, the O2 generated via ozone dissociation could combine with the photogenerated electrons to form superoxide radicals which are also conductive to the toluene degradation.展开更多
采用水热法在FTO(fluorine-doped tin oxide)基底上制备不同形貌的锐钛矿结构TiO_(2)薄膜。通过不断增大反应前驱物中盐酸浓度,TiO_(2)薄膜由球状颗粒薄膜逐渐演变生长成大面积高能(001)面裸露的TiO_(2)纳米片阵列薄膜。通过对形貌演化...采用水热法在FTO(fluorine-doped tin oxide)基底上制备不同形貌的锐钛矿结构TiO_(2)薄膜。通过不断增大反应前驱物中盐酸浓度,TiO_(2)薄膜由球状颗粒薄膜逐渐演变生长成大面积高能(001)面裸露的TiO_(2)纳米片阵列薄膜。通过对形貌演化规律及X射线衍射图谱变化规律进行分析,提出了不同形貌TiO_(2)薄膜的生长演化机制,并对盐酸在其中的作用进行了说明。为了进一步改善TiO_(2)薄膜的性能,采用连续离子层吸附反应法对不同形貌的TiO_(2)薄膜进行CdS量子点敏化。采用紫外可见吸收光谱分析法和三电极体系对复合薄膜的光吸收性能和光电化学(PEC)性能进行了研究,实验数据显示CdS/TiO_(2)复合薄膜的光电化学性能皆明显优于单纯TiO_(2)薄膜,而且纳米片阵列薄膜的性能明显优于其他形貌薄膜,说明了大面积高能(001)面裸露的TiO_(2)纳米片阵列薄膜的性能优越性。展开更多
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.
基金supported by the National Natural Science Foundation of China(Nos.21406164,21466035 and 51203111)the National Basic Research Program of China("973"Program,Nos.2012CB720100 and 2014CB239300)
文摘Response surface methodology(RSM)was employed to optimize the control parameters of TiO_(2)/graphene with exposed{001}facets during synthesis,and its enhanced photocatalytic activities were evaluated in the photodegradation of toluene.Experimental results were in good agreement with the predicted results obtained using RSM with a correlation coefficient(R^(2))of 0.9345.When 22.06 mg of graphite oxide(GO)and 2.09 mL of hydrofluoric acid(HF)were added and a hydrothermal time of 28 h was used,a maximum efficiency in the degradation of toluene was achieved.X-ray diffraction(XRD),transmission electron microscopy(TEM),and scanning electron microscopy(SEM)were employed to characterize the obtained hybrid photocatalyst.The electron transferred between Ti and C retarded the combination of electron–hole pairs and hastened the transferring of electrons,which enhanced the photocatalytic activity.
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the National Natural Science Foundation of China (U1632273, 21673214,U1732272, U1832165).
文摘This study investigated the positive effect of surface modification with ozone on the photocatalytic performance of anatase TiO2 with dominated(001) facets for toluene degradation.The performance of photocatalyst was tested on a home-made volatile organic compounds degradation system. The ozone modification, toluene adsorption and degradation mechanism were established by a combination of various characterization methods, in situ diffuse reflectance infrared fourier transform spectroscopy, and density functional theory calculation.The surface modification with ozone can significantly enhance the photocatalytic degradation performance for toluene. The abundant unsaturated coordinated 5 c-Ti sites on(001)facets act as the adsorption sites for ozone. The formed Ti–O bonds reacted with H2O to generate a large amount of isolated Ti5 c-OH which act as the adsorption sites for toluene,and thus significantly increase the adsorption capacity for toluene. The outstanding photocatalytic performance of ozone-modified TiO2 is due to its high adsorption ability for toluene and the abundant surface hydroxyl groups, which produce very reactive OH·radicals under irradiation. Furthermore, the O2 generated via ozone dissociation could combine with the photogenerated electrons to form superoxide radicals which are also conductive to the toluene degradation.
文摘采用水热法在FTO(fluorine-doped tin oxide)基底上制备不同形貌的锐钛矿结构TiO_(2)薄膜。通过不断增大反应前驱物中盐酸浓度,TiO_(2)薄膜由球状颗粒薄膜逐渐演变生长成大面积高能(001)面裸露的TiO_(2)纳米片阵列薄膜。通过对形貌演化规律及X射线衍射图谱变化规律进行分析,提出了不同形貌TiO_(2)薄膜的生长演化机制,并对盐酸在其中的作用进行了说明。为了进一步改善TiO_(2)薄膜的性能,采用连续离子层吸附反应法对不同形貌的TiO_(2)薄膜进行CdS量子点敏化。采用紫外可见吸收光谱分析法和三电极体系对复合薄膜的光吸收性能和光电化学(PEC)性能进行了研究,实验数据显示CdS/TiO_(2)复合薄膜的光电化学性能皆明显优于单纯TiO_(2)薄膜,而且纳米片阵列薄膜的性能明显优于其他形貌薄膜,说明了大面积高能(001)面裸露的TiO_(2)纳米片阵列薄膜的性能优越性。