A series of photocatalysts of un-doped, single-doped and co-doped nanometer titanium diox- ide (TiO2) have been successfully prepared by template method using Fe(NO3)3.9H2O, La(NO3)3.6H2O, and tetrabutyl titanat...A series of photocatalysts of un-doped, single-doped and co-doped nanometer titanium diox- ide (TiO2) have been successfully prepared by template method using Fe(NO3)3.9H2O, La(NO3)3.6H2O, and tetrabutyl titanate as precursors and glucan as template. Scanning electron microscopy, X-ray diffraction, and N2 adsorption-desorption measurement were employed to characterize the morphology, crystal structure and surface structure of the samples. The photo-absorbance of the obtained catalysts was measured by UV-Vis absorption spectroscopy, and the photocatalytic activities of the prepared samples under UV and visible light were estimated by measuring the degradation rate of methyl orange in an aqueous solution. The characterizations indicated that the prepared photocatalysts consisted of anatase phase and possessed high surface area of ca. 163-176 m2/g. It was shown that the Fe and La co-doped nano-TiO2 could be activated by visible light and could thus be used as an effective catalyst in photo-oxidation reactions. The synergistic effect of Fe and La co-doping played an important role in improving the photocatalytic activity. In addition, the possibility of cyclic usage of co-doped nano-TiO2 was also confirmed, the photocatalytic activity of codoped nano-TiO2 remained above 89.6% of the fresh sample after being used four times.展开更多
[Objective]This paper aimed at studying the liquefaction technology of chestnut shells [Method]Effects on chestnut shells liquefaction of six catalysts were studied,which were sodium hydroxide,sodium carbonate,acetic ...[Objective]This paper aimed at studying the liquefaction technology of chestnut shells [Method]Effects on chestnut shells liquefaction of six catalysts were studied,which were sodium hydroxide,sodium carbonate,acetic acid(99.5%),phosphoric acid(85%),hydrochloric acid(37%),sulfuric acid(98%).The research had analyzed the liquefaction effects of chestnut shells in presence of phenol and at liquefaction temperatures of 130,150 and 170 ℃,in which the proportion of added quantities of concentrated sulfuric acid,phosphoric acid,concentrated hydrochloric acid to phenol were 1%-6%.Properties of phenolic resin made from formaldehyde and phenol-liquefied products of chestnut shells catalyzed by concentrated sulfuric acid with an added amount of 4% at 150 ℃(WPF)were analyzed and compared with traditional phenolic formaldehyde resin(PF).[Result]Acid catalysts were better than alkaline ones in the phenol-liquefaction of chestnut shells,and the liquefaction ratio increased with the increasing of acidic intensity.The liquefaction ratio had attained the maximum as 92.11 % when catalyzed by concentrated sulfuric acid with an added amount of 4% at 150 ℃.The phenolic resin made from the liquefied products of chestnut shells was basically in accordance with the standard of GB/T 14732-93 when the mass ratio of chestnut shells powders to phenol was 1∶3.[Conclusion]It was possible to produce phenolic resin with liquefied chestnut shells.展开更多
In order to improve the photocatalytic performance of mesoporous titania under visible light, a series of photocatalysts of S and Ag co-doped mesoporous titania have been successfully prepared by template method using...In order to improve the photocatalytic performance of mesoporous titania under visible light, a series of photocatalysts of S and Ag co-doped mesoporous titania have been successfully prepared by template method using thiourea, AgNO3 and tetrabutyl titanate as precursors and Pluronic P123 (EO20PO70EO20) as template. Scanning electron microscopy (SEM), X-ray diffraction (XRD), nitrogen adsorption-desorption measurements, and UV-visible spectroscopy (UV-Vis) were employed to characterize the morphology, crystal structure, surface structure, and optical absorption properties of the samples. The microcrystal of the photocatalysts consisted of anatase phase and was approximately present in the form of spherical particle. The photocatalytic performance was studied by photodegradation methyl orange (MO) in water under UV and visible light irradiation. The calcination temperature and the doping content influenced the photoactivity. In addition, the possibility of cyclic usage of co-doped mesoporous titania was also confirmed, the photocatalytic activity of mesoporous titania remained above 89% of that of the fresh sample after being used four times. It was shown that the co-doped mesoporous titania could be activated by visible light and could thus be potentially applied for the treatment of water contaminated by organic pollutants. The synergistic effect of sulfur and silver co-doping played an important role in improving the photocatalytic activity.展开更多
Ultrafine noble metal nanoparticles (Pt, Pd, or Au) co-catalyst loaded on the surface of rutile and brookite TiO2 were prepared via a simple photo-deposition strategy under high vacuum conditions. The properties of ...Ultrafine noble metal nanoparticles (Pt, Pd, or Au) co-catalyst loaded on the surface of rutile and brookite TiO2 were prepared via a simple photo-deposition strategy under high vacuum conditions. The properties of the prepared samples were determined by different characterization techniques, including X-ray diffraction, transmission electron microscopy, diffuse reflectance ultraviolet-visible spectroscopy, and photoluminescence spectroscopy. The photocatalytic performance of the samples was evaluated by monitoring the reforming of methanol. Co-catalyst loading greatly improved the photocatalytic activity of TiO2. Specifically, Pt-TiO2 displayed the highest photocatalytic activity among all samples studied, followed by Pd-TiO2 and then Au-TiO2. Furthermore, this photocatalytic behavior was not influenced by the intrinsic nature of the TiO2 semiconductor photocatalyst. Similar photocatalytic activity trends were achieved with both sets of noble metal-loaded photocatalysts prepared using rutile and brookite TiO2 as supports. By examining the physicochemical and photocatalytic properties, the factors controlling the photocatalytic activity of the noble metal-loaded TiO2 samples were discussed in detail.展开更多
Nickel nanowire and nanotube arrays as supports for Pt-Pd catalyst were prepared by elec- troless deposition with anodic aluminum oxide template. Pt-Pd composite catalyst was de- posited on the arrays by displacement ...Nickel nanowire and nanotube arrays as supports for Pt-Pd catalyst were prepared by elec- troless deposition with anodic aluminum oxide template. Pt-Pd composite catalyst was de- posited on the arrays by displacement reaction. SEM images show that the nickel nanowires have an average diameter of I00 nm and the nickel nanotubes have an average inner diameter of 200 nm. EDS scanning reveals that elemental Pt and Pd disperse uniformly on the arrays. Cyclic voltammetry study indicates that the nickel nanotube array loaded with Pt-Pd pos- sesses a higher electrochemical activity for ethanol oxidation than the nickel nanowire array with Pt-Pd.展开更多
A ZSM-5/MOR co-crystalline zeolite was synthesized without using the template. The physico-chemical properties of the zeolite were characterized by XRD, FT-IR, SEM and TPD and then compared with the co-crystalline zeo...A ZSM-5/MOR co-crystalline zeolite was synthesized without using the template. The physico-chemical properties of the zeolite were characterized by XRD, FT-IR, SEM and TPD and then compared with the co-crystalline zeolite synthesized with a template. Analytical results indicated that they were similar in structure and composition. The influences ofpH value and Si/Al ratio on synthesis were studied. It was found that a high pH value or a low Si/AI ratio could provide better environment for mordenite (MOR) crystallization. The zeolites applied as catalysts in naphtha catalytic cracking for producing ethylene and propylene showed outstanding catalytic performance with the total yield of ethylene and propylene reaching 55 m%. The process could achieve most favorable efficiency when the catalyst contained 5 m% of MOR.展开更多
Doping heteroatoms into carbon matrix was an efficient strategy to achieve a high-performance non-precious metal oxygen reduction electrocatalyst. Herein, an in situ templated synthesis strategy has been demonstrated ...Doping heteroatoms into carbon matrix was an efficient strategy to achieve a high-performance non-precious metal oxygen reduction electrocatalyst. Herein, an in situ templated synthesis strategy has been demonstrated to fabricate nitrogen, sulfur and iron-tridoped mesoporous carbon nanosheets(NSFC) with FeCl3 as the two-dimensional template. And a protic salt was used as the carbon, nitrogen and sulfur source, which realized one-step preparation of catalyst materials and the co-doping of various heteroatoms simultaneously. As a result, the optimized NSFC catalyst possessed comparable catalytic activity and selectivity, while superior durability and methanol permeability resistance to commercial 30 wt% Pt/C catalyst in alkaline media. Such excellent performance should be ascribed to the efficient multiple-element doping into the large-specific-surface-area and highly stable carbon nanosheets realized by the in situ synthesis route with a novel FeCl3 template.展开更多
A biomorphic CeO2microtube with multiple-pore structure was fabricated by using the cotton as biotemplate,throughcerium nitrate solution infiltration and thermal decomposition.Field emission scanning electron microsco...A biomorphic CeO2microtube with multiple-pore structure was fabricated by using the cotton as biotemplate,throughcerium nitrate solution infiltration and thermal decomposition.Field emission scanning electron microscope(FESEM),powder X-raydiffraction(XRD),transmission electron microscope(TEM),N2adsorption?desorption isotherms,temperature-programmedreduction(TPR)and CO oxidation were used to characterize the samples.The results indicated that the synthesized products werecomposed of crystallites with grain size about9nm and exhibited a fibrous morphology similar to the original template andpossessed a specific surface area(BET)of62.3m2/g.Compared with the conventional CeO2particles,the synthesized materialsshowed a superior catalytic activity for CO oxidation.For the synthesized fibrous CeO2,the CO conversion at320°C was above90%and a100%CO conversion was obtained at410°C.展开更多
Highly active Fe-N_x sites that effectively improve the performance of non-precious metal electrocatalysts for oxygen reduction reactions(ORRs) are desirable. Herein, we propose a strategy for introducing a carbon t...Highly active Fe-N_x sites that effectively improve the performance of non-precious metal electrocatalysts for oxygen reduction reactions(ORRs) are desirable. Herein, we propose a strategy for introducing a carbon template into a melamine/Fe-salt mixture to inductively generate highly active Fe-N_x sites for ORR. Using 57 Fe M?sbauer spectroscopy, X-ray photoelectron spectroscopy, and X-ray diffraction, we studied the structural composition of the Fe and N co-doped carbon catalysts.Interestingly, the results showed that this system not only converted inactive Fe and Fe-carbides into active Fe-N_4 and other Fe-nitrides, but also improved their intrinsic activities.展开更多
Well-aligned open-ended multi-walled carbon nanotube (MWCNT) arrays were prepared via chemical vapor deposition (CVD) method in porous anodic aluminum oxide (AAO) templates without depositing any transition meta...Well-aligned open-ended multi-walled carbon nanotube (MWCNT) arrays were prepared via chemical vapor deposition (CVD) method in porous anodic aluminum oxide (AAO) templates without depositing any transition metals as catalyst. Effects of the CVD temperature and heat treatment were studied in detail. Well-aligned open-ended MWCNT arrays were obtained at the CVD temperature above 600℃; when CVD temperature is reduced to around 550℃, CNTs, CNFs and other structures existed at the same time; no CNTs or carbon nanofibres (CNFs) could be fouad as the CVD temperature is below 500℃, and only amorphous carbon in the porous AAO template was found. Experimental results showed that the AAO template is catalytic during the CVD process, and it has the following two effects: to catalyze thermal decomposition of acetylene and to catalyze conversion of carbon decomposed from acetylene into CNTs or CNFs. Heat treatment could improve the graphitization degree, but it might also introduce new defects.展开更多
Molecular mechanics and quantum mechanics simulations, as molecular simulation methods, were performed to investigate the effects of different surfaces, the promoter Co/Ni, the active phase of MoS2 or WS2, the content...Molecular mechanics and quantum mechanics simulations, as molecular simulation methods, were performed to investigate the effects of different surfaces, the promoter Co/Ni, the active phase of MoS2 or WS2, the content of Si and other factors on the order of interaction between the MoS2 (WS2) single slab and the support surface. The influence of Si content was studied by molecular mechanics, and an advantageous Si content was found. Various surfaces, promoters and active phases also played an important role in the interaction between the support surfaces and active phases, and some significant trends were found out. Quantum mechanics simulation was performed to study the possible effect of electrostatic interaction between the support and the active phase, upon which the calculations suggested that the existence of a favorable Si content was possible. The electronic effects of Co/Ni promoter and the intensity of Co/Mo/Ni/W/Li/AI/Si species bonded to the alumina support were also investigated by quantum mechanics, and it was found that the different electronic effects of Co and Ni might bring forth some obvious influences on the interaction between the support and the active phase. And the results of comparing the intensity of Co/Mo/Ni/W/Li/AI/Si species bonded to the support can also explain the different interaction intensity in various catalyst systems.展开更多
The mesoporous Ti O2 has been synthesized by evaporation induced self assembly(EISA) method. The thermogravimetric/differential scanning calorimetric(TG/DSC), X-ray diffraction(XRD), high-resolution transmission elect...The mesoporous Ti O2 has been synthesized by evaporation induced self assembly(EISA) method. The thermogravimetric/differential scanning calorimetric(TG/DSC), X-ray diffraction(XRD), high-resolution transmission electron microscopy(HR-TEM) and N2 adsorption desorption and adsorption are used to study the effects of the synthesized process condition on the microstructure of the as-synthesized mesoporous Ti O2. The photocatalytic performances of as-synthesized samples are evaluated by the degradation of the formaldehyde under ultraviolet light irradiations. The results demonstrate that the as-synthesized mesoporous Ti O2 are anatase with the uniform size about 20-40 nm. The sample is prepared using cetyltrimethyl ammonium bromide(CTAB) as the template with average pore size distribution of 8.12 nm, specific surface area of 68.47 m2/g and pore volume of 0.213 m L/g. The samples show decomposition of formaldehyde 95.8% under ultraviolet light irradiations for 90 min. These results provide a basic experimental process for preparation mesoporous Ti O2, which will posses a broad prospect in terms of the applications in improving indoor air quality.展开更多
Titanium dioxide (TiO2) is widely employed as a solid photocatalyst for solar energy conversion and envi- ronmental remediation. The ability to construct porous TiO2 with controlled particle size and narrowed bandga...Titanium dioxide (TiO2) is widely employed as a solid photocatalyst for solar energy conversion and envi- ronmental remediation. The ability to construct porous TiO2 with controlled particle size and narrowed bandgap is an essential requirement for the design of highly efficient and recyclable photocatalysts. Here, we report a template- free acetic acid induced method for the synthesis of visible- light responsive carbon-doped TiO2 microplates with high crystallinity and mesoporous structure. It is shown that the electron-withdrawing bidentate carboxylate ligands derived from acetic acid can narrow the bandgap of TiO2 (1.84 eV) substantially. Moreover, the resultant microplate photo- catalysts exhibit excellent photocatalytic efficiency and solid-liquid separation performance, which will be bene- ficial for future industrial applications.展开更多
Here we report a hydrothermal approach to build and tailor the hierarchical structure of brookite TiO_2 crystal under multiple hierarchical scales. Benefiting from the hierarchical structure and the existence of oxyge...Here we report a hydrothermal approach to build and tailor the hierarchical structure of brookite TiO_2 crystal under multiple hierarchical scales. Benefiting from the hierarchical structure and the existence of oxygen vacancy,these as-prepared hierarchical brookite TiO_2 crystals can not only enhance photocatalytic activity, but also demonstrate their potential in the treatment of superficial malignant tumor.展开更多
Developing low-cost, high-performance elec- trocatalysts for the oxygen reduction reaction (ORR) is crucial for implementation of fuel cells and metal-air batteries into practical applications. Graphene-based cataly...Developing low-cost, high-performance elec- trocatalysts for the oxygen reduction reaction (ORR) is crucial for implementation of fuel cells and metal-air batteries into practical applications. Graphene-based catalysts have been extensively investigated for ORR in alkaline electrolytes. However, their performance in acidic electrolytes still requires further improvement compared to the Pt/C catalyst. Here we report a self-templating approach to prepare graphene-based sandwich-like porous carbon nanosheets for efficient ORR in both alkaline and acidic electrolytes. Graphene oxides were first used to adsorb m-phenylenediamine molecules which can form a nitrogen-rich polymer network after oxidative poly- merization. Then iron (Fe) salt was introduced into the polymer network and transformed into ORR active Fe-N-C sites along with Fe, FeS, and FEN0.05 nanopartides after pyr- olysis, generating ORR active sandwich-like carbon na- nosheets. Due to the presence of multiple ORR active sites. The as-obtained catalyst exhibited prominent ORR activity with a half-wave potential -30 mV more positive than Pt/C in 0.1 mol L-1 KOH, while the half-wave potential of the catalyst was only -40 mV lower than that of commercial Pt/C in 0.1 mol L-1 HClO4. The unique planar sandwich-like structure could expose abundant active sites for ORR. Meanwhile, the graphene layer and porous structure could simultaneously enhance electrical conductivity and facilitate mass transport. The prominent electrocatalytic activity and durability in both alkaline and acidic electrolytes indicate that these carbon na- nosheets hold great potential as alternatives to precious metal- based catalysts, as demonstrated in zinc-air batteries and proton exchange membrane fuel cells.展开更多
Herein is reported the soft-templating synthesis of visible-light photoactive bismuth ferrite (BiFeO3) nanoarchitectures in the form of thin fihns using a poly(ethylene-co-butylene)-block-poly(ethylene oxide) di...Herein is reported the soft-templating synthesis of visible-light photoactive bismuth ferrite (BiFeO3) nanoarchitectures in the form of thin fihns using a poly(ethylene-co-butylene)-block-poly(ethylene oxide) diblock copolymer as the structure-directing agent. We establish that (1) the self-assembled materials employed in this work are highly crystalline after annealing at 550 ℃ in air and that (2) neither the bismuth-poor Bi2Fe4O9 phase nor other impurity phases are formed. We further show that there is a distinct restructuring of the high quality cubic pore network of amorphous BiFeO3 during crystallization. This restructuring leads to films with a unique architecture that is composed of anisotropic crystallites intermingled with a continuous mesoporosity. While this article focuses on the characterization of these novel materials by electron microscopy, krypton physisorption, grazing incidence small-angle X-ray scattering, time-of-flight secondary ion mass spectrometry, X-ray photoelectron spectroscopy, UV-vis and Raman spectroscopy, we also examine the photocatalytic properties and show the benefits of the combination of mesoporosity and nanocrystallinity. Templated BiFeO3 thin films (25% porosity) with a direct optical band gap at 2.9 eV exhibit a catalytic activity for the degradation of rhodamine B much better than that of nontemplated samples. We attribute this improvement to the nanoscale porosity, which provides for more available active sites on the photocatalyst.展开更多
Controlled synthesis of hierarchically assembled titanium dioxide (TiO2) nano- structures is important for practical applications in environmental purification and solar energy conversion. We present here the fabric...Controlled synthesis of hierarchically assembled titanium dioxide (TiO2) nano- structures is important for practical applications in environmental purification and solar energy conversion. We present here the fabrication of interconnected TiO2 nanotubes as a macroscopic bulk material by using a porous carbon nanotube (CNT) sponge as a template. The basic idea is to uniformly coat an amorphous titania layer onto the CNT surface by the infiltration of a TiO2 precursor into the sponge followed by a subsequent hydrolysis process. After calcination, the CNTs are completely removed and the titania is simultaneously crystallized, which results in a porous macrostructure composed of interconnected anatase TiO2 nanotubes. The TiO2 nanotube macrostructures show comparable photocatalytic activities to commercial products (AEROXIDE TiO2 P25) for the degradation of rhodamine B (RhB). Moreover, the TiO2 nanotube macrostructures can be settled and separated from water within 12 h after photocatalysis, whereas P25 remains suspended in solution after weeks. Thus the TiO2 nanotube macrostructures offer the advantage of easy catalyst separation and recycle and can be a promising candidate for wastewater treatment.展开更多
In various temperatures, the effects of inorganic acids on the free phenol level in liquefaction products were investigated. In this paper, the free phenol level was used as an indicator to evaluate liquefaction effic...In various temperatures, the effects of inorganic acids on the free phenol level in liquefaction products were investigated. In this paper, the free phenol level was used as an indicator to evaluate liquefaction efficiency. Results showed that sulfuric acid was the best among the 4 acids. Under the condition of reaction temperature 150 ~C, reaction time 1.5 h, liquefaction ratio (liquid ! particleboard) 4 and content of sulfuric acid 6%, the free phenol level in the liquefaction products of waste particleboard is 36.95%, and that of original particleboard is 24.27%.展开更多
To improve the contact between platinum catalyst and titanium substrate, a layer of TiO2 nanotube arrays has been synthesized before depositing Pt nanoflowers by pulse electrodeposition. Dramatic improvements in elect...To improve the contact between platinum catalyst and titanium substrate, a layer of TiO2 nanotube arrays has been synthesized before depositing Pt nanoflowers by pulse electrodeposition. Dramatic improvements in electrocatalytic activity (3x) and stability (60x) for methanol oxidation were found, suggesting promising applications in direct methanol fuel cells. The 3x and 60x improvements persist for Pt/Pd catalysts used to overcome the CO poisoning problem.展开更多
文摘A series of photocatalysts of un-doped, single-doped and co-doped nanometer titanium diox- ide (TiO2) have been successfully prepared by template method using Fe(NO3)3.9H2O, La(NO3)3.6H2O, and tetrabutyl titanate as precursors and glucan as template. Scanning electron microscopy, X-ray diffraction, and N2 adsorption-desorption measurement were employed to characterize the morphology, crystal structure and surface structure of the samples. The photo-absorbance of the obtained catalysts was measured by UV-Vis absorption spectroscopy, and the photocatalytic activities of the prepared samples under UV and visible light were estimated by measuring the degradation rate of methyl orange in an aqueous solution. The characterizations indicated that the prepared photocatalysts consisted of anatase phase and possessed high surface area of ca. 163-176 m2/g. It was shown that the Fe and La co-doped nano-TiO2 could be activated by visible light and could thus be used as an effective catalyst in photo-oxidation reactions. The synergistic effect of Fe and La co-doping played an important role in improving the photocatalytic activity. In addition, the possibility of cyclic usage of co-doped nano-TiO2 was also confirmed, the photocatalytic activity of codoped nano-TiO2 remained above 89.6% of the fresh sample after being used four times.
基金Supported by Project of Beijing Municipal Science and Technology Commission(Z07090500550704)the Key Scientific and Technological Project of Henan Province(102102210447)~~
文摘[Objective]This paper aimed at studying the liquefaction technology of chestnut shells [Method]Effects on chestnut shells liquefaction of six catalysts were studied,which were sodium hydroxide,sodium carbonate,acetic acid(99.5%),phosphoric acid(85%),hydrochloric acid(37%),sulfuric acid(98%).The research had analyzed the liquefaction effects of chestnut shells in presence of phenol and at liquefaction temperatures of 130,150 and 170 ℃,in which the proportion of added quantities of concentrated sulfuric acid,phosphoric acid,concentrated hydrochloric acid to phenol were 1%-6%.Properties of phenolic resin made from formaldehyde and phenol-liquefied products of chestnut shells catalyzed by concentrated sulfuric acid with an added amount of 4% at 150 ℃(WPF)were analyzed and compared with traditional phenolic formaldehyde resin(PF).[Result]Acid catalysts were better than alkaline ones in the phenol-liquefaction of chestnut shells,and the liquefaction ratio increased with the increasing of acidic intensity.The liquefaction ratio had attained the maximum as 92.11 % when catalyzed by concentrated sulfuric acid with an added amount of 4% at 150 ℃.The phenolic resin made from the liquefied products of chestnut shells was basically in accordance with the standard of GB/T 14732-93 when the mass ratio of chestnut shells powders to phenol was 1∶3.[Conclusion]It was possible to produce phenolic resin with liquefied chestnut shells.
基金This work was supported by the National Natural Sci- ence Foundation of China (No.41373127) and the Liaoning Provincial Natural Science Foundation of China (No.2013020121).
文摘In order to improve the photocatalytic performance of mesoporous titania under visible light, a series of photocatalysts of S and Ag co-doped mesoporous titania have been successfully prepared by template method using thiourea, AgNO3 and tetrabutyl titanate as precursors and Pluronic P123 (EO20PO70EO20) as template. Scanning electron microscopy (SEM), X-ray diffraction (XRD), nitrogen adsorption-desorption measurements, and UV-visible spectroscopy (UV-Vis) were employed to characterize the morphology, crystal structure, surface structure, and optical absorption properties of the samples. The microcrystal of the photocatalysts consisted of anatase phase and was approximately present in the form of spherical particle. The photocatalytic performance was studied by photodegradation methyl orange (MO) in water under UV and visible light irradiation. The calcination temperature and the doping content influenced the photoactivity. In addition, the possibility of cyclic usage of co-doped mesoporous titania was also confirmed, the photocatalytic activity of mesoporous titania remained above 89% of that of the fresh sample after being used four times. It was shown that the co-doped mesoporous titania could be activated by visible light and could thus be potentially applied for the treatment of water contaminated by organic pollutants. The synergistic effect of sulfur and silver co-doping played an important role in improving the photocatalytic activity.
基金supported by the National Natural Science Foundation of China(21307035)the Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)~~
文摘Ultrafine noble metal nanoparticles (Pt, Pd, or Au) co-catalyst loaded on the surface of rutile and brookite TiO2 were prepared via a simple photo-deposition strategy under high vacuum conditions. The properties of the prepared samples were determined by different characterization techniques, including X-ray diffraction, transmission electron microscopy, diffuse reflectance ultraviolet-visible spectroscopy, and photoluminescence spectroscopy. The photocatalytic performance of the samples was evaluated by monitoring the reforming of methanol. Co-catalyst loading greatly improved the photocatalytic activity of TiO2. Specifically, Pt-TiO2 displayed the highest photocatalytic activity among all samples studied, followed by Pd-TiO2 and then Au-TiO2. Furthermore, this photocatalytic behavior was not influenced by the intrinsic nature of the TiO2 semiconductor photocatalyst. Similar photocatalytic activity trends were achieved with both sets of noble metal-loaded photocatalysts prepared using rutile and brookite TiO2 as supports. By examining the physicochemical and photocatalytic properties, the factors controlling the photocatalytic activity of the noble metal-loaded TiO2 samples were discussed in detail.
文摘Nickel nanowire and nanotube arrays as supports for Pt-Pd catalyst were prepared by elec- troless deposition with anodic aluminum oxide template. Pt-Pd composite catalyst was de- posited on the arrays by displacement reaction. SEM images show that the nickel nanowires have an average diameter of I00 nm and the nickel nanotubes have an average inner diameter of 200 nm. EDS scanning reveals that elemental Pt and Pd disperse uniformly on the arrays. Cyclic voltammetry study indicates that the nickel nanotube array loaded with Pt-Pd pos- sesses a higher electrochemical activity for ethanol oxidation than the nickel nanowire array with Pt-Pd.
基金funded by the National Basic Research Program of China (Project No. 2003CB615804) the joint funding of the National Natural Science Foundation of China and SINOPEC (NO.20736011)
文摘A ZSM-5/MOR co-crystalline zeolite was synthesized without using the template. The physico-chemical properties of the zeolite were characterized by XRD, FT-IR, SEM and TPD and then compared with the co-crystalline zeolite synthesized with a template. Analytical results indicated that they were similar in structure and composition. The influences ofpH value and Si/Al ratio on synthesis were studied. It was found that a high pH value or a low Si/AI ratio could provide better environment for mordenite (MOR) crystallization. The zeolites applied as catalysts in naphtha catalytic cracking for producing ethylene and propylene showed outstanding catalytic performance with the total yield of ethylene and propylene reaching 55 m%. The process could achieve most favorable efficiency when the catalyst contained 5 m% of MOR.
基金supported by the National Natural Science Foundation of China(21273114,21771107)Natural Science Foundation of Jiangsu Province(BK20161484)+3 种基金the Fundamental Research Funds for the Central Universities(NE2015003)the "Six Talent Peaks Program" of Jiangsu Province(2013-XNY-010)Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutionthe Foundation of Graduate Innovation Center in NUAA(kfjj20160613)~~
文摘Doping heteroatoms into carbon matrix was an efficient strategy to achieve a high-performance non-precious metal oxygen reduction electrocatalyst. Herein, an in situ templated synthesis strategy has been demonstrated to fabricate nitrogen, sulfur and iron-tridoped mesoporous carbon nanosheets(NSFC) with FeCl3 as the two-dimensional template. And a protic salt was used as the carbon, nitrogen and sulfur source, which realized one-step preparation of catalyst materials and the co-doping of various heteroatoms simultaneously. As a result, the optimized NSFC catalyst possessed comparable catalytic activity and selectivity, while superior durability and methanol permeability resistance to commercial 30 wt% Pt/C catalyst in alkaline media. Such excellent performance should be ascribed to the efficient multiple-element doping into the large-specific-surface-area and highly stable carbon nanosheets realized by the in situ synthesis route with a novel FeCl3 template.
基金Projects(21277094,51478285,21407111) supported by the National Natural Science Foundation of ChinaProjects(BK20140280,BK20151198) supported by the Natural Science Foundation of Jiangsu Province,China+4 种基金Project(14KJA430004) supported by Collegiate Natural Science Fund of Jiangsu Province,ChinaProject supported by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD),ChinaProject supported by Jiangsu Collaborative Innovation Center of Technology and Material for Water Treatment,ChinaProject supported Excellent Innovation Team in Science and Technology of Education Department of Jiangsu Province,ChinaProjects(SJHG1304,SJHG1310,SJHG1404) supported by the Jiangsu Key Laboratory for Environment Functional Materials,China
文摘A biomorphic CeO2microtube with multiple-pore structure was fabricated by using the cotton as biotemplate,throughcerium nitrate solution infiltration and thermal decomposition.Field emission scanning electron microscope(FESEM),powder X-raydiffraction(XRD),transmission electron microscope(TEM),N2adsorption?desorption isotherms,temperature-programmedreduction(TPR)and CO oxidation were used to characterize the samples.The results indicated that the synthesized products werecomposed of crystallites with grain size about9nm and exhibited a fibrous morphology similar to the original template andpossessed a specific surface area(BET)of62.3m2/g.Compared with the conventional CeO2particles,the synthesized materialsshowed a superior catalytic activity for CO oxidation.For the synthesized fibrous CeO2,the CO conversion at320°C was above90%and a100%CO conversion was obtained at410°C.
文摘Highly active Fe-N_x sites that effectively improve the performance of non-precious metal electrocatalysts for oxygen reduction reactions(ORRs) are desirable. Herein, we propose a strategy for introducing a carbon template into a melamine/Fe-salt mixture to inductively generate highly active Fe-N_x sites for ORR. Using 57 Fe M?sbauer spectroscopy, X-ray photoelectron spectroscopy, and X-ray diffraction, we studied the structural composition of the Fe and N co-doped carbon catalysts.Interestingly, the results showed that this system not only converted inactive Fe and Fe-carbides into active Fe-N_4 and other Fe-nitrides, but also improved their intrinsic activities.
基金This project was supported by the National High Technology Research and Development Program of China (863 Program, No. 2004AA302030) and Na- tional Natural Science Foundation of China (NSFC No. 60574095). Tests and analysis are supported by the United Foundation for Testing &: Analysis in Hefei, Chi- nese Academy of Sciences.
文摘Well-aligned open-ended multi-walled carbon nanotube (MWCNT) arrays were prepared via chemical vapor deposition (CVD) method in porous anodic aluminum oxide (AAO) templates without depositing any transition metals as catalyst. Effects of the CVD temperature and heat treatment were studied in detail. Well-aligned open-ended MWCNT arrays were obtained at the CVD temperature above 600℃; when CVD temperature is reduced to around 550℃, CNTs, CNFs and other structures existed at the same time; no CNTs or carbon nanofibres (CNFs) could be fouad as the CVD temperature is below 500℃, and only amorphous carbon in the porous AAO template was found. Experimental results showed that the AAO template is catalytic during the CVD process, and it has the following two effects: to catalyze thermal decomposition of acetylene and to catalyze conversion of carbon decomposed from acetylene into CNTs or CNFs. Heat treatment could improve the graphitization degree, but it might also introduce new defects.
文摘Molecular mechanics and quantum mechanics simulations, as molecular simulation methods, were performed to investigate the effects of different surfaces, the promoter Co/Ni, the active phase of MoS2 or WS2, the content of Si and other factors on the order of interaction between the MoS2 (WS2) single slab and the support surface. The influence of Si content was studied by molecular mechanics, and an advantageous Si content was found. Various surfaces, promoters and active phases also played an important role in the interaction between the support surfaces and active phases, and some significant trends were found out. Quantum mechanics simulation was performed to study the possible effect of electrostatic interaction between the support and the active phase, upon which the calculations suggested that the existence of a favorable Si content was possible. The electronic effects of Co/Ni promoter and the intensity of Co/Mo/Ni/W/Li/AI/Si species bonded to the alumina support were also investigated by quantum mechanics, and it was found that the different electronic effects of Co and Ni might bring forth some obvious influences on the interaction between the support and the active phase. And the results of comparing the intensity of Co/Mo/Ni/W/Li/AI/Si species bonded to the support can also explain the different interaction intensity in various catalyst systems.
基金Projects(51102026,51272032) supported by the Program for the National Natural Science Foundation of ChinaProject(11A014) supported by the Scientific Research Fund of Hunan Provincial Education DepartmentProject supported by the Aid Program for Science and Technology Innovative Research Team in Higher Educational Instituions of Hunan Province,China
文摘The mesoporous Ti O2 has been synthesized by evaporation induced self assembly(EISA) method. The thermogravimetric/differential scanning calorimetric(TG/DSC), X-ray diffraction(XRD), high-resolution transmission electron microscopy(HR-TEM) and N2 adsorption desorption and adsorption are used to study the effects of the synthesized process condition on the microstructure of the as-synthesized mesoporous Ti O2. The photocatalytic performances of as-synthesized samples are evaluated by the degradation of the formaldehyde under ultraviolet light irradiations. The results demonstrate that the as-synthesized mesoporous Ti O2 are anatase with the uniform size about 20-40 nm. The sample is prepared using cetyltrimethyl ammonium bromide(CTAB) as the template with average pore size distribution of 8.12 nm, specific surface area of 68.47 m2/g and pore volume of 0.213 m L/g. The samples show decomposition of formaldehyde 95.8% under ultraviolet light irradiations for 90 min. These results provide a basic experimental process for preparation mesoporous Ti O2, which will posses a broad prospect in terms of the applications in improving indoor air quality.
基金Acknowledgments This work was supported by the National Natural Science Foundation of China (20966006), the Natural Science Foun- dation of the Inner Mongolia Autonomous Region (2014MS0218), and the Program for Innovative Research Team in Universities of Inner Mongolia Autonomous Region (NMGIRT-A1603).
文摘Titanium dioxide (TiO2) is widely employed as a solid photocatalyst for solar energy conversion and envi- ronmental remediation. The ability to construct porous TiO2 with controlled particle size and narrowed bandgap is an essential requirement for the design of highly efficient and recyclable photocatalysts. Here, we report a template- free acetic acid induced method for the synthesis of visible- light responsive carbon-doped TiO2 microplates with high crystallinity and mesoporous structure. It is shown that the electron-withdrawing bidentate carboxylate ligands derived from acetic acid can narrow the bandgap of TiO2 (1.84 eV) substantially. Moreover, the resultant microplate photo- catalysts exhibit excellent photocatalytic efficiency and solid-liquid separation performance, which will be bene- ficial for future industrial applications.
基金supported by the National Natural Science Foundation of China (21573068)Program of Shanghai Subject Chief Scientist (15XD1501300)+1 种基金the Scientific Research Foundation for the Returned Overseas Chinese Scholars, State Education Ministrythe Fundamental Research Funds for the Central Universities (WD1313009)
文摘Here we report a hydrothermal approach to build and tailor the hierarchical structure of brookite TiO_2 crystal under multiple hierarchical scales. Benefiting from the hierarchical structure and the existence of oxygen vacancy,these as-prepared hierarchical brookite TiO_2 crystals can not only enhance photocatalytic activity, but also demonstrate their potential in the treatment of superficial malignant tumor.
基金supported by the National Basic Research Program of China (973 Program, 2015CB351903)the National Key Research and Development Program (2017YFA0207301)+1 种基金the National Natural Science Foundation of China (51402282, 21474095 and 21476104)CAS Key Research Program of Frontier Sciences (QYZDB-SSW-SLH018)
文摘Developing low-cost, high-performance elec- trocatalysts for the oxygen reduction reaction (ORR) is crucial for implementation of fuel cells and metal-air batteries into practical applications. Graphene-based catalysts have been extensively investigated for ORR in alkaline electrolytes. However, their performance in acidic electrolytes still requires further improvement compared to the Pt/C catalyst. Here we report a self-templating approach to prepare graphene-based sandwich-like porous carbon nanosheets for efficient ORR in both alkaline and acidic electrolytes. Graphene oxides were first used to adsorb m-phenylenediamine molecules which can form a nitrogen-rich polymer network after oxidative poly- merization. Then iron (Fe) salt was introduced into the polymer network and transformed into ORR active Fe-N-C sites along with Fe, FeS, and FEN0.05 nanopartides after pyr- olysis, generating ORR active sandwich-like carbon na- nosheets. Due to the presence of multiple ORR active sites. The as-obtained catalyst exhibited prominent ORR activity with a half-wave potential -30 mV more positive than Pt/C in 0.1 mol L-1 KOH, while the half-wave potential of the catalyst was only -40 mV lower than that of commercial Pt/C in 0.1 mol L-1 HClO4. The unique planar sandwich-like structure could expose abundant active sites for ORR. Meanwhile, the graphene layer and porous structure could simultaneously enhance electrical conductivity and facilitate mass transport. The prominent electrocatalytic activity and durability in both alkaline and acidic electrolytes indicate that these carbon na- nosheets hold great potential as alternatives to precious metal- based catalysts, as demonstrated in zinc-air batteries and proton exchange membrane fuel cells.
文摘Herein is reported the soft-templating synthesis of visible-light photoactive bismuth ferrite (BiFeO3) nanoarchitectures in the form of thin fihns using a poly(ethylene-co-butylene)-block-poly(ethylene oxide) diblock copolymer as the structure-directing agent. We establish that (1) the self-assembled materials employed in this work are highly crystalline after annealing at 550 ℃ in air and that (2) neither the bismuth-poor Bi2Fe4O9 phase nor other impurity phases are formed. We further show that there is a distinct restructuring of the high quality cubic pore network of amorphous BiFeO3 during crystallization. This restructuring leads to films with a unique architecture that is composed of anisotropic crystallites intermingled with a continuous mesoporosity. While this article focuses on the characterization of these novel materials by electron microscopy, krypton physisorption, grazing incidence small-angle X-ray scattering, time-of-flight secondary ion mass spectrometry, X-ray photoelectron spectroscopy, UV-vis and Raman spectroscopy, we also examine the photocatalytic properties and show the benefits of the combination of mesoporosity and nanocrystallinity. Templated BiFeO3 thin films (25% porosity) with a direct optical band gap at 2.9 eV exhibit a catalytic activity for the degradation of rhodamine B much better than that of nontemplated samples. We attribute this improvement to the nanoscale porosity, which provides for more available active sites on the photocatalyst.
文摘Controlled synthesis of hierarchically assembled titanium dioxide (TiO2) nano- structures is important for practical applications in environmental purification and solar energy conversion. We present here the fabrication of interconnected TiO2 nanotubes as a macroscopic bulk material by using a porous carbon nanotube (CNT) sponge as a template. The basic idea is to uniformly coat an amorphous titania layer onto the CNT surface by the infiltration of a TiO2 precursor into the sponge followed by a subsequent hydrolysis process. After calcination, the CNTs are completely removed and the titania is simultaneously crystallized, which results in a porous macrostructure composed of interconnected anatase TiO2 nanotubes. The TiO2 nanotube macrostructures show comparable photocatalytic activities to commercial products (AEROXIDE TiO2 P25) for the degradation of rhodamine B (RhB). Moreover, the TiO2 nanotube macrostructures can be settled and separated from water within 12 h after photocatalysis, whereas P25 remains suspended in solution after weeks. Thus the TiO2 nanotube macrostructures offer the advantage of easy catalyst separation and recycle and can be a promising candidate for wastewater treatment.
文摘In various temperatures, the effects of inorganic acids on the free phenol level in liquefaction products were investigated. In this paper, the free phenol level was used as an indicator to evaluate liquefaction efficiency. Results showed that sulfuric acid was the best among the 4 acids. Under the condition of reaction temperature 150 ~C, reaction time 1.5 h, liquefaction ratio (liquid ! particleboard) 4 and content of sulfuric acid 6%, the free phenol level in the liquefaction products of waste particleboard is 36.95%, and that of original particleboard is 24.27%.
文摘To improve the contact between platinum catalyst and titanium substrate, a layer of TiO2 nanotube arrays has been synthesized before depositing Pt nanoflowers by pulse electrodeposition. Dramatic improvements in electrocatalytic activity (3x) and stability (60x) for methanol oxidation were found, suggesting promising applications in direct methanol fuel cells. The 3x and 60x improvements persist for Pt/Pd catalysts used to overcome the CO poisoning problem.