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1.
The objective of this study was to evaluate the performance of a photocatalysis/H2O2/metal membrane hybrid system in the degradation of humic acid. A metal membrane of nominal pore size 0.5 μm was used in the
experiment for separation of TiO2 particles. Hydrogen peroxide was tested as an oxidant. The efficiency of removal of CODCr and color increased rapidly for initial hydrogen peroxide concentrations up to 50 mg L−1. The efficiency of removal of CODCr and color by 50 mg L−1 initial hydrogen peroxide concentration was approximately 95 and 98%, respectively. However, addition of hydrogen peroxide
over 50 mg L−1 inhibited the efficiency of the system. Addition of hydrogen peroxide to a UV/TiO2 system enhanced efficiency of removal of CODCr and color compared with no addition of hydrogen peroxide. This may be ascribed to capture electrons ejected from TiO2 and to the production of OH radicals. Application of the metal membrane in the UV/TiO2/H2O2 system enhanced the efficiency of removal of CODCr and color because of adsorption by the metal membrane surface and the production of OH radicals. By application of a metal
membrane with a nominal pore size of 0.5 μm, TiO2 particles were effectively separated from the treated water by metal membrane rejection. The photocatalytic metal membrane
had much less resistance than the humic acid, TiO2, and humic acid/TiO2 because of the degradation of humic acid by the photocatalytic reaction. 相似文献
2.
The photocatalytic degradation of natural organic matter (NOM) would be an attractive option in the treatment of drinking water. The performance of a submerged photocatalytic membrane reactor (PMR) was investigated with regard to the removal of NOM and the control of membrane fouling. In particular, this work focused on the adsorption and desorption of humic acids (HA) and lake water NOM at the surface of TiO2 photocatalyts and ferrihydrite (FH) adsorbents in the PMR for water treatment. The addition of FH particles with a large sorption capacity helped remove the NOM released from TiO2 particles, but FH suspended in water affected the photocatalysis of lake water NOM with a low specific UV absorbance (SUVA) value. To prevent the UV light being scattered by FH without any photocatalytic activity, FH particles were attached to a submerged microfiltration (MF) membrane, which contributed to a greater removal of NOM during long-term PMR operation. The further removal of NOM from aqueous solution was achieved due to the synergistic effect of TiO2 photocatalysis and FH adsorption in PMR while minimizing the influence of photoinduced desorption of NOM. No significant membrane fouling occurred when the submerged PMR was operated even at high flux levels (>25 L/m2 h), as long as photocatalytic decomposition took place. 相似文献
3.
T. Ishihara K. Nishida H. Nishiguchi Y. Takita K. Chaki 《Research on Chemical Intermediates》2006,32(3):253-262
A new reforming process was studied using Ni/SiO2 with a hydrogen-permeating membrane reactor. Nickel catalyst supported on SiO2 is highly active for CH4-H2O-O2 reaction in membrane reactor and the reaction close to CH4 + 0.35O2 + 1.3H2O → CO2 + 3.3H2 proceeds at 873 K. Since the selectivity to carbon and CO2 increased and decreased with decreasing contact time respectively, it is considered that the reaction was started by decomposition
of CH4 followed by oxidation of C and water shift reaction. Therefore, the reaction mechanism was different from so-called autothermal
reforming (ATR) reaction. 相似文献
4.
Methanol was synthesized from CO2 and H2 using a silica/alumina composite membrane reactor, which improved methanol conversion to 150% of the value in conventional
reactor, by in situ removal of water formed in catalytic reaction.
This revised version was published online in June 2006 with corrections to the Cover Date. 相似文献
5.
Ignazio Renato Bellobono Riccardo Bianchi Giulia de Martini Paola Maria Tozzi Mauro Luigi Bonardi Flavia Groppi Mauro Rossi 《Journal of Chemometrics》2008,22(7):425-435
Kinetic fitting of substrate disappearance and of total organic carbon (TOC) mineralization of organic micropollutants, in water and air, by photocatalytic membranes immobilizing titanium dioxide, was carried out. A model was used in which mineralization of substrate to CO2 is supposed to occur, with kinetic constant k1, through one single intermediate, mediating the behaviour of all the numerous real intermediates formed in the path to CO2, kinetic constant of formation of the latter being k2. A competitive Langmuirian‐type adsorption of both substrate and ‘intermediate’ was also supposed to be operative, as expressed by pseudo‐thermodynamic constants K1 and K2 respectively, these constants possessing a, partly at least, kinetic significance. Nonlinear models could be fitted to data by using the least‐squares method. The very satisfactory matching is shown for the laboratory‐scale mineralization kinetics of methane, as model molecule of aliphatic contaminants, both in the gas phase and in aqueous solution. Furthermore, in pilot plant experiments, using phenol, as model molecule of aromatics, modelling of quantum yields was carried out, as a function of concentration and of adsorbed radiant power. Kinetics of hydroxyl radicals reacting between themselves, leading to hydrogen peroxide, other than with substrate or intermediates leading to mineralization, was considered, paralleled by a second competition kinetics due to superoxide anion radical and its conjugate acid, equally leading to mineralization. In this model the contribution of hydroxyl radicals to mineralization decreases with irradiance, while the contribution of superoxide anion radical and its conjugate acid increases. If the regression equations of these two contributions are considered together, in a linear combination, the surface model perfectly fits the experimental data. Copyright © 2008 John Wiley & Sons, Ltd. 相似文献
6.
Mariana Ionita Livia Elena Crica Stefan Ioan Voicu Andreea Madalina Pandele Horia Iovu 《先进技术聚合物》2016,27(3):350-357
Cellulose triacetate (AC)/graphene oxide (GO) porous membranes were successfully fabricated by combining ultrasonication and phase inversion method. The structures and morphologies of the resultant composite membranes were investigated by X‐ray diffraction (XRD), scanning electron microscopy, and transmission electron microscopy, respectively. Microscopic and X‐ray diffraction measurements revealed that GO sheets were uniformly dispersed within the AC matrix. The pore size and structure were modulated by changing GO concentration from 0.25 to 1 wt%. Membrane thermal properties were also studied. Among all tested membranes, the most favorable GO amount was 1 wt%, giving Td3% of 274°C, which represents a 22°C enhancement compared with AC. Conversely, the membranes showed improved barrier properties against water and ethanol. The decrease of both ethanol and water fluxes was assigned to the stabilization of composite membrane structure, as a result of GO progressive addition. Bovine serum albumin rejection assay indicated an increasing from 78% in the case of CA membrane to 99% in the case of CA/GO 1 wt% of the rejection degree after 90 min. Copyright © 2015 John Wiley & Sons, Ltd. 相似文献
7.
Hydrogen production from coke oven gas over LiNi/γ-Al2O3 catalyst modified by rare earth metal oxide in a membrane reactor
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Zhibin Yang Yunyan Zhang Weizhong Ding Yuwen Zhang Peijun Shen Yuding Zhou Yong Liu Shaoqing Huang Xionggang Lu 《天然气化学杂志》2009,18(4):407-414
The performance of LiNi/r-Al2O3 catalysts modified by rare earth metal oxide (La2O3 or CeO2) packed on BCFNO membrane reactor was
discussed for the partial oxidation of methane (POM) in coke oven gas (COG) at 875 ◦C. The NiO/r-Al2O3 catalysts with different amounts of
La2O3 and CeO2 were prepared with the same preparation method and under the same condition in order to compare the reaction performance
(oxygen permeation, CH4 conversion, H2 and CO selectivity) on the membrane reactor. The results show that the oxygen permeation flux
increased significantly with LiNiREOx/r-Al2O3 (RE = La or Ce) catalysts by adding the element of rare earth especially the Ce during the
POM in COG. Such as, the Li15wt%CeO29wt%NiO/
-Al2O3 catalyst with an oxygen permeation flux of 24.71 ml·cm−2·min−1 and a high
CH4 conversion was obtained in 875 ◦C. The resulted high oxygen permeation flux may be due to the added Ce that inhibited the strong
interaction between Ni and Al2O3 to form the NiAl2O4 phase. In addition, the introduction of Ce leads up to an important property of storing
and releasing oxygen. 相似文献
8.
Pei Chen Xinbing Chen Xiangshu Chen Hidetoshi Kita 《Journal of membrane science》2009,330(1-2):369-378
The preparation of the supported titanium silicalite-1 (TS-1) zeolite membrane with inexpensive tetrapropylammonium bromide (TPABr)/weak base synthesis system was studied by three methods, and the catalytic activity of the obtained TS-1 zeolite membrane was evaluated with the oxidation of 2-propanol (IPA) under pervaporation condition. It was found that TS-1 zeolite membrane could be successfully prepared with “seeding” or “seeding in situ” method, but could not be achieved with “in situ” method. Adding a little amount of promoter ions of PO43− into the synthesis gel was of benefit to the catalytic activity of the prepared TS-1 zeolite membrane, but had no obvious effect on the membrane layer formation on the mullite porous support. For “seeding” method, the membrane prepared with the synthesis gel having molar composition of SiO2:0.1TPABr:0.9Et2NH:0.03TiO2:80H2O:0.06H3PO4 at 150 °C for 48 h showed the highest oxidation conversion of IPA of 72% accompanied by a flux of 0.35 kg/m2 h. Further more, much higher IPA oxidation conversion of 76% accompanied by a flux of 0.65 kg/m2 h was obtained for the TS-1 zeolite membrane prepared with the same synthesis gel by “seeding in situ” method at 150 °C for 72 h. 相似文献
9.
Peter J. Dowding James W. Goodwin Brian Vincent 《Colloids and surfaces. A, Physicochemical and engineering aspects》2001,180(3):301-309
The work described focuses on a two-stage process for the production of large porous suspension polymer beads of defined particle size and narrow size distribution. Emulsification has been performed using purpose built cross-flow membrane equipment, which allows controlled production of large emulsion droplets with a much narrower size distribution. The work described compares the production of large emulsion droplets of monomer prepared both by agitation and using a cross-flow membrane. The effects of variations in the pore size of the membrane and flow-rates on the size of the emulsion droplets produced are also investigated. The second stage of the process is polymerisation of performed monomer emulsion droplets using a continuous tubular reactor. Samples polymerised using such a method show a narrower size distribution than similar systems polymerised as a batch. 相似文献
10.
The emergence of cuprous oxide (Cu2O) as a visible light active semiconductor for photocatalytic and photoelectrochemical applications has elevated significantly over the past decade. With photocorrosion identified as a severe issue for Cu2O, its photoactivity has been greatly restricted. Given that Cu2O redox potentials are located in between its band gap, the possible occurrence of self-photoreduction or self-oxidation upon illumination is inevitable. Various efforts have been directed to implement effective strategies in enhancing the photostability of Cu2O. In particular, most of the studies focused on improving the charge transfer from Cu2O to reactants or co-catalyst to avoid accumulation of charge within the particles. This review presents recent research progresses for the development of strategies to suppress Cu2O photocorrosion in regards to its intrinsic properties and charge kinetics. It is shown that effective transport of electrons or holes out of Cu2O photocatalyst by engineering its crystal structure, tuning its reaction environment or depositing secondary elements could effectively inhibit Cu2O from experiencing self-photodecomposition. Understanding of the charge dynamics with respect to its photocorrosion is pivotal to optimize the design of Cu2O photocatalyst for enhanced performance in the future. 相似文献
11.
《Arabian Journal of Chemistry》2019,12(7):897-907
A hybrid catalyst composed of a platinum thin layer and modified with manganese oxide (MnOx) is recommended for the oxygen evolution reaction (OER). The Pt layer of the catalyst was physically sputtered onto a TiOx-coated Si substrate (this TiOx layer was sputtered inbetween the Si substrate and Pt layer to improve their adhesion and prevent their mutual diffusion). On top of the Pt layer, another thin TiOx layer (∼60 nm) was spun before the electrochemical deposition of MnOx. The investigation focused primarily to evaluate the impact of the catalyst’s annealing in oxygen atmosphere on its catalytic activity toward OER. Interestingly, before the modification with MnOx, a large catalytic enhancement both in activity (∼228 mV negative shift at 20 mA cm−2 if compared to conventional bare Pt catalysts) and stability was achieved at the catalyst annealed at 600 °C toward OER in 0.5 M KOH. Surprisingly, the addition of MnOx to the catalyst synergized a boosted activity amplifying the negative shift to 470 mV at the same current density. Bunch of materials and electrochemical techniques were combined to reveal important remarks about the catalyst’s morphology, structure, composition and intrinsic activity which was attributed to electronic rather than geometric factors. 相似文献
12.
Kazuki Akamatsu Masataka Nakane Takashi Sugawara Tadashi Hattori Shin-ichi Nakao 《Journal of membrane science》2008
We have successfully developed a membrane reactor for decomposing hydrogen sulfide into hydrogen using an amorphous silica membrane for the first time. The membrane was prepared by the CVD method with tetramethoxysilane and oxygen, and showed excellent hydrogen permeance at 873 K of the order of 10−7 mol m−2 s−1 Pa−1 and high hydrogen/nitrogen permselectivity of 104. The membrane reactor constructed with our membrane and a commercially available catalyst decomposed hydrogen sulfide into hydrogen with higher conversion than the equilibrium conversion. This conversion enhancement was because of the selective extraction of hydrogen from the reaction side to the permeate side by the silica membrane. 相似文献
13.
F-doped TiO2 (FTO) powders were synthesized by spray pyrolysis (SP) from an aqueous solution of H2TiF6. The resulting FTO powders possessed spherical particles with a rough surface morphology and a strong surface acidity. The fluorine concentrations in the FTO powders calculated from XPS spectra significantly depended on SP temperature and ranged from 2.76 to 9.40 at.%. The FTO powder prepared at SP temperature of 1173 K demonstrated the highest photocatalytic activity for the decomposition of gas-phase acetaldehyde under both ultraviolet (UV) and visible light (vis) irradiations, and it was higher than that of commercial P 25. This high photocatalytic activity was ascribed to several beneficial effects produced by F-doping: enhancement of surface acidity, creation of oxygen vacancies, and increase of active sites. It was interesting to point out that the vis photocatalytic activity of FTO powders was achieved by the creation of surface oxygen vacancies rather than the improvement of optical absorption property of bulk TiO2 in vis region. 相似文献
14.
A membrane reactor consisting of two recirculating flow systems connected via a membrane module has been constructed and used to study the dehydrogenation of cyclohexane. When the reactor is operated differentially it is possible to obtain the same information that is generated when using more conventional steady flow reactors. The batch system has the advantages of easily varying the ratio of membrane area to reactor volume and sampling a very wide range of effective Damköhler numbers. These are important variables in design studies. This ability has been demonstrated for the dehydrogenation of cyclohexane. The batch system reproduced results from studies using a more conventional flow reactor. In addition, with the batch reactor it was possible to experimentally confirm predictions that were based upon computer simulation but which were outside the range of experimental study for the conventional reactors used. 相似文献
15.
《印度化学会志》2021,98(11):100213
Synthesis of nanoparticles having low chemical toxicity has been interest of researchers for decades. Utilization of plant phytochemicals as reducing agent is now a globally recognized alternative technique for environmental friendly and low-cost production of nanoparticles. This work reports a facile green synthesis protocol of Nickel Oxide nanoparticles (NiO NPs) using fresh tea leaf extract. The synthesized nanoparticles have been characterized through various analytical techniques like Powder XRD (P-XRD), Fourier Transform Infrared Spectroscopy (FT-IR), Transmission electron microscopy (TEM), Scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS). The XRD results reveal the formation of crystalline nickel oxide nanoparticles. FTIR spectrum displays the existence of different polyphenolic groups over NiO NPs surface. TEM and SEM images indicate the formation of slightly agglomerated spherical nanoparticles with particle size 3–5 nm. The nanoparticles were used towards the photocatalytic degradation of both cationic, anionic dyes and their mixtures under optimum conditions in the presence of UV light irradiation. More than 95% degradation was observed for all the dye solutions with 30 mg L-1 catalytic dose. Moreover, the degradation efficiency of the nanoparticle was studied by altering various parameters like pH, initial dye concentration and amount of catalytic dose. Pseudo first order kinetic model was employed in all the reactions. A detailed mechanism and kinetics of the all the reactions were studied. Interestingly, the catalyst showed excellent recyclability up-to 4th cycles with very low catalytic activity loss. 相似文献
16.
甲苯是一种最常见的室内有毒挥发性有机物(VOCs),目前消除方法主要有吸附、催化燃烧和光催化氧化,其中光催化是一种最高效和经济可行的方法,能在较温和条件下将甲苯完全矿化为 CO2.作为研究最广泛的光催化剂, TiO2在应用中通常有锐钛矿(ATiO2)和金红石(RTiO2)两种物相,但单物相 TiO2的低量子产率和光生电子-空穴对的快速复合严重限制了它的应用.本文选择兼具锐钛矿和金红石两种物相的 P25为催化剂载体,通过负载少量 ZnO和构建多组分并具备多通道载流子分离功能的异质结以提高 TiO2基光催化剂的性能.
利用一步浸渍法制备了一系列 ZnO/P25复合光催化剂,考察了其光催化降解气相甲苯性能. X射线粉末衍射结果表明, ZnO/P25异质光催化剂是由 ATiO2, RTiO2和红锌矿三种物相结构组成.高分辨透射电镜结果表明, ZnO/P25具备三相异质结 ZnO(002)/ATiO2(101)/RTiO2(110).紫外可见光谱、荧光光谱和光电流表征结果表明, ZnO/P25所形成的三相异质结不但增强了光吸收能力,还实现了多通道电子/空穴分离.催化降解实验表明, ZnO/P25异质光催化剂能在室温紫外光辐射下将甲苯完全矿化为 CO2和 H2O.基于三相异质结和多通道光生电子-空穴对分离的形成及促进作用, ZnO/P25光催化活性和速率均明显高于 P25.本文报道的多通道载流子分离理念可为高效光催化剂设计和应用提供一种新思路. 相似文献
利用一步浸渍法制备了一系列 ZnO/P25复合光催化剂,考察了其光催化降解气相甲苯性能. X射线粉末衍射结果表明, ZnO/P25异质光催化剂是由 ATiO2, RTiO2和红锌矿三种物相结构组成.高分辨透射电镜结果表明, ZnO/P25具备三相异质结 ZnO(002)/ATiO2(101)/RTiO2(110).紫外可见光谱、荧光光谱和光电流表征结果表明, ZnO/P25所形成的三相异质结不但增强了光吸收能力,还实现了多通道电子/空穴分离.催化降解实验表明, ZnO/P25异质光催化剂能在室温紫外光辐射下将甲苯完全矿化为 CO2和 H2O.基于三相异质结和多通道光生电子-空穴对分离的形成及促进作用, ZnO/P25光催化活性和速率均明显高于 P25.本文报道的多通道载流子分离理念可为高效光催化剂设计和应用提供一种新思路. 相似文献
17.
Fast and effective protein digestion is a vital process for mass spectrometry (MS) based protein analysis. This study introduces a porous polymer membrane enzyme reactor (PPMER) coupled to nanoflow liquid chromatography-tandem MS (nLC-ESI-MS/MS) for on-line digestion and analysis of proteins. Poly (styrene-co-maleic anhydride) (PS-co-MAn) was fabricated by the breath figure method to make a porous polymer membrane in which the MAn group was covalently bound to enzyme. Based on this strategy, microscale PPMER (μPPMER) was constructed for on-line connection with the nLC-ESI-MS/MS system. Its capability for enzymatic digestion with bovine serum albumin (BSA) was evaluated with varied digestion periods. The on-line proteolysis of BSA and subsequent analysis with μPPMER-nLC-ESI-MS/MS revealed that peptide sequence coverage increased from 10.3% (digestion time 10 min) to 89.1% (digestion time 30 min). μPPMER can efficiently digest proteins due to the microscopic confinement effect, showing its potential application in fast protein identification and protease immobilization. Applications of on-line digestion using μPPMER with human plasma and urinary proteome samples showed that the developed on-line method yielded equivalent or better performance in protein coverage and identified more membrane proteins than the in-solution method. This may be due to easy accommodation of hydrophobic membrane proteins within membrane pores. 相似文献
18.
T. Tsuru T. Morita H. Shintani T. Yoshioka M. Asaeda 《Journal of membrane science》2008,316(1-2):53-62
Hydrogen production by steam reforming of methane using catalytic membrane reactors was investigated first by simulation, then by experimentation. The membrane reactor simulation, using an isothermal and plug-flow model with selective permeation from reactant stream to permeate stream, was conducted to evaluate the effect of permselectivity on membrane reactor performance – such as methane conversion and hydrogen yield – at pressures as high as 1000 kPa. The simulation study, with a target for methane conversion of 0.8, showed that hydrogen yield and production rate have approximately the same dependency on operating conditions, such as reaction pressure, if the permeance ratio of hydrogen over nitrogen ((H2/N2)) is larger than 100 and of H2 over H2O is larger than 15. Catalytic membrane reactors, consisting of a microporous Ni-doped SiO2 top layer and a catalytic support, were prepared and applied experimentally for steam reforming of methane at 500 °C. A bimodal catalytic support, which allows large diffusivity and high dispersion of the metal catalyst, was prepared for the enhancement of membrane catalytic activity. Catalytic membranes having H2 permeances in the range of 2–5 × 10−6 m3 m−2 s−1 kPa−1, with H2/N2 of 25–500 and H2/H2O of 6–15, were examined for steam reforming of methane. Increased performance for the production of hydrogen was experimentally obtained with an increase in reaction-side pressure (as high as 500 kPa), which agreed with the theoretical simulation with no fitting parameters. 相似文献
19.
Michael Dolan Narendra Dave Leigh Morpeth Richard Donelson Daniel Liang Michael Kellam Song Song 《Journal of membrane science》2009
Amorphous alloy membranes composed primarily of Ni and early transition metals (ETMs) are an inexpensive alternative to Pd-based alloy membranes, and these materials are therefore of particular interest for the large-scale production of hydrogen from carbon-based fuels. Catalytic membrane reactors can produce hydrogen directly from coal-derived synthesis gas at 400 °C, by combining a commercial water–gas-shift (WGS) catalyst with a hydrogen-selective membrane. In order to explore the suitability of Ni-based amorphous alloys for this application, the thermal stability and hydrogen permeation characteristics of Ni–ETM amorphous alloy membranes has been examined. A fundamental limitation of these materials is that hydrogen permeability is inversely proportional to the thermal stability of the alloy. Alloy design is therefore a compromise between hydrogen production rate and durability. Amorphous Ni60Nb40−XZrX membranes have been tested at 400 °C in pure hydrogen, and in simulated coal-derived gas streams with high steam, CO and CO2 levels, without severe degradation or corrosion-induced failure. Ni–Nb–Zr amorphous alloys are therefore prospective materials for use in a catalytic membrane reactor for coal-derived syngas. 相似文献
20.
Chih Ming Ma Young Ku Wen Wang Fu Tien Jeng 《Reaction Kinetics and Catalysis Letters》2008,94(2):199-206
The main objective of this study was to develop a simple, energy-efficient photoreactor for operating at room temperature.
In this work, the design of a new gas-phase optical fiber photoreactor (OFP) was introduced which operated under various parameters,
such as the UV light intensity and the initial concentration for the photocatalytic decomposition of acetone. Experimental
results indicated that increasing the UV light intensity or decreasing the initial concentrations of acetone by a UV/TiO2 process would result in improving the decomposition and mineralization efficiencies. The apparent quantum yield of the novel
optical fiber reactor is about 2 to 3 times greater than that of the traditional annular reactor. 相似文献