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1.
A series of highly-hydrophobic MIL-53-Al (MIL = Materials of Institut Lavoisier) frameworks synthesized via decoration of the Al-OH groups by alkyl phosphonic acid were developed as adsorbents for removing acetone from humid gas streams. The newly prepared materials were characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscope (SEM), N2 adsorption-desorption and thermogravimetric analysis (TGA). Their adsorption behaviors toward acetone vapor under dry and wet conditions were studied subsequently. Results showed that alkyl phosphonic acid was successfully grafted into MIL-53-Al skeleton through coordinating interaction with Al3+ generating [email protected]x (x = 12, 14, 18). The [email protected]x exhibited similar crystal structure and thermal stability to parent MIL-53-Al. Furthermore, the modified materials showed significantly enhanced hydrophobicity. The water vapor uptake of [email protected]14 decreased by 72.55% at 75% relative humidity (RH). Dynamic adsorption experiments demonstrated that water vapor had almost no effect on the acetone adsorption performance of [email protected]14. Under the condition of 90% RH, the acetone adsorption capacity of [email protected]14 was 102.98% higher than that of MIL-53-Al. Notably, [email protected]14 presented excellent adsorption reversibility and regeneration performance in 10 adsorption-desorption cycles. Taken together, the strategy of metal-OH group modification is an attractive way to improve the acetone adsorption performance over metal-organic frameworks (MOFs) under humid conditions. Besides, [email protected]14 would be deemed as a promising candidate for capturing acetone in high moisture environment.  相似文献   

2.
MIL-53(Fe) was successfully prepared and deposited on the surface carboxylated polyester (PET) fiber by an optimized conventional solvothermal or industrialized high temperature pressure exhaustion (HTPE) process to develop a PET fiber supported MIL-53(Fe) photocatalyst ([email protected]) for the degradation of polyvinyl alcohol (PVA) in water under light emitting diode (LED) visible irradiation. On the basis of several characterizations, [email protected] was tested for the photocalytic ability and degradation mechanism. It was found that temperature elevation significantly enhanced the formation and deposition of MIL-53(Fe) with better photocatalytic activity. However, higher temperature than 130°C was not in favor of its photocatalytic activity. Increasing the number of surface carboxyl groups of the modified PET fiber could cause a liner improvement in MIL-53(Fe) loading content and photocatalytic ability. High visible irradiation intensity also dramatically increased photocatalytic ability and PVA degradation efficiency of [email protected] Na2S2O8 was used to replace H2O2 as electron acceptor for further promoting PVA degradation in this system. [email protected] prepared by HTPE process showed higher MIL-53(Fe) loading content and slightly lower PVA degradation efficiency than that prepared by solvothermal process at the same conditions. These findings provided a practical strategy for the large-scale production of the supported MIL-53(Fe) as a photocatalyst in the future.  相似文献   

3.
Nitroaromatic explosives are major pollutants produced during wars that cause serious environmental and health problems. The removal of a typical nitroaromatic explosive, 2,4,6-trinitrotoluene (TNT), from aqueous solution, was conducted using a new recyclable magnetic nano-adsorbent ([email protected]2NH2). This adsorbent was prepared by grafting amino groups onto [email protected]2 particles with a well-defined core-shell structure and demonstrated monodispersity in solution. The removal performance of the nano-adsorbent towards TNT was found to be 2.57 and 4.92 times higher than that towards two analogous explosives, 2,4-dinitrotoluene (2,4-DNT) and 2-nitrotoluene (2-NT), respectively, under neutral conditions. The difference in the removal performance among the three compounds was further compared in terms of the effects of different conditions (pH value, ionic strength, humic acid concentration, adsorbent modification degree and dosage, etc.) and the electrostatic potential distributions of the three compounds. The most significant elevation is owing to modification of amino on [email protected]2 which made a 20.7% increase in adsorption efficiency of TNT. The experimental data were well fit by the pseudo-second-order kinetic model and the Freundlich adsorption isotherm model, indicating multilayer adsorption on a heterogeneous surface. The experimental results and theoretical considerations show that the interactions between [email protected]2NH2 NPs and TNT correspond to dipole-dipole and hydrophobic interactions. These interactions should be considered in the design of an adsorbent. Furthermore, the adaptability to aqueous environment and excellent regeneration capacity of [email protected]2NH2 NPs makes these remediation materials promising for applications.  相似文献   

4.
In this paper, highly stable, powerful, and recyclable magnetic nanoparticles tethered N-heterocyclic carbene-palladium(II) ((CH3)3[email protected]3O4) as magnetic nanocatalyst was successfully synthesized from a simplistic multistep synthesis under aerobic conditions through easily available low-cost chemicals. Newly synthesized (CH3)3[email protected]3O4 magnetic nanocatalyst was characterized from various analytical tools and catalytic potential of the (CH3)3[email protected]3O4 magnetic nanocatalyst was studied for the catalytic reduction of toxic 4-nitrophenol (4-NP), hexavalent chromium (Cr(VI)), Methylene Blue (MB) and Methyl Orange (MO) at room temperature in aqueous media. UV-Visible spectroscopy was employed to monitor the reduction reactions. New (CH3)3[email protected]3O4 magnetic nanocatalyst exhibited excellent catalytic activity for the reduction of toxic environmental pollutants. Moreover, (CH3)3[email protected]3O4 magnetic nanocatalyst could be easily and rapidly separated from the reaction mixture with the help of an external magnet and recycled minimum five times in reduction of 4-NP, MB, MO and four times in Cr(VI) without significant loss of catalytic potential and remains stable even after reuse.  相似文献   

5.
The effects of four conditioning approaches:Acid,Acid-zero-valent iron(ZVI)/peroxydisulfate(PMS),Fe(Ⅱ)/PMS and ZVI/PMS,on wastewater activated sludge(WAS) dewatering and organics distribution in supernatant and extracellular polymeric substances(EPS) layers were investigated.The highest reduction in bound water and the most WAS destruction was achieved by Acid-ZVI/PMS,and the optimum conditions were pH 3,ZVI dosage 0.15 g/g dry solid(DS),oxone dosage 0.07 g/g DS and reaction time 10.6 min with the reductions in capillary suction time(CST) and water content(Wc) as 19.67% and 8.49%,respectively.Four conditioning approaches could result in TOC increase in EPS layers and supernatant,and protein(PN) content in tightly bound EPS(TB-EPS).After conditioning,organics in EPS layers could migrate to supernatant.Polysaccharide(PS) was easier to migrate to supernatant than PN.In addition,Acid,Acid-ZVI/PMS or Fe(Ⅱ)/PMS conditioning promoted the release of some polysaccharides containing ring vibrations v P=O,v C-O-C,v C-O-P functional groups from TB-EPS.ESR spectra proved that both radicals of SO_4~-· and·OH contributed to dewatering and organics transformation and migration.CST value of WAS positively correlated with the ratios of PN/PS in LB-EPS and total EPS,while it negatively correlated with TOC,PN content and PS content in TB-EPS,as well as PS content in supernatant and LB-EPS.BWC negatively correlated to zeta potential and TOC value,PN content,and HA content in supernatant.  相似文献   

6.
Urea oxidation reaction (UOR) provides a method for hydrogen production besides wastewater treatment, but the current limited catalytic activity has prevented the application. Herein, we develop a novel H2O2 treatment strategy for tailoring the surface oxygen ligand of NiFe-layered double hydroxides (NiFe-LDH). The sample after H2O2 treatment (NiFeO-LDH) shows significant enhancement on UOR efficiency, with the potential of 1.37 V (RHE) to reach a current density of 10 mA/cm2. The boost is attributed to the richness adsorption O ligand on NiFeO-LDH as revealed by XPS and Raman analysis. DFT calculation indicates formation of two possible types of oxygen ligands: adsorbed oxygen on the surface and exposed from hydroxyl group, lowered the desorption energy of CO2 product, which lead to the lowered onset potential. This strategy is further extended to NiFe-LDH nano sheet on Ni foam to reach a higher current density of 440 mA/cm2 of UOR at 1.8 V (RHE). The facile surface O ligand manipulation is also expected to give chance to many other electro-catalytic oxidations.  相似文献   

7.
The widely used carbamazepine(CBZ) is one of the most persistent pharmaceuticals and suffers insufficient removal efficiency by conventional wastewater treatment.A synthesized Co-based perovskite(LaCoO_3) was used to activate peroxymonosulfate(PMS) in order to degrade CBZ.Results showed that LaCoO_3 exhibited an excellent performance in PMS activation and CBZ degradation at neutral pH,with low cobalt leaching.The results of FT-IR and XPS verified the high structurally and chemically stability of LaCoO_3 in PMS activation.Electron spin resonance(ESR) analysis suggested the generation of radical species,such as sulfate radicals(SO_4·~-) and hydroxyl radicals(·OH).Radical quenching experiments further revealed the responsibility of SO_4·~-as the dominant oxidant for CBZ oxidation.Ten products were detected via the oxidation of CBZ,with the olefinic double bond attacked by SO_4·~-as the initial step.Hydroxylation,hydrolysis,cyclization and dehydration were involved along the transformation of CBZ.The toxicity of CBZ solution was significantly reduced after treating by PMS/LaCoO_3.  相似文献   

8.
The simultaneous electro-oxidation of Ni (II)-citrate and electrodeposition recovery of nickel metal were attempted in a combined electro-oxidation-electrodeposition reactor with a boron-doped diamond (BDD) anode and a polished titanium cathode. Effects of initial nickel citrate concentration, current density, initial pH, electrode spacing, electrolyte type, and initial electrolyte dosage on electrochemical performance were examined. The efficiencies of Ni (II)-citrate removal and nickel metal recovery were determined to be 100% and over 72%, respectively, under the optimized conditions (10 mA/cm2, pH 4.09, 80 mmol/L Na2SO4, initial Ni (II)-citrate concentration of 75 mg/L, electrode spacing of 1 cm, and 180 min of electrolysis). Energy consumption increased with increased current density, and the energy consumption was 0.032 kWh/L at a current density of 10 mA/cm2 (pH 6.58). The deposits at the cathode were characterized by scanning electron microscopy (SEM), energy-dispersive spectrometry (EDS), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). These characterization results indicated that the purity of metallic nickel in cathodic deposition was over 95%. The electrochemical system exhibited a prospective approach to oxidize metal complexes and recover metallic nickel.  相似文献   

9.
Degradation of organic contaminants with simultaneous recycling of Ag+ from silver-containing organic wastewater such as photographic effluents is desired. Although photoelectrocatalysis (PEC) technology is a good candidate for this type of wastewater, its reaction kinetics still needs to be improved. Herein, peroxymonosulfate (PMS) was employed to enhance the PEC kinetics for oxidation of phenol (PhOH) at the anode and reduction of Ag+ at the cathode. The degradation efficiency of phenol (PhOH, 0.1 mmol/L) was increased from 42.8% to 96.9% by adding 5 mmol/L PMS at a potential of 0.25 V. Meanwhile, the Ag (by wt%) deposited on the cathode was 28.1% (Ag2O) in PEC process, while that of Ag (by wt%) was 69.7% (Ag0) by adding PMS. According to the electrochemistry analysis, PMS, as photoelectrons acceptor, enhances the separation efficiency of charges and the direct h+ oxidation of PhOH at the photoanode. Meantime, the increasing cathode potential avoided H2 evolution and strongly alkaline at the surface of cathode, thus enabling the deposition of Ag+ in the form of metallic silver with the help of PMS. In addition, PMS combined with PEC process was effective in treating photographic effluents.  相似文献   

10.
Indoor air quality (IAQ) directly affects the health of occupants. Household manufacturing equipment (HME) used for hobbies or educational purposes is a new and unexplored source of air pollution. In this study, we evaluated the characteristics of particulate and gaseous pollutants produced by a household laser processing equipment (HLPE). Various target materials were tested using a commercial HLPE under various operating conditions of laser power and sheath air flow rate. The mode diameters of the emitted particles gradually decreased as laser power increased, while the particle number concentration (PNC) and particle emission rate (PER) increased. In addition, as the sheath air flow rate quadrupled from 10 to 40 L/min, the mode diameter of the emitted particles decreased by nearly 25%, but the effect on the PNC was insignificant. When the laser induced the target materials at 53 mW, the mode diameters of particles were <150 nm, and PNCs were >2.0 × 104 particles/cm3. Particularly, analyses of sampled aerosols indicated that harmful substances such as sulfur and barium were present in particles emitted from leather. The carcinogenic gaseous pollutants such as acrylonitrile, acetaldehyde, 1,3-butadiene, benzene, and C8 aromatics (ethylbenzene) were emitted from all target materials. In an actual indoor environment, the PNC of inhalable ultrafine particles (UFPs) was >5 × 104 particles/cm3 during 30 min of HLPE operation. Our results suggest that more meticulous control methods are needed, including the use of less harmful target materials along with filters or adsorbents that prevent emission of pollutants.  相似文献   

11.
铁改性掺氮碳纤维活化过一硫酸盐降解双酚A   总被引:2,自引:2,他引:0  
通过静电纺丝制备了Fe和N掺杂改性的碳纳米纤维(Fe-N-CNF),研究了该催化剂活化过一硫酸盐(PMS)降解双酚A(BPA)的性能.以聚丙烯腈为前驱体通过添加FeCl3、尿素、NH4Cl、均苯四甲酸二酐等配制溶胶进行静电纺丝,预氧化并高温碳化后获得Fe-N-CNF,研究了Fe-N-CNF投加量、PMS投加量、溶液初始pH对BPA降解效果的影响.结果表明,当Fe-N-CNF投加量为1 g·L-1,PMS投加量为2 mmol·L-1,初始pH为5时,30 min内对初始浓度为20 mg·L-1 BPA的降解率可达100%.自由基淬灭实验和电子自旋共振波谱(ESR)分析证明,该体系中起主要作用的活性氧物种是O2·-1O2.同时研究了Fe-N-CNF/PMS体系对多种有机污染物的降解效果.  相似文献   

12.
Ultraviolet (UV)/monochloramine (NH2Cl) as an advanced oxidation process was firstly applied for Aspergillus spores inactivation. This study aims to: i) clarify the inactivation and photoreactivation characteristics of UV/NH2Cl process, ii) compared with UV/Cl2 in inactivation efficiency, photoreactivation and energy consumption. The results illustrated that UV/NH2Cl showed better inactivation efficiency than that of UV alone and UV/Cl2, and could effectively control the photoreactivation. For instance, the inactivation rates for Aspergillus flavus, Aspergillus niger and Aspergillus fumigatus in the processes of UV/NH2Cl (2.0 mg/L) was 0.034, 0.030 and 0.061 cm2/mJ, respectively, which were higher than that of UV alone (0.027, 0.026 and 0.024 cm2/mJ) and UV/Cl2 (0.023, 0.026 and 0.031 cm2/mJ). However, there was no synergistic effect for Aspergillus flavus and Aspergillus fumigatus. As for Aspergillus niger, the best synergistic effect can reach 1.86-log10. This may be due to their different resistance to disinfectants, which were related to the size, an outer layer of rodlets (hydrophobins) and pigments. After UV/NH2Cl inactivation, the degree of cell membrane damage and intracellular reactive oxygen species were higher than that of UV alone. UV/NH2Cl had the advantages of high inactivation efficiency and inhibition of photoreactivation, which provides a new entry point for the disinfection of waterborne fungi.  相似文献   

13.
利用共沉淀法成功制备出绿色、高效、具有磁性的介孔Fe/Cu双金属非均相催化剂(Fe-Cu-400),通过X射线衍射仪(XRD)、比表面积测试仪(BET)、场发射扫描电镜(FESEM)及X射线能谱仪(EDS)等表征手段对催化剂的结构、形貌等进行分析,并用制备的Fe-Cu-400催化剂活化过一硫酸盐(PMS)降解四环素(TC),研究了不同反应条件对降解效果的影响.结果表明Fe-Cu-400/PMS体系具有较好的降解效果,随着PMS浓度和初始p H的提高,TC降解效率明显增加;无机阴离子(H2PO-4、HCO-3、Cl-)均对TC的降解有不同程度的促进作用,而NO-3对TC的降解则表现出较弱的抑制作用.Fe-Cu-400在循环使用5次后仍具有较好活化性能.通过自由基抑制实验和XPS测试分析了Fe-Cu-400/PMS体系的活化机制和分解产生的主要活性物种.通过LC-MS结合TOC分析,推测出TC经水解、脱甲基、脱羟基和脱氨基作用达到降解和矿化.  相似文献   

14.
采用超声波(US)和活性碳纤维(ACF)协同活化过一硫酸盐(PMS)产生硫酸根自由基(SO_4~-·)降解偶氮染料酸性橙7(AO7).在US/ACF/PMS体系中,当ACF投加量为0.3 g·L~(-1),n(PMS)/n(AO7)为20/1,US功率密度为10 W·cm~(-2)时,反应30 min后,AO7完全降解.其中,初始pH对AO7降解有较大的影响,pH为2.0时AO7降解效果最好;Cl~-对US/ACF/PMS体系降解AO7有促进作用,Cl-浓度越高,AO7降解速率越快;且ACF在重复使用4次时,协同US活化PMS对AO7仍具有较好的脱色率.通过总有机碳分析发现,US/ACF/PMS体系对染料AO7具有一定的矿化率.采用紫外可见光谱、气相色谱-质谱(GC/MS)对AO7降解过程进行了分析,表明AO7分子中偶氮键及萘环结构均被破坏,并进一步矿化为CO_2和H_2O.  相似文献   

15.
Strongly acidic wastewater produced in nonferrous metal smelting industries often contains high concentrations of Ni(II), which is a valuable metal. In this study, the precipitation of Ni(II) from strongly acidic wastewater using sodium dimethyldithiocarbamate (DDTC) as the precipitant was evaluated. The effects of various factors on precipitation were investigated, and the precipitation mechanism was also identified. Finally, the nickel in the precipitates was recovered following a pyrometallurgical method. The results show that, under optimised conditions (DDTC:Ni(II) molar ratio = 4:1; temperature = 25 °C), the Ni(II) removal efficiency reached 99.3% after 10 min. In strongly acidic wastewater, the dithiocarbamate group of DDTC can react with Ni(II) to form DDTCNi precipitates. Further recovery experiments revealed that high-purity NiO can be obtained by the calcination of DDTCNi precipitates, with the nickel recovery efficiency reaching 98.2%. The gas released during the calcination process was composed of NO2, CS2, H2O, CO2, and SO2. These results provide a basis for an effective Ni(II) recovery method from strongly acidic wastewater.  相似文献   

16.
Electrochemical degradation of 2,4-dichlorophenol (2,4-DCP) in aqueous solution was investigated over Ti/SnO2-Sb anode. The factors influencing the degradation rate, such as applied current density (2-40 mA/cm2), pH (3-11) and initial concentration (5-200 mg/L) were evaluated. The degradation of 2,4-DCP followed apparent pseudo first-order kinetics. The degradation ratio on Ti/SnO2-Sb anode attained > 99.9% after 20 min of electrolysis at initial 5-200 mg/L concentrations at a constant current density of 30 mA/cm2 with a 10 mmol/L sodium sulphate (Na2SO4) supporting electrolyte solution. The results showed that 2,4-DCP (100 mg/L) degradation and total organic carbon (TOC) removal ratio achieved 99.9% and 92.8%, respectively, at the optimal conditions after 30 min electrolysis. Under this condition, the degradation rate constant (k) and the degradation half-life (t1/2) were 0.21 min-1 and (2.8±0.2) min, respectively. Mainly carboxylic acids (propanoic acid, maleic acid, propanedioic acid, acetic acid and oxalic acid) were detected as intermediates. The energy efficiencies for 2,4-DCP degradation (5-200 mg/L) with Ti/SnO2-Sb anode ranged from 0.672 to 1.602 g/kWh. The Ti/SnO2-Sb anode with a high activity to rapid organic oxidation could be employed to degrade chlorophenols, particularly 2,4-DCP in wastewater.  相似文献   

17.
阴极原位产H2O2强化光电催化降解水中EDTA的研究   总被引:1,自引:1,他引:0  
本研究构建了以活性碳纤维(Activated Carbon Fiber,ACF)为阴极,TiO_2/Ti与Ru O_2/Ti为双阳极的光电催化体系.该体系中,Ru O_2/Ti电阳极和TiO_2/Ti光阳极均有氧化作用,可同时氧化降解污染物;且电阳极具有较强析氧作用,能产生大量O_2;ACF阴极具有还原作用,可将体系中产生的O_2原位还原为H_2O_2;H_2O_2在紫外光下产生·OH,进而强化光电催化与电催化氧化过程,实现对水中乙二胺四乙酸二钠(EDTA)的高效去除.本论文详细考察了电流密度、pH、曝气等因素对EDTA降解效果的影响.结果表明,在EDTA初始浓度为300 mg·L~(-1)、溶液初始pH=4.84、电流密度为12 m A·cm~(-2)和光电流密度为0.012 m A·cm~(-2)的条件下,反应90 min后,EDTA降解率高于90%.该催化体系实现了EDTA的高效降解.  相似文献   

18.
电氧化杀藻过程中藻细胞活性变化的研究   总被引:5,自引:1,他引:4  
梁文艳  王珂  阮铃铃  隋丽丽 《环境科学》2010,31(6):1464-1469
由Ti/RuO2棒为阳极、不锈钢管为阴极组成电氧化管式反应装置,采用TTC-脱氢酶活性和中性红染色的活性测定方法,研究了电氧化杀藻中藻活性变化以及影响因素.结果显示,在8mA/cm2下处理30min后,以藻细胞密度计的杀藻率仅为45%,而此时TTC-脱氢酶活性下降了94%,中性红染色率为100%,藻细胞已无法再生长,已全部失活,表明活性指标比细胞密度更能准确反映杀藻处理效果.电解液种类对杀藻存在明显影响,常用电解液Na2SO4和NaNO3的杀藻效果相近,Na2SO4浓度对杀藻效果影响不大.但当电解液中含有0.1mmol/LNaCl时,杀藻效果明显提高,5min后的脱氢酶下降了87%,中性红染色率达到82%.藻样初始浓度对杀藻效果影响较大,细胞密度增大,杀藻效果急剧下降,以天然水为电解液,细胞密度达到水华时的4.4×107个/L,只需处理1min可将藻细胞全部灭活.  相似文献   

19.
In this work a novel anode configuration consisting of an iron mesh double layer is proposed for the electrochemical treatment of wastewater. The removal of Reactive Black 5 dye(RB5) from synthetic contaminated water was used as a model system. At a constant anode surface area, identical process operating parameters and batch process mode, the iron mesh double layer electrode showed better performance compared to the conventional single layer iron mesh. The double layer electrode was characterized by RB5 and chemical oxygen demand(COD) removal efficiency of 98.2% and 97.7%, respectively, kinetic rate constant of 0.0385/min, diffusion coefficient of 4.9 × 10~(-5)cm~2/sec and electrical energy consumption of 20.53 kWh/kgdye removed. In the continuous flow system, the optimum conditions suggested by Response Surface Methodology(RSM) are: initial solution p H of 6.29,current density of 1.6 m A/cm~2, electrolyte dose of 0.15 g/L and flow rate of 11.47 m L/min which resulted in an RB5 removal efficiency of 81.62%.  相似文献   

20.
以一种Cu-MOF(HKUST-1)为模板,将其经不同温度的热处理制备铜氧化物,研究了热处理温度对产物组成及形貌的影响,并通过产物在一系列条件下活化过一硫酸氢钾(PMS)降解水体中罗丹明B(Rh B)的实验探究了其催化性能.XRD、SEM、XPS等表征结果表明,随着热处理温度的升高,产物由Cu2O/CuO混合物逐渐转化为纯相CuO,且模板HKUST-1的原有正八面体结构坍塌加剧.Rh B降解实验的结果显示,催化剂对PMS的活化性能随热处理温度的升高而加强.在中性pH条件下,当PMS投加量为1.00 mmol·L~(-1),CuO-650用量为0.20 g·L~(-1)时,反应时间进行90 min基本可实现Rh B(浓度为0.10mmol·L~(-1))的完全降解.此外,CuO-650还具有pH适用范围较广,铜离子溶出量较低(pH=3条件下为1.309 mg·L~(-1),pH=7条件下为0.987 mg·L~(-1)),循环稳定性较佳的特点,进一步证明CuO-650是一种很有潜力的PMS催化剂.  相似文献   

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