The design and synthesis of non-precious metal dual-functional electrocatalysts through the modulation of electronic structure are important for the development of renewable hydrogen energy.Herein,MnS_(2)/MnO_(2)-CC h...The design and synthesis of non-precious metal dual-functional electrocatalysts through the modulation of electronic structure are important for the development of renewable hydrogen energy.Herein,MnS_(2)/MnO_(2)-CC heterostructure dual-functional catalysts with ultrathin nanosheets were prepared by a twostep electrodeposition method for efficient acidic hydrogen evolution reaction(HER) and degradation of organic wastewater(such as methylene blue(MB)).The electronic structure of Mn atoms at the MnS_(2)/MnO_(2)-CC heterostructure interface is reconfigured under the joint action of S and O atoms.Theoretical calculations show that the Mn d-band electron distribution in MnS_(2)/MnO_(2)-CC catalyst has higher occupied states near the Fermi level compared to the MnO_(2) and MnS_(2) catalysts,which indicates that MnS_(2)/MnO_(2)-CC catalyst has better electron transfer capability and catalytic activity.The MnS_(2)/MnO_(2)-CC catalysts require overpotential of only 66 and 116 mV to reach current density of 10 and 100 mA cm^(-2)in MB/H_(2)SO_(4) media.The MnS_(2)/MnO_(2)-CC catalyst also has a low Tafel slope(26.72 mV dec^(-1)) and excellent stability(the performance does not decay after 20 h of testing).In addition,the MB removal efficiency of the MnS_(2)/MnO_(2)-CC catalyst with a better kinetic rate(0.0226) can reach 97.76%,which is much higher than that of the MnO_(x)-CC catalyst(72.10%).This strategy provides a new way to develop efficient and stable non-precious metal dual-functional electrocatalysts for HER and organic wastewater degradation.展开更多
Investigation was made into the degradation of organic compounds by a dielectric barrier corona discharge (DBCD) system. The DBCD, consisting of a quartz tube, a concentric high voltage electrode and a net wrapped t...Investigation was made into the degradation of organic compounds by a dielectric barrier corona discharge (DBCD) system. The DBCD, consisting of a quartz tube, a concentric high voltage electrode and a net wrapped to the external wall (used as ground electrode), was introduced to generate active species which were sprayed into the organic solution through an aerator fixed on the bottom of the tube. The effect of four factors-the discharge voltage, gas flow rate, solution conductivity, and pH of wastewater, on the degradation efficiency of phenol was assessed. The obtained results demonstrated that this process was an effective method for phenol degradation. The degradation rate was enhanced with the increase in power supplied. The degradation efficiency in alkaline conditions was higher than those in acid and neutral conditions. The optimal gas flow rate for phenol degradation in the system was 1.6 L/min, while the solution conductivity had little effect on the degradation.展开更多
Metal organic frameworks(MOFs)is a research hotspot in the solar fuel production and photo-degradation of pollutants field due to high surface area,rich metal/organic species,large pore volume,and adjustability of str...Metal organic frameworks(MOFs)is a research hotspot in the solar fuel production and photo-degradation of pollutants field due to high surface area,rich metal/organic species,large pore volume,and adjustability of structures and compositions.Therefore,in this review,we first summarized the design factors of photocatalytic materials based on MOF from the perspective of"star"MOF.The modification strategies of MOFs-based photocatalysts were discussed to improve its photocatalytic activity and specific applications were summarized as well,including photocatalytic CO_(2)reduction,photocatalytic water splitting and photo-degradation of pollutants.Finally,the advantages and disadvantages of MOFs-based photocatalysts were discussed,the current challenges were highlighted,and suggestions for future research directions were proposed.展开更多
Metal-based perovskite oxides have contributed significantly to the advanced oxidation processes(AOPs)due to their diverse active sites and excellent compositional/structural flexibility.In this study,we specially des...Metal-based perovskite oxides have contributed significantly to the advanced oxidation processes(AOPs)due to their diverse active sites and excellent compositional/structural flexibility.In this study,we specially designed a perovskite oxide with abundant oxygen vacancies,SrCo_(0.8)Fe_(0.2)O_(3)(SCF),and firstly applied it as a catalyst in peroxymonosulfate(PMS) activation towards organic pollutants degradation.The result revealed that the prepared SCF catalyst exhibited excellent performance on organic compounds degradation.Besides,SCF showed much better activity than La_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3)(LSCF) in terms of reaction rate and stability for the degradation of the organic compounds.Based on the analysis of scanning electron microscope,transmission electron microscope,X-ray diffraction,N_(2) adsorption-desorption,X-ray photoelectron spectroscopy and electron paramagnetic resonance,it was confirmed that the perovskite catalysts with high content of Sr doping at A-site could effectively create a defect-rich surface and optimize its physicochemical properties,which was responsible for the excellent heterogeneous catalytic activity of SCF.SCF can generate three highly active species:~1 O_(2),SO_(4)^(-)· and ·OH in PMS activation,revealing the degradation process of organic compounds was a coupled multiple active species in both radical and nonradical pathway.Moreover,it was mainly in a radical pathway in the degradation through PMS activation on SCF and SO_(4)^(-)· radicals produced were the dominant species in SCF/PMS system.This study demonstrated that perovskite-type catalysts could enrich OVs efficiently by doping strategy and regulate the PMS activation towards sulfate radical-based AOPs.展开更多
Persulfate decontamination technologies utilizing radical‐driven processes are powerful tools for the treatment of a broad range of impurities.However,the design of high‐performance catalytic activators with multi‐...Persulfate decontamination technologies utilizing radical‐driven processes are powerful tools for the treatment of a broad range of impurities.However,the design of high‐performance catalytic activators with multi‐functionality remains a great challenge.Therefore,in this study,three‐dimensional multifunctional FexOy/N‐GN/CNTs(N‐GN:nitrogen‐doped graphene,CNTs:carbon nanotubes)heterojunctions,which can be employed as microwave absorbers and catalysts,were synthesized via a solvothermal method and applied to activate peroxymonosulfate for the degradation of methylene blue(MB).X‐ray diffraction(XRD),Fourier transform infrared spectrometer(FTIR),scanning electron microscope(SEM),and X‐ray photoelectron microscopy(XPS)analyses revealed that the FexOy were anchored in‐situ onto the N‐GN network.Using MB as the model organic dye,various factors,such as degradation systems,PMS loading,initial organic pollutant concentration,and catalyst dosage were optimized.The results revealed that the remarkable efficiency was attributable to the synergistic effects of carbon,nitrogen,and iron‐based species.The oxidation system corresponded to the pseudo‐first‐order kinetic with a k value of^0.33 min^-1.It was demonstrated that both SO4^-and OH^-were the predominant reactive species through quenching experiments.Because these heterojunctions were employed as microwave absorbers and have a semiconductor‐like texture,the Fe/N co‐rich hierarchical porous carbon skeleton favored electron transport and storage.These heterojunctions increase the options for transitional metal catalysts and highlights the importance of designing other heterojunctions for specific applications,such as supercapacitors,energy storage,CO2 capture,and oxygen reduction electrocatalysts.展开更多
The multifunctionality and the advantages of thermal plasma for the fast inactivation of viable cells and degradation of organic compounds dissolved in waste water are presented.A complete bacterial inactivation proce...The multifunctionality and the advantages of thermal plasma for the fast inactivation of viable cells and degradation of organic compounds dissolved in waste water are presented.A complete bacterial inactivation process was observed and studied using a thermal plasma treatment source with very short application times,in particular for Staphylococcus aureus bundle spore survival.The survival curves and analyses of the experimental data of the initial and final densities of S.aureus bacteria show a dramatic inhibitory effect of the plasma discharge on the residual bacteria survival ratio.As the exposure time increased,the inactivation process rate increased for direct exposure more than it did for indirect exposure.The evaluation of direct and indirect exposure was based on the analysis of the ultraviolet spectrum from the absorbance spectra of the organic compound dye called benzene sulfonate(C(16)H(11)N2Na O4S)and of viable cells called S.aureus.Organic compounds were degraded and viable cells were killed in a short time by thermal plasma.Moreover,analyses of total carbon,total organic carbon,and total inorganic carbon showed a fast decrease in organically bound carbon,however,this was not as fast as the absorbance spectra revealed by the exposure time increasing more for direct exposure than indirect exposure.After 100 s of exposure to the organic compound dye the removal had a maximun of 40%for samples with indirect exposure to the plasma and a maximum of 90%for samples with the direct exposure.For both samples,where some organic contaminants still remained in treated water,four electrolytes(KCl,Na Cl,Na2SO4,and CH3COONa)were added to be effective for complete sterilization,reaching a purity of 100%.A proposal is made for an optimized thermal plasma water purification system(TPWPS)to improve fast inactivation of microbes and the degradation of organic compounds dissolved in water(especially for direct exposure rather than indirect exposure)using a hybrid plasma torch with an electrical power of 125 kW(500 V–250 A)producing a high-temperature(10 000 K–19 000 K)plasma jet with a maximum gas consumption of 28 mg s^-1.展开更多
The response of mangrove ecosystems to the Asian monsoon in the future global warming can be understood by reconstructing the development of mangrove forests during the Holocene climatic optimum(HCO), using proxies ...The response of mangrove ecosystems to the Asian monsoon in the future global warming can be understood by reconstructing the development of mangrove forests during the Holocene climatic optimum(HCO), using proxies preserved in coastal sediments. The total organic matter in sediments of a segmented core, with calibrated age ranges between 5.6 and 7.7 cal. ka BP and corresponding to the HCO, from the Qinzhou Bay in Guangxi, China, is quantitatively partitioned into three end-members according to their sources: mangrove-derived, terrigenous,and marine phytoplanktonic, using a three-end-member model depicted by organic carbon isotope(δ13Corg) and the molar ratio of total organic carbon to total nitrogen(C/N). The percentage of mangrove-derived organic matter(MOM) contribution is used as a proxy for mangrove development. Three visible drops in MOM contribution occurred at ca. 7.3, ca. 6.9, and ca. 6.2 cal. ka BP, respectively, are recognized against a relatively stable and higher MOM contribution level, indicating that three distinct mangrove forest degradations occurred in the Qinzhou Bay during the HCO. The three mangrove forest degradations approximately correspond to the time of the strengthened/weakened Asian winter/summer monsoon. This indicates that even during a period favorable for the mangrove development, such as the HCO, climatic extremes, such as cold and dry events driven by the strengthened/weakened Asian winter/summer monsoon, can trigger the degradation of mangrove forests.展开更多
The hypoxic phenomena of seawater have been found in the Changjiang esturay and its adjacent area for several decades. To study organic matter degradation in seasonal hypoxic seawater, series of stimulated incubation ...The hypoxic phenomena of seawater have been found in the Changjiang esturay and its adjacent area for several decades. To study organic matter degradation in seasonal hypoxic seawater, series of stimulated incubation experiments with S keletonema costatum in seawater under different oxygen saturations were conducted. By tracking variations of lipids originated from the alga, time-dependent concentrations of neutral lipids(hexadecanol, otctadecanol, cholesterol, brassicasterol and phytol) and fatty acids(12:0, 14:0, 16:0, 16:1, 18:0, 18:1(9), 20:5 and 22:6) were obtained during three month of incubation. The results indicate that residence time, oxygen saturation, bacterial community and the structure of lipids were key factors controlling preservation and degradation of lipids in seawater. The degradation rate constants calculated from multi-G model showed that under same oxygen saturation, algal fatty acid degraded faster than neutral lipids, and unsaturated fatty acids degraded faster than saturated fatty acids. Our new discovery showed that degradation rate constant had linear positive correlation with oxygen saturation of seawater, indicating the critical role of oxygen on degradation of algal lipids in hypoxic seawater. The results of this study will be helpful to understand organic carbon cycling in seawater and marine environment more deeply. Future field experiments and investigation should be conducted tracking control factors, especially the role of oxygen saturation on organic matter degradation in natural environment.展开更多
In this work, electrospray technique combined sol-gel method was used to prepare porous TiO2 film. X-ray Photoelectron Spectroscopy (XPS), X-Ray Diffraction (XRD), and Scanning Electron Microscope (SEM) analyses were ...In this work, electrospray technique combined sol-gel method was used to prepare porous TiO2 film. X-ray Photoelectron Spectroscopy (XPS), X-Ray Diffraction (XRD), and Scanning Electron Microscope (SEM) analyses were conducted to examine the chemical composition, phase structure, and surface morphology of the sprayed TiO2 film. After calcined at 450℃ in air atmosphere for 2 h, mesoporous TiO2 nano-spheres clusters were formed on the surface of silicon wafer and the average size of nano-spheres was 250 nm. Ti presented as Ti 4+ oxidation state in TiO2 film, and the TiO2 film exhibited the anatase phase. The sprayed porous TiO2 films were employed as photocatalyst to degrade organic phosphorus in water samples. Compared with the TiO2 film prepared by Sol-Gel spin-coating method, the porous TiO2 film deposited by electrospray combined sol-gel method showed higher photocatalytic activity.展开更多
Microbial activity and interaction are the important driving factors in the start-up phase of food waste composting at low temperature.The aim of this study was to explore the effect of inoculating Bacillus lichenifor...Microbial activity and interaction are the important driving factors in the start-up phase of food waste composting at low temperature.The aim of this study was to explore the effect of inoculating Bacillus licheniformis on the degradation of organic components and the potential microbe-driven mechanism from the aspects of organic matter degradation,enzyme activity,microbial community interaction,and microbial metabolic function.The results showed that after inoculating B.licheniformis,temperature increased to 47.8℃ on day2,and the degradation of readily degraded carbohydrates(RDC)increased by 31.2%,and the bioheat production increased by 16.5%.There was an obvious enhancement of extracellular enzymes activities after inoculation,especially amylase activity,which increased by 7.68 times on day 4.The inoculated B.licheniformis colonized in composting as key genus in the start-up phase.Modular network analysis and Mantel test indicated that inoculation drove the cooperation between microbial network modules who were responsible for various organic components(RDC,lipid,protein,and lignocellulose)degradation in the start-up phase.Metabolic function prediction suggested that carbohydrate metabolisms including starch and sucrose metabolism,glycolysis/gluconeogenesis,pyruvate metabolism,etc.,were improved by increasing the abundance of related functional genes after inoculation.In conclusion,inoculating B.licheniformis accelerated organic degradation by driving the cooperation between microbial network modules and enhancing microbial metabolism in the start-up phase of composting.展开更多
LuFeO3 crystallites of different sizes and morphologies were synthesized via a hydrothermal route. The sonocatalytic properties of the as-synthesized samples were investigated by degrading various organic dyes, includ...LuFeO3 crystallites of different sizes and morphologies were synthesized via a hydrothermal route. The sonocatalytic properties of the as-synthesized samples were investigated by degrading various organic dyes, including acid orange 7 (AOT), rhodamine B (RhB), methyl orange (MO), and methylene blue (MB), under ultrasonic irradiation, revealing that they exhibit excellent sonocatalytic activity toward the degradation of these dyes. Particularly, the synthesized bar-like particles with lengths of-3 μm and widths of-1μm have the highest sonocatalytic activity, and the degradation percentage of AO7 reaches 89% after 30 min of sonocatalysis. The effects of inorganic anions such as CI-, NO3-, SO42-, PO43-, and HCO3- on the sonocatalysis efficiency were investigated. Hydroxyl radicals (·OH) detected by fiuorimetry using terephthalic acid as a probe molecule were found to be produced over the ultrasonic-irradiated LuFeO3 particles. The addition of ethanol, which acts as a· OH scavenger, leads to quenching of "OH radicals and a simultaneous decrease in the dye degrada- tion. This suggests that "OH is the dominant active species responsible for the dye degradation.展开更多
Although both the aerobic photocatalytic oxidation of organic pollutants into CO2 and the anaerobic photocatalytic reduction of CO2 into solar fuels have been intensively studied,few efforts have been devoted to combi...Although both the aerobic photocatalytic oxidation of organic pollutants into CO2 and the anaerobic photocatalytic reduction of CO2 into solar fuels have been intensively studied,few efforts have been devoted to combining these carbon-involved photocatalytic oxidation-reduction processes together,by which an artificial photocatalytic carbon cycling process can be established.The key challenge lies in the exploitation of efficient bifunctional photocatalysts,capable of triggering both aerobic oxidation and anaerobic reduction reactions.In this work,a bifunctional ternary g-C3N4/Bi/BiVO4 hybrid photocatalyst is successfully constructed,which not only demonstrates superior aerobic photocatalytic oxidation performance in degrading an organic pollutant(using the dye,Rhodamine B as a model),but also exhibits impressive photocatalytic CO2 reduction performance under anaerobic conditions.Moreover,a direct conversion of Rhodamine B to solar fuels in a one-pot anaerobic reactor can be achieved with the as-prepared ternary g-C3N4/Bi/BiVO4 hybrid photocatalyst.The excellent bifunctional photocatalytic performance of the g-C3N4/Bi/BiVO4 photocatalyst is associated with the formation of efficient S-scheme hybrid junctions,which contribute to promoting the appropriate charge dynamics,and sustaining favorable charge potentials.The formation of the S-scheme heterojunction is supported by scavenger studies and density functional theory calculations.Moreover,the in-situ formed plasmonic metallic Bi nanoparticles in the S-scheme hybrid g-C3N4/Bi/BiVO4 photocatalyst enhances vectorial interfacial electron transfer.This novel bifunctional S-scheme g-C3N4/Bi/BiVO4 hybrid photocatalyst system provides new insights for the further development of an integrated aerobic-anaerobic reaction system for photocatalytic carbon cycling.展开更多
In this paper, a research was made on the treatment of distillation ammonia wastewater from Tai'an Coke-Plant by SBR(sequencing batch reactors). The feasibility and cost effectiveness was tested. Performance of SB...In this paper, a research was made on the treatment of distillation ammonia wastewater from Tai'an Coke-Plant by SBR(sequencing batch reactors). The feasibility and cost effectiveness was tested. Performance of SBR process treating organic substance and ammonia was presented for different operating pattern and aeration time. The mechanism of the simultaneous nitrification and denitrification from coke plant were analysed on SBR process.展开更多
Thermal catalytic degradation of organic pollutants conducted in the dark at room temperature under atmospheric pressure without the need of external chemicals and energy sources has attracted a lot of attention over ...Thermal catalytic degradation of organic pollutants conducted in the dark at room temperature under atmospheric pressure without the need of external chemicals and energy sources has attracted a lot of attention over the last two decades. It provides unparalleled advantages over other advanced oxidation processes (AOPs) in treating domestic and industrial contaminated wastewater from the viewpoint of energy/chemical conservation and ease of operation. Rich knowledge has been accumulated in terms of the synthesis and application of thermal catalysts though controversies remain regarding their underlying mechanisms. This review sheds light on the proposed thermo- catalysis mechanism for the first time and presents the development of thermal catalysts under dark ambient conditions with a focus on catalyst materials, catalytic activity, and mechanism. The present review aims to provide mechanistic insights into the rational design of novel and efficient catalysts, and their underlying mechanisms as well as the emerging challenges and perspectives in thermo-catalysis under dark ambient conditions used for the practical and efficient treatment of contaminated wastewater.展开更多
According to a great deal of experimental findings and the oretical analysis, theperformance of SBR process treating organic substance and ammonia was presented for different operating pattern and aeration time.When t...According to a great deal of experimental findings and the oretical analysis, theperformance of SBR process treating organic substance and ammonia was presented for different operating pattern and aeration time.When the operation mode is feeding water,anoxie mixing 2.5 h, settlement, and draining for 1.5 h, the coke plant wastewater can be treated well by the SBR method.展开更多
The study herein investigated the effectiveness of simultaneous use of ozone and hydrogen peroxide(O_3/H_2O_2 process) to degrade o-phenylenediamine(o-PDA) in a simulated wastewater. A rotor–stator reactor(RSR) was e...The study herein investigated the effectiveness of simultaneous use of ozone and hydrogen peroxide(O_3/H_2O_2 process) to degrade o-phenylenediamine(o-PDA) in a simulated wastewater. A rotor–stator reactor(RSR) was employed to create a high-gravity environment in order to enhance ozone-liquid mass transfer rate and possibly improve the degradation rate of o-PDA. The degradation efficiency of o-PDA(η) as well as the overall gas-phase volumetric mass transfer coefficient(KGa) were determined under different operating conditions of H_2O_2 concentration, initial o-PDA concentration, temperature of reaction, initial p H and rotation speed of RSR in attempt to establish the optimal conditions. Chemical oxygen demand reduction rate(rCOD) of wastewater treated at a particular set of conditions was also analyzed. Additionally, the intermediate products of degradation were identified using a gas chromatography-mass spectrometer(GC/MS) to further evaluate the extent of o-PDA degradation as well as establish its possible degradation pathway. Results were validated by comparison with those of sole use of ozone(O_3 process), and it was noted that η, KGa and rCODachieved by O_3/H_2O_2 process was 24.4%,31.6% and 25.2% respectively higher than those of O_3 process, indicating that H_2O_2 can greatly enhance ozonation of o-PDA. This work further demonstrates that an RSR can significantly intensify ozone-liquid mass transfer rate and thus provides a feasible intensification means for the ozonation of o-PDA as well as other recalcitrant organics.展开更多
A BiVO_4 photoanode with exposed(040) facets was prepared to enhance its photoelectrochemical performance.The exposure of the(040) crystal planes of the BiVO_4 film was induced by adding NaCl to the precursor solution...A BiVO_4 photoanode with exposed(040) facets was prepared to enhance its photoelectrochemical performance.The exposure of the(040) crystal planes of the BiVO_4 film was induced by adding NaCl to the precursor solution. The asprepared BiVO_4 photoanode exhibits higher solar-light absorption and charge-separation efficiency compared to those of an anode prepared without adding Na Cl. To our knowledge,the photocurrent density(1.26 m A cm^(-2) at 1.23 V vs. RHE) of as-prepared BiVO_4 photoanode is the highest according to the reports for bare BiVO_4 films under simulated AM1.5 G solar light, and the incident photon-to-current conversion efficiency is above 35% at 400 nm. The photoelectrochemical(PEC)water-splitting performance was also dramatically improvedwith a hydrogen evolution rate of 9.11 lmol cm^(-2) h^(-1), which is five times compared with the BiVO_4 photoanode prepared without NaCl(1.82 lmol cm^(-2) h^(-1)). Intensity-modulated photocurrent spectroscopy and transient photocurrent measurements show a higher charge-carrier-transfer rate for this photoanode. These results demonstrate a promising approach for the development of high-performance BiVO_4 photoanodes which can be used for efficient PEC water splitting and degradation of organic pollutants.展开更多
According to a great deal of experimental findings and theoretical analysis, when the COD of inlet is 1 000-1 200 mg/L, NH3--N is 200~250 mg/L, the periodic time of operation is 24 h, the aeration time is 16 h and the...According to a great deal of experimental findings and theoretical analysis, when the COD of inlet is 1 000-1 200 mg/L, NH3--N is 200~250 mg/L, the periodic time of operation is 24 h, the aeration time is 16 h and the sludge density is 5 000-7 000 mg/L, COD of outlet is 150-200 mg/L, NH3--N is less than 25 mg/L, the volume load of COD and NH3--N remove 0.50 and 0.12 kg/(m3od) respectively. Meanwhile, studied the influence of various crafts parameter change on the treating effect and absorbing the yielding water of the SBR reactor with pulverized coal ash for improving the removing effect of COD and chromaticity further.展开更多
The structures of 26 different congeners of polychlorinated biphenyls(PCBs, including monothrough deca-chlorinated) were optimized using density functional theory(DFT) calculations with the 6-31+G(d,p) basis se...The structures of 26 different congeners of polychlorinated biphenyls(PCBs, including monothrough deca-chlorinated) were optimized using density functional theory(DFT) calculations with the 6-31+G(d,p) basis set. The activation energies for the dechlorination of these systems were calculated for direct photodegradation and photosensitized degradation reaction pathways in the presence of natural organic matter(NOM). The dechlorination mechanism of these PCBs and the ring-opening reaction mechanisms(using QST3 method) of the photosensitive degradation products were analyzed. The results showed that(i) the activation energy for the photosensitized degradation of PCBs was much lower than that of direct photodegradation;(ii) the degradation activities(i.e., C–Cl bond cleavage energies) were the same for both degradation pathways and followed the order ortho 〉 meta 〉 para;(iii) the degradation activities of asymmetric PCBs were higher than those of the corresponding symmetrical PCBs for the direct photodegradation and it was completely opposite in the photosensitive degradation;(iv) there was no correlation between the dissociation energy and the number of C–Cl bonds for the direct photodegradation and dechlorination products were all biphenyl;(v) the degradation activity of PCBs decreased as the number of C–Cl bonds increased in the presence of NOM; and(vi) even when the dechlorination reaction was incomplete, it produced chlorophenol. Furthermore, the free radicals of NOM led to the ring-opening reactions of PCBs via an initial addition step. The main site of these ring-opening reactions was the ortho position. Notably, the likelihood of ring-opening reactions occurring involving the degradation products increased as the degradation degree of PCBs increased.展开更多
The effective,stable,and secure catalysts are essential for sulfate radical(SO_(4)·−)-based advanced oxidation processes(SR-AOPs)to the degradation of organic contaminants in water.Heterogeneous supported cobalt-...The effective,stable,and secure catalysts are essential for sulfate radical(SO_(4)·−)-based advanced oxidation processes(SR-AOPs)to the degradation of organic contaminants in water.Heterogeneous supported cobalt-based catalysts are commonly used to activate peroxymonosulfate(PMS)to achieve the degradation.In this work,we synthesized Co_(3)O_(4)@Al_(2)O_(3)three-dimensional(3D)mesoporous nanocomposite(denoted as Co_(3)O_(4)@Al_(2)O_(33)DPNC)in just one step by calcining cheap and green deep eutectic solvent(DES)solution containing Co salt.Co_(3)O_(4)@Al_(2)O_(33)DPNC with the high specific surface area(93.246 m^(2)/g),uniform pore distribution(3.829 nm)and rich porosity(0.255 cm^(3)/g)were attained in a beautiful hierarchical structure which exhibited the open 3D propeller-like microstructure,two-dimensional lamellar substructure with rich folds,as well as the decoration of highly dispersed Co_(3)O_(4)nanoparticles on mesoporous amorphous Al_(2)O_(3).The excellent chemical and thermal stability of Al_(2)O_(3)ensures the high stability of the catalyst,and the formation of the complex hierarchical structure makes the active Co_(3)O_(4)be homogenously dispersed for effective catalysis.The catalyst demonstrated outstanding performance for catalytic degradations of organic pollutants(acetaminophen,oxytetracycline,5-sulfosalicylic acid,orange G and Rhodamine B)by generated SO_(4)·−,·OH and^(1)O_(2).With a very low cobalt content(equal to 28.2 mg/L of Co),the catalyst exhibited very high stability and excellent reusability in the recycling usages,while the leaching of the cobalt element(<0.145 mg/L)was also at a low level.Our catalyst achieved effective degradations of acetaminophen in cycles without losing its stable hierarchical nanostructure.展开更多
基金supported by The Key Laboratory of Advanced Functional Materials, Ministry of Education of China, Beijing University of Technologythe National Natural Science Foundation of China (NSFC, 52070006)。
文摘The design and synthesis of non-precious metal dual-functional electrocatalysts through the modulation of electronic structure are important for the development of renewable hydrogen energy.Herein,MnS_(2)/MnO_(2)-CC heterostructure dual-functional catalysts with ultrathin nanosheets were prepared by a twostep electrodeposition method for efficient acidic hydrogen evolution reaction(HER) and degradation of organic wastewater(such as methylene blue(MB)).The electronic structure of Mn atoms at the MnS_(2)/MnO_(2)-CC heterostructure interface is reconfigured under the joint action of S and O atoms.Theoretical calculations show that the Mn d-band electron distribution in MnS_(2)/MnO_(2)-CC catalyst has higher occupied states near the Fermi level compared to the MnO_(2) and MnS_(2) catalysts,which indicates that MnS_(2)/MnO_(2)-CC catalyst has better electron transfer capability and catalytic activity.The MnS_(2)/MnO_(2)-CC catalysts require overpotential of only 66 and 116 mV to reach current density of 10 and 100 mA cm^(-2)in MB/H_(2)SO_(4) media.The MnS_(2)/MnO_(2)-CC catalyst also has a low Tafel slope(26.72 mV dec^(-1)) and excellent stability(the performance does not decay after 20 h of testing).In addition,the MB removal efficiency of the MnS_(2)/MnO_(2)-CC catalyst with a better kinetic rate(0.0226) can reach 97.76%,which is much higher than that of the MnO_(x)-CC catalyst(72.10%).This strategy provides a new way to develop efficient and stable non-precious metal dual-functional electrocatalysts for HER and organic wastewater degradation.
基金supported by Ministry of Education of the People's Republic of China (20070141004)
文摘Investigation was made into the degradation of organic compounds by a dielectric barrier corona discharge (DBCD) system. The DBCD, consisting of a quartz tube, a concentric high voltage electrode and a net wrapped to the external wall (used as ground electrode), was introduced to generate active species which were sprayed into the organic solution through an aerator fixed on the bottom of the tube. The effect of four factors-the discharge voltage, gas flow rate, solution conductivity, and pH of wastewater, on the degradation efficiency of phenol was assessed. The obtained results demonstrated that this process was an effective method for phenol degradation. The degradation rate was enhanced with the increase in power supplied. The degradation efficiency in alkaline conditions was higher than those in acid and neutral conditions. The optimal gas flow rate for phenol degradation in the system was 1.6 L/min, while the solution conductivity had little effect on the degradation.
文摘Metal organic frameworks(MOFs)is a research hotspot in the solar fuel production and photo-degradation of pollutants field due to high surface area,rich metal/organic species,large pore volume,and adjustability of structures and compositions.Therefore,in this review,we first summarized the design factors of photocatalytic materials based on MOF from the perspective of"star"MOF.The modification strategies of MOFs-based photocatalysts were discussed to improve its photocatalytic activity and specific applications were summarized as well,including photocatalytic CO_(2)reduction,photocatalytic water splitting and photo-degradation of pollutants.Finally,the advantages and disadvantages of MOFs-based photocatalysts were discussed,the current challenges were highlighted,and suggestions for future research directions were proposed.
基金supported by the National Key Research and Development Program of China (Project No.2018YFB1502903)。
文摘Metal-based perovskite oxides have contributed significantly to the advanced oxidation processes(AOPs)due to their diverse active sites and excellent compositional/structural flexibility.In this study,we specially designed a perovskite oxide with abundant oxygen vacancies,SrCo_(0.8)Fe_(0.2)O_(3)(SCF),and firstly applied it as a catalyst in peroxymonosulfate(PMS) activation towards organic pollutants degradation.The result revealed that the prepared SCF catalyst exhibited excellent performance on organic compounds degradation.Besides,SCF showed much better activity than La_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3)(LSCF) in terms of reaction rate and stability for the degradation of the organic compounds.Based on the analysis of scanning electron microscope,transmission electron microscope,X-ray diffraction,N_(2) adsorption-desorption,X-ray photoelectron spectroscopy and electron paramagnetic resonance,it was confirmed that the perovskite catalysts with high content of Sr doping at A-site could effectively create a defect-rich surface and optimize its physicochemical properties,which was responsible for the excellent heterogeneous catalytic activity of SCF.SCF can generate three highly active species:~1 O_(2),SO_(4)^(-)· and ·OH in PMS activation,revealing the degradation process of organic compounds was a coupled multiple active species in both radical and nonradical pathway.Moreover,it was mainly in a radical pathway in the degradation through PMS activation on SCF and SO_(4)^(-)· radicals produced were the dominant species in SCF/PMS system.This study demonstrated that perovskite-type catalysts could enrich OVs efficiently by doping strategy and regulate the PMS activation towards sulfate radical-based AOPs.
基金supported by the National Natural Science Foundation of China(21676039)Innovative talents in Liaoning universities and colleges(LR2017045)the Opening Foundation of State Key Laboratory of Inorganic Synthesis and Preparative Chemistry of Jilin University(2016–04)~~
文摘Persulfate decontamination technologies utilizing radical‐driven processes are powerful tools for the treatment of a broad range of impurities.However,the design of high‐performance catalytic activators with multi‐functionality remains a great challenge.Therefore,in this study,three‐dimensional multifunctional FexOy/N‐GN/CNTs(N‐GN:nitrogen‐doped graphene,CNTs:carbon nanotubes)heterojunctions,which can be employed as microwave absorbers and catalysts,were synthesized via a solvothermal method and applied to activate peroxymonosulfate for the degradation of methylene blue(MB).X‐ray diffraction(XRD),Fourier transform infrared spectrometer(FTIR),scanning electron microscope(SEM),and X‐ray photoelectron microscopy(XPS)analyses revealed that the FexOy were anchored in‐situ onto the N‐GN network.Using MB as the model organic dye,various factors,such as degradation systems,PMS loading,initial organic pollutant concentration,and catalyst dosage were optimized.The results revealed that the remarkable efficiency was attributable to the synergistic effects of carbon,nitrogen,and iron‐based species.The oxidation system corresponded to the pseudo‐first‐order kinetic with a k value of^0.33 min^-1.It was demonstrated that both SO4^-and OH^-were the predominant reactive species through quenching experiments.Because these heterojunctions were employed as microwave absorbers and have a semiconductor‐like texture,the Fe/N co‐rich hierarchical porous carbon skeleton favored electron transport and storage.These heterojunctions increase the options for transitional metal catalysts and highlights the importance of designing other heterojunctions for specific applications,such as supercapacitors,energy storage,CO2 capture,and oxygen reduction electrocatalysts.
基金financial support from MEPhI in the framework of the Russian Academic Excellence Project
文摘The multifunctionality and the advantages of thermal plasma for the fast inactivation of viable cells and degradation of organic compounds dissolved in waste water are presented.A complete bacterial inactivation process was observed and studied using a thermal plasma treatment source with very short application times,in particular for Staphylococcus aureus bundle spore survival.The survival curves and analyses of the experimental data of the initial and final densities of S.aureus bacteria show a dramatic inhibitory effect of the plasma discharge on the residual bacteria survival ratio.As the exposure time increased,the inactivation process rate increased for direct exposure more than it did for indirect exposure.The evaluation of direct and indirect exposure was based on the analysis of the ultraviolet spectrum from the absorbance spectra of the organic compound dye called benzene sulfonate(C(16)H(11)N2Na O4S)and of viable cells called S.aureus.Organic compounds were degraded and viable cells were killed in a short time by thermal plasma.Moreover,analyses of total carbon,total organic carbon,and total inorganic carbon showed a fast decrease in organically bound carbon,however,this was not as fast as the absorbance spectra revealed by the exposure time increasing more for direct exposure than indirect exposure.After 100 s of exposure to the organic compound dye the removal had a maximun of 40%for samples with indirect exposure to the plasma and a maximum of 90%for samples with the direct exposure.For both samples,where some organic contaminants still remained in treated water,four electrolytes(KCl,Na Cl,Na2SO4,and CH3COONa)were added to be effective for complete sterilization,reaching a purity of 100%.A proposal is made for an optimized thermal plasma water purification system(TPWPS)to improve fast inactivation of microbes and the degradation of organic compounds dissolved in water(especially for direct exposure rather than indirect exposure)using a hybrid plasma torch with an electrical power of 125 kW(500 V–250 A)producing a high-temperature(10 000 K–19 000 K)plasma jet with a maximum gas consumption of 28 mg s^-1.
基金The National Basic Research Program (973 Program) of China under contract No.2010CB951203the National Natural Science Foundation of China under contract Nos 41376075,41576061 and 41206057
文摘The response of mangrove ecosystems to the Asian monsoon in the future global warming can be understood by reconstructing the development of mangrove forests during the Holocene climatic optimum(HCO), using proxies preserved in coastal sediments. The total organic matter in sediments of a segmented core, with calibrated age ranges between 5.6 and 7.7 cal. ka BP and corresponding to the HCO, from the Qinzhou Bay in Guangxi, China, is quantitatively partitioned into three end-members according to their sources: mangrove-derived, terrigenous,and marine phytoplanktonic, using a three-end-member model depicted by organic carbon isotope(δ13Corg) and the molar ratio of total organic carbon to total nitrogen(C/N). The percentage of mangrove-derived organic matter(MOM) contribution is used as a proxy for mangrove development. Three visible drops in MOM contribution occurred at ca. 7.3, ca. 6.9, and ca. 6.2 cal. ka BP, respectively, are recognized against a relatively stable and higher MOM contribution level, indicating that three distinct mangrove forest degradations occurred in the Qinzhou Bay during the HCO. The three mangrove forest degradations approximately correspond to the time of the strengthened/weakened Asian winter/summer monsoon. This indicates that even during a period favorable for the mangrove development, such as the HCO, climatic extremes, such as cold and dry events driven by the strengthened/weakened Asian winter/summer monsoon, can trigger the degradation of mangrove forests.
基金Supported by the National Natural Science Foundation of China for Creative Groups(No.41521064)the National Natural Science Foundation of China(No.41676067)+2 种基金the Fundamental Funds for Central Universities(No.201762030)the National Key Research and Development Program of China(No.2016YFA0601302)the Natural Science Foundation of Shandong Province(No.ZR2010DM001)
文摘The hypoxic phenomena of seawater have been found in the Changjiang esturay and its adjacent area for several decades. To study organic matter degradation in seasonal hypoxic seawater, series of stimulated incubation experiments with S keletonema costatum in seawater under different oxygen saturations were conducted. By tracking variations of lipids originated from the alga, time-dependent concentrations of neutral lipids(hexadecanol, otctadecanol, cholesterol, brassicasterol and phytol) and fatty acids(12:0, 14:0, 16:0, 16:1, 18:0, 18:1(9), 20:5 and 22:6) were obtained during three month of incubation. The results indicate that residence time, oxygen saturation, bacterial community and the structure of lipids were key factors controlling preservation and degradation of lipids in seawater. The degradation rate constants calculated from multi-G model showed that under same oxygen saturation, algal fatty acid degraded faster than neutral lipids, and unsaturated fatty acids degraded faster than saturated fatty acids. Our new discovery showed that degradation rate constant had linear positive correlation with oxygen saturation of seawater, indicating the critical role of oxygen on degradation of algal lipids in hypoxic seawater. The results of this study will be helpful to understand organic carbon cycling in seawater and marine environment more deeply. Future field experiments and investigation should be conducted tracking control factors, especially the role of oxygen saturation on organic matter degradation in natural environment.
基金Supported by the National Basic Research Program of China (No. 2009CB320300)National Natural Science Foundation of China (No. 61072023)National High Technology Research and Development Programs (No.2012AA040506, No. 2012AA101608)
文摘In this work, electrospray technique combined sol-gel method was used to prepare porous TiO2 film. X-ray Photoelectron Spectroscopy (XPS), X-Ray Diffraction (XRD), and Scanning Electron Microscope (SEM) analyses were conducted to examine the chemical composition, phase structure, and surface morphology of the sprayed TiO2 film. After calcined at 450℃ in air atmosphere for 2 h, mesoporous TiO2 nano-spheres clusters were formed on the surface of silicon wafer and the average size of nano-spheres was 250 nm. Ti presented as Ti 4+ oxidation state in TiO2 film, and the TiO2 film exhibited the anatase phase. The sprayed porous TiO2 films were employed as photocatalyst to degrade organic phosphorus in water samples. Compared with the TiO2 film prepared by Sol-Gel spin-coating method, the porous TiO2 film deposited by electrospray combined sol-gel method showed higher photocatalytic activity.
基金supported by the Open Research Fund Program of State Environmental Protection Key Laboratory of Food Chain Pollution Control(No.FC2022YB01)the National Natural Science Foundation of China(No.32071552)+1 种基金the Independent Research Project of Science and Technology Innovation Base in Tibet Autonomous Region(No.XZ2022JR0007G)China Agricultural University-Dabeinong Group Professional degree graduate joint training reform project(No.CAUDBN PDG-JTRP).
文摘Microbial activity and interaction are the important driving factors in the start-up phase of food waste composting at low temperature.The aim of this study was to explore the effect of inoculating Bacillus licheniformis on the degradation of organic components and the potential microbe-driven mechanism from the aspects of organic matter degradation,enzyme activity,microbial community interaction,and microbial metabolic function.The results showed that after inoculating B.licheniformis,temperature increased to 47.8℃ on day2,and the degradation of readily degraded carbohydrates(RDC)increased by 31.2%,and the bioheat production increased by 16.5%.There was an obvious enhancement of extracellular enzymes activities after inoculation,especially amylase activity,which increased by 7.68 times on day 4.The inoculated B.licheniformis colonized in composting as key genus in the start-up phase.Modular network analysis and Mantel test indicated that inoculation drove the cooperation between microbial network modules who were responsible for various organic components(RDC,lipid,protein,and lignocellulose)degradation in the start-up phase.Metabolic function prediction suggested that carbohydrate metabolisms including starch and sucrose metabolism,glycolysis/gluconeogenesis,pyruvate metabolism,etc.,were improved by increasing the abundance of related functional genes after inoculation.In conclusion,inoculating B.licheniformis accelerated organic degradation by driving the cooperation between microbial network modules and enhancing microbial metabolism in the start-up phase of composting.
基金supported by the National Natural Science Foundation of China(51262018)the Fundamental Research Funds for Universities of Gansu Province(056003)the Hongliu Outstanding Talents Foundation of Lanzhou University of Technology(J201205)~~
文摘LuFeO3 crystallites of different sizes and morphologies were synthesized via a hydrothermal route. The sonocatalytic properties of the as-synthesized samples were investigated by degrading various organic dyes, including acid orange 7 (AOT), rhodamine B (RhB), methyl orange (MO), and methylene blue (MB), under ultrasonic irradiation, revealing that they exhibit excellent sonocatalytic activity toward the degradation of these dyes. Particularly, the synthesized bar-like particles with lengths of-3 μm and widths of-1μm have the highest sonocatalytic activity, and the degradation percentage of AO7 reaches 89% after 30 min of sonocatalysis. The effects of inorganic anions such as CI-, NO3-, SO42-, PO43-, and HCO3- on the sonocatalysis efficiency were investigated. Hydroxyl radicals (·OH) detected by fiuorimetry using terephthalic acid as a probe molecule were found to be produced over the ultrasonic-irradiated LuFeO3 particles. The addition of ethanol, which acts as a· OH scavenger, leads to quenching of "OH radicals and a simultaneous decrease in the dye degrada- tion. This suggests that "OH is the dominant active species responsible for the dye degradation.
基金financially supported by the National Natural Science Foundation of China(51872341,51572209)the Start-up Funds for High-Level Talents of Sun Yat-sen University(38000-31131105)+1 种基金the Fundamental Research Funds for the Central Universities(19lgzd29)the Science and Technology Program of Guangzhou(201707010095)~~
文摘Although both the aerobic photocatalytic oxidation of organic pollutants into CO2 and the anaerobic photocatalytic reduction of CO2 into solar fuels have been intensively studied,few efforts have been devoted to combining these carbon-involved photocatalytic oxidation-reduction processes together,by which an artificial photocatalytic carbon cycling process can be established.The key challenge lies in the exploitation of efficient bifunctional photocatalysts,capable of triggering both aerobic oxidation and anaerobic reduction reactions.In this work,a bifunctional ternary g-C3N4/Bi/BiVO4 hybrid photocatalyst is successfully constructed,which not only demonstrates superior aerobic photocatalytic oxidation performance in degrading an organic pollutant(using the dye,Rhodamine B as a model),but also exhibits impressive photocatalytic CO2 reduction performance under anaerobic conditions.Moreover,a direct conversion of Rhodamine B to solar fuels in a one-pot anaerobic reactor can be achieved with the as-prepared ternary g-C3N4/Bi/BiVO4 hybrid photocatalyst.The excellent bifunctional photocatalytic performance of the g-C3N4/Bi/BiVO4 photocatalyst is associated with the formation of efficient S-scheme hybrid junctions,which contribute to promoting the appropriate charge dynamics,and sustaining favorable charge potentials.The formation of the S-scheme heterojunction is supported by scavenger studies and density functional theory calculations.Moreover,the in-situ formed plasmonic metallic Bi nanoparticles in the S-scheme hybrid g-C3N4/Bi/BiVO4 photocatalyst enhances vectorial interfacial electron transfer.This novel bifunctional S-scheme g-C3N4/Bi/BiVO4 hybrid photocatalyst system provides new insights for the further development of an integrated aerobic-anaerobic reaction system for photocatalytic carbon cycling.
文摘In this paper, a research was made on the treatment of distillation ammonia wastewater from Tai'an Coke-Plant by SBR(sequencing batch reactors). The feasibility and cost effectiveness was tested. Performance of SBR process treating organic substance and ammonia was presented for different operating pattern and aeration time. The mechanism of the simultaneous nitrification and denitrification from coke plant were analysed on SBR process.
基金funding support by the National Natural Science Foundation of China (51674091, 51104048)~~
文摘Thermal catalytic degradation of organic pollutants conducted in the dark at room temperature under atmospheric pressure without the need of external chemicals and energy sources has attracted a lot of attention over the last two decades. It provides unparalleled advantages over other advanced oxidation processes (AOPs) in treating domestic and industrial contaminated wastewater from the viewpoint of energy/chemical conservation and ease of operation. Rich knowledge has been accumulated in terms of the synthesis and application of thermal catalysts though controversies remain regarding their underlying mechanisms. This review sheds light on the proposed thermo- catalysis mechanism for the first time and presents the development of thermal catalysts under dark ambient conditions with a focus on catalyst materials, catalytic activity, and mechanism. The present review aims to provide mechanistic insights into the rational design of novel and efficient catalysts, and their underlying mechanisms as well as the emerging challenges and perspectives in thermo-catalysis under dark ambient conditions used for the practical and efficient treatment of contaminated wastewater.
文摘According to a great deal of experimental findings and the oretical analysis, theperformance of SBR process treating organic substance and ammonia was presented for different operating pattern and aeration time.When the operation mode is feeding water,anoxie mixing 2.5 h, settlement, and draining for 1.5 h, the coke plant wastewater can be treated well by the SBR method.
基金Supported by the National Natural Science Foundation of China(21276013,21676008)Specialized Research Fund for the Doctoral Program of Higher Education of China(20130010110001)
文摘The study herein investigated the effectiveness of simultaneous use of ozone and hydrogen peroxide(O_3/H_2O_2 process) to degrade o-phenylenediamine(o-PDA) in a simulated wastewater. A rotor–stator reactor(RSR) was employed to create a high-gravity environment in order to enhance ozone-liquid mass transfer rate and possibly improve the degradation rate of o-PDA. The degradation efficiency of o-PDA(η) as well as the overall gas-phase volumetric mass transfer coefficient(KGa) were determined under different operating conditions of H_2O_2 concentration, initial o-PDA concentration, temperature of reaction, initial p H and rotation speed of RSR in attempt to establish the optimal conditions. Chemical oxygen demand reduction rate(rCOD) of wastewater treated at a particular set of conditions was also analyzed. Additionally, the intermediate products of degradation were identified using a gas chromatography-mass spectrometer(GC/MS) to further evaluate the extent of o-PDA degradation as well as establish its possible degradation pathway. Results were validated by comparison with those of sole use of ozone(O_3 process), and it was noted that η, KGa and rCODachieved by O_3/H_2O_2 process was 24.4%,31.6% and 25.2% respectively higher than those of O_3 process, indicating that H_2O_2 can greatly enhance ozonation of o-PDA. This work further demonstrates that an RSR can significantly intensify ozone-liquid mass transfer rate and thus provides a feasible intensification means for the ozonation of o-PDA as well as other recalcitrant organics.
基金financial support provided by the National Nature Science Foundation of China(No.21576162,No.51578332,and No.21507085)the Shanghai Yangfan Program(14YF1401500)
文摘A BiVO_4 photoanode with exposed(040) facets was prepared to enhance its photoelectrochemical performance.The exposure of the(040) crystal planes of the BiVO_4 film was induced by adding NaCl to the precursor solution. The asprepared BiVO_4 photoanode exhibits higher solar-light absorption and charge-separation efficiency compared to those of an anode prepared without adding Na Cl. To our knowledge,the photocurrent density(1.26 m A cm^(-2) at 1.23 V vs. RHE) of as-prepared BiVO_4 photoanode is the highest according to the reports for bare BiVO_4 films under simulated AM1.5 G solar light, and the incident photon-to-current conversion efficiency is above 35% at 400 nm. The photoelectrochemical(PEC)water-splitting performance was also dramatically improvedwith a hydrogen evolution rate of 9.11 lmol cm^(-2) h^(-1), which is five times compared with the BiVO_4 photoanode prepared without NaCl(1.82 lmol cm^(-2) h^(-1)). Intensity-modulated photocurrent spectroscopy and transient photocurrent measurements show a higher charge-carrier-transfer rate for this photoanode. These results demonstrate a promising approach for the development of high-performance BiVO_4 photoanodes which can be used for efficient PEC water splitting and degradation of organic pollutants.
文摘According to a great deal of experimental findings and theoretical analysis, when the COD of inlet is 1 000-1 200 mg/L, NH3--N is 200~250 mg/L, the periodic time of operation is 24 h, the aeration time is 16 h and the sludge density is 5 000-7 000 mg/L, COD of outlet is 150-200 mg/L, NH3--N is less than 25 mg/L, the volume load of COD and NH3--N remove 0.50 and 0.12 kg/(m3od) respectively. Meanwhile, studied the influence of various crafts parameter change on the treating effect and absorbing the yielding water of the SBR reactor with pulverized coal ash for improving the removing effect of COD and chromaticity further.
基金supported by the Fundamental Research Funds for the Central Universities in 2013(JB2013146)the Key Projects in the National Science&Technology Pillar Program in the Eleventh Five-Year Plan Period(2008BAC43B01)
文摘The structures of 26 different congeners of polychlorinated biphenyls(PCBs, including monothrough deca-chlorinated) were optimized using density functional theory(DFT) calculations with the 6-31+G(d,p) basis set. The activation energies for the dechlorination of these systems were calculated for direct photodegradation and photosensitized degradation reaction pathways in the presence of natural organic matter(NOM). The dechlorination mechanism of these PCBs and the ring-opening reaction mechanisms(using QST3 method) of the photosensitive degradation products were analyzed. The results showed that(i) the activation energy for the photosensitized degradation of PCBs was much lower than that of direct photodegradation;(ii) the degradation activities(i.e., C–Cl bond cleavage energies) were the same for both degradation pathways and followed the order ortho 〉 meta 〉 para;(iii) the degradation activities of asymmetric PCBs were higher than those of the corresponding symmetrical PCBs for the direct photodegradation and it was completely opposite in the photosensitive degradation;(iv) there was no correlation between the dissociation energy and the number of C–Cl bonds for the direct photodegradation and dechlorination products were all biphenyl;(v) the degradation activity of PCBs decreased as the number of C–Cl bonds increased in the presence of NOM; and(vi) even when the dechlorination reaction was incomplete, it produced chlorophenol. Furthermore, the free radicals of NOM led to the ring-opening reactions of PCBs via an initial addition step. The main site of these ring-opening reactions was the ortho position. Notably, the likelihood of ring-opening reactions occurring involving the degradation products increased as the degradation degree of PCBs increased.
基金supported by the National Natural Science Foundation of China(Nos.22274149,22074137,22274147 and 21721003)Jilin Province Science and Technology Development Plan Project(No.20210506012ZP)。
文摘The effective,stable,and secure catalysts are essential for sulfate radical(SO_(4)·−)-based advanced oxidation processes(SR-AOPs)to the degradation of organic contaminants in water.Heterogeneous supported cobalt-based catalysts are commonly used to activate peroxymonosulfate(PMS)to achieve the degradation.In this work,we synthesized Co_(3)O_(4)@Al_(2)O_(3)three-dimensional(3D)mesoporous nanocomposite(denoted as Co_(3)O_(4)@Al_(2)O_(33)DPNC)in just one step by calcining cheap and green deep eutectic solvent(DES)solution containing Co salt.Co_(3)O_(4)@Al_(2)O_(33)DPNC with the high specific surface area(93.246 m^(2)/g),uniform pore distribution(3.829 nm)and rich porosity(0.255 cm^(3)/g)were attained in a beautiful hierarchical structure which exhibited the open 3D propeller-like microstructure,two-dimensional lamellar substructure with rich folds,as well as the decoration of highly dispersed Co_(3)O_(4)nanoparticles on mesoporous amorphous Al_(2)O_(3).The excellent chemical and thermal stability of Al_(2)O_(3)ensures the high stability of the catalyst,and the formation of the complex hierarchical structure makes the active Co_(3)O_(4)be homogenously dispersed for effective catalysis.The catalyst demonstrated outstanding performance for catalytic degradations of organic pollutants(acetaminophen,oxytetracycline,5-sulfosalicylic acid,orange G and Rhodamine B)by generated SO_(4)·−,·OH and^(1)O_(2).With a very low cobalt content(equal to 28.2 mg/L of Co),the catalyst exhibited very high stability and excellent reusability in the recycling usages,while the leaching of the cobalt element(<0.145 mg/L)was also at a low level.Our catalyst achieved effective degradations of acetaminophen in cycles without losing its stable hierarchical nanostructure.