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catalytic ozonation of NH_(4)^(+)-N in wastewater over composite metal oxide catalyst

Journal of Rare Earths 2022年第1期40卷 73-84页

作者： Caiqing He Yunnen Chen Lin Guo Ruoyu Yin Tingsheng Qiu Jiangxi Key Laboratory of Mining&Metallurgy Environmental Pollution Control Jiangxi University of Science and TechnologyGanzhou 341000China

Large amounts of water containing-ammonium nitrogen(NH_(4)^(+)-N)have attracted increasing attention.catalytic ozonation technology,involving the generation of hydroxyl radical(OH)with strong oxidation ability,was originally utilized to degrade organic-containing wastewater.In this paper,Ce/MnOx composite metal oxide catalysts prepared with different preparation conditions were used to degrade wastewater containing inorganic pollutant(NH_(4)^(+)-N).The as-prepared catalyst features were characterized using X-ray diffraction(XRD),Brunauer-Emmett-Teller method(BET),scanning electron microscopy(SEM),energy dispersive X-ray spectroscopy(EDS),Fourier transform infrared spectroscopy(FTIR),X-ray photoelectron spectroscopy(XPS)and H_(2)-temperature programmed reduction(H_(2)-TPR)techniques.The results show that the catalyst,prepared by conditions with precipitant Na_(2)CO_(3) and Ce/Mn molar ratio 1:2 calcined at 400℃for 3 h in pH 11.0,displays the optimal performance,with the removal rate of NH_(4)^(+)-N and selectivity to gaseous nitrogen,88.14 wt%and 53.67 wt%,respectively.The effects of several operating factors including solution pH,initial NH_(4)^(+)-N concentrations and scavengers were evaluated.In addition,XRD patterns of catalyst with the best performance and the comparative study on decontamination of NH_(4)^(+)-N by various processes(O_(3),catalyst and catalyst/O_(3))show that the primary metal oxides are CeO_(2) and MnO_(2) in Ce/MnOx composite metal oxide catalysts,which have a synergistic effect on the catalytic ozonation of NH_(4)^(+)-N,and the new phase MnO_(2) plays a great role.After 5 consecutive use cycles,the degradation efficiency is declined slightly,and can still achieve better than 70 wt%over 1 h reaction.Additionally,the application of catalytic ozonation for actual wastewater on the removal rate of NH_(4)^(+)-N was investigated.Possible mechanism and degradation pathway of NH_(4)^(+)-N were also proposed.In a word,the application of CeO_(2)-MnO_(2) composite metal oxide catalysts in catalytic o

关键词： Ammonium nitrogen Catalyst Wastewater catalytic ozonation Rare earths

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catalytic ozonation in advanced treatment of kitchen wastewater:multi-scale simulation and pilot-scale study

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Frontiers of Environmental Science & Engineering 2023年第12期17卷 47-58页

作者： Zuoyong Zhou Ni Yan Mengxi Yin Tengfei Ren Shuning Chen Kechao Lu Xiaoxin Cao Xia Huang Xiaoyuan Zhang State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China

catalytic ozonation is regarded as a promising technology in the advanced treatment of refractory organic wastewater.Packed-bed reactors are widely used in practical applications due to simple structures,installation and operation.However,mass transfer of packed-bed reactors is relatively restrained and amplified deviations usually occurred in scale-up application.Herein,a multi-scale packed-bed model of catalytic ozonation was established to guide pilot tests.First,a laboratory-scale test was conducted to obtain kinetic parameters needed for modeling.Then,a multi-scale packed-bed model was developed to research the effects of water distribution structure,catalyst particle size,and hydraulic retention time(HRT)on catalytic ozonation.It was found that the performance of packed bed reactor was increased with evenly distributed water inlet,HRT of 60 min,and catalyst diameter of about 3-7 mm.Last,an optimized reactor was manufactured and a pilot-scale test was conducted to treat kitchen wastewater using catalytic ozonation process.In the pilot-scale test with an ozone dosage of 50 mg/L and HRT of 60 min,the packed-bed reactor filled with catalysts I was able to reduce chemical oxygen demand(COD)from 117 to 59 mg/L.The performance of the catalytic ozonation process in the packed-bed reactor for the advanced treatment of actual kitchen wastewater was investigated via both multi-scale simulation and pilot-scale tests in this study,which provided a practical method for optimizing the reactors of treating refractory organic wastewater.

关键词： catalytic ozonation Multi-scale simulation Pilot-scale study Kitchen wastewater

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Development, dilemma and potential strategies for the application of nanocatalysts in wastewater catalytic ozonation: A review

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Journal of Environmental Sciences 2023年第2期124卷 330-349页

作者： Xiaoguang Jin Changyong Wu Liya Fu Xiangmiao Tian Panxin Wang Yuexi Zhou Jiane Zuo State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing 100012China School of Environment Tsinghua UniversityBeijing 100084China Research Center of Environmental Pollution Control Engineering Technology Chinese Research Academy of Environment SciencesBeijing 100012China

With the continuous development of nanomaterials in recent years,the application of nanocatalysts in catalytic ozone oxidation has attracted more and more researchers’attention due to their excellent catalytic properties.In this review,we systematically summarized the current research status of nanocatalysts mainly involving material categories,mechanisms and catalytic efficiency.Based on summary and analysis,we found most of the reported nanocatalysts were in the stage of laboratory research,which was caused by the nanocatalysts defects such as easy aggregation,difficult separation,and easy leakage.These defects might result in severe resource waste,economic loss and potentially adverse effects imposed on the ecosystem and human health.Aiming at solving these defects,we further analyzed the reasons and the existing reports,and revealed that coupling nano-catalyst and membrane,supported nanocatalysts and magnetic nanocatalysts had promising potential in solving these problems and promoting the actual application of nanocatalysts in wastewater treatment.Furthermore,the advantages,shortages and our perspectives of these methods are summarized and discussed.

关键词： catalytic ozonation Nanocatalyst limitation Membrane Supported nanocatalysts Magnetic nanocatalysts

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Interlayer-confined two-dimensional manganese oxide-carbon nanotube catalytic ozonation membrane for efficient water purification

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Frontiers of Chemical Science and Engineering 2022年第5期16卷 731-744页

作者： Dean Xu Tong Ding Yuqing Sun Shilong Li Wenheng Jing State Key Laboratory of Materials-Oriented Chemical Engineering Nanjing Tech UniversityNanjing 210009China

catalytic ozonation technology has attracted copious attention in water purification owing to its favorable oxidative degradation of pollutants and mitigation of membrane fouling capacity.However,its extensive industrial application has been restricted by the low ozone utilization and limited mass transfer of the short-lived radical species.Interlayer space-confined catalysis has been theoretically proven to be a viable strategy for achieving high catalytic efficiency.Here,a two-dimensional MnO_(2)-incorporated ceramic membrane with tunable interspacing,which was obtained via the intercalation of a carbon nanotube,was designed as a catalytic ozonation membrane reactor for degrading methylene blue.Benefiting from the abundant catalytic active sites on the surface of two-dimensional MnO_(2) as well as the ultralow mass transfer resistance of fluids due to the nanolayer confinement,an excellent mineralization effect,i.e.,1.2 mg O_(3)(aq)mg^(-1) TOC removal(a total organic carbon removal rate of 71.5%),was achieved within a hydraulic retention time of 0.045 s of pollutant degradation.Further,the effects of hydraulic retention time and interlayer spacing on methylene blue removal were investigated.Moreover,the mechanism of the catalytic ozonation employing catalytic ozonation membrane was proposed based on the contribution of the Mn(III/IV)redox pair to electron transfer to generate the reactive oxygen species.This innovative twodimensional confinement catalytic ozonation membrane could act as a nanoreactor and separator to efficiently oxidize organic pollutants and enhance the control of membrane fouling during water purification.

关键词： catalytic membrane reactor catalytic ozonation nanoconfinement two-dimensional manganese oxide

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Fe_(3)C@C/C for catalytic ozonation of silicon-containing wastewater:Dual improvement of silicon resistance and catalytic effect

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Journal of Materials Science & Technology 2023年第5期136卷 65-77页

作者： Shengzhe Wang Lei Ma Rui Wang Chengyu Jin Ying Zhao Xuefei Tan Yanan Zhang Mengyang Liu Chenxing Yao Huangzhao Wei Chenglin Sun Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China Beijing Key Laboratory of Fuels Cleaning and Advanced catalytic Emission Reduction Technology/College of Chemical Engineering Beijing Institute of Petrochemical TechnologyBeijing 102617China College of Materials and Chemical Engineering Heilongjiang Institute of TechnologyHarbin 150050China School of Light Industry and Chemical Engineering Dalian Polytechnic UniversityDalian 116034China

The improvement of catalysts’stability under harsh reaction conditions is vital for their practical applica-bility.Herein,iron carbide(Fe_(3)C)nanoparticles were encapsulated in graphitic carbon in situ and a carbon ball served as the carrier.The synthesized Fe_(3)C@C/C was first utilized to treat an m-cresol wastewater containing Si via catalytic ozonation.Compared with the commercial Fe/Al_(2)O_(3)catalyst,the resistance to Si of the Fe_(3)C@C/C was improved 22.68 times,while the TOC removal rate increased by a factor of 2.9,and it remained stable during 10 cycles and 12000 min of continuous reaction,which further demon-strated its potential for diverse applications.The catalyst exhibits improved resistance to Si because of the dual protection from the carbon-encapsulated structure and carbon carrier.Density functional theory calculations show that the encapsulation of Fe_(3)C using carbon significantly increases the resistance to adsorption of Si on its active sites.In addition,the activation of O_(3)is unimpeded on the Fe_(3)C adsorption sites by the protection from C,thus the generation of reactive oxygen species(ROS)by ozone is largely promoted.The mechanism associated with the resistance of the Fe_(3)C@C/C catalyst to Si and its elevated activity are also elucidated.

关键词： catalytic ozonation Silicon-resistant catalyst Carbon-encapsulated Fe_(3)C@C/C Density functional theory

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Heterogeneous catalytic ozonation by amorphous boron for degradation of atrazine in water

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Chinese Chemical Letters 2023年第5期34卷 408-413页

作者： Zirong Song Jie Li Hongxin Xu Yu Li Yaxiong Zeng Baohong Guan College of Environmental and Resource Sciences Zhejiang UniversityHangzhou 320058China Yiwu Water Construction Group Co. Ltd.Yiwu 322000China College of Chemical and Biological Engineering Zhejiang UniversityHangzhou 320013China

As one of the most promising and practical advanced oxidation processes(AOPs),the catalytic ozonation is triggered by the active components of catalyst,which are usually derived from metals or metal oxides.To avoid the metal pollution from catalyst,here the amorphous boron(A-boron)is used as a metalfree catalyst for catalytic ozonation to produce free radicals for effective degradation of atrazine(ATZ),the world-widely used herbicide and also a widespread pollutant in environment.A-boron exhibits an outstanding performance for catalytic ozonation to remove ATZ from water.As A-boron is introduced into ozonation,the degradation efficiency in 10 min is promoted to 97.1%,much higher than that of 15.1%under ozonation.The mechanism is that the B-B bonds and internal suboxide B in A-boron serve as the main active sites to donate electrons to accelerate ozone decomposition to produce reactive oxygen species(ROS),including·O_(2)^(-)and^(1)O_(2),and further enhance ATZ degradation via ROS reactions.Moreover,the A-boron is still highly active with a degradation efficiency of ATZ over 95%in 10 min even after four successive cycles.This work shows A-boron could be an alternative for the active components of metal or metal oxide in catalytic ozonation.

关键词： Amorphous boron catalytic ozonation Reactive oxygen species Atrazine Advanced oxidation processes

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catalytic ozonation treatment of papermaking wastewater by Ag-doped NiFe2O4 : Performance and mechanism

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Journal of Environmental Sciences 2020年第11期32卷 75-84页

作者： Junyu Zhao Jiashun Cao Yujie Zhao Teng Zhang Di Zheng Chao Li Key Laboratory of Integrated Regulation and Resource Development on Shallow Lakes Ministry of EducationHohai UniversityNanjing 210098China College of Environment Hohai UniversityNanjing 210098China China United Engineering Corporation Limited Zhejiang 310000China

The catalytic ozonation treatment of secondary biochemical effluent for papermaking wastewater by Ag-doped nickel ferrite was investigated.Ag-doped catalysts prepared by sol-gel method were characterized,illustrating that Ag entirely entered the crystalline of Ni Fe2O4 and changed the surface properties.The addition of catalyst enhanced the removal efficiency of chemical oxygen demand and total organic carbon.The results of gas chromatography-mass spectrometer,ultraviolet light absorbance at 254 nm and threedimensional fluorescence excitation-emission matrix suggested that aromatic compounds were efficiently degraded and toxic substances,such as dibutyl phthalate.In addition,the radical scavenging experiments confirmed the hydroxyl radicals acted as the main reactive oxygen species and the surface properties of catalysts played an important role in the reaction.Overall,this work validated potential applications of Ag-doped Ni Fe2O4 catalyzed ozonation process of biologically recalcitrant wastewater.

关键词： Papermaking wastewater Secondary effluent Nickel ferrite Ag-doping catalytic ozonation

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catalytic ozonation of volatile organic compounds(ethyl acetate)at normal temperature

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Chinese Journal of Chemical Engineering 2021年第4期34卷 159-167页

作者： Jiahao Cui Shejiang Liu Hua Xue Xianqin Wang Ziquan Hao Rui Liu Wei Shang Dan Zhao Hui Ding School of Environmental Science and Engineering Tianjin UniversityTianjin 300072China School of Chemical Engineering and Technology Tianjin UniversityTianjin 300072China Tianjin Key Laboratory of Indoor Air Environmental Quality Control School of Environmental Science and EngineeringTianjin UniversityTianjin 300072China

catalytic treatments of VOCs at normal temperature can greatly reduce the cost and temperature of processing,and improve the safety factor in line with the requirements of green chemistry.Activated carbon fiber(ACF)was pretreated with 10%H_(2)SO_(4)by single factor optimization to increase specific surface area and pore volume obviously.The catalytic ozonation performance of ACF loaded with Au,Ag,Pt and Pd noble metals on ethyl acetate was investigated and Pd/ACF was selected as the optimal catalyst which had certain stability.Pd is uniformly distributed on the surface of ACF,and Palladium mainly exists in the form of Pd0 with a amount of Pd+2.The specific surface area of the catalysts gradually decreases as the loading increases.The activation energy of ethyl acetate calculated by Arrhenius equation is 113 kJ mol 1.With 1%Pd loading and the concentration ratio of ozone to ethyl acetate is 3:1,catalytic ozonation performance is maximized and the conversion rate of ethyl acetate reached to 60%in 3050℃Cat 15,00030,000 h^1.

关键词： catalytic ozonation Normal temperature Activated carbon fiber Ethyl acetate Noble metal catalysts

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Effects of operating conditions on iron(hydr)oxides evolution and ciprofloxacin degradation in potassium ferrate-ozone stepwise oxidation system

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Journal of Environmental Sciences 2024年第1期135卷 367-378页

作者： Xiaochen Li Yifan Wang Ning Wang Mei Li Maomao Bai Jingtao Xu Hongbo Wang School of Municipal and Environmental Engineering Shandong Jianzhu UniversityJinan 250101China Resources and Environment Innovation Institute Shandong Jianzhu UniversityJinan 250101China

In this study,a stepwise oxidation system of potassium ferrate(K_(2)FeO_(4))combined with ozone(O+3)was used to degrade ciprofloxacin(CIP).The effects of pH and pre-oxidation time of K_(2)FeO_(4) on the evolution of K_(2)FeO_(4) reduction products(iron(hydr)oxides)and CIP degradation were investigated.It was found that in addition to its own oxidation capacity,K_(2)FeO_(4) can also influence the treatment effect of CIP by changing the catalyst content.The presence of iron(hydr)oxides effectively enhanced the mineralization rate of CIP by catalyzing ozonation.The pH value can influence the content and types of the components with catalytic ozonation effect in iron(hydr)oxides.The K_(2)FeO_(4) pre-oxidation stage can produce more iron(hydr)oxides with catalytic components for subsequent ozonation,but the evolution of iron(hydr)oxides components was influenced by O_(3) treatment.It can also avoid the waste of oxidation capacity owing to the oxidation of iron(hydr)oxides by O_(3) and free radicals.The intermediate degradation products were identified by Fourier transform ion cyclotron resonance mass spectrometry(FT-ICR-MS).Besides,the degradation pathways were proposed.Among the degradation products of CIP,the product with broken quinolone ring structure only appeared in the stepwise oxidation system.

关键词： Potassium ferrate reduction products catalytic ozonation Ciprofloxacin Potassium ferrate pre-oxidation time

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Pretreatment of cyanided tailings by catalytic ozonation with Mn^(2+)/O^3

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Journal of Environmental Sciences 2015年第2期27卷 14-21页

作者： Yulong Li Dengxin Li Jiebing Li Jin wang Asif Hussain Hao Ji Yijie Zhai College of Environmental Science and Engineering State Environmental Protection Engineering Center for Pollution Treatment and Control in Textile Industry Donghua University

The increasing amount of cyanided tailings produced as a by-product has gained significant attention in recent years because of the rapid development of the gold industry and extensive exploitation of gold mineral resources. The effective use of these secondary resources is becoming an important and urgent problem for all environmental protection staff. Manganese-catalyzed ozonation for the pre-oxidation of cyanided tailings was studied and the effects of Mn2＋dosage, initial sulfuric acid concentration, ozone volume flow, temperature and agitation speed on pretreatment were examined. The optimum reaction conditions were observed to be： ore pulp density 2.5%, agitation speed 700 r/min,temperature 60°C, Mn2＋dosage 40 g/L, ozone volume flow 80 L/hr, initial sulfuric acid concentration 1 mol/L, and reaction time 6 hr. Under these conditions, the leaching rate of Fe and weight loss could reach 94.85% and 48.89% respectively. The leaching process of cyanided tailings by Mn2＋/O3 was analyzed, and it was found that the leaching of pyrite depends on synergetic oxidation by high-valent manganese and O3, in which the former played an important part.

关键词： Cyanided tailings Pretreatment Mn2＋/O3 catalytic ozonation

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