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Catalytic activities and mechanism of formaldehyde oxidation over gold supported on MnO

Guanglong PANG,Donghui WANG,Yunhong ZHANG,Chunyan MA,Zhengping HAO

《环境科学与工程前沿（英文）》 2016年 第10卷 第3期   页码 447-457 doi: 10.1007/s11783-015-0808-8

摘要： MnO microspheres with various surface structures were prepared using the hydrothermal method, and Au/MnO catalysts were synthesized using the sol-gel method. We obtained three MnO microspheres and Au/MnO samples: coherent solid spheres covered with wire-like nanostructures, solid spheres with nanosheets, and hierarchical hollow microspheres with nanoplatelets and nanorods. We investigated the properties and catalytic activities of formaldehyde oxidation at room temperature. Crystalline structures of MnO are the main factor affecting the catalytic activities of these samples, and γ-MnO shows high catalytic performance. The excellent redox properties are responsible for the catalytic ability of γ-MnO . The gold-supported interaction can change the redox properties of catalysts and accelerate surface oxygen species transition, which can account for the catalytic activity enhancement of Au/MnO . We also studied intermediate species. The dioxymethylene (DOM) and formate species formed on the catalyst surface were considered intermediates, and were ultimately transformed into hydrocarbonate and carbonate and then decomposed into CO . A proposed mechanism of formaldehyde oxidation over Au/MnO catalysts was also obtained.

关键词： MnO2 microspheres     Au/MnO2     formaldehyde oxidation     γ-MnO2    

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Modified iron-molybdate catalysts with various metal oxides by a mechanochemical method: enhanced formaldehydeyield in methanol partial oxidation

Xue Liu, Lingtao Kong, Shengtao Xu, Chaofan Liu, Fengyun Ma

《化学科学与工程前沿（英文）》 2021年 第15卷 第5期   页码 1099-1110 doi: 10.1007/s11705-020-2008-8

摘要： A mechanochemical method was employed to prepare modified iron molybdate catalysts with various metal salts as precursors. The physicochemical properties of the iron molybdate catalysts were characterized, and their performances in catalyzing the reaction from methanol to formaldehyde (HCHO) were evaluated. Iron molybdate catalysts doped with Co(NO ) ·6H O and Al(NO ) ·9H O resulted in high HCHO yields. Compared with a commercial catalyst, the HCHO yields in the reaction with the modified catalyst at an optimal Co/Mo molar ratio reached 97.37%. According to chemical state analysis, the formation of CoO and the efficient decrease in the MoO sublimation rate could be important factors enhancing the HCHO yield in reactions catalyzed with iron molybdate doped with different Co/Mo mole ratios.

关键词： iron molybdate catalyst     metal oxides     methanol to formaldehyde     Co/Mo ratio     formaldehyde yield    

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Synthesis of TiO2 nano-particles and their photocatalytic activity for formaldehyde and methyl orange

XIAO Xinyan, ZHANG Huiping, CHEN Huanqin, LIAO Dongliang

《化学科学与工程前沿（英文）》 2007年 第1卷 第2期   页码 178-183 doi: 10.1007/s11705-007-0033-5

摘要： TiO nano-particles were synthesized by sol-gel technique and characterized by X-ray diffractometer (XRD) and transmission electron microscope (TEM). Their photocatalytic activities for formaldehyde (FA) and methyl orange (MO) degradation were tested using degradation rate (η) as an evaluation index. Based on the orthogonal test results, the optimal condition for TiO preparation was obtained. Results showed that particle sizes were in the range of 10 40 nm, and that prepared TiO had better photocatalytic activity than P25. A simplified model was developed to evaluate the apparent quantum efficiency (Φapp) of this photocatalytic reaction system.

关键词： prepared     photocatalytic activity     apparent     photocatalytic     orthogonal    

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Phenolic compounds removal by wet air oxidation based processes

Linbi Zhou, Hongbin Cao, Claude Descorme, Yongbing Xie

《环境科学与工程前沿（英文）》 2018年 第12卷 第1期 doi: 10.1007/s11783-017-0970-2

摘要： Wet air oxidation (WAO) and catalytic wet air oxidation (CWAO) are efficient processes to degrade organic pollutants in water. In this paper, we especially reviewed the WAO and CWAO processes for phenolic compounds degradation. It provides a comprehensive introduction to the CWAO processes that could be beneficial to the scientists entering this field of research. The influence of different reaction parameters, such as temperature, oxygen pressure, pH, stirring speed are analyzed in detail; Homogenous catalysts and heterogeneous catalysts including carbon materials, transitional metal oxides and noble metals are extensively discussed, among which Cu based catalysts and Ru catalysts were shown to be the most active. Three different kinds of the reactor implemented for the CWAO (autoclave, packed bed and membrane reactors) are illustrated and compared. To enhance the degradation efficiency and reduce the cost of the CWAO process, biological degradation can be combined to develop an integrated technology.

关键词： Wet air oxidation     Catalytic wet air oxidation     Phenolic compounds     Heterogeneous catalysts     Mechanism    

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β-Cyclodextrin promoted oxidation of primary amines to nitriles in water

Dongpo SHI, Hongbing JI, Zhong LI

《化学科学与工程前沿（英文）》 2009年 第3卷 第2期   页码 196-200 doi: 10.1007/s11705-009-0051-6

摘要： A facile, efficient and substrate-selective oxidation of the primary amines with NaClO as oxidant catalyzed by cyclodextrin ( CD) has been developed in water for the first time, and the behavior of cyclodextrin that catalyzed the primary amines to nitriles in water was investigated. It was found that the primary amines which could form host-guest complexes with cyclodextrin were oxidized to nitriles with excellent yields at ambient temperature. The results show that cyclodextrin worked not only as a solubilizing agent but also as a catalyst in these reactions.

关键词： substrate-selective     amines oxidation     β-cyclodextrin    

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Solvent-free mechanochemical mild oxidation method to enhance adsorption properties of chitosan

《环境科学与工程前沿（英文）》 2021年 第15卷 第6期 doi: 10.1007/s11783-021-1416-4

摘要：

• Solvent-free chitosan oxidation is obtained by rapid mechanochemical reaction.

关键词： Chitosan     High energy ball milling     Mechanochemistry     Oxidation    

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Plasma-assisted oxidation of benzoic acid

Anna Khlyustova, Nikolay Sirotkin

《化学科学与工程前沿（英文）》 2020年 第14卷 第4期   页码 513-521 doi: 10.1007/s11705-019-1825-0

摘要： Plasma-assisted oxidation of organic compounds is one of the developing technologies for wastewater treatment. Plasmas effectively accelerate degradation processes due to plasma generated reactive species and ultra-violet radiation. Oxidation of benzoic acid in aqueous solutions by the atmospheric pressure glow discharge and underwater diaphragm discharge was studied and monitored by fluorescence and spectrophotometric methods. Discharge type and solution pH affect the formation rates of mono- and dihydroxybenzoic acids. Dihydroxyl derivatives were formed only by glow discharge action. The yields of hydroxyl radical were estimated on the kinetics data for the hydroxylation of benzoic acid. The steps of the hydroxylation processes and further oxidation were described.

关键词： atmospheric pressure glow discharge     underwater diaphragm discharge     oxidation     benzoic acid     hydroxyl radical    

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Novel coprecipitation–oxidation method for recovering iron from steel waste pickling liquor

Shejiang Liu, Hongyang Yang, Yongkui Yang, Yupeng Guo, Yun Qi

《环境科学与工程前沿（英文）》 2017年 第11卷 第1期 doi: 10.1007/s11783-017-0902-1

摘要： Coprecipitation–oxidation method was developed to recover the iron from wastewater. Fe O nanoparticles were well synthesized from steel waste pickling liquor. Promoters greatly improved the properties of synthesized Fe O nanoparticle. Real-time control of the Fe /Fe molar ratio was achieved by ORP monitoring. Waste pickling liquors (WPLs) containing high concentrations of iron and acid are hazardous waste products from the steel pickling processes. A novel combined coprecipitation–oxidation method for iron recovery by Fe O nanoparticle production from the WPLs was developed in this study. An oxidation–reduction potential monitoring method was developed for real-time control of the Fe /Fe molar ratio. The key coprecipitation–oxidation parameters were determined using the orthogonal experimental design method. The use of promoters greatly improved the Fe O nanoparticle crystallinity, size, magnetization, and dispersion. X-ray diffraction patterns showed that the produced Fe O nanoparticles were single phase. The Fe O nanoparticles were approximately spherical and slightly agglomerated. Vibrating sample magnetometry showed that the Fe O nanoparticles produced from the WPLs had good magnetic properties, with a saturation magnetization of 80.206 emu·g and a remanence of 10.500 emu·g . The results show that this novel coprecipitation–oxidation method has great potential for recycling iron in WPLs.

关键词： Waste pickling liquor     Coprecipitation–oxidation     Fe3O4 nanoparticles     Oxidation–reduction potential     Promoter    

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Electricity-driven ammonia oxidation and acetate production in microbial electrosynthesis systems

《环境科学与工程前沿（英文）》 2022年 第16卷 第4期 doi: 10.1007/s11783-021-1476-5

摘要：

• MES was constructed for simultaneous ammonia removal and acetate production.

关键词： Biocathode     Carbon dioxide     Electrochemical oxidation     Graphite anode     Boron-doped diamond    

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Application of permanganate in the oxidation of micropollutants: a mini review

Xiaohong GUAN, Di HE, Jun MA, Guanghao CHEN

《环境科学与工程前沿（英文）》 2010年 第4卷 第4期   页码 405-413 doi: 10.1007/s11783-010-0252-8

摘要： As a green oxidant, permanganate has received considerable attention for the removal of micropollutants in drinking water treatment. To provide a better understanding of the oxidation of organic micropollutants with permanganate, the oxidation kinetics of 32 micropollutants were compiled. The pollutants include algal toxins, endocrine disrupting chemicals (EDCs), and pharmaceuticals. The oxidation kinetics of micropollutants by permanganate were found to be first order with respect to both contaminant and permanganate concentrations from which second-order rate constants ( ″) were obtained. Permanganate oxidized the heterocyclic aromatics with vinyl moiety (i.e., microcystins, carbamazepine, and dichlorvos) by the addition of double bonds. For the polycyclic aromatic hydrocarbons (PAHs) with alkyl groups, permanganate attacked the benzylic C-H through abstraction of hydrogen. The mechanism for the oxidation of phenolic EDCs by permanganate was a single electron transfer and aromatic ring cleavage. The presence of background matrices could enhance the oxidation of some phenolic EDCs by permanganate, including phenol, chlorinated phenols, bisphenol A, and trichlosan. The toxicity of dichlorvos solution increased after permanganate oxidation, and the estrogenic activity of bisphnol A/estrone increased significantly at the beginning of permanganate oxidation. Therefore, the toxicity of degradation products or intermediates should be determined in the permanganate oxidation processes to better evaluate the applicability of permanganate. The influence of background ions on the permanganate oxidation process is far from clear and should be elucidated in the future studies to better predict the performance of permanganate oxidation of micropollutants. Moreover, methods should be employed to catalyze the permanganate oxidation process to achieve better removal of micropollutants.

关键词： pharmaceuticals     endocrine disrupting chemicals (EDCs)     algal toxins     permanganate     oxidation    

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“ALL FREE” — a novel design concept of applying partial oxidation process to vehicle

Ling LIN, Wenshuang LIN, Qingbiao LI, Yao ZHOU,

《化学科学与工程前沿（英文）》 2010年 第4卷 第2期   页码 207-212 doi: 10.1007/s11705-009-0240-3

摘要： With the rapid expansion of the global motor vehicle population, the transportation sector has taken up a growing proportion among all the carbon dioxide emission-related sectors. To contribute to solutions of the carbon dioxide-oriented problem in transportation, this paper proposes the “ALL FREE” concept that applies partial oxidation process instead of the conventional complete oxidation to vehicle engines. In such an engine, the fuels are partially oxidized into corresponding chemical products, which, as a result, enable the process to be theoretically free of CO, while the heat output of the partial oxidation could drive the vehicle. On the other hand, the resulting products are of great value, which could decrease or even counteract the cost of fuels in transportation. In this paper, the thermodynamic and kinetic data (e.g., the heat output and heat release rate) of five selected partial oxidation reactions were calculated at length to demonstrate and exemplify the theoretical feasibility of the “ALL FREE” concept. It turned out that the partial oxidation of -butane to maleic anhydride has the most potential to meet the basic requirements of this concept. To sum up, this design concept is of significant application potential for the reduction of CO emissions in the transportation industry, although there remain many technical challenges.

关键词： oxidation process     CO     complete oxidation     ALL FREE     -butane    

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Microwave-assisted catalytic oxidation of gaseous toluene with a Cu-Mn-Ce/cordierite honeycomb catalyst

Longli Bo, Shaoyuan Sun

《化学科学与工程前沿（英文）》 2019年 第13卷 第2期   页码 385-392 doi: 10.1007/s11705-018-1738-3

摘要： A novel Cu-Mn-Ce/cordierite honeycomb catalyst was prepared by an incipient wetness method and the catalyst was characterized. The active ingredients were present as various spinel species of Cu, Mn and Ce oxides with different valences and they were unevenly dispersed over the surface of the catalyst. The catalytic oxidation of gaseous toluene was primarily investigated using a fixed bed reactor under microwave heating in the continuous flow mode. Under the optimal conditions of 6.7 wt-% loading of the active component, a bed temperature of 200°C, a flow rate of 0.12 m ·h and an initial concentration of toluene of 1000 mg·m , the removal and mineralization efficiencies of toluene were 98% and 70%, respectively. Thus the use of the microwave effectively improved the oxidation of toluene and this is attributed to dipole polarization and hotspot effects. After four consecutive cycles (a total of 1980 min), the Cu-Mn-Ce/cordierite catalyst still exhibited excellent catalytic activity and structural stability, and the toluene removal was higher than 90%. This work demonstrates the possibility of treating volatile organic compounds in exhaust gases by microwave-assisted catalytic oxidation.

关键词： microwave     catalytic oxidation     toluene     Cu-Mn-Ce/cordierite     mineralization    

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Characterization of electrode fouling during electrochemical oxidation of phenolic pollutant

Xuefeng Liu, Shijie You, Fang Ma, Hao Zhou

《环境科学与工程前沿（英文）》 2021年 第15卷 第4期 doi: 10.1007/s11783-020-1345-7

摘要： Abstract • Electrode fouling is characterized by non-destructive characterization. • Electrode fouling is highly dependent on electrochemical process. • Active chlorine can prevent the formation of polymeric fouling film. Electrode fouling is a problem that commonly occurs during electro-oxidation water purification. This study focused on identifying the fouling behavior of Pt electrode associated with the formation of polymeric layer during electro-oxidation of phenol. The in situ electrochemical measurements and non-destructive observation of the electrode morphology were reported. The results demonstrated that the electrode fouling was highly dependent on thermodynamic process of electrode that was controlled by anode potential. At anode potential lower than 1.0 V vs SHE, the direct electro-oxidation caused the electrode fouling by the formation of polymeric film. The fouling layer decreased the electrochemically active surface area from 8.38 cm2 to 1.57 cm2, indicated by the formation of polymeric film with thickness of 2.3 mm, increase in mass growing at a rate of 3.26 μg/cm2/min. The degree to which the anode was fouled was independent of anion in the electrolyte. In comparison, at anode potential higher than 2.7 V vs SHE, the anions (e.g., chloride) could exert a major influence to the behavior of electrode fouling. The presence of chloride was shown to mitigate the fouling of electrode significantly through preventing the formation of polymeric film by active chlorine (e.g., Cl• and Cl2) produced from anodic oxidation of chloride. Since chloride is the most abundant anionic species existing in both natural and engineered water system, this study not only offers a deep insight into the mechanism of electrode fouling, but also suggests strategies for anti-fouling in the presence of chloride in electro-oxidation process.

关键词： Electro-oxidation     Electrode fouling     Polymeric film     Chloride ions    

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Biological conversion pathways of sulfate reduction ammonium oxidation in anammox consortia

Zhen Bi, Deqing Wanyan, Xiang Li, Yong Huang

《环境科学与工程前沿（英文）》 2020年 第14卷 第3期 doi: 10.1007/s11783-019-1217-1

摘要： The SRAO phenomena tended to occur only under certain conditions. High amount of biomass and non-anaerobic condition is requirement for SRAO. Anammox bacteria cannot oxidize ammonium with sulfate as electron acceptor. AOB and AnAOB are mainly responsible for ammonium conversion. Heterotrophic sulfate reduction mainly contributed to sulfate conversion. For over two decades, sulfate reduction with ammonium oxidation (SRAO) had been reported from laboratory experiments. SRAO was considered an autotrophic process mediated by anammox bacteria, in which ammonium as electron donor was oxidized by the electron acceptor sulfate. This process had been attributed to observed transformations of nitrogenous and sulfurous compounds in natural environments. Results obtained differed largely for the conversion mole ratios (ammonium/sulfate), and even the intermediate and final products of sulfate reduction. Thus, the hypothesis of biological conversion pathways of ammonium and sulfate in anammox consortia is implausible. In this study, continuous reactor experiments (with working volume of 3.8L) and batch tests were conducted under normal anaerobic (0.2≤DO<0.5 mg/L) / strict anaerobic (DO<0.2 mg/L) conditions with different biomass proportions to verify the SRAO phenomena and identify possible pathways behind substrate conversion. Key findings were that SRAO occurred only in cases of high amounts of inoculant biomass under normal anaerobic condition, while absent under strict anaerobic conditions for same anammox consortia. Mass balance and stoichiometry were checked based on experimental results and the thermodynamics proposed by previous studies were critically discussed. Thus anammox bacteria do not possess the ability to oxidize ammonium with sulfate as electron acceptor and the assumed SRAO could, in fact, be a combination of aerobic ammonium oxidation, anammox and heterotrophic sulfate reduction processes.

关键词： Anammox bacteria     Autotrophic     Biological conversion     Sulfate reducing ammonium oxidation (SRAO)    

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Advances and perspectives in catalysts for liquid-phase oxidation of cyclohexane

Hui LI, Yuanbin SHE, Tao WANG

《化学科学与工程前沿（英文）》 2012年 第6卷 第3期   页码 356-368 doi: 10.1007/s11705-012-0903-3

摘要： The latest progress and developments in catalysts for the oxidation of cyclohexane are reviewed. Catalytic systems for the oxidation of cyclohexane including metal supported, metal oxides, molecular sieves, metal substituted polyoxometalates, photocatalysts, organocatalysts, Gif systems, metal-organic catalysts and metalloporphyrins are discussed with a particular emphasis on metalloporphyrin catalytic systems. The advantages and disadvantages of these methods are summarized and analyzed. Finally, the development trends in the oxidation technology of cyclohexane are examined.

关键词： cyclohexane     liquid-phase oxidation     catalysis    

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标题 作者 时间 类型 操作

Catalytic activities and mechanism of formaldehyde oxidation over gold supported on MnO

Guanglong PANG,Donghui WANG,Yunhong ZHANG,Chunyan MA,Zhengping HAO

期刊论文

Modified iron-molybdate catalysts with various metal oxides by a mechanochemical method: enhanced formaldehydeyield in methanol partial oxidation

Xue Liu, Lingtao Kong, Shengtao Xu, Chaofan Liu, Fengyun Ma

期刊论文

Synthesis of TiO2 nano-particles and their photocatalytic activity for formaldehyde and methyl orange

XIAO Xinyan, ZHANG Huiping, CHEN Huanqin, LIAO Dongliang

期刊论文

Phenolic compounds removal by wet air oxidation based processes

Linbi Zhou, Hongbin Cao, Claude Descorme, Yongbing Xie

期刊论文

β-Cyclodextrin promoted oxidation of primary amines to nitriles in water

Dongpo SHI, Hongbing JI, Zhong LI

期刊论文

Solvent-free mechanochemical mild oxidation method to enhance adsorption properties of chitosan

期刊论文

Plasma-assisted oxidation of benzoic acid

Anna Khlyustova, Nikolay Sirotkin

期刊论文

Novel coprecipitation–oxidation method for recovering iron from steel waste pickling liquor

Shejiang Liu, Hongyang Yang, Yongkui Yang, Yupeng Guo, Yun Qi

期刊论文

Electricity-driven ammonia oxidation and acetate production in microbial electrosynthesis systems

期刊论文

Application of permanganate in the oxidation of micropollutants: a mini review

Xiaohong GUAN, Di HE, Jun MA, Guanghao CHEN

期刊论文

“ALL FREE” — a novel design concept of applying partial oxidation process to vehicle

Ling LIN, Wenshuang LIN, Qingbiao LI, Yao ZHOU,

期刊论文

Microwave-assisted catalytic oxidation of gaseous toluene with a Cu-Mn-Ce/cordierite honeycomb catalyst

Longli Bo, Shaoyuan Sun

期刊论文

Characterization of electrode fouling during electrochemical oxidation of phenolic pollutant

Xuefeng Liu, Shijie You, Fang Ma, Hao Zhou

期刊论文

Biological conversion pathways of sulfate reduction ammonium oxidation in anammox consortia

Zhen Bi, Deqing Wanyan, Xiang Li, Yong Huang

期刊论文

Advances and perspectives in catalysts for liquid-phase oxidation of cyclohexane

Hui LI, Yuanbin SHE, Tao WANG

期刊论文