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Kinetics and mechanism of nitrobenzene degradation by hydroxyl radicals-based ozonation process enhanced

Weizhou Jiao, Shengjuan Shao, Peizhen Yang, Kechang Gao, Youzhi Liu

《化学科学与工程前沿（英文）》 2021年 第15卷 第5期   页码 1197-1205 doi: 10.1007/s11705-020-1998-6

摘要： This study investigated the indirect oxidation of nitrobenzene (NB) by hydroxyl radicals (·OH) in a rotating packed bed (RPB) using competitive kinetics method with -nitrochlorobenzene as a reference compound. The rate constants of NB with ·OH are calculated to be between (1.465±0.113) × 10 L/(mol·s) and (2.497±0.192) × 10 L/(mol·s). The experimental data are fitted by the modified Arrhenius equation, where the activation energy is 4877.74 J/mol, the order of NB concentration, rotation speed, and initial pH is 0.2425, 0.1400 and 0.0167, respectively. The ozonation process of NB could be enhanced by RPB, which is especially effective for highly concentrated NB-containing wastewater under alkaline conditions. The high gravity technology can accelerate ozone mass transfer and self-decomposition of ozone to produce more ·OH, resulting in an increase in the indirect oxidation rate of NB by ·OH and consequently effective degradation of NB in wastewater.

关键词： high gravity technology     hydroxyl radicals     nitrobenzene     reaction kinetics    

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Simultaneous removal of trihalomethanes by bimetallic Ag/Zn: kinetics study

Ahmed H A DABWAN, Satoshi KANECO, Hideyuki KATSUMATA, Kiyoyuki EGUSA, Tohru SUZUKI, Kiyohisa OHTA,

《化学科学与工程前沿（英文）》 2010年 第4卷 第3期   页码 322-327 doi: 10.1007/s11705-009-0261-y

摘要： In the present work, bimetallic silver/zinc was applied into the degradation of trihalomethanes, THMs: CHCl, CHBrCl, CHBrCl, and CHBr. The kinetics reaction rates and removal efficiencies of the THM compound mixtures, in the aqueous solutions, were investigated. Batch experiments were conducted under mild conditions, ambient temperature, and pressure. The primary degradation reaction followed a pseudo-first-order kinetic law. The first-order rate constants and the degradation efficiencies followed the decreasing order of CHBr>CHBrCl>CHBrCl>CHCl. The bond dissociation energy and hydrophilic/hydrophobic characteristics of the THM compounds may become the most important parameters affecting the degradation kinetics and efficiency by bimetallic Ag/Zn.

关键词： reaction     first-order     dissociation     degradation reaction     aqueous    

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New insight into effect of potential on degradation of Fe-N-C catalyst for ORR

Yanyan GAO, Manman QI, Liang HE, Haiping CHEN, Wenzhe LUO, Ming HOU, Zhigang SHAO

《能源前沿（英文）》 2021年 第15卷 第2期   页码 421-430 doi: 10.1007/s11708-021-0727-2

摘要： In recent years, Fe-N-C catalyst is particularly attractive due to its high oxygen reduction reaction (ORR) activity and low cost for proton exchange membrane fuel cells (PEMFCs). However, the durability problems still pose challenge to the application of Fe-N-C catalyst. Although considerable work has been done to investigate the degradation mechanisms of Fe-N-C catalyst, most of them are simply focused on the active-site decay, the carbon oxidation, and the demetalation problems. In fact, the 2e pathway in the ORR process of Fe-N-C catalyst would result in the formation of H O , which is proved to be a key degradation source. In this paper, a new insight into the effect of potential on degradation of Fe-N-C catalyst was provided by quantifying the H O intermediate. In this case, stability tests were conducted by the potential-static method in O saturated 0.1 mol/L HClO . During the tests, H O was quantified by rotating ring disk electrode (RRDE). The results show that compared with the loading voltage of 0.4 V, 0.8 V, and 1.0 V, the catalysts being kept at 0.6 V exhibit a highest H O yield. It is found that it is the combined effect of electrochemical oxidation and chemical oxidation (by aggressive radicals like H O /radicals) that triggered the highest H O release rate, with the latter as the major cause.

关键词： proton exchange membrane fuel cells (PEMFCs)     oxygen reduction reaction (ORR)     Fe-N-C catalyst     potential     H2O2     degradation    

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Influence of construction-induced damage on the degradation of freeze–thawed lightweight cellular concrete

《结构与土木工程前沿（英文）》 2021年 第15卷 第3期   页码 781-792 doi: 10.1007/s11709-021-0733-9

摘要： During the construction of lightweight cellular concrete (LCC), material damage frequently occurs, causing the degradation and deterioration of the mechanical performance, durability, and subgrade quality of LCC. The construction-induced damage can be more significant than those from the service environment of LCC, such as freeze–thaw (F–T) action in cold regions. However, the effect of construction-induced damage on LCC during F–T cycles is often ignored and the deterioration mechanisms are not yet clarified. In this study, we investigated the factors causing damage during construction using a sample preparation method established to simulate the damage in the laboratory setting. We conducted F–T cycle tests and microstructural characterization to study the effect of microstructural damage on the overall strength of LCC with different water contents under F–T actions. We established the relationship between the pore-area ratio and F–T cycle times, pore-area ratio, and strength, as well as the F–T cycle times and strength under different damage forms. The damage evolution is provided with the rationality of the damage equation, verified by comparing the measured and predicted damage variables. This study would serve as a guide for the construction and performance of LCC in cold regions.

关键词： lightweight cellular concrete     construction-induced damage     freeze-thaw action     microstructure     degradation mechanism    

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Efficient degradation of orange II by ZnMn

Qingzhuo Ni, Hao Cheng, Jianfeng Ma, Yong Kong, Sridhar Komarneni

《化学科学与工程前沿（英文）》 2020年 第14卷 第6期   页码 956-966 doi: 10.1007/s11705-019-1907-z

摘要： A ZnMn O catalyst has been synthesized via a sucrose-aided combustion method and characterized by various analytical techniques. It is composed of numerous nanoparticles (15–110 nm) assembled into a porous structure with a specific surface area (SSA) of 19.1 m ·g . Its catalytic activity has been investigated for the degradation of orange II dye using three different systems, i.e., the photocatalysis system with visible light, the chemocatalysis system with bisulfite, and the photo-chemical catalysis system with both visible light and bisulfite. The last system exhibits the maximum degradation efficiency of 90%, much higher than the photocatalysis system (15%) and the chemocatalysis system (67%). The recycling experiments indicate that the ZnMn O catalyst has high stability and reusability and is thus a green and eximious catalyst. Furthermore, the potential degradation mechanisms applicable to the three systems are discussed with relevant theoretical analysis and scavenging experiments for radicals. The active species such as Mn(III), O , h , e , SO and HO are proposed to be responsible for the excellent degradation results in the photo-chemical catalysis system with the ZnMn O catalyst.

关键词： ZnMn2O4     photo-chemical catalysis     bisulfite     dye degradation    

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Promotive effect of pyridine on indole degradation by activated sludge under anoxic conditions

LI Yongmei, GU Guowei, LI Wenshu

《环境科学与工程前沿（英文）》 2007年 第1卷 第4期   页码 493-497 doi: 10.1007/s11783-007-0079-0

摘要： Batch experiments were carried out to investigate the promotive effect of pyridine on indole degradation under denitrifying conditions. The seed sludge was obtained from a local coal-coking wastewater treatment facility and was acc

关键词： wastewater treatment     coal-coking wastewater     promotive     degradation    

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anchored alginate/poly(acrylic acid/acrylamide) double-network hydrogel composites for efficient catalytic degradation

《化学科学与工程前沿（英文）》 2023年 第17卷 第7期   页码 893-905 doi: 10.1007/s11705-022-2290-8

摘要： A novel alginate/poly(acrylic acid/acrylamide) double-network hydrogel composite with silver nanoparticles was successfully fabricated using the sol–gel method. The presence of carboxyl and amide groups in the network structure provided abundant active sites for complexing silver ions, facilitating the in situ reduction and confinement of silver nanoparticles. In batch experiments, the optimal silver loading was 20%, and 5 mmol·L–1 of p-nitrophenol was completely degraded in 113 s with a rate constant value of 4.057 × 10−2 s–1. In the tap water system and simulated seawater system, the degradation time of p-nitrophenol at the same concentration was 261 and 276 s, respectively, with a conversion rate above 99%. In the fixed-bed experiment, the conversion rate remained above 74% after 3 h at a flowing rate of 7 mL·min–1. After 8 cycling tests, the conversion rate remained at 98.7%. Moreover, the catalyst exhibited outstanding performance in the degradation experiment of four typical organic dyes.

关键词： double-network hydrogel     dye degradation     silver nanoparticles     alginate    

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Sustainable wood-based nanotechnologies for photocatalytic degradation of organic contaminants in aquatic

《环境科学与工程前沿（英文）》 2021年 第15卷 第4期 doi: 10.1007/s11783-020-1346-6

摘要：

•Wood and its reassemblies are ideal substrates to develop novel photocatalysts.

关键词： Wood     Nanocatalysts     Photodegradation     Organic contaminants     Composites    

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Thermodynamic analysis of reaction pathways and equilibrium yields for catalytic pyrolysis of naphtha

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1700-1712 doi: 10.1007/s11705-022-2207-6

摘要： The chain length and hydrocarbon type significantly affect the production of light olefins during the catalytic pyrolysis of naphtha. Herein, for a better catalyst design and operation parameters optimization, the reaction pathways and equilibrium yields for the catalytic pyrolysis of C5–8 n/iso/cyclo-paraffins were analyzed thermodynamically. The results revealed that the thermodynamically favorable reaction pathways for n/iso-paraffins and cyclo-paraffins were the protolytic and hydrogen transfer cracking pathways, respectively. However, the formation of light paraffin severely limits the maximum selectivity toward light olefins. The dehydrogenation cracking pathway of n/iso-paraffins and the protolytic cracking pathway of cyclo-paraffins demonstrated significantly improved selectivity for light olefins. The results are thus useful as a direction for future catalyst improvements, facilitating superior reaction pathways to enhance light olefins. In addition, the equilibrium yield of light olefins increased with increasing the chain length, and the introduction of cyclo-paraffin inhibits the formation of light olefins. High temperatures and low pressures favor the formation of ethylene, and moderate temperatures and low pressures favor the formation of propylene. n-Hexane and cyclohexane mixtures gave maximum ethylene and propylene yield of approximately 49.90% and 55.77%, respectively. This work provides theoretical guidance for the development of superior catalysts and the selection of proper operation parameters for the catalytic pyrolysis of C5–8 n/iso/cyclo-paraffins from a thermodynamic point of view.

关键词： naphtha     catalytic pyrolysis     reaction pathway     equilibrium yield    

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Thermal degradation kinetics and lifetime estimation for polycarbonate/polymethylphenylsilsesquioxane

Jiangbo WANG, Zhong XIN

《化学科学与工程前沿（英文）》 2009年 第3卷 第2期   页码 167-171 doi: 10.1007/s11705-009-0006-y

摘要： The thermal degradation behaviors of polycarbonate/polymethylphenylsilsesquioxane (FRPC) composites were investigated by thermogravimetric analysis (TGA) under isothermal conditions in nitrogen atmosphere. The isothermal kinetics equation was used to describe the thermal degradation process. The results showed that activation energy ( ), in the case of isothermal degradation, was a quick increasing function of conversion (α) for polycarbonate (PC) but was a strong and decreasing function of conversion for FRPC. Under the isothermal condition, the addition of polymethylphenylsilsesquioxane (PMPSQ) retardanted the thermal degradation and enhanced the thermal stability of PC during the early and middle stages of thermal degradation. It also indicated a possible existence of a difference in nucleation, nuclei growth, and gas diffusion mechanism in the thermal degradation process between PC and FRPC. Meanwhile, the addition of PMPSQ influenced the lifetime of PC, but the composite still met the demand in manufacturing and application.

关键词： polycarbonate     polymethylphenylsilsesquioxane     thermal degradation kinetics     activation energy     lifetime    

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bismuth oxyiodide with highly exposed (110) facets on curved carbon nitride for the photocatalytic degradation

《化学科学与工程前沿（英文）》 2022年 第16卷 第7期   页码 1125-1138 doi: 10.1007/s11705-021-2116-0

摘要： Crystalline materials with specific facet atomic arrangements and crystal facet structures exhibit unique functions according to their facet effects, quantum size effects and physical and chemical properties. In this study, a novel high-exposure (110) facet of bismuth oxyiodide (BiOI) was prepared (denoted as BiOI-110), and designed as nanosheets rich in oxygen vacancies by crystal facet design and regulation. Graphitic carbon nitride was designed as curved carbon nitride with dibromopyrazine, denoted as DCN, which contributed to a significant structural distortion in plane symmetry and improved the separation of charge carriers. Novel heterostructured BiOI-110/DCN nanosheets with a high-exposure (110) facet and abundant oxygen vacancies were successfully designed to enhance the photocatalytic degradation of organic pollutants. It was demonstrated that complete and tight contact between BiOI-110 and DCN was achieved by changing the size and crystal facet of BiOI. Oxytetracycline (OTC) and methyl blue dyes were used as targets for pollutant degradation, and 85.6% and 96.5% photocatalytic degradation efficiencies, respectively, were observed in the optimal proportion of 7% BiOI-110/DCN. The experimental results and electron spin resonance analysis showed that •O2– and h+ played a major role in the process of pollutant degradation. Additionally, high-resolution liquid chromatography-mass spectrography was used to identify the reaction intermediates of OTC, and the possible degradation pathway of this pollutant was proposed. Finally, the excellent reusability of BiOI-110/DCN nanomaterials was confirmed, providing a new approach for the removal of antibiotics that are difficult to biodegrade. Overall, crystal facet design has been proven to have broad prospects in improving the water environment.

关键词： high-exposure (110) facet     oxygen vacancy-rich     BiOI-110/DCN heterojunction     photocatalytic degradation     visible-light-response    

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UV-LED/P25-based photocatalysis for effective degradation of isothiazolone biocide

《环境科学与工程前沿（英文）》 2021年 第15卷 第5期 doi: 10.1007/s11783-020-1379-x

摘要：

• UV-LED with shorter wavelength was beneficial for photocatalytic degradation.

关键词： Degradation     Photocatalytic     LED     CMIT     P25    

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Mechanistic insights into the selective photocatalytic degradation of dyes over TiO/ZSM-11

《环境科学与工程前沿（英文）》 2023年 第17卷 第8期 doi: 10.1007/s11783-023-1701-5

摘要：

● TiO2/ZSM-11 was prepared by a facile solid state dispersion method.

关键词： Selective dye degradation     Photocatalysis     TiO2     ZSM-11     Chemisorption    

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Photocatalytic degradation of methyl orange using ZnO/TiO composites

Ming GE , Changsheng GUO , Xingwang ZHU , Lili MA , Wei HU , Yuqiu WANG , Zhenan HAN ,

《环境科学与工程前沿（英文）》 2009年 第3卷 第3期   页码 271-280 doi: 10.1007/s11783-009-0035-2

摘要： ZnO/TiO composites were synthesized by using the solvothermal method and ultrasonic precipitation followed by heat treatment in order to investigate their photocatalytic degradation of methyl orange (MO) in aqueous suspension under UV irradiation. The composition and surface structure of the catalyst were characterized by X-ray diffraction (XRD), field emission scanning electron microscope (FE-SEM), and transmission electron microscopy (TEM). The degradation efficiencies of MO at various pH values were obtained. The highest degradation efficiencies were obtained before 30min and after 60min at pH 11.0 and pH 2.0, respectively. A sample analysis was conducted using liquid chromatography coupled with electrospray ionization ion-trap mass spectrometry. Six intermediates were found during the photocatalytic degradation process of quinonoid MO. The degradation pathway of quinonoid MO was also proposed.

关键词： photocatalytic degradation     methyl orange     ZnO/TiO2 composites     high performance liquid chromatography mass spectrometry (HPLC-MS)    

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Acid Orange 7 degradation using methane as the sole carbon source and electron donor

《环境科学与工程前沿（英文）》 2022年 第16卷 第3期 doi: 10.1007/s11783-021-1468-5

摘要：

• AO7 degradation was coupled with anaerobic methane oxidation.

关键词： Azo dyes     AO7 degradation     Anaerobic methane oxidation     Microbial community     ANME-2d    

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标题 作者 时间 类型 操作

Kinetics and mechanism of nitrobenzene degradation by hydroxyl radicals-based ozonation process enhanced

Weizhou Jiao, Shengjuan Shao, Peizhen Yang, Kechang Gao, Youzhi Liu

期刊论文

Simultaneous removal of trihalomethanes by bimetallic Ag/Zn: kinetics study

Ahmed H A DABWAN, Satoshi KANECO, Hideyuki KATSUMATA, Kiyoyuki EGUSA, Tohru SUZUKI, Kiyohisa OHTA,

期刊论文

New insight into effect of potential on degradation of Fe-N-C catalyst for ORR

Yanyan GAO, Manman QI, Liang HE, Haiping CHEN, Wenzhe LUO, Ming HOU, Zhigang SHAO

期刊论文

Influence of construction-induced damage on the degradation of freeze–thawed lightweight cellular concrete

期刊论文

Efficient degradation of orange II by ZnMn

Qingzhuo Ni, Hao Cheng, Jianfeng Ma, Yong Kong, Sridhar Komarneni

期刊论文

Promotive effect of pyridine on indole degradation by activated sludge under anoxic conditions

LI Yongmei, GU Guowei, LI Wenshu

期刊论文

anchored alginate/poly(acrylic acid/acrylamide) double-network hydrogel composites for efficient catalytic degradation

期刊论文

Sustainable wood-based nanotechnologies for photocatalytic degradation of organic contaminants in aquatic

期刊论文

Thermodynamic analysis of reaction pathways and equilibrium yields for catalytic pyrolysis of naphtha

期刊论文

Thermal degradation kinetics and lifetime estimation for polycarbonate/polymethylphenylsilsesquioxane

Jiangbo WANG, Zhong XIN

期刊论文

bismuth oxyiodide with highly exposed (110) facets on curved carbon nitride for the photocatalytic degradation

期刊论文

UV-LED/P25-based photocatalysis for effective degradation of isothiazolone biocide

期刊论文

Mechanistic insights into the selective photocatalytic degradation of dyes over TiO/ZSM-11

期刊论文

Photocatalytic degradation of methyl orange using ZnO/TiO composites

Ming GE , Changsheng GUO , Xingwang ZHU , Lili MA , Wei HU , Yuqiu WANG , Zhenan HAN ,

期刊论文

Acid Orange 7 degradation using methane as the sole carbon source and electron donor

期刊论文