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Catalytic ozonation performance and surface property of supported Fe

Zhendong YANG, Aihua LV, Yulun NIE, Chun HU

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 451-456 doi: 10.1007/s11783-013-0509-0

摘要： Fe O was supported on mesoporous Al O or SiO (50 wt.%) using an incipient wetness impregnation method, and Fe O /Al O exhibited higher catalytic efficiency for the degradation of 2,4-dichlorophenoxyacetic acid and -chlorobenzoic acid aqueous solution with ozone. The effect and morphology of supported Fe O on catalytic ozonation performance were investigated based on the characterization results of X-ray diffraction, X-ray photoelectron spectroscopy, BET analysis and Fourier transform infrared spectroscopy. The results indicated that the physical and chemical properties of the catalyst supports especially their Lewis acid sites had a significant influence on the catalytic activity. In comparison with SiO , more Lewis acid sites existed on the surface of Al O , resulting in higher catalytic ozonation activity. During the reaction process, no significant Fe ions release was observed. Moreover, Fe O /Al O exhibited stable structure and activity after successive cyclic experiments. The results indicated that the catalyst is a promising ozonation catalyst with magnetic separation in drinking water treatment.

关键词： heterogeneous catalytic ozonation     iron oxides     supports     surface Lewis acid sites    

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Catalytic activity of cerium-doped Ru/AlO during ozonation of dimethyl phthalate

ZHOU Yunrui, ZHU Wanpeng, CHEN Xun

《环境科学与工程前沿（英文）》 2008年 第2卷 第3期   页码 354-357 doi: 10.1007/s11783-008-0059-z

摘要： In this paper, factors influencing the mineralization of dimethyl phthalate (DMP) during catalytic ozonation with a cerium-doped Ru/AlO catalyst were studied. The catalytic contribution was calculated through the results of a comparison experiment. It showed that doping cerium significantly enhanced catalytic activity. The total organic carbon (TOC) removal over the doped catalyst at 100 min reached 75.1%, 61.3% using Ru/AlO catalyst and only 14.0% using ozone alone. Catalytic activity reached the maximum when 0.2% of ruthenium and 1.0% of cerium were simultaneously loaded onto AlO support. Results of experiments on oxidation by ozone alone, adsorption of the catalyst, Ce ion’s and heterogeneous catalytic ozonation confirmed that the contribution of heterogeneous catalytic ozonation was about 50%, which showed the obvious effect of Ru–Ce/AlO on catalytic activity.

关键词： Ru–Ce/AlO     dimethyl phthalate     mineralization     comparison experiment     catalytic ozonation    

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

《化学科学与工程前沿（英文）》 2022年 第16卷 第5期   页码 731-744 doi: 10.1007/s11705-021-2110-6

摘要： 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 MnO2-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 MnO2 as well as the ultralow mass transfer resistance of fluids due to the nanolayer confinement, an excellent mineralization effect, i.e., 1.2 mg O3(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 two-dimensional 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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Adsorption in combination with ozonation for the treatment of textile waste water: a critical review

Shraddha Khamparia,Dipika Kaur Jaspal

《环境科学与工程前沿（英文）》 2017年 第11卷 第1期 doi: 10.1007/s11783-017-0899-5

摘要： A combination of adsorption with ozonation proved best for dye removal. Toxicity of the textile effluents can be remarkably reduced by combined method. Wide scope for choice of natural materials for treatment of textile dyes. Intrusion of synthetic textile dyes in the ecosystem has been recognized as a serious issue worldwide. The effluents generated from textiles contain large amount of recalcitrant unfixed dyes which are regarded as emerging contaminants in the field of waste water study. Removal of various toxic dyes often includes diverse and complex set of physico-chemical, biological and advanced oxidation processes adopted for treatment. Adsorption in itself is a well-known technique utilized for treatment of textile effluents using a variety of adsorbents. In addition, ozonation deals with effective removal of dyes using high oxidising power of ozone. The review summarizes dye removal study by a combination of ozonation and adsorption methods. Also, to acquire an effective interpretation of this combined approach of treating wastewater, a thorough study has been made which is deliberated here. Results asserts that, with the combined ability of ozone and a catalyst/adsorbent, there is high possibility of total elimination of dyes from waste water. Several synthetically prepared materials have been used along with few natural materials during the combined treatment. However, considering practical applicability, some areas were identified during the study where work needs to be done for effective implementation of the combined treatment.

关键词： Adsorption     Ozonation     Catalytic Ozonation     Textile dyes     Mineralization    

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Catalytic ozonation of reactive red X-3B in aqueous solution under low pressure: decolorization and OH

Hong SUN,Min SUN,Yaobin ZHANG,Xie QUAN

《环境科学与工程前沿（英文）》 2015年 第9卷 第4期   页码 591-595 doi: 10.1007/s11783-014-0694-5

摘要： Catalytic ozonation of Reactive Red X-3B in aqueous solution had been carried out in an ozone oxidation reactor where Mn-Fe-ceramic honeycomb was used as the catalysts. The presence of Mn-Fe-ceramic honeycomb catalyst could obviously improve the decoloration efficiency of Reactive Red X-3B and the utilization efficiency of ozone compared to the results from non-catalytic ozonation. Adsorption of Reactive Red X-3B had no obviously influence on the degradation efficiency. Addition of tert-butanol significantly decreased the degradation efficiency, indicating that the degradation of Reactive Red X-3B followed the mechanism of hydroxyl radical (OH·) oxidation. The operating variables such as reaction pressure and ozone supply had a positive influence on the degradation efficiency, mainly attributing to facilitate the ozone decomposition and OH· formation.

关键词： catalytic ozonation     reactive red X-3B     ceramic honeycomb     hydroxyl radical (OH·)    

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Catalytic ozonation of organic compounds in water over the catalyst of RuO

Jianbing WANG,Guoqing WANG,Chunli YANG,Shaoxia YANG,Qing HUANG

《环境科学与工程前沿（英文）》 2015年 第9卷 第4期   页码 615-624 doi: 10.1007/s11783-014-0706-5

摘要： This research investigates the performances of RuO /ZrO -CeO in catalytic ozonation for water treatment. The results show that RuO /ZrO -CeO was active for the catalytic ozonation of oxalic acid and possessed higher stability than RuO /Al O and Ru/AC. In the catalytic ozonation of dimethyl phthalate (DMP), RuO /ZrO -CeO did not enhance the DMP degradation rate but significantly improved the total organic carbon (TOC) removal rate. The TOC removal in catalytic ozonation was 56% more than that in noncatalytic ozonation. However this does not mean the catalyst was very active because the contribution of catalysis to the overall TOC removal was only 30%. The adsorption of the intermediates on RuO /ZrO -CeO played an important role on the overall TOC removal while the adsorption of DMP on it was negligible. This adsorption difference was due to their different ozonation rates. In the catalytic ozonation of disinfection byproduct precursors with RuO /ZrO -CeO , the reductions of the haloacetic acid and trihalomethane formation potentials (HAAFPs and THMFPs) for the natural water samples were 38%–57% and 50%–64%, respectively. The catalyst significantly promoted the reduction of HAAFPs but insignificantly improved the reduction of THMFPs as ozone reacts fast with the THMs precursors. These results illustrate the good promise of RuO /ZrO -CeO in catalytic ozonation for water treatment.

关键词： ozonation     ruthenium     oxalic acid     dimethyl phthalate     disinfection byproduct    

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Inhibition of bromate formation by reduced graphene oxide supported cerium dioxide during ozonation of

Bei Ye, Zhuo Chen, Xinzheng Li, Jianan Liu, Qianyuan Wu, Cheng Yang, Hongying Hu, Ronghe Wang

《环境科学与工程前沿（英文）》 2019年 第13卷 第6期 doi: 10.1007/s11783-019-1170-z

摘要： GO or RGO promotes bromate formation during ozonation of bromide-containing water. CeO2/RGO significantly inhibits bromate formation compared to RGO during ozonation. CeO2/RGO shows an enhancement on DEET degradation efficiency during ozonation. Ozone (O3) is widely used in drinking water disinfection and wastewater treatment. However, when applied to bromide-containing water, ozone induces the formation of bromate, which is carcinogenic. Our previous study found that graphene oxide (GO) can enhance the degradation efficiency of micropollutants during ozonation. However, in this study, GO was found to promote bromate formation during ozonation of bromide-containing waters, with bromate yields from the O3/GO process more than twice those obtained using ozone alone. The promoted bromate formation was attributed to increased hydroxyl radical production, as confirmed by the significant reduction (almost 75%) in bromate yield after adding t-butanol (TBA). Cerium oxide (less than 5 mg/L) supported on reduced GO (xCeO2/RGO) significantly inhibited bromate formation during ozonation compared with reduced GO alone, and the optimal Ce atomic percentage (x) was determined to be 0.36%, achieving an inhibition rate of approximately 73%. Fourier transform infrared (FT-IR) spectra indicated the transformation of GO into RGO after hydrothermal treatment, and transmission electron microscope (TEM) results showed that CeO2 nanoparticles were well dispersed on the RGO surface. The X-ray photoelectron spectroscopy (XPS) spectra results demonstrated that the Ce3+/Ce4+ ratio in xCeO2/RGO was almost 3‒4 times higher than that in pure CeO2, which might be attributed to the charge transfer effect from GO to CeO2. Furthermore, Ce3+ on the xCeO2/RGO surface could quench Br⋅ and BrO⋅ to further inhibit bromate formation. Meanwhile, 0.36CeO2/RGO could also enhance the degradation efficiency of N,N-diethyl-m-toluamide (DEET) in synthetic and reclaimed water during ozonation.

关键词： Bromate     Catalytic ozonation     Graphene oxide     Cerium dioxide    

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Significant enhancement in catalytic ozonationefficacy: From granular to super-fine powdered activated

Tianyi Chen, Wancong Gu, Gen Li, Qiuying Wang, Peng Liang, Xiaoyuan Zhang, Xia Huang

《环境科学与工程前沿（英文）》 2018年 第12卷 第1期 doi: 10.1007/s11783-018-1022-2

摘要： In this study, super-fine powdered activated carbon (SPAC) hasbeen proposed and investigated as a novel catalyst for the catalyticozonation of oxalate for the first time. SPAC was prepared from commercialgranular activated carbon (GAC) by ball milling. SPAC exhibited highexternal surface area with a far greater member of meso- and macropores(563% increase in volume). The catalytic performances of activatedcarbons (ACs) of 8 sizes were compared and the rate constant for pseudofirst-order total organic carbon removal increased from 0.012 min to 0.568 min (47-fold increase) withthe decrease in size of AC from 20 to 40 mesh (863 mm) to SPAC (~1.0 mm). Furthermore, the diffusion resistance of SPAC decreased17-fold compared with GAC. The ratio of oxalate degradation by surfacereaction increased by 57%. The rate of transformationof ozone to radicals by SPAC was 330 times that of GAC. The resultssuggest that a series of changes stimulated by ball milling, includinga larger ratio of external surface area, less diffusion resistance,significant surface reaction and potential oxidized surface all contributedto enhancing catalytic ozonation performance. This study demonstratedthat SPAC is a simple and effective catalyst for enhancing catalyticozonation efficacy.

关键词： Super-fine activated carbon     Catalytic ozonation     External surface area     Surface reaction     Hydroxyl radical    

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Synthesis of nanofluids composed of deep eutectic solvents and metal-modified MCM-41 particles as multifunctional promoters for fuel oil desulfurization

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1776-1787 doi: 10.1007/s11705-023-2314-z

摘要： Compared with traditional hydrodesulfurization, new nonhydrodesulfurization methods have the advantage of a high removal efficiency for thiophene compounds under mild conditions. However, independent nonhydrodesulfurization technologies are faced with their own shortcomings, such as limitations of the desulfurization performance and regeneration of materials. To overcome these limitations, four nanofluids were prepared by dispersing different metal-modified MCM-41 particles in deep eutectic solvent as multifunctional promoters to develop a comprehensive desulfurization method. Based on the excellent adsorbability and high catalytic activity of the dispersed particles and the outstanding extractability of deep eutectic solvent in nanofluids, a high sulfur removal of 99.33% was achieved for model oil under mild conditions in 15 min. The nanofluids also showed excellent reusability due to their high structural stability. In addition, NF@Cu/Al-MCM-41-2.5% exhibited the best desulfurization performance among the prepared nanofluids. This result was obtained because the introduction of Al ions increased the number of acid sites and defect sites to improve the catalytic activity and adsorbability, and the best affinity of Cu/Al-MCM-41 for the deep eutectic solvent favored the reaction mass transfer. This work opens the door to the development of a comprehensive nonhydrodesulfurization method based on the design of nanofluid materials.

关键词： fuel oil desulfurization     nanofluids     catalytic ozonation    

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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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面向绿色化工应用的陶瓷催化膜反应器的设计与制备 Feature Article

张广儒, 金万勤, 徐南平

《工程（英文）》 2018年 第4卷 第6期   页码 848-860 doi: 10.1016/j.eng.2017.05.001

摘要：

催化膜反应器将反应和分离耦合在一个单元，在化工生产中被视为一种绿色的化工新工艺。而在催化膜反应器中采用陶瓷膜可以使膜反应器的应用范围扩展到一些苛刻环境。本文介绍了基于气体分离的致密陶瓷催化膜反应器和基于非均相体系分离的多孔陶瓷催化膜反应器，评述了近10 年两种不同种类的膜反应器的最新进展以及本课题组的相关工作。面向能源、环境领域的应用，对膜反应器的设计、制备及应用展开重点讨论。针对各个膜反应器，从膜及膜反应器构型入手，以典型的催化反应为例，对膜反应器的设计及优化进行详细论述，最后探讨了进一步发展所面临的瓶颈和可能取得突破的方向，以及膜与膜反应器未来发展应重点关注的领域。

关键词： 致密膜     多孔膜     催化膜反应器     气体分离     非均相催化    

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Mechanisms for simultaneous ozonation of sulfamethoxazole and natural organic matters in secondary effluent

《环境科学与工程前沿（英文）》 2021年 第15卷 第4期 doi: 10.1007/s11783-020-1368-0

摘要：

• SMX was mainly degraded by hydrolysis, isoxazole oxidation and double-bond addition.

关键词： Sulfamethoxazole     Ozonation     Natural organic matters     Secondary effluent     Degradation mechanism    

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Pathway of the ozonation of 2,4,6-trichlorophenol in aqueous solution

PI Yunzheng, WANG Jianlong

《环境科学与工程前沿（英文）》 2007年 第1卷 第2期   页码 179-183 doi: 10.1007/s11783-007-0031-3

摘要： The reaction mechanism and pathway of the ozonation of 2,4,6-trichlorophenol (2,4,6-TCP) in aqueous solution were investigated. The removal efficiency and the variation of HO, Cl, formic acid, and oxalic acid were studied during the semi-batch ozonation experiments (continuous for ozone gas supply, fixed volume of water sample). The results showed that when there was no scavenger, the removal efficiency of 0.1 mmol/L 2,4,6-TCP could reach 99% within 6 min by adding 24 mg/L ozone. The reaction of molecular ozone with 2,4,6-TCP resulted in the formation of HO. The maximal concentration of HO detected during the ozonation could reach 22.5% of the original concentration of 2,4,6-TCP. The reaction of ozone with HO resulted in the generation of a lot of OH° radicals. Therefore, 2,4,6-TCP was degraded to formic acid and oxalic acid by ozone and OH° radicals together. With the inhibition of OH°radicals, ozone molecule firstly degraded 2,4,6-TCP to form chlorinated quinone, which was subsequently oxidized to formic acid and oxalic acid. Two reaction pathways of the degradation of 2,4,6-TCP by ozone and O/OH° were proposed in this study.
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Effect of effluent organic matter on ozonation of bezafibrate

Huan HE,Qian SUI,Shuguang LU,Wentao ZHAO,Zhaofu QIU,Gang YU

《环境科学与工程前沿（英文）》 2015年 第9卷 第6期   页码 962-969 doi: 10.1007/s11783-015-0772-3

摘要： The influence of three effluent organic matter (EfOM) model compounds, humic acid (HA), bovine serum albumin (BSA), and sodium alginate (AGS), on the ozonation of bezafibrate (BF), a typical pharmaceutical and personal care product (PPCP), was investigated. The results show that ozonation efficiently removed BF from aqueous solution with removal efficiencies>95% within 8 min for all conditions. The reaction rate of BF decreased with increasing model compounds concentrations and the influence was more pronounced for HA and BSA, while less pronounced for AGS. Although BF concentration was significantly reduced, the degree of mineralization achieved was only approximately 11%. The addition of HA and BSA improved the mineralization of the solution, while the influence of AGS was minor. The acute toxicity of BF solution during ozonation was determined using the Luminescent bacteria test, and the toxicity exhibited an initial increase and a successive reduction. An overall decreased acute toxicity was observed with an increase of HA. The presence of BSA increased the formation rate of toxicity intermediates and resulted in inhibition peak forward.

关键词： ozonation     bezafibrate     acute toxicity     humic acid     bovine serum albumin     sodium alginate    

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Identification of resistant pharmaceuticals in ozonation using QSAR modeling and their fate in electro-peroxone

《环境科学与工程前沿（英文）》 2021年 第15卷 第5期 doi: 10.1007/s11783-021-1394-6

摘要：

• Effect of converting ozonation to E-peroxone was studied on pharmaceutical removal.

关键词： Ozone     Electro-peroxone     Wastewater     Quantitative structure activity relationship     Advanced oxidation processes    

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标题 作者 时间 类型 操作

Catalytic ozonation performance and surface property of supported Fe

Zhendong YANG, Aihua LV, Yulun NIE, Chun HU

期刊论文

Catalytic activity of cerium-doped Ru/AlO during ozonation of dimethyl phthalate

ZHOU Yunrui, ZHU Wanpeng, CHEN Xun

期刊论文

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

期刊论文

Adsorption in combination with ozonation for the treatment of textile waste water: a critical review

Shraddha Khamparia,Dipika Kaur Jaspal

期刊论文

Catalytic ozonation of reactive red X-3B in aqueous solution under low pressure: decolorization and OH

Hong SUN,Min SUN,Yaobin ZHANG,Xie QUAN

期刊论文

Catalytic ozonation of organic compounds in water over the catalyst of RuO

Jianbing WANG,Guoqing WANG,Chunli YANG,Shaoxia YANG,Qing HUANG

期刊论文

Inhibition of bromate formation by reduced graphene oxide supported cerium dioxide during ozonation of

Bei Ye, Zhuo Chen, Xinzheng Li, Jianan Liu, Qianyuan Wu, Cheng Yang, Hongying Hu, Ronghe Wang

期刊论文

Significant enhancement in catalytic ozonationefficacy: From granular to super-fine powdered activated

Tianyi Chen, Wancong Gu, Gen Li, Qiuying Wang, Peng Liang, Xiaoyuan Zhang, Xia Huang

期刊论文

Synthesis of nanofluids composed of deep eutectic solvents and metal-modified MCM-41 particles as multifunctional promoters for fuel oil desulfurization

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

面向绿色化工应用的陶瓷催化膜反应器的设计与制备

张广儒, 金万勤, 徐南平

期刊论文

Mechanisms for simultaneous ozonation of sulfamethoxazole and natural organic matters in secondary effluent

期刊论文

Pathway of the ozonation of 2,4,6-trichlorophenol in aqueous solution

PI Yunzheng, WANG Jianlong

期刊论文

Effect of effluent organic matter on ozonation of bezafibrate

Huan HE,Qian SUI,Shuguang LU,Wentao ZHAO,Zhaofu QIU,Gang YU

期刊论文

Identification of resistant pharmaceuticals in ozonation using QSAR modeling and their fate in electro-peroxone

期刊论文