Journal of Water Process Engineering
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2020
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IF 3.465
Yu Li,Luchao Wu,Yun Wang,Peng Ke,Jie Xu,Baohong Guan
Ozone decomposition into free radicals, which can be facilitated by enhancing electron transfer between ozone and catalyst, is an important segment in catalytic ozonation. We doped cerium uniformly on γ-Al 2 O 3 with an impregnation–calcination method to enhance electron transfer in catalytic ozonation of phenol in aqueous solution. The removal efficiency of phenol is raised from 39.7% by ozonation alone to 46.3% by catalytic ozonation with Ce/Al 2 O 3 in 50 min reaction. A higher Ce 3+ /Ce 4+ ratio in Ce/Al 2 O 3 witnesses a higher electron transfer rate in catalytic ozonation and thus a higher degradation efficiency of phenol, illustrating that the activity of Ce/Al 2 O 3 depends on the valence state of Ce. The electron transfer cycle is formed by the electron donation from Ce 3+ to ozone molecule and the electron acceptance of Ce 4+ from adjacent lattice oxygen. After getting the electron, the ozone molecule is decomposed to generate free radical of ·OH on the surface of Ce/Al 2 O 3 . The continuous flow experiments exhibit a stable and high catalytic activity of Ce/Al 2 O 3 for catalytic ozonation, implying the feasibility in practical application.
研究领域:
环境科学
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催化材料
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2019
·
IF 5.108
Weirui Chen,Yixiang Bao,Xukai Li,Jun Huang,Yiming Tang,Laisheng Li
Mesoporous Fe-Cu@SiO 2 core-shell catalyst was synthesized and assessed for its catalytic activity in the ozonation of salicylic acid (SA). The synthesized catalyst was characterized by XRD, TEM, SEM, XPS, H 2 -TPR, etc. Fe-Cu@SiO 2 exhibited a regular spherical shape and had the surface area at 1216 m 2 g −1 . The wrapping of metal components and their strong interaction prevented metal leaching. Fe-Cu@SiO 2 showed the highest activity for SA mineralization when compared with Fe@SiO 2 and Cu@SiO 2 . In Fe-Cu@SiO 2 /O 3 , 88% TOC was removed, which was 2.5 times as much as that in sole ozonation. SA degradation efficiency in Fe-Cu@SiO 2 /O 3 increased with initial pH. O 3 , ·OH and H 2 O 2 were the main reactive oxygen species accounting for SA mineralization. Due to their scavenging effect of ·OH, NH 4 + , NO 3 − and humic acids would inhibit the degradation efficiency of Fe-Cu@SiO 2 /O 3 . Acidic sites, oxygen vacancies and the Fe-Cu(I/II) electron transfer were responsible for ozone decomposition and ·OH generation. SA mineralization proceeded through the ·OH mechanism. Moreover, SA mineralization in O 3 and Fe-Cu@SiO 2 /O 3 both exhibited a two-stage pseudo first-order kinetics (stage I: 0–45 min; stage II: 45–120 min). The degradation intermediates were detected to investigate the reaction pathway. ORP and EEM were used to monitor the degradation process. Great difference was found for carboxylic acids accumulation in O 3 and Fe-Cu@SiO 2 /O 3 . The accelerated removal of oxalic acid and humic acid-like intermediates were responsible for the two-stage pseudo first-order kinetics.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
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2012
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IF 2.947
Liu Hao,Deng Huiping,Shi Jun
Pyrene and fluoranthene, typical polycyclic aromatic hydrocarbons, are very difficult to be removed from water due to their hydrophilic nature and relatively low reactivity towards ozone. In the study, Ce-loaded activated carbon (Ce-AC) is prepared and used as catalyst to promote pyrene and fluoranthene degradation by ozone. The catalytic activity of Ce-AC is investigated under various experiment conditions. Results indicate both of pyrene and fluoranthene removals are significantly enhanced in Ce-AC + O 3 due to effective generation of hydroxyl radicals ( OH), as compared to ozonation alone and AC + O 3 . The mineral matter present in the activated carbon positively contributes to remove fluoranthene and the optimized cerium loading of AC is 0.3% in ozonation process. Moreover, the toxicity of pyrene is more than that of fluoranthene and the reaction solution's toxicity is substantially reduced by catalytic ozonation with Ce-AC.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2017
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IF 3.387
Ruimei Fang,Haibao Huang,Wenjun Huang,Jian Ji,Qiuyu Feng,Yajie Shu,Yujie Zhan,Gaoyuan Liu,Ruijie Xie
Coal based activated carbon (AC) was pretreated by peracetic acid solution and used for supporting Mn catalyst towards oxidation of gaseous benzene by catalytic ozonation . The as-obtained activated carbon was characterized by XPS, BET, SEM, and TG technologies. It indicates that peracetic acid solution modification not only raised the quantity of chemisorbed oxygen or water, and hydroxyl group on activated carbon material surface, but also increased the specific surface area and benzene adsorption capacity of activated carbon. Benzene could be completely removed in 300 min and CO 2 selectivity reached to 61.9% over Mn/AC-modified catalyst. A possible catalytic ozonation mechanism of activated carbon which was treated by peracetic acid solution supported Mn catalyst for oxidation of benzene was proposed.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Yizhen Cheng,Jing Kang,Pengwei Yan,Jimin Shen,Zhonglin Chen,Xinwei Zhu,Qiang Tan,Linlu Shen,Shuyu Wang,Shaobin Wang
Herein, a highly dispersed catalyst (ZnO x -500) was synthesized for heterogeneous catalytic ozonation (HCO), which had a simple ZnO crystal phase but riched in oxygen vacancies (OVs). The O 3 /ZnO x -500 system exhibited both superior catalytic activity and stability after several cycles, providing a promising strategy for atrazine (ATZ) removal. The strong inhibition of phosphoric acid validated the dominant role of the hydroxyl group (−OH) from water molecule (H 2 O) dissociation on the zinc site near OVs. Density functional theory calculation further revealed that OVs on (100) and (101) planes could make more zinc sites exposed and facilitate the formation of hydrated −OH, which was easier to approach O 3 for its decomposition to generate hydroxyl radical ( • OH). This work revealed the intrinsic relationship between OVs and hydrated −OH in an aqueous solution, providing new insight into the solid-liquid interface mechanism of HCO.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Weirui Chen,Weijie Chen,Yimin Luo,Yanqi Feng,Xukai Li,Jing Wang,Ping Li,Liying Bin,Bing Tang,Laisheng Li
g-C 3 N 4 (CN) based catalysts were effective for photocatalytic ozonation (PCO), but their stability during reaction remained a mystery. This study investigated the change on PCO activity and stability of CN induced by F or I doping. Compared with CN, F-CN had the greater VB potential while I-CN had a greater CB position, which both led to their better O 3 activation. F-CN and I-CN PCO showed the greater oxalic acid (OA) degradation than that of CN PCO process. Though the enhanced activity, both F-CN and I-CN demonstrated the lower stability compared with that of CN. Because of the existing of reactive oxygen species (ROS) like •OH, •O 2 - and h vb + , CN, F-CN and I-CN were partially oxidized, generating NO 3 - and organic molecules such as cyanuric acid. h vb + and •OH mainly accounted for the decomposition of three CN. Triazine ring oxidation resulted in internal tearing and edge fracture as well as the formation of O-containing groups on all CN-based catalysts. O contents in catalysts initially increased and then decreased with reaction time, indicating that surface O-containing groups were unstable. The structural destroy could be eased with the present of organic pollutants. This study deepened the understanding of fate of CN based catalysts during PCO application.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
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2024
·Vol. 14
·期 12
·885
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IF 3.8
Yulin Sun,Yiwei Zhang,Baoqing Hou,Yong He,Wubin Weng,Yanqun Zhu,Zhihua Wang
Formaldehyde (HCHO) is known as one of the important indoor organic pollutants. How to remove and decompose the low concentration of formaldehyde at room temperature is important for indoor environments. Catalytic ozonation is an efficient method to thoroughly remove HCHO at room temperature, with high efficiency and few byproducts. A series of MnOx/γ-Al2O3catalysts were prepared in this work via the impregnation method and treated with different reagents (acid, alkali, and H2O2) to evaluate their catalytic activity for HCHO removal. The results showed that MnAl-II (acid treatment) performed well in activity tests, reaching a nearly 100% HCHO conversion at an O3/HCHO of 2.0 and attaining a CO2selectivity of above 95% at an O3/HCHO of 3.0 at 30 °C, with almost no ozone residual existing. The larger specific surface area, abundant oxygen vacancies, and higher number of acid sites contributed to the excellent performance of MnAl-II. Stability and H2O resistance tests of MnAl-II were also conducted. To reveal the intermediate product formation and further investigate the reaction mechanism of HCHO ozonation, in-situ DRIFTS measurement was carried out combined with DFT calculations.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Cuili Xing,Xinyi Yao,Kaiwei Zheng,Yang Liu,Yuankui Sun,Xiaohong Guan
Efficient removal of recalcitrant Cr(III)-organic complexes is always challenged by slow decomplexation process and the possible accumulation of highly toxic Cr(VI). Herein, a sulfidated zero-valent iron coupled ozonation strategy (S-ZVI/O 3 ) was proposed to achieve efficient decomplexation and simultaneous abatement of Cr(III)-EDTA without Cr(VI) accumulation. Results revealed that S-ZVI could catalyze O 3 to enhance removal of Cr(III)-EDTA and total organic carbon. Moreover, 88.3 % of total Cr was sequestrated by S-ZVI/O 3 and the corresponding kinetic constant was 3.1 times higher than that of ZVI/O 3 . Mechanistically, electron paramagnetic resonance and probing tests verified HO • was the dominant reactive oxidation species for decomplexation of Cr(III)-EDTA in both S-ZVI/O 3 and ZVI/O 3 . More attractively, it was found that structural Fe(II) was the major O 3 activator in S-ZVI/O 3 , whereas dissolved Fe 2+ accounted for O 3 catalyzation in ZVI/O 3 . The X-ray absorption spectroscopy analysis revealed that sulfidation treatment could enhance corrosion of ZVI with the formation of sufficient Fe(II) species. The in-situ formed Fe(II) could not only transform undesired Cr(VI) back to Cr(III) but also co-precipitate with Cr(III) to form solid Fe-Cr hydroxides. Besides Cr(III)-EDTA, S-ZVI/O 3 is also applicable to other EDTA complexed heavy metals. This work would provide a new method for the heavy metal complexes removal from water.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Scientific Reports
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2021
·Vol. 11
·期 1
·1-13
·
IF 4.38
Tang Xi,Zhang Yifei,Li Weiqi,Geng Jinju,Ren Hongqiang,Xu Ke
Humic acid (HA) is the main component of organic matter in effluent from wastewater treatment. The effective removal of HA is significant. In this study, a novel catalyst was prepared using a transition metal oxide as the active component and Al 2 O 3 as a granular carrier. The mechanism of catalytic ozonation of HA under neutral pH conditions and its efficiency were investigated. Under the chosen conditions (an ozone concentration of 2.2 mg/L, 50 mg/L HA solution, catalyst dosage of 5 g/L and initial pH of 6.49), the Cu/Ce–Al 2 O 3 bimetallic catalyst led to 54.79% TOC removal rate after 30 min; the removal rate by ozone alone was only 20.49%. The characteristics of organic compounds determined by FT-IR and GC–MS showed that organic compounds were degraded significantly by the catalytic treatment. The addition of catalysts could effectively degrade toxic intermediates and reduce the acute toxicity produced by ozonation. Humic acid substances were largely removed and transformed into biodegradable intermediates. This study proposes a new and efficient ozonation catalyst for practical applications in advanced wastewater treatment.
研究领域:
环境科学
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化学工程
·
毒理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2014
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IF 2.235
Jun Chen,Weijie Wen,Linjun Kong,Shuanghong Tian,Fuchuan Ding,Ya Xiong
Magnetically separable MnFe2O4 was prepared successfully by a sol–gel combustion method. The synthesized MnFe2O4 was characterized by X-ray diffraction (XRD), scanning electronic microscopy (SEM), Brunauer–Emmett–Teller (BET) surface area, zeta potential, and magnetic hysteresis loops. The catalytic activity of MnFe2O4 was evaluated by the ozonation of 4-chlorophenol (4-CP) at different solution pH value, ozone gas concentration, MnFe2O4 dosage, and initial 4-CP concentration. The ozone consumption was monitored and the ·OH exposure was calculated in different processes. It was found that MnFe2O4 was highly effective in catalyzing ozone decomposition and favored to generate more hydroxyl radicals. Moreover, the synergistically catalytic effect between Mn and Fe in MnFe2O4 was confirmed. Finally, lifetime of MnFe2O4 was measured in a novel integrated membrane-heterogeneous catalytic ozonation reactor designed for the first time. All the experimental results show that MnFe2O4 is a highly recoverable, efficient, and durable catalyst in the ozonation.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL ENGINEERING SCIENCE
·
2022
·Vol. 39
·期 1
·56-63
·
IF 2.172
Jie Zhang,Ben Dong,Jing Liu,Wuxu Yang,Sijie Ge,Shilong He
In this article, Mn doping on Ce-based γ-Al2O3 (i.e., Mn-Ce-γ-Al2O3) was synthesized and then employed as catalysts to study the removal of phenol from aqueous solutions through catalytic ozonation process. The results showed that the phenol removal was remarkably increased to 97.50% if Mn-Ce-γ-Al2O3 was adopted as the catalyst. In addition, the kinetic rate of the reaction was increased, approximately, about 1.49 times when using Ce-γ-Al2O3 catalyst with Mn doping. Moreover, X-ray diffraction, transmission electron microscopy, Brunner-Emmet-Teller measurements, and X-ray photoelectron spectroscopy techniques were used to comprehensively characterize the physicochemical properties of the synthesized Mn-Ce-γ-Al2O3 catalyst, including the phases, morphologies, textural properties, and dispersity of the surface active species. More uniform channel mesoporous structures were obtained after Mn doping on Ce-γ-Al2O3, which could enhance the gas-liquid mass transfer rate, surface hydroxyl groups, Ce3+/Ce4+ ratio, and the formation of Mn-Ce solid solution. In this study, the effects of Mn doping on Ce-based γ-Al2O3 on phenol degradation were investigated and the removal mechanisms were suggested for a better understanding of the improved removal efficiency.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Yingjie Wen,Xu Chen,Linfeng Su,Shuqian Dong,Li Yi,Peilei He,Wen Yang,Zhiyi Lu
The catalytic ozonation-based advanced oxidation process (AOP) is applied to remove nondegradable chemical oxygen demand (COD), while the application in industry is limited by the economics and activity of catalysts. In this study, we demonstrate that by taking atrazine (ATZ) as a model pollutant, the removal rates of catalytic ozonation were negatively correlated with the interlayer water content of metal-modified montmorillonite (M x @MMT), instead of the loadings metals. Among the modified MMT, Zn 0.1 @MMT achieved 83.2% degradation of ATZ within 15 min, and corresponding removal rates of COD and total organic carbon (TOC) reached 40.3% and 46.5%, respectively. Detailed EPR and quenching experiments identified that hydroxyl radicals (HO•) were the main reactive oxygen species and QTOF/MS/MS analysis helped to propose a possible degradation pathway of ATZ. Moreover, the catalytic performance of Zn 0.1 @MMT under different conditions was also systematically evaluated.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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