ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2024
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IF 10.8
Yang Guo,Erzhuo Zhao,Jingfei Long,Gang Yu,Yujue Wang
Heterogeneous surface processes such as adsorption and oxidation with surface-adsorbed reactive oxygen species (ROSad, e.g., adsorbed oxygen atom (*Oad) and hydroxyl radicals (•OHad)) have been suggested to play an important role in pollutant abatement during heterogeneous catalytic ozonation (HCO). However, to date, there is no reliable method to quantitatively evaluate the contribution of heterogeneous surface processes to pollutant abatement (fS) during HCO. In this study, we developed a method by combining probe compound-based experiments with kinetic modeling to distinguish heterogeneous surface processes from homogeneous bulk reactions with aqueous O3 and ROS (•OH and superoxide radicals (O2•–) in the abatement of various pollutants (e.g., atrazine, ibuprofen, tetrachloroethylene, and perfluorooctanoic acid) during HCO with reduced graphene oxide. The results show that the pollutants that have a low affinity for the rGO surface (e.g., ibuprofen and tetrachloroethylene) were essentially abated by homogeneous bulk reactions, while the contribution of heterogeneous surface processes was negligible (fS < 5%). In contrast, heterogeneous surface processes played an important or even dominant role in the abatement of pollutants that have a high surface affinity (e.g., fS = 32–82% for atrazine and perfluorooctanoic acid). This study is a critical first step in quantitatively evaluating the role of heterogeneous surface processes for pollutant abatement during HCO, which is crucial to understanding the mechanism of HCO and designing catalysts for effective pollutant abatement.
研究领域:
环境科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Siyi Zhou,Hao Cheng,Sridhar Komarneni,Jianfeng Ma
In this study, a cobalt-doped nickel disulfide (Co-Ni 3 S 2 ) catalyst was prepared by a one-step hydrothermal method, which was grown on the surface of firm and dense three-dimensional porous nickel foam (NF). Although researchers have conducted extensive research on heterogeneous catalytic ozonation (HCO) over the past decades, the development of highly efficient, easily separable, stable, and recyclable HCO catalysts is still a bottleneck for practical applications. Taking p-nitrophenol (PNP) as the targeted pollutant, the synergistic effect of Co-Ni 3 S 2 /NF composites and ozone was studied. The results show that Co-Ni 3 S 2 /NF with different doping ratios can degrade PNP by more than 99% within 40 minutes, showing high activity. At the same time, in the cycle experiment, Co-Ni 3 S 2 /NF showed good stability and recyclability compared with the powder catalyst and therefore, the former could reduce water treatment cost. We also found that in the Co-Ni 3 S 2 /NF/O 3 system, the production rates of 1 O 2 , •OH and O 2 •- can be greatly improved, and the process of degradation is synergistic with both non-radicals and free radicals.
研究领域:
环境科学
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材料科学
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催化化学
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产品关联
DOI
高影响因子
RSC Advances
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2022
·Vol. 12
·期 48
·31024-31031
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IF 4.036
Jia Yuan,Yang Li,Yun Guo,Zhiwei Wang
Ozonation process is a promising yet challenging method for the removal of refractory organic matter due to the sluggish reaction for generating hydroxyl radical (˙OH) at a neutral pH condition. Herein, an efficient heterogeneous catalytic ozonation system using CeO2/Al2O3 catalyst was developed to remove dimethyl phthalate (DMP) from wastewater. Under a neutral condition of pH = 6, this system achieved almost 100% DMP removal within 15 min at an optimized catalyst dosage of 30 g L−1 and the ozone flow rate of 22.5 mg min−1. Moreover, the catalytic ozonation system exhibited a stable degradation performance of DMP in a wider pH range (pH = 5–10). The results of electron paramagnetic resonance (EPR) and quantitative tests confirmed the ultrafast conversion of O3 to ˙OH (0.774 μM min−1) on the surface of CeO2 based ceramic catalyst. The quenching experiments further supported the predominant role of ˙OH in the mineralization of DMP. These results highlight the potential of using the heterogeneous catalytic ozonation system for the efficient removal of refractory organic matter from wastewater.
研究领域:
环境工程
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化学工程
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水处理
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Yizhen Cheng,Xiaoyu Zhu,Pengwei Yan,Binyuan Wang,Jing Kang,Jimin Shen,Qiang Tan,Xinwei Zhu,Tianhao She,Jinxiang Zuo,Shengxin Zhao,Zhonglin Chen
Novel zero-valent iron (ZVI) and zero-valent zinc (ZVZ) bimetal-supported biochar (ZF@BC) was developed for heterogeneous catalytic ozonation (HCO), which demonstrated the unique dual synergistic adsorption and catalysis-induced effective O 3 triggering and interfacial decontamination. ZF@BC exhibited impressive catalytic and structure stabilities for 2-methyl-4-chlorophenoxyacetic acid (MCPA) degradation during long-lasting HCO, which can resist interference from a complex water quality background. Abundant electron-rich oxygen-containing functional groups and defects on BC contributed to the adsorption of MCPA and O 3 , respectively, while the introduced ZVZ was anticipated to expedite O 3 decomposition by facilitating single-electron transfer reduction of O 2 and establishing a robust connection with ZVI. Continuous efficacy of bimetal in three stages enhanced the efficiency of O 3 utilization and hydroxyl radicals ( • OH) yield, thereby safely mitigating the associated toxicity of MCPA after treatment. The development of O 3 /ZF@BC introduced a sustainable, long-term decontamination strategy and provided valuable insights for the advancement of HCO.
研究领域:
环境科学
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水处理
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催化
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
WATER RESEARCH
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2021
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IF 11.236
Shi-Qi Tian,Jing-Yao Qi,Yun-Peng Wang,Yu-Lei Liu,Lu Wang,Jun Ma
After reaction with permanganate or ferrate, the resulted Mn-loaded and Fe-loaded biochar (MnOx/biochar and FeOx/biochar) exhibited excellent catalytic ozonation activity. O 3 (2.5 mg/L) eliminated 48% of atrazine (ATZ, 5 μM) within 30 min at pH 7.0, while under identical conditions, ozonation efficiency of ATZ increased to 83% and 100% in MnOx/biochar and FeOx/biochar (20 mg/L) heterogeneous catalytic systems, respectively. Radical scavenger experiment and electron paramagnetic resonance (EPR) analysis confirmed that hydroxyl radical (•OH) was the dominant oxidant. Total Lewis acid sites on MnOx/biochar and FeOx/biochar were 3.5 and 4.1 times of that on the raw biochar, which induced enhanced adsorption of O 3 and its subsequent decomposition into •OH. Electron transfer via redox pairs on MnOx/biochar and FeOx/biochar was observed by cyclic voltammetry scans, which also functioned in the improved catalytic capacity. Degradation pathways of ATZ in MnOx/biochar and FeOx/biochar ozonation systems were proposed, with 34.6% and 44.8% of dechlorination effect accomplished within 30 min of reaction, which was improved by 4.1 and 5.3 times compared to pure ozonation. After 12-hour treatment, acute toxicity of ATZ oxidation products was reduced from 38.3% of pure ozonation system to 14.5% and 6.3% of activated ozonation systems with MnOx/biochar and FeOx/biochar, respectively. Mn-loaded biochar and Fe-loaded biochar have great potential for heterogeneous catalytic ozonation of polluted water.
研究领域:
环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
Journal of Cleaner Production
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2022
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IF 11.072
Linfeng Su,Xu Chen,Hui Wang,Yude Wang,Zhiyi Lu
The ozone activation reaction is becoming more popular with the treatment of organic pollutants, while the key to improving the efficiency heavily lies in the selection of active catalysts. In this study, we demonstrate that synthetic 4A zeolite with a high surface oxygen vacancy density and acidity exhibits excellent activity toward the ozonation process, where the removal rates of atrazine (ATZ) reached 87.5% at 6 min, and the removal rates of Chemical Oxygen Demand (COD) and Total Organic Carbon (TOC) reached 66.7% and 35.8% at 15 min, respectively. Compared with commercial 4A zeolite and synthetic 4A zeolite with acid treatment, the ozonation activities of 4A zeolites positively correlate with the surface acidity. Mechanistic investigations have identified that hydroxyl radicals are the main reactive oxygen species , and thus, the degradation pathway of ATZ is provided. Moreover, the influences of catalyst dosage, reaction temperature, pH and cycling stability on ozonation performance are systematically evaluated.
研究领域:
环境科学
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催化
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水处理
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Shanli Wang,Mingyan Zhang,Chao Li,Licong Xu,Wenbin Jiang,Deyou Yu,Minghua Wu,Bin Yu
Manipulating the electron density of active sties to develop highly efficient catalysts is expected to be one of the most ideal approaches to facilitate overall efficiency of the heterogenous catalytic ozonation (HCO) process. In this study, we demonstrate a fluorine-doping engineering to optimize the HCO activity of aluminum oxide through an improved sol–gel method using NH 4 F (NF-Al 2 O 3 ) and HF (HF-Al 2 O 3 ) as the fluorine source. We provide evidence that the fluorine atom is successfully incorporated into crystal structure of NF-Al 2 O 3 via the formation of Al-F-Al bonds, accompany with the generation of oxygen vacancy defects , which allow for ozone molecule adsorption and activation. In contrast, the fabricated HF-Al 2 O 3 only features the presence of Al x F y ·nH 2 O instead of Al-F-Al structure probably due to the unexpected etching reaction. The introduction of fluorine atom largely decreases the local electron density of neighboring Al of NF-Al 2 O 3 catalyst evidenced by the two-fold increment in the amount of strong Lewis acid sites. Consequently, the HCO activity of NF-Al 2 O 3 catalyst is found promotion by 42.9% over pure Al 2 O 3 in terms of the degradation kinetic rate constant ( k obs ). The NF-Al 2 O 3 catalyst exhibits a powerful capacity to selectively catalyze ozone molecule into singlet oxygen ( 1 O 2 ), rendering the HCO system with high-tolerance to coexisting water matrixes (e.g., humic acid, chlorine ions, carbonate). Moreover, NF-Al 2 O 3 initiated HCO system can effectively purify wastewaters from textile industry with high-quality enough to be reused for textile dyeing. Therefore, our study provides a novel strategy to develop effective HCO catalysts for promoting wastewater treatment and reuse.
研究领域:
环境科学
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催化
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水处理
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材料科学
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产品关联
DOI
高影响因子
Nanoscale
·
2023
·Vol. 15
·期 12
·5909-5918
·
IF 6.7
Wenjie Wu,Saiyu Bu,Liang Bai,Yuanting Su,Yenan Song,Haitao Sun,Guangyin Zhen,Ke Dong,Lunhua Deng,Qinghong Yuan,Chengbin Jing,Zhuo Sun
Non-thermal plasma (NTP) degradation of volatile organic compounds (VOCs) into CO2 and H2O is a promising strategy for addressing ever-growing environment pollution. However, its practical implementation is hindered by low conversion efficiency and emissions of noxious by-products. Herein, an advanced low-oxygen-pressure calcination process is developed to fine-tune the oxygen vacancy concentration of MOF-derived TiO2 nanocrystals. Vo-poor and Vo-rich TiO2 catalysts were placed in the back of an NTP reactor to convert harmful ozone molecules into ROS that decompose VOCs via heterogeneous catalytic ozonation processes. The results indicate that Vo-TiO2-5/NTP with the highest Vo concentration exhibited superior catalytic activity in the degradation of toluene compared to NTP-only and TiO2/NTP, achieving a maximum 96% elimination efficiency and 76% COx selectivity at an SIE of 540 J L−1. Mechanistic analysis reveals that the 1O2, ˙O2− and ˙OH species derived from the activation of O3 molecules on Vo sites contribute to the decomposition of toluene over the Vo-rich TiO2 surface. With the aid of advanced characterization and density functional theory calculations, the roles of oxygen vacancies in manipulating the synergistic capability of post-NTP systems were explored, and were attributed to increased O3 adsorption ability and enhanced charge transfer dynamics. This work presents novel insights into the design of high-efficiency NTP catalysts structured with active Vo sites.
研究领域:
环境科学
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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