Water
·
2022
·Vol. 14
·期 16
·2569
·
IF 3.53
Weifan Gao,Guichang Zhang,Xiaoping Zhang,Shaoqi Zhou,Zihao Wang
The catalytic capability of original carbon nitride (CN) is limited by a small specific surface area and high electron–hole recombination rate. In this study, WO3-loaded porous carbon nanosheets (MCA-CN/WO3) were synthesized by thermal treatment with melamine, cyanuric acid and WCl6. The MCA-CN/WO3could degrade 98% of the methylene blue (MB) within 30 min in the photo-Fenton-like process, displaying better catalytic activity than the original CN (30%), pure MCA-CN (63%) and original CN/WO3(87%). The results of photoluminescence and electrochemical impedance spectroscopy demonstrated that the Z-scheme heterojunction of MCA-CN/WO3inhibited the recombination of electrons and holes. In addition, the porous nanosheet structure accelerated the electron transfer and provided abundant active sites for MB degradation. A radical quenching experiment indicated that the Z-scheme heterojunction facilitated the decomposition of H2O2to produce1O2for MB degradation. The possible degradation pathways of MB were proposed.Keywords:photo-Fenton-like process;WO3-loaded porous carbon nitride nanosheet;Z-scheme heterojunction;MB degradation
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Tong Liu,Yang Liu,Peng Zhou,Zhaokun Xiong,Heng Zhang,Chuanshu He,Ye Du,Gang Yao,Bo Lai
As one of the most promising advanced oxidation processes , the activation of S(IV) by iron-based materials to produce SO 4 •− has become a hot technology for the degradation of organic pollutants . However, the mechanism of radical chain reactions has not been clearly explored. Herein, we established a novel AOP system based on the combination of zero-valent iron (ZVI) and potassium pyrosulfite (PPS). Combined with the degradation trends of CBZ and the change of DO concentration, the system was proposed to be divided into a slow initiation stage in 5 min and a rapid degradation stage in 5 − 10 min. Through a series of quenching experiments, electron paramagnetic resonance tests and several probe experiments, the mechanisms of two radical chain reactions were proposed between ZVI and PPS: the first one produced O 2 •− and HO • , and the other produced SO 3 •− , SO 5 •− , SO 4 •− and HO • . The two-stage reaction and two radical production paths of the ZVI/PPS system were proposed for the first time, which provided theoretical guidance for the practical application of the ZVI/PPS system. The ZVI/PPS system has been found to have excellent environmental adaptability in the treatment of industrial wastewater .
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2022
·Vol. 119
·期 30
·e2202682119
·
IF 12.779
Mingjie Huang,Yu-Sheng Li,Chuan-Qi Zhang,Chao Cui,Qing-Qing Huang,Mengkai Li,Zhimin Qiang,Tao Zhou,Xiaohui Wu,Han-Qing Yu
Heterogeneous peroxymonosulfate (PMS)–based advanced oxidation processes (AOPs) have shown a great potential for pollutant degradation, but their feasibility for large-scale water treatment application has not been demonstrated. Herein, we develop a facile coprecipitation method for the scalable production (∼10 kg) of the Cu-Fe-Mn spinel oxide (CuFeMnO). Such a catalyst has rich oxygen vacancies and symmetry-breaking sites, which endorse it with a superior PMS-catalytic capacity. We find that the working reactive species and their contributions are highly dependent on the properties of target organic pollutants. For the organics with electron-donating group (e.g., -OH), high-valent metal species are mainly responsible for the pollutant degradation, whereas for the organics with electron-withdrawing group (e.g., -COOH and -NO2), hydroxyl radical (•OH) as the secondary oxidant also plays an important role. We demonstrate that the CuFeMnO–PMS system is able to achieve efficient and stable removal of the pollutants in the secondary effluent from a municipal wastewater plant at both bench and pilot scales. Moreover, we explore the application prospect of this PMS-based AOP process for large-scale wastewater treatment. This work describes an opportunity to scalably prepare robust spinel oxide catalysts for water purification and is beneficial to the practical applications of the heterogeneous PMS-AOPs.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Yingqing Guo,Zhenyu Jin,Xiaolu Li,Feng Wang,Yuanyuan Yan,Leiyu Feng
Water pollution caused by antibiotic abuse has become an urgent environmental problem. In this study, nitrogen-doped carbon materials which were prepared with reindeer manure via a thermal annealing method (shortened as DF X , X representing the thermal temperature) were applied to the removal of tetracycline hydrochloride (TH) in wastewater. According to the results, the DF700 material had the best adsorption ability, and could catalyze the degradation of TH by potassium persulfate (PS). At the initial concentration of 35 mg/L, about 69.8% of TH could be removed within two hours after the catalytic oxidation . The material characterization showed that DF700, which was doped with 2.4% nitrogen atoms , had a large specific surface area and mesoporous structures, resulting in excellent adsorption and catalytic properties. Furthermore, the degradation reaction by PS over the nitrogen-doped carbon materials was confirmed a nonradical oxidation process.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Pei Chen,Ningning Dong,Junjie Zhang,Wei Wang,Fatang Tan,Xinyun Wang,Xueliang Qiao,Po Keung Wong
In this study, zinc peroxide (ZnO 2 ) with broad energy gap was firstly used for visible-light-induced photocatalytic degradation of tetracycline (TC) and inactivation of Escherichia coli ( E. coli ). A small amount of ZnO 2 (10 mg) could efficiently degrade 100 mL of 50 mg/L TC in a wide pH range (4–12), and the degradation performance was rarely suppressed by common matrix species and natural water sources. Also, 100 mg/L ZnO 2 could inactivate around 7-log E. coli cells within 60 min under visible-light irradiation. Quenching experiments and electron paramagnetic resonance (EPR) results confirmed that superoxide radical (•O 2 − ) and singlet oxygen ( 1 O 2 ) were the main reactive oxygen species (ROS), which were attributed to the self-sensitization of TC and the photoexcitation of released H 2 O 2 under the catalysis of Zn(OH) 2 from the hydrolysis of partial ZnO 2 , respectively. The pathways of TC degradation and processes of visible-light-induced TC degradation and E. coli inactivation were proposed and deduced in detail. This work presented the enhanced visible-light photocatalytic activities of ZnO 2 for antibiotic degradation and bacterial inactivation, and provided a deep insight into the mechanisms of visible-light-induced TC degradation and E. coli inactivation over ZnO 2 .
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 48
·72764-72776
·
IF 5.19
Zhong Dan,Feng Weinan,Ma Wencheng,Liu Xinyue,Ma Jun,Zhou Ziyi,Du Xuan,He Fu
Goethite and lepidocrocite, as the main compositions of pipe deposits in the water distribution network, could be used as a catalyst for advanced oxidation processes (AOPs). This research utilizes them to activate PDS/H 2 O 2 and PMS/H 2 O 2 degrading the 2,4,6-trichlorophenol, respectively. To describe the incomplete degradation of pollutants and reflect the induction period, a modified first-order model has been proposed and used to analyze degradation differences under several key affecting factors. The results revealed that the PDS/H 2 O 2 system has a synergy effect in the 2,4,6-trichlorophenol degradation process. The possible degradation pathways and intermediate products were confirmed by gas chromatograph-mass spectrometry (GC–MS). The paper provides a new idea for the effective use of pipe deposits to remove chlorophenols from drinking water, which is of great significance to ensure water quality safety.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Jingdong Yang,Yu Li,Zequn Yang,Kaimin Shih,Guang-Guo Ying,Yong Feng
The presence of 1,4-dioxane in various water streams poses a threat to the health of human beings. In this study, the oxidative combination of ozone with peroxymonosulfate (PMS) was for the first time used to remove 1,4-dioxane from water. Near complete abatement of 1,4-dioxane was achieved by ozone-PMS after reaction of only 15 min and the degradation kinetics was found to be positively correlated with doses of PMS and ozone. Ozone-PMS oxidation had the optimum performance at slight base pH values. Both sulfate radicals and hydroxyl radicals were generated in ozone-PMS oxidation and these radicals resulted in the degradation of 1,4-dioxane. The effects of common water constituents and real water matrices were investigated. It was found that bicarbonate ions with a concentration up to 10 mM had a slight promoting effect, while either chloride ions or natural organic matter inhibited only slightly the degradation. Meanwhile, no obvious difference in the degradation of 1,4-dioxane was found among the real water matrices and deionized water , which demonstrates that ozone-PMS oxidation has high tolerance and stability. The results from this study demonstrate that ozone-PMS may be a promising technology for the removal of 1,4-dioxane from various water matrices.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
·
IF 11.357
Jiahuan Li,Shaojie Ren,Xiao Qiu,Shan Zhao,Rui Wang,Yunkun Wang
To combat the spread of antibiotic resistance into the environment, we should adequately manage wastewater effluent treatment to achieve simultaneous removal of antibiotics, antibiotic resistant bacteria (ARB), and antibiotic resistance genes (ARGs). Herein, we fabricate a multifunctional electroactive poly(vinylidene fluoride) ultrafiltration membrane (C/PVDF) by phase inversion on conductive carbon cloth. The membrane possesses not only excellent retention toward ARB and ARGs but also exhibits high oxidation capacity as an electrode. Notably, sulfamethoxazole degradation involving hydroxylation and hydrolysis by the anode membrane is predominant, and the degradation efficiency is up to 81.5% at +4 V. Both electro-filtration processes exhibit significant ARB inactivation, anode filtration is superior to cathode filtration. Moreover, the degradation of intracellular ARGs (iARGs) located in the genome is more efficient than those located in the plasmid, and these degradation efficiencies at −2 V are higher than +2 V. The degradation efficiencies of extracellular ARGs (eARGs) are opposite and are lower than iARGs. Compared with regular filtration, the normalized flux of electroactive ultrafiltration membrane is improved by 18.0% at −2 V, 15.9% at +2 V, and 30.4% at +4 V during treating wastewater effluent, confirming its antifouling properties and feasibility for practical application.
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APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Yan Ding,Kangping Cui,Xueyan Liu,Chen-Xuan Li,Zhi Guo,Minshu Cui,Yihan Chen
Herein, a new axial g-C 3 N 4 coordinated iron(III) phthalocyanine (FeP/CN) was fabricated for peroxymonosulfate (PMS) activation. Around 100% degradation of acetaminophen (AP), 2,4-dichlorophenol (2,4-DP), sulfadiazine (SDZ), and methyl orange (MO) (30 mg L -1 ) were achieved within 20 min by adding 0.02 g L -1 FeP/CN 5 (3.62 wt% Fe) and 0.2 mM PMS. High-valent iron-oxo species (Fe IV =O) was demonstrated as the main reactive species, which mediated a two-electron transfer process with pollutants. Characterizations and computational analysis revealed that the axial g-C 3 N 4 ligand provided Fe(III) coordination environments to generate Fe IV =O species directly through PMS activation, and increased the reactivity of the Fe IV =O species in pollutants oxidation due to the narrowed HOMO-LUMO gap. Besides, small displacement of Fe atom (0.23 Å) from the macrocycles plane due to the axial g-C 3 N 4 ligand decreased the iron demetalization rate from 3.54% to 0.28% in the catalyst/PMS system. This work offered an excellent strategy to design high-efficiency catalysts for Fe IV =O generation.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yanan Shang,Xinning Liu,Yanwei Li,Yue Gao,Baoyu Gao,Xing Xu,Qinyan Yue
The synthesis of a highly efficient and stable single atom catalyst (SAC) for peroxydisulfate (PDS) activation remains a challenge. Herein, a reconstructed iron single atom catalyst (Fe-SAC) with both abundant conjugated π-π sp 2 structured carbon and reactive Fe-N 4 sites was first reported to improve the decomposition of organics in PDS/SACs systems. Enhanced organics adsorption can be achieved by the conjugated π-π sp 2 structured carbon via π-π interaction to decrease the migration distance of reactive species to organic molecules. In addition, PDS tended to be attached onto the Fe-N 4 sites accompanied by the peroxymonosulfate (PMS) generation via S-O breakage of PDS, accelerating the generation of radicals. As a result, organics decomposition via PDS activation by reconstructed Fe-SAC was significantly higher (∼6 times) than the conventional Fe-SAC because of the synergistic effect of the resulting dual reaction sites. This work provides a new strategy to enhance the catalytic performances in PDS/SACs systems.
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CHINESE JOURNAL OF CATALYSIS
·
2022
·
IF 12.92
Yu-Lan Wu,Ming-Yu Qi,Chang-Long Tan,Zi-Rong Tang,Yi-Jun Xu
ABSTRACT Simultaneously utilizing photogenerated electrons and holes to convert renewable biomass and its derivatives into corresponding value-added products and hydrogen (H 2 ) is a promising strategy to deal with the energy and environmental crisis. Herein, we report a facile hydrothermal method to construct a direct Z-scheme CdS/WO 3 binary composite for photocatalytic coupling redox reaction, simultaneously producing H 2 and selectively converting aromatic alcohols into aromatic aldehydes in one pot. Compared with bare CdS and WO 3 , the CdS/WO 3 binary composite exhibits significantly enhanced performance for this photocatalytic coupled redox reaction, which is ascribed to the extended light harvesting range, efficient charge carrier separation rate and optimized redox capability of CdS/WO 3 composite. Furthermore, the feasibility of converting various aromatic alcohols to corresponding aldehydes coupled with H 2 evolution on the CdS/WO 3 photocatalyst is proved and a reasonable reaction mechanism is proposed. It is hoped that this work can provide a new insight into the construction of direct Z-scheme photocatalysts to effectively utilize the photogenerated electrons and holes for photocatalytic coupled redox reaction.
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Water
·
2022
·Vol. 14
·期 18
·2811
·
IF 3.53
Zhixiong Liu,Wenlei Qin,Lei Sun,Huiyu Dong,Xiangjuan Yuan,Fei Pan,Dongsheng Xia
The degradation of acyclovir (ACY) and atenolol (ATL) in the UV/peroxydisulfate (UV/PDS) process has been systematically considered, focusing on the degradation kinetics, theoretical models, and reaction pathways via applying a microfluidic UV reaction system. The removal efficiencies of ACY and ATL were >94.8%, and the apparent degradation rate constants (kobs) were 0.0931 and 0.1938 min−1at pH 6.0 in the UV/PDS system. The sulfate radical (SO4•−) and hydroxyl radical (•OH) were identified as the major reactive radicals. The pH-dependent reaction rate constants of ACY and ATL with•OH and SO4•−were measured via the competing kinetics. Meanwhile, the contributions of•OH and SO4•−for ACY and ATL degradation were calculated by the radical steady-state hypothesis, and the results revealed that SO4•−occupied a decisive position (>84.5%) for the elimination of ACY and ATL. The contribution of•OH became more significant with the increasing pH, while SO4•−was still dominant. Moreover, ACY and ATL degradation performance were systematically evaluated via the experiments and Kintecus model under different operational parameters (Cl−, Br−, HCO3−, NOM, etc.) in the UV/PDS process. Furthermore, the plausible reaction pathways of ACY and ATL were elucidated based on the Fukui function theory and ultra-performance liquid chromatography-tandem quadrupole time-of-flight mass spectrometry (UPLC-QTOF-MS) analysis. The UV/PDS process has been demonstrated to be an efficient and potential application for micropollutants mitigation.Keywords:UV/PDS;micropollutants;radical contribution rates;kinetic models;degradation pathways
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