ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2023
·Vol. 30
·期 24
·66303-66313
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IF 5.8
Xu Zhimin,Ju Shaohua,Gao Peng,Lin Junjian,Niu Yifan,Meng Fei,Li Shunling,Li Fangfang,Du Jiahao,Xu Li,Peng Hongbo,Pan Bo
In this study, ferrous composites (Fe x O 4 ) were prepared by microreactor to activate peroxydisulfate (PDS) for the degradation of bisphenol A (BPA) with visible (Vis) light irradiation. X-ray diffraction (XRD), energy-dispersive spectrometry (EDS), X-ray photoelectron spectroscopy (XPS), and scanning electron microscope (SEM) were used to characterize the morphology and crystal phase of Fe X O 4 . Photoluminescence (PL) spectroscopy combined with amperometric tests were used to determine the role of PDS on the performance of photocatalytic reaction. The main reactive species and intermediates for BPA removal were determined by electron paramagnetic resonance (EPR) measurement and quenching experiments. The result indicated that singlet state oxygen ( 1 O 2 ) contributed more to the BPA degradation than that of other reactive radicals (·OH, SO 4 ·− and ·O 2 − ); these reactive radicals and 1 O 2 formed by the reaction between photo-generated electrons (e − ) and holes (h + ) of Fe x O 4 and PDS. During this process, the consumption of e − and h + also improved their separation efficiency and thus enhanced the degradation of BPA. In addition, the photocatalytic activity of Fe x O 4 in Vis/Fe x O 4 /PDS system was 3.2-fold and 6.6-fold higher than that of single Fe x O 4 and PDS under Vis light, respectively. The Fe 2+ /Fe 3+ cycle could effectively drive the photocatalytic activation of PDS through indirect electron transfer and the formation of reactive radicals. This work illustrated that the degradation of BPA was rapidly in Vis/Fe x O 4 /PDS system mainly through 1 O 2 , which further improve our understanding on the efficient removal of organic contaminants in the environment.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Mukhtiar Ali,Xin Song,Qing Wang,Zhuanxia Zhang,Meng Zhang,Xing Chen,Zhiwen Tang,Xin Liu
In this study, a set of comprehensive experiments were conducted to explore the effects of temperature on the biodegradation, bioavailability , and generation of reactive oxygen species (ROS) by thermally enhanced biodegradation (TEB) under benzene and BaP co-contaminated conditions. The biodegradation rates of benzene increased from 57.4% to 88.7% and 84.9%, and the biodegradation efficiency of BaP was enhanced from 15.8% to 34.6% and 28.6%, when the temperature was raised from the ambient temperature of 15 °C to 45 °C and 30 °C, respectively. In addition, the bioavailability analysis results demonstrated that the water- and butanol-extractable BaP increased with elevated temperatures. High enzymatic activities and PAH-RHD α gene in gram-positive bacteria favored the long-term elevated temperatures (30 and 45 °C) compared to gram-negative bacteria. Moreover, ROS species (O 2 •− and •OH) generation was detected which were scavenged by the increased superoxide dismutase and catalase activities at elevated temperatures. Soil properties (pH, TOC , moisture, total iron, Fe 3+ , and Fe 2+ ) were affected by the temperature treatments, revealing that metal-organic-associated reactions occurred during the TEB of benzene–BaP co-contamination. The results concluded that biodegradation of benzene–BaP co-contamination was greatly improved at 45 °C and that microbial activities enhanced the biodegradation under TEB via the increased bioavailability and generation and degradation of ROS.
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Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Yiqing Liu,Shixiang Wang,Zhenran Wang,Yongsheng Fu,Runyu Zhou
A novel FeCu anchored coal gangue (FeCu-CG) composite was prepared by a two-step (acidation and subsequent chemical reduction) method and applied in catalytic activation of peracetic acid (PAA) for sulfamethoxazole (SMX) removal in water. The BET, XPS, SEM , EDS, and XRD characterization of FeCu-CG indicated that it had a porous structure with the S BET area of 36.38 m² g −1 and nano-FeCu particles were successfully loaded in the CG carrier, which provided electrons and Fe(II) for PAA decomposition through the bimetallic corrosion reaction. The hydroxyl radical (HO • ) was verified to be largely responsible for SMX elimination in FeCu-CG/PAA system. More than 96.4 % of SMX was removed by FeCu-CG/PAA in 40 min at initial pH ranging from 5.0 to 9.0. Increasing FeCu-CG dosage from 0.1 to 1.0 g L −1 could enhance SMX degradation in FeCu-CG/PAA system, but higher dosage inhibited SMX removal owing to the aggregation of FeCu-CG particles. Coexisting dissolved organic matter (DOM), HCO 3 - and Cl - suppressed SMX degradation. The degradation pathways of SMX by FeCu-CG/PAA were proffered including hydroxylation, amino oxidation , bond cleavage and coupling reaction based on five detected degradation products .
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Jian Ke,Hailun Zhao,Shangkun Zhu,Zixuan Zheng,Qiulian Yang,Yanhua Liu,Ruixin Guo,Jianqiu Chen
The safe disposal of excess sludge generated from chemical wastewater treatment processes has attracted worldwide concern because of its high yield and toxicity. In our work, purified terephthalic acid excess sludge-derived biochar (PTABC) was prepared via one-step pyrolysis without additives. The prepared catalyst was demonstrated to degrade sulfamethoxazole (SMX) via the activation of peroxymonosulfate (PMS). The inhibitory effects of anions were negligible. The reactive oxygen species were investigated based on the radical scavenging experiments and electron paramagnetic resonance technique. Additionally, the electron transfer process was investigated via electrochemical measurements. The results show that the non-radical pathways take a leading role in the degradation of SMX and the corresponding contributions of sulfate radical (SO 4 •– ), hydroxyl radical (•OH) and non-radical pathways in PTABC-700/PMS system for SMX degradation were 12.59%, 3.28%, and 84.13%, respectively. Active sites of PTABC-700 responsible for SMX degradation were also proposed. Overall, this study provides a promising strategy for converting excess sludge into functional catalysts and achieving treatment of SMX-contaminated wastewater.
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ENVIRONMENTAL RESEARCH
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2023
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IF 8.3
Jinbin Lai,Ting Tang,Xiaodong Du,Rui Wang,Jiahao Liang,Dehao Song,Zhi Dang,Guining Lu
As emerging pollutants continue to be discovered, studies on the degradation behavior of emerging pollutants have proliferated, but few studies have focused on the reactivity of the new pollutants themselves. The work investigated the oxidation of a representative roadway runoff-derived organic contaminant , 1,3-diphenylguanidine (DPG) by goethite activated persulfate (PS). DPG exhibited the highest degradation rate ( k d = 0.42 h −1 ) with present of PS and goethite at pH 5.0, then started to decrease with increasing pH. Chloride ion inhibited DPG degradation by scavenging HO·. Both HO· and SO 4 − · were generated in goethite activated PS system. Competitive kinetic experiments and flash photolysis experiments were conducted to investigate free radical reaction rate. The second-order reaction rate constants for DPG reacting with HO· and SO 4 − · were quantified ( k DPG + HO·, k DPG + SO4 - · ), which both reached above 10 9 M −1 s −1 . Chemical structures of five products were identified, four of them were previously detected in DPG photodegradation , bromination and chlorination processes. By density functional theory (DFT) calculations, ortho- and para- C were more easily attacked by both HO· and SO 4 − ·. ion of H on N by HO· and SO 4 − · were the favorable pathways, and the product TP-210 might be generated by cyclization of DPG radical from abstraction of H on N (3). The results of this study help us to better understand the reactivity of DPG with SO 4 − · and HO·.
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RESEARCH ON CHEMICAL INTERMEDIATES
·
2023
·Vol. 49
·期 7
·2793-2806
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IF 3.3
Zhang Xinxi,Cao Min,Liu Da,Lei Juying,Zhang Jinlong,Liu Yongdi,Zhou Liang
Advanced oxidation processes based on peroxymonosulfate (PMS) activation are widely used for the removal of antibiotic contaminants. However, the commonly used transition metal catalysts suffer from secondary contamination due to ions leaching during the activation of PMS. Herein, the oxygen and nitrogen co-doped carbon material (Nv-NC-2) with abundant mesopores was obtained by simple high-temperature calcination using covalent organic frameworks (COFs) as precursors and NH 4 Cl as an activator. The Nv-NC-2/PMS system exhibited excellent levofloxacin removal efficiency under a wide pH and complex water environment with anions interference. The C=O in Nv-NC-2 was identified as the main active sites through degradation experiments and XPS. Furthermore, the electron paramagnetic resonance, quenching experiments and probe capture experiments demonstrated 1 O 2 and \({\text{O}}_{2}^{ - }\) were dominant active species. This study enhances the catalytic activity of COFs-derived carbon materials through a simple activation technique, which provides a novel method for surface modification of carbon materials.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Jinxin Li,Dan Zhong,Feiyu Li,Kefei Li,Wencheng Ma,Jun Ma,Jingna Zhang,Aoshuang Sun
A bifunctional electro-Fenton (EF) cathode with Fe 3 O 4 -LaFeO 3 /C embedded graphite felt (GF) was synthesized through a hydrothermal process, which was used for in situ electrochemical formation of active oxygen species (ROS) for coal pyrolysis wastewater (CPW) removal. Experimental results illustrated that the mineralization efficiency of dimethylphenol (DMP) was achieved at 90.7 % within 150 min reaction. On the basis of quenching test and free radical detection, the ∙OH and ∙O 2 − were the detectable ROS in the hetero-EF system for DMP removal. Meanwhile, the formed oxygen vacancies (OVs) and the redox of Fe 2+ /Fe 3+ promoted the oxygen adsorption and H 2 O 2 activation. Density functional theory (DFT) calculations further discussed that the Fe 3 O 4 -LaFeO 3 interface possessed more downward spin density of states in the conduction band, resulting in a higher total density of states (DOS) value near the Fermi level. Moreover, the Fe 3 O 4 -LaFeO 3 /C/GF cathode displayed good recyclability with low metal ion dissolution for 5 times (99.5 % DMP removal and 78.6 % TOC removal) and underlying actual CPW application potential (80.2 % of COD removal and 100 % of total phenol (Tph) removal). Overall, this work invented a novel and stable bifunctional cathode for the efficient removal of refractory CPW in the hetero-EF system.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Yishuai Pan,Xiaoshan Zheng,Guoqiang Zhao,Zepeng Rao,Wanchao Yu,Baoliang Chen,Chiheng Chu
The hydroxyl radical (•OH) is a potent oxidant and key reactive species in mediating element cycles and pollutant dynamics in the natural environment. The natural source of •OH is historically linked to photochemical processes (e.g., photoactivation of natural organic matter or iron minerals) or redox chemical processes (e.g., reaction of microbe-excreted or reduced iron/natural organic matter/sulfide-released electrons with O2 in soils and sediments). This study revealed a ubiquitous source of •OH production via water vapor condensation on iron mineral surfaces. Distinct •OH productions (15–478 nM via water vapor condensation) were observed on all investigated iron minerals of abundant natural occurrence (i.e., goethite, hematite, and magnetite). The spontaneous •OH productions were triggered by contact electrification and Fenton-like activation of hydrogen peroxide (H2O2) at the water–iron mineral interface. Those •OH drove efficient transformation of organic pollutants associated on iron mineral surfaces. After 240 cycles of water vapor condensation and evaporation, bisphenol A and carbamazepine degraded by 25%–100% and 16%–51%, respectively, forming •OH-mediated arene/alkene hydroxylation products. Our findings largely broaden the natural source of •OH. Given the ubiquitous existence of iron minerals on Earth’s surface, those newly discovered •OH could play a role in the transformation of pollutants and organic carbon associated with iron mineral surfaces.
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CHEMOSPHERE
·
2023
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IF 8.8
Youyou Hu,Jialin Guo,Wei Wang,Yanqing He,Zhengkui Li
Metal-nitrogen-site catalysts are widely recognized as effective heterogeneous catalysts in peroxymonosulfate (PMS)-based advanced oxidation processes . However, the selective oxidation mechanism for organic pollutants is still contradictory. In this work, manganese-nitrogen active centers and tunable nitrogen vacancies were synchronously constructed on graphitic carbon nitride (LMCN) through l -cysteine-assisted thermal polymerization to reveal different antibiotic degradation mechanisms. Benefiting from the synergism of manganese-nitrogen bond and nitrogen vacancies, the LMCN catalyst exhibited excellent catalytic activity for the degradation of tetracycline (TC) and sulfamethoxazole (SMX) antibiotics with first-order kinetic rate constants of 0.136 min −1 and 0.047 min −1 , which were higher than those of other catalysts. Electron transfer dominated TC degradation at low redox potentials , while electron transfer and high-valent manganese (Mn (V)) were responsible for SMX degradation at high redox potentials. Further experimental studies unveiled that the pivotal role of nitrogen vacancies is to promote electron transfer pathway and Mn(V) generation, while nitrogen-coordinated manganese as the primary catalytic active site determines Mn(V) generation. In addition, the antibiotic degradation pathways were proposed and the toxicity of byproducts was analyzed. This work provides an inspiring idea for the controlled generation of reactive oxygen species by targeted activation of PMS.
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International Journal of Nanomedicine
·
2023
·
IF 8
Peiru Si,Jiaxing Lei,Chen Yang,Peipei Zhang,Xiaojiao Li,Shaohua Zheng,Qingqing Li,Jiye Zhang
Introduction Hepatic ischemia-reperfusion injury (HIRI) is the main reason for liver dysfunction or failure after liver resection and liver transplantation. As excess accumulation of reactive oxygen species (ROS) is the leading factor, ceria nanoparticle, a cyclic reversible antioxidant, is an excellent candidate for HIRI.Methods Manganese doped mesoporous hollow ceria nanoparticles (MnOx-CeO2 NPs) were prepared, and the physicochemical characteristics, such as particle size, morphology, microstructure, etc. were elucidated. The in vivo safety and liver targeting effect were examined after i.v. injection. The anti-HIRI was determined by a mouse HIRI model.Results MnOx-CeO2 NPs with 0.40% Mn doped exhibited the strongest ROS-scavenging capability, which may due to the increased specific surface area and surface oxygen concentration. The nanoparticles accumulated in the liver after i.v. injection and exhibited good biocompatibility. In the HIRI mice model, MnOx-CeO2 NPs significantly reduced the serum ALT and AST level, decreased the MDA level and increased the SOD level in the liver, prevent pathological damages in the liver.Conclusion MnOx-CeO2 NPs were successfully prepared and it could significantly inhibit the HIRI after i.v. injection.
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ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Jiajun Liu,Xionghao Zhang,Junda Li,Yi Feng,Li Feng,Shuai Han,Tingyu Pan,Taiheng Zhang,Shenyu Wu,Zijie Ke,Bingzhi Liu,Huaili Zheng
In this study, an advanced oxidation process with E/Ce(IV) synergistic PMS (E/Ce(IV)/PMS) was established for the efficient removal of Reactive Blue 19 (RB19). The catalytic oxidation performance of different coupling systems was examined and the synergistic effect of E/Ce(IV) with PMS in the system was substantiated. The oxidative removal of RB19 in E/Ce(IV)/PMS was excellent, achieving a removal efficiency of 94.47% and a reasonable power consumption (EE/O value was 3.27 kWh·m −3 ). The effect of pH, current density, Ce(IV) concentration, PMS concentration, initial RB19 concentration and water matrix on the removal efficiency of RB19 were explored. Additionally, quenching and EPR experiments showed that the solution contains different radicals such as SO 4 ·− , HO∙ and 1 O 2 , where 1 O 2 and SO 4 ·− played key roles, but HO∙ just acted a weaker role. Ce ion trapping experiment confirmed that Ce(IV) was involved in the reaction process and played a major role (29.91%). RB19 was subject to three possible degradation pathways, and the intermediate products displayed well biochemical properties. To conclude, the degradation mechanism of RB19 was explored and discussed. In the presence of current, E/Ce(IV)/PMS performed a rapid Ce(IV)/Ce(III) cycle, continuously generating strong catalytic oxidation Ce(IV), The reactive radicals derived from the decomposition of PMS, in conjunction with Ce(IV) and direct electro-oxidation, efficiently destroyed the molecular structure of RB19 and showed an efficient removal rate.
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Journal of Cleaner Production
·
2023
·
IF 11.1
Zheng Fang,Zifeng Lin,Ping Chen,Mengying Feng,Haijin Liu,Zhenjun Xiao,Zili Lin,Dagaung Li,Dezhu Liu,Yudan Zhang,Wenying Lv,Guoguang Liu
Advanced oxidation processes (AOPs) are highly efficient for the removal of antibiotics from water. The activation of hydrogen peroxide (H 2 O 2 ) by ultraviolet (UV) has garnered increasing attention. This study describes the enhanced photochemical degradation of emerging contaminants in water using a UV-activated calcium peroxide (UV/CaO 2 ) system, wherein CaO 2 can gently produce H 2 O 2 when exposed to UV light . The UV/CaO 2 system can expeditiously and efficiently eradicate ciprofloxacin (CIP), in which hydroxyl radicals (•OH) and superoxide anions (O 2 •- ) played critical roles. The superlative rate constant was 0.024 min −1 at an optimal dosage of 0.1 g L −1 , which was a 16-fold increase over the rate of pure UV photolysis. The UV/CaO 2 system had an excellent defluorination capacity (80% within 60 min). Further, this technology was intensely evaluated over a wide range of pH for the removal of CIP, including H 2 O 2 yields, defluorination rates, as well as correlations with the reactive species generated during the reactions for numerical analysis. The UV/CaO 2 system had an excellent anti-interference capacity over a wide pH range. Three major degradation pathways were proposed for the degradation of CIP, together with predictions of the physiological toxicity of these transformation intermediates. This study provides strong technical support for the promotion of this UV/CaO 2 water treatment platform, as well as the decontamination and defluorination of water matrixes contaminated with fluoroquinolones.
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