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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2019 ·Vol. 26 ·期 36 ·36410-36422 · IF 2.914

Catalytic degradation of organic pollutants in Fe(III)/peroxymonosulfate (PMS) system: performance, influencing factors, and pathway

Latif Abdul,Kai Sun,Si Youbin

This study demonstrated, for the first time, Fe(III)/peroximonosulphate (PMS) could be an efficient advanced oxidation process (AOP) for wastewater treatment. Bisphenol A (BPA) was chosen as a model pollutant in the present study. Fe(III)-activated PMS system proved very effective to eliminate 92.18% of BPA (20 mg/L) for 30-min reaction time at 0.50 mM PMS, 1.5 g/L Fe(III), pH 7.0. The maximum degradation of BPA occurred at neutral pH, while it was suppressed at both strongly acidic and alkaline conditions. Organic and inorganic ions can interfere with system efficiency either positively or negatively, so their interaction was thoroughly investigated. Furthermore, the presence of organic acids also affected BPA degradation rate, especially the addition of 10 mM citric acid decreased the degradation rate from 92.18 to 66.08%. Radical scavenging experiments showed that SO 4 •– was the dominant reactive species in Fe(III)/PMS system. A total of 5 BPA intermediates were found by using LC/MS. A possible degradation pathway was proposed which underwent through bridge cleavage and hydroxylation processes. Acute toxicity of the BPA degradation products was assessed using Escherichia coli growth inhibition test . These findings proved to be promising and economical to deal with wastewater using iron mineral for the elimination of organic pollutants. Graphical abstract

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JOURNAL OF HAZARDOUS MATERIALS · 2019 · IF 7.65

A stable and easily prepared copper oxide catalyst for degradation of organic pollutants by peroxymonosulfate activation

Songxue Wang,Shanshan Gao,Jiayu Tian,Qiao Wang,Tianyu Wang,Xiujuan Hao,Fuyi Cui

A direct one-step calcination preparation of CuO catalyst (CuO-3) using polyethylene glycol (PEG) as nonionic polymeric structure directing agent was developed for activation of peroxymonosulfate (PMS). The morphological and physicochemical properties of the CuO-3 were characterized and the catalytic activity for degradation of organic pollutants was evaluated. The resultant CuO-3 with significantly enhanced surface area exhibited excellent catalytic performance of phenolic organic pollutants degradation. The reaction mechanism of the PMS/CuO system was systematically investigated with a series of radical quenching tests and the analysis of electron paramagnetic resonance (EPR) spectroscopy. Quite different from traditional hydroxyl radicals ( OH) and sulfate radical (SO 4 − ) based advanced oxidation processes, singlet oxygen ( 1 O 2 ) was identified as the dominate reactive species responsible for the degradation of organic pollutants. Moreover, the main formation pathway of 1 O 2 was also investigated. The results indicated that the superoxide radical (O 2 − ) was involved in the generation of 1 O 2 as a crucial precursor. Also, the PMS/CuO-3 system exhibited satisfactory stability and reusability under neutral conditions as well as high removal of organic pollutants in the presence of inorganic anions. This work not only provides a novel and stable preparation method for CuO catalyst, but also gives a deeper insight into the mechanisms of PMS activation by CuO.

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ENGINEERING IN LIFE SCIENCES · 2019 ·Vol. 19 ·期 11 ·815-824 · IF 1.936

Immobilization of laccase onto modified PU/RC nanofiber via atom transfer radical polymerization method and application in removal of bisphenol A

Xin Li,Dawei Li,Pengfei Lv,Jinyan Hu,Quan Feng,Qufu Wei

In this study, 2-hydroxyethyl methacrylate (HEMA) was used as the monomers for surface grafting on electrospun PU/RC nanofiber membrane via atom transfer radical polymerization (ATRP) method, and the PU/RC-poly(HEMA) nanofiber membrane was investigated as a carrier for LAC. Free and immobilized LAC was characterized, and efficiency of bisphenol A (BPA) removal was determined. The results indicated that the PU/RC-poly(HEMA)-LAC showed relatively higher pH stability, temperature stability, and storage stability than free and PU/RC-LAC; moreover, more than 60% of the PU/RC-poly(HEMA)-LAC activity was retained after 10 cycles of ABTS treatment. Notably, the BPA removal efficiency of PU/RC-poly(HEMA)-LAC membrane generally ranged from 87.3 to 75.4% for the five cycles. Therefore, the PU/RC-poly(HEMA) nanofiber membrane has great potential as a carrier for the LAC immobilization for various industrial applications and bioremediation.

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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Recycling of nitrogen-containing waste diapers for catalytic contaminant oxidation: Occurrence of radical and non-radical pathways

Yue Yang,Mengyuan Wang,Penghui Shi,Junfeng Wu,Yulin Min,Qunjie Xu,Yifei Guo

The transformation of waste biomass into nitrogen-doped carbon-based functional materials is recognized as an economical route for energy production and conversion. Waste diapers contain urea that could be used as a nitrogen source, were considered renewable biomass. BPA, a widely used environmental endocrine disruptor, produces estrogen effects in the human body and is characterized by low concentrations and high toxicity in the environment. Here, a simple method of obtaining cobalt embedded waste diaper carbon (Co-WDC) using abandoned diapers is reported and used for an advanced oxidation process. Co-WDC completely removed 20 mg L −1 BPA from a solution within 6 min with a degradation rate constant of 0.68 min −1 . The LC–MS test revealed that BPA is decomposed into small molecules, and TOC was greatly reduced. Electron paramagnetic resonance and quenching experiments demonstrated the Co-WDC degradation system acted through two pathways, radical and non-radical pathway where 1 O 2 was the dominant species. Material characterization and discussion of the mechanism revealed that the introduction of Co mainly formed a metal-nitrogen structure that induced peroxymonosulfate to produce 1 O 2 , which participated in BPA degradation in the Co-WDC system. This work should generate interest in the recycling of waste biomass for peroxymonosulfate activation and environmental modification.

CAS / MDL: 80-05-7 71-48-7 57-13-6
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MICROCHEMICAL JOURNAL · 2019 · IF 3.206

Development and application of a novel electrochemical sensor based on AuNPS and difunctional monomer-MIPs for the selective determination of Tetrabromobisphenol-S in water samples

Kwabena Agyarko Sarpong,Kun Zhang,Yu Luan,Yunfei Cao,Wanzhen Xu

Tetrabromobisphenol-S (TBBPS) is a Brominated Flame Retardants (BFRs). TBBPS in trace quantities is lethal and do not only alter the normal performance of the endocrine system but can directly or indirectly provoke hepatoxicity and carcinogenic diseases. Herein, we fabricate a facile electrochemical sensor and investigate its application towards the determination of TBBPS through imprinting technique. TBBPS imprinting was carried out in the presence of methacrylic acid (MAA) and 4-aminothiophenol (4-ATP) functional monomers (DiM) over gold nanoparticles (AuNPs) modified carbon paste electrode (CPE). Transmission electron microscopy (TEM) was used to characterize the imprinted sensor. Performance was thoroughly investigated using both cyclic voltammetry (CV) and differential pulse voltammetry (DPV). The proposed sensor showed detection behavior towards TBBPS in standard solutions with different concentrations range of 0.1 nM-10 nM and with a detection limit of 0.029 nM. The developed MIP(DiM)@AuNPs/CPE sensor had enhanced recognition capacity compared to MIP electrochemical sensors developed with a mono functional monomer (MIP(MoM)@AuNPs/CPE) and non-imprinted sensors. In addition, the low cost; easier preparation; excellent stability; and good selectivity of MIP(DiM)@AuNPs/CPE electrochemical sensor makes it an attractive alternative to high instrumentation detection techniques.

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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Simultaneous Cr(VI) reduction and bisphenol A degradation by a 3D Z-scheme Bi2S3-BiVO4 graphene aerogel under visible light

Qianwei Liang,Sittipranee Ploychompoo,Jingda Chen,Tingting Zhou,Hanjin Luo

Rational design strategy and facile synthesis method of photocatalysts with high efficiency and stability have been still a significant challenge for the removal of environmental contaminants. In this study, a three dimensional (3D) all-solid-state Z-scheme heterojunction photocatalytic system containing bismuth sulphide (Bi 2 S 3 ) and bismuth vanadate (BiVO 4 ) was constructed as Bi 2 S 3 -BiVO 4 graphene aerogel (SVGA) by a facile hydrothermal method. The potential application of as-synthesized SVGA was demonstrated to remove Cr(VI) and bisphenol A (BPA) simultaneously in aqueous media via the synergy of adsorption and photocatalysis under visible light irradiation. The removal rates of Cr(VI) and BPA both nearly reached 100% after adsorption for 40 min and photocatalysis for 120 min under visible light (λ > 420 nm), which was much better than the removal efficiency of individual Bi 2 S 3 and BiVO 4 , as well as Bi 2 S 3 graphene aerogel (SGA) and BiVO 4 graphene aerogel (VGA) samples. The rGO played an important role as photoinduced electron transfer mediator between Bi 2 S 3 and BiVO 4 , which promoted the photogenerated electrons transfer efficiency and enhanced photocatalytic ability of SVGA efficiently. The harmful Cr(VI) was conserved into hypotoxic Cr(III) and BPA was degraded into CO 2 and H 2 O after photocatalysis on SVGA, and the fabricated SVGA also presented favorable stability and satisfactory application effect in practical water samples, implied that such photocatalyst has a promising application for simultaneous removal of heavy metals and organics from aqueous environment.

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NEW JOURNAL OF CHEMISTRY · 2019 ·Vol. 44 ·期 4 ·1245-1252 · IF 3.069

A novel cobalt doped MOF-based photocatalyst with great applicability as an efficient mediator of peroxydisulfate activation for enhanced degradation of organic pollutants

Shi-Wen Lv,Jing-Min Liu,Ning Zhao,Chun-Yang Li,Zhi-Hao Wang,Shuo Wang

The issue of environmental pollution is currently more and more serious, and developing an effective method with universal applicability for removing various contaminants is pretty necessary. Herein, a novel photocatalyst denoted as Co-doped MIL-53-NH2(Fe : Co 4 : 1) was constructed via a feasible solvothermal method, which served as an efficient mediator to activate peroxydisulfate for degrading various organic pollutants. Results from the current work indicated that doping Co with an appropriate proportion could enhance the optical absorption intensity of MIL-53-NH2 and reduce the band gap. Furthermore, a Co ion acting as a mediator could facilitate the charge transfer through a Co3+/Co2+ redox pathway, and thereby suppress the recombination of photogenerated electron–hole pairs. More interestingly, the Co-doped MIL-53-NH2 exhibited excellent and extensive degradation abilities for various organic pollutants including bisphenol A (BPA), antibiotics and organic dyes in the presence of peroxydisulfate (PS) under visible light irradiation. It was also found that ˙OH and SO4−˙ were the major contributors to the catalytic process. Total organic carbon (TOC) analysis indicated that the majority of the contaminants were degraded into CO2 and H2O. Even in the real samples, the developed Co-doped MIL-53-NH2/PS/solar system still possessed excellent performance for the degradation of BPA. Possible photocatalytic mechanisms and the kinetics were also investigated. Besides, the Co-doped MIL-53-NH2 had good catalytic reusability and stability. To sum up, this study provides a promising approach for removing organic pollutants from wastewater.

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JOURNAL OF SEPARATION SCIENCE · 2019 ·Vol. 43 ·期 5 ·987-995 · IF 2.516

Highly ordered molecularly imprinted mesoporous silica for selective removal of bisphenol A from wastewater

Jinyi Wu,Lei Tan,Yuling Li,Xiaotong Wu,Yong Liang

Selective removal of bisphenol A from wastewater is quite challenging primarily because of its low concentration and matrix complexity. To this end, according to the molecular structure of bisphenol A, we designed a functional monomer for the preparation of molecularly imprinted mesoporous silica using click chemistry reaction. The resultant bisphenol A imprinted mesoporous silica was characterized by transmission electron microscopy, small angle X-ray diffraction, and N 2 adsorption–desorption experiments. The results indicated that the bisphenol A imprinted mesoporous silica possessed a highly ordered periodic hexagonal mesostructure with the Brunauer–Emmett–Teller surface area of 944.28 m 2 /g. The bisphenol A imprinted mesoporous silica showed fast adsorption kinetics and the saturated adsorption capacity reached up to 88.6 mg/g at pH 6.5, and with relative selectivity factors ranged from 1.06 to 3.20. The adsorption efficiency of the bisphenol A imprinted mesoporous silica was above 97.96% after five extraction/elution cycles. The bisphenol A imprinted mesoporous silica was further applied to the selective removal of bisphenol A from real wastewater samples and showed great promise in practical applications.

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CHEMOSPHERE · 2019 · IF 5.108

Activation of dissolved molecular oxygen by Cu(0) for bisphenol a degradation: Role of Cu(0) and formation of reactive oxygen species

Jiajun Long,Longqian Xu,Linghui Zhao,Huaqiang Chu,Yunfeng Mao,Deli Wu

In this study, Cu(0) was synthesized with NaBH 4 as a reducing agent for Cu(II) and used to activate dissolved molecular oxygen (O 2 ) under acidic conditions. The Cu(0) synthesized had much higher activity than the purchased. The roles of Cu was clarified and the formation of reactive oxygen species was discussed through direct detection for the first time. By detecting the valence change of Cu in a CuO system, Bisphenol A (BPA) was found to accelerate the transformation of Cu(II) to Cu(I). Besides, the evidence from electron spin resonance (ESR) studies and scavenging tests revealed the new roles of Cu(0) that Cu(0) could not only convert O 2 to produce ·O 2 − , but also catalyze H 2 O 2 to ·OH. The results from this study offer evidence of new reaction pathways in Cu-activated O 2 systems and deepen understanding of the reaction between Cu species and O 2 .

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APPLIED CATALYSIS B-ENVIRONMENTAL · 2019 · IF 14.229

Preforming abundant surface cobalt hydroxyl groups on low crystalline flowerlike Co3(Si2O5)2(OH)2 for enhancing catalytic degradation performances with a critical nonradical reaction

Zhong-Shuai Zhu,Xiao-Jie Yu,Jin Qu,Ya-Qiong Jing,Yasmine Abdelkrim,Zhong-Zhen Yu

Low crystalline flowerlike cobalt silicate hydroxide (Co 3 (Si 2 O 5 ) 2 (OH) 2 , CoSiO x ) is synthesized by a one-pot hydrothermal approach. Abundant highly active Co OH + is preformed on the surface of CoSiO x , while the low crystallinity of CoSiO x leads to the formation of active 1 O 2 caused by the generation of oxygen vacancy in the valence change cycle between Co 2+ and Co 3+ . The optimal CoSiO x with a high specific surface area of 665.2 m 2  g −1 could expose surface Co OH + , thus rapidly activate peroxymonosulfate (PMS) and accelerate catalytic efficiencies. As a result, at least 11 kinds of organic pollutants could be degraded with 33–242% higher efficiencies than reported. In addition to the common SO 4 - and OH, large amounts of active 1 O 2 endow the CoSiO x /PMS system with superb catalytic performances in diverse conditions, suggesting the excellent adaptability for practical usage. This work provides a new protocol to advance the PMS activation process for high-performance cobalt based heterogeneous catalysts.

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APPLIED CATALYSIS B-ENVIRONMENTAL · 2019 · IF 14.229

A photo-switch for peroxydisulfate non-radical/radical activation over layered CuFe oxide: Rational degradation pathway choice for pollutants

Junqin Liu,Pingxiao Wu,ShanShan Yang,Saeed Rehman,Zubair Ahmed,Nengwu Zhu,Zhi Dang,Zehua Liu

This work presents a novel strategy for peroxydisulfate (PDS) activation under controlled non-radical/radical mechanism, which is based on a photo-switch over layered CuFe oxide (CFO). The non-radical mechanism is attained by CFO under dark environment, and the radical mechanism is achieved through the visible light irradiation. Electron paramagnetic resonance (EPR) and density functional theory (DFT) studies demonstrate the non-radical activation mechanism is conducted by the polarization effect of CFO to PDS molecule. The radical mechanism could be elucidated by the one-electron reduction of the PDS by excited electrons on conduction band of CFO. Products analyses based on HPLC-MS and Fukui functions suggest that the non-radical degradation pathway could decrease the generation of halide intermediates, whereas the radical pathway may not be observed with this property. Quantitative structure-activity relationships (QSARs) were established between the observed pseudo-first-order rates of various phenolic pollutants and the classical descriptors (i.e., Hammett constant, Pka, E HOMO and E LUMO ) in the non-radical and radical systems, respectively, to give instructions of pathway choice for different pollutants. Considering the non-radical/radical pathway both have their own unique strengths (e.g., non-radical pathway has high selectivity to pollutants and high utilization efficiency of oxidant, and radical pathway has considerable degradation rate and strong mineralization ability), these pathways should be chosen wisely for pollutant degradation according to reality conditions.

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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

M88/PS/Vis system for degradation of bisphenol A: Environmental factors, degradation pathways, and toxicity evaluation

Jiawei Lin,Yongyou Hu,Luxiang Wang,Donghui Liang,Xian Ruan,Sicheng Shao

In this study, we synthesized a typical iron-based metal-organic framework, MIL-88B (Fe), and constructed a MIL-88B (Fe)/persulfate/visible light (M88/PS/Vis) system for photocatalytic degradation of bisphenol A (BPA) in aqueous solution. The removal efficiency, environmental factors, and degradation mechanism and pathways were explored. The results showed that there were synergistic effects in the M88/PS/Vis system: BPA (10 mg/L) could be removed completely within 25 min with 0.6 g/L M88 and 2 mM PS under visible light, while the removal rates with individual M88/Vis or M88/PS was only 26.0% and 34.1%, respectively. In addition, the BPA degradation rate in the M88/PS/Vis system (0.107 min −1 ) was 4.7 times higher than that in the M88/PS system (0.023 min −1 ) and 8.9 times higher than that in the M88/Vis system (0.012 min −1 ), respectively. Additionally, environmental factors could strongly impact the degradation of BPA in the studied system in which O 2 − and SO 4 − played a dominant role. More importantly, risk assessment in the BPA/M88/PS/Vis system was, for the first time, estimated in our study via the “ecological structure activity relationships” program at three trophic levels and Cell Counting Kit-8 method. Although there were some intermediates with higher biological toxicity than BPA and increased the toxicity of solution, most intermediates were one or more level less toxic than BPA. In most cases, the toxicity of solutions were lower than the initial samples, which demonstrated the effectiveness of M88/PS/Vis system in the reduction of toxicity of BPA, and the toxicity hazard in general could be effectively avoided by prolonging the duration of light exposure. This research provides a profound understanding of the potential application of PS activation by photocatalyst for both BPA removal and toxicity shift under visible light.

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