APPLIED SURFACE SCIENCE
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2020
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IF 6.182
Binrong Li,Yanhua Cui,Yonghai Feng,Chundu Wu,Yongsheng Yan,Minjia Meng
The directional design of interfacial defects is a promising way to promote charge separation but simultaneously a great challenge due to their random formation in heterojunction. Herein, an alternative Bi 12 O 17 Cl 2 /Bi 2 WO 6 heterojunction with interfacial defects formed spontaneously is prepared by controlling the growth of Bi 2 WO 6 on the edges of Bi 12 O 17 Cl 2 nanobelts via ion exchange process. These interfacial defects can efficiently increase the carrier density and serve as charge separation centers to extend the lifetime of carriers and activate O 2 to O 2 − and further to OH. The zigzag interfaces and irregular edges facilitate the interaction between active sites and reactants. The heterojunction morphology and the interfacial defect concentration can be controlled by tuning the solvothermal time. Consequently, the optimal Bi 12 O 17 Cl 2 /Bi 2 WO 6 heterojunction exhibits significantly enhanced visible light photocatalytic performance toward the degradation of phenols, antibiotics and dyes as compared to that of mono-Bi Bi 12 O 17 Cl 2 and Bi 2 WO 6 photocatalyst.
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WATER RESEARCH
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2020
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IF 9.13
Jun Wang,Xiaoguang Duan,Jian Gao,Yi Shen,Xiaohui Feng,Zijun Yu,Xiaoyao Tan,Shaomin Liu,Shaobin Wang
A rational design of structure-tailored and functionalized nanocarbons for peroxymonosulfate (PMS) activation is important in metal-free catalysis for degradation of water contaminants. In this work, we employed ionic liquids (ILs) for synthesis of porous carbon materials (PCMs) as a PMS activator for oxidative removal of naproxen and systematically investigated the functions of structure defects, oxygen functional groups and heteroatom doping toward the catalytic oxidation. A positive linear correlation between reaction rate constants and carbon defect ratios of PCMs revealed that the structural defects played an important role in PMS activation. Electron paramagnetic resonance (EPR) spectra, radical quenching experiments and electrochemical analysis tests verified nonradical-dominated oxidations via electron transfer and 1 O 2 . Structural vacancies, ketonic C=O groups and graphitic-N atoms on carbons have been revealed to be the active sites for the nonradical pathways via direct electron transfer or generation of O 2 •− / 1 O 2 . This work provides new insight into the reaction mechanism and structure-performance relationships of the catalytic centers in nonradical oxidation.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Hongchao Li,Jieshu Qian,Bingcai Pan
Co-based carbonaceous materials are among the most effective heterogeneous catalysts to activate peroxymonosulfate (PMS) for the degradation of organic pollutants in water. However, present examples normally suffer the aggregation of catalyst and/or the leakage of active Co species especially when the Co content is high, resulting in a loss of reactivity and potential environmental risk. In this study, we report the use of a mixture of Co phthalocyanine and melamine as precursor for the preparation of a carbonaceous catalyst with N-coordinated Co (Co-NG) for PMS activation . The presence of Co phthalocyanine in the precursor facilitates the uniform distribution of Co species in carbonaceous substrate with high Co content of 8.0 wt%, thus exhibiting remarkable catalytic reactivity for the degradation of a variety of organic pollutants. More importantly, the strong coordination by N atoms significantly enhances the Co stability and reduces the Co leaching during cyclic use. Experiment results demonstrate that both sulfate radicals (SO 4 •− ) and hydroxyl radicals (HO • ) contribute to the pollutant degradation with SO 4 •− as the main reactive species. Other reaction parameters including solution pH, the presence of inorganic anions, and natural organic matters were also investigated and evaluated. We reckon this study provides new insights for the design of efficient Co-based carbonaceous catalysts with high Co stability for water treatment application.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Qiuyi Ji,Xinying Cheng,Yijie Wu,Weiming Xiang,Huan He,Zhe Xu,Chenmin Xu,Chengdu Qi,Shiyin Li,Limin Zhang,Shaogui Yang
A novel PDI/PS/Vis system was constructed and the photocatalytic activity of PDI with various degrees of self-assembly was explored. Perylene diimide (PDI) as photocatalysts possesses excellent charge separation efficiency and the electron injection from the PDI to persulfate (PS) can produce active species more efficiently. With the PDI/PS/Vis system, 5 mg/L bisphenol A (BPA, 50 mL) could be completely removed in 15 min with 0.5 g/L photocatalyst and 1.5 mM PS under visible light (λ>420 nm). Nearly 71.1 % of BPA was mineralized after 1 h degradation. Radical quenching tests and electron paramagnetic resonance (EPR) spectra revealed that h + , ·O 2 − , ·OH and SO 4 ·- all contributed to organics elimination with radical process. Based on the results of theoretical calculations and toxicity assessment, BPA will eventually be converted into non-toxic ring-opening products. Therefore, the highly efficient PDI/PS/Vis system has great potential for application in water environment remediation.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Xinxin Long,Shengjiong Yang,Xiaojie Qiu,Dahu Ding,Chuanping Feng,Rongzhi Chen,JihuaTan,Xinming Wang,Nan Chen,Qin Lei
A facile coprecipitation-thermal method is reported to prepare spinel cobalt ferrites CoFe 2 O 4 nanoparticles (NPs) with a well-defined mesoporous dominated structure using hybrid cobalt-ion hexacyanoferrate (CoFeHCF) NPs as a template. The properties of the synthesized catalysts are evidenced by various characterization methods. And the effects of time, pH, catalyst/oxidant/BPA dosage, coexisting ions and natural organic matter (NOM) on catalytic degradation of bisphenol A (BPA) are investigated. The as-prepared CoFe 2 O 4 shows a high catalytic performance of 97% elimination for 45 μM BPA in 40 min. The excellent catalytic performance could be attributed to the large specific surface area (66.18 m 2 /g) and high content of cobalt (the atomic ratio of Fe/Co is 1.86) of CoFe 2 O 4 NPs. Slightly alkaline pH, higher catalyst dosage and anions including Cl − and CO 3 2− /HCO 3 − are favorable for BPA degradation. Especially, 81.57% mineralization of BPA could be achieved in 60 min under the optimization system. The catalytic capacity of CoFe 2 O 4 could be regenerated by simple washing and drying at 200℃, which is much lower than the crystal temperature. SO 4 ∙ − and HO∙ are the primary reactive species responsible for BPA oxidation while SO 4 ∙ − might play a dominant role. This work provides a novel method to produce CoFe 2 O 4 nanocatalysts for contaminant degradation and encourage the extended application of CoFeHCF in the environment.
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ACS Applied Bio Materials
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2020
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IF 0
Ning Zhao,Jing-Min Liu,Fei-Er Yang,Shi-Wen Lv,Jin Wang,Shuo Wang
It is of great significance to establish a simple method for sensitively detecting metal ions and antibiotics for food safety. Herein, two crystalline polyimide covalent organic frameworks (COFs) were constructed via a green method, in which no organic solvents were used. Results suggested that both COF-1 and COF-2 with π-conjugated frameworks emitted strong fluorescence originating from the n−π* transition in N,N-dimethylformamide and the alkaline aqueous solution. More interestingly, both COF-1 and COF-2 showed excellent sensing performance for various metal ions and typical antibiotics. Taking COF-1 as the specific research object, the as-synthesized COF-1 exhibited noticeable turn-off fluorescence behaviors for 10 metal ions and 2 antibiotics. A high linear correlation coefficient, a wide linear range, and a low detection limit were achieved in real samples. The aggregation effect and π–π reaction were the possible fluorescence quenching mechanisms. In short, this work provides insights into the synthesis and application of fluorescent sensors based on COFs in food detection fields.
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MICROCHEMICAL JOURNAL
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2020
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IF 3.594
Wenfei Zhao,Xu Jing,Yaqin Tian,Cuiping Feng
A novel approach using magnetic Fe 3 O 4 @ porous activated carbon effervescent tablet-assisted deep eutectic solvent-based dispersive liquid–liquid microextraction (META-DES-DLLME) combined with HPLC was developed for the measurement of phenolic endocrine disrupting chemicals (bisphenol A, p - tert -octylphenol, nonylphenol) in environmental water. In the proposed method, deep eutectic solvents synthesized by 1-dodecanol and hexyltrimethylammonium bromide were applied as extraction solvent. A magnetic effervescent tablet, containing a foaming agent and a new magnetic material, combined the dispersion of the extraction solvent and the magnetic recovery into one step. The influence of parameters, including the composition and volume of DESs, the type and amount of acid, the amount of sodium bicarbonate, the composition and amount of Fe 3 O 4 @ porous activated carbon, the pH, and the amount of sodium chloride, were optimized. Under the optimized conditions, accuracy and precision were demonstrated over the whole concentration range of 10–1000 μg L -1 . The extraction recovery ranged from 81.0 to 94.7% with a relative standard deviation of 1.2–6.7%, and the LOD and LOQ ranged from 0.82 to 1.7 μg L -1 and 2.7–5.5 μg L -1 , respectively. The method was successfully applied to extract and analyse the phenolic endocrine disrupting chemicals in environmental water.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2020
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IF 5.774
Guanghui Wang,Jialing Dai,Qiuyan Luo,Nansheng Deng
In this work, a novel titanium dioxide@aspartic acid-β-cyclodextrin@reduced graphene oxide (TiO 2 @ACD@RGO) composite photocatalyst was successfully synthesized by photochemical method and characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), Fourier transform- infrared spectroscopy (FT-IR), Raman spectroscopy, Brunauer-Emmett-Teller (BET), X-ray photoelectron spectroscopy (XPS) and thermogravimetric analysis (TGA). The photocatalytic degradation behavior of bisphenol A (BPA) was investigated under UV irradiation (λ < 365 nm), the mechanism of photocatalytic degradation of BPA on TiO 2 @ACD@RGO was explained, and the stability and reusability of TiO 2 @ACD@RGO composite was also evaluated. The photocatalytic investigations showed that the TiO 2 @ACD@RGO possessed high photocatalytic efficiency for the degradation of BPA, which was better than that of TiO 2 and TiO 2 @RGO. The reaction constant of TiO 2 @ACD@RGO for BPA was 0.739 mg/L·min, which was 1.34 times of TiO 2 @RGO and 1.87 times of TiO 2 , respectively. The predominant reactive oxygen species for BPA degradation was identified to be the O 2 − and h + . The high photocatalytic activity was attributed to the improvement of the electron transfer and mass transfer at the TiO 2 @ACD@RGO interface. Additionally, the TiO 2 @ACD@RGO presented excellent stability and reusability after five cycles.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Lihan Pan,Wen Shi,Tapas Sen,Lingzhi Wang,Jinlong Zhang
The role of high-valent Fe has rarely been explored in persulfate-based heterogeneous reaction. Herein, the existence of Fe(IV) is verified in a visible light-assisted FeTiO 3 /persulfate system using methyl phenyl sulfoxide as the probe. The FeTiO 3 /persulfate/light system is capable of selectively degrading aromatic compounds with lower ionization potentials including tetracycline and bisphenol A by photo-generated high-valent Fe(IV). The contributions from SO 4 ·- , · OH and 1 O 2 are excluded. The comparable efficiency in the dark requires higher dosages and suffers from a rapid deactivation. Based on XPS, Raman and EPR analyses, the poor dark activity is caused by the formation of a complex between in situ formed Fe(III) and SO 4 2- on the FeTiO 3 surface; this complex is, however, the key intermediate for Fe(IV) production under the light irradiation. This study reveals the long-ignored role of SO 4 2- as an abundant species in iron-based persulfate systems. We also call for re-evaluating the real oxidation mechanism in other persulfate-based reactions considering the different oxidation mechanisms of radicals and high-valent iron.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Zhuoqian Li,Kai Li,Shuanglong Ma,Bingjun Dang,Yi Li,Haichao Fu,Jinge Du,Qingxiang Meng
A convenient and efficient method to fabricate isolated Fe single-atom catalysts deposited on Myriophyllum aquaticum -based biochar (ISA-Fe/MC) is reported for peroxymonosulfate-based organics degradation. Firstly, the Fe nanoparticles anchored on the hierarchical porous biochar (nano-Fe/MC) can be obtained by utilizing K 2 FeO 4 as a synchronous activation and graphitization agent. Subsequently, ISA-Fe/MC was achieved by HCl etching of nano-Fe/MC to remove the excess Fe nanoparticles. Compared with nano-Fe/MC, ISA-Fe/MC demonstrated outperformed catalytic capacity towards PMS activation for phenol degradation. The combination of super high surface area, hierarchical porous structure, graphitization structure and atomically dispersed Fe species should be responsible for prominent catalytic oxidation ability and outstanding resistance to common anions and humic acid. Based on the chemical scavengers, EPR experiments and electrochemistry tests, the SO 4 •– dominated radical degradation pathway for nano-Fe/MC and electron transfer reigned non-radical degradation pathway for ISA-Fe/MC was revealed. In contrast to nano-Fe/MC, density functional theory calculations demonstrated the enhanced density of states around Fermi level in ISA-Fe/MC meaning the increased catalytic performance and more electron transfer between single-atom Fe to adjacent graphitic C and N which could serve as electron transfer channel for PMS activation.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2020
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IF 6.551
Yaxin Sun,Xinying Wang,Yuanyuan Zhou,Junhong Zhang,Weiqi Cui,Enyin Wang,Juan Du,Bo Wei,Xia Xu
Human exposure to bisphenol A (BPA) is unavoidable in daily life. Recently, research has showen that BPA could induce oxidative imbalance, thereby causing reproductive toxicity and liver dysfunction. Accumulated evidence has demonstrated that metformin possesses strong anti-oxidative properties. This study aimed to study the mechanism underlying the hepatic-protective effect of metformin on liver injury induced by BPA in rats via the UPLC-MS/MS metabolomics approach. Forty-two male rats were randomly divided into six groups ( n = 7), namely the saline group (control), the corn oil group (vehicle), the metformin group (Met), the bisphenol A group (BPA), the bisphenol A and metformin group (BPA + Met), and the bisphenol A and diammonium glycyrrhizinate (positive control) group (BPA + DG). Serum was collected for biochemical analysis and metabolomics, and liver tissue was collected for histopathology and metabolomics in each group. We found that metformin could significantly reduce the levels of liver function enzymes (ALT, AST and GGT) and ameliorate inflammatory cell infiltration and hepatocyte necrosis induced by BPA. On the other hand, metformin could significantly enhance the total antioxidant capacity in BPA rats. Notably, metabolomics data indicated that the principal altered metabolic pathways based on the 26 differential metabolites in liver tissue, and 21 in serum among vehicle, BPA and BPA + Met groups, respectively, including cysteine and methionine metabolism, glutathione metabolism, and arginine biosynthesis and purine metabolism. Additionally, metformin significantly increased cystathionine β synthase (CBS) and cystathionine γ lyase (CSE), thus reducing serum levels of homocysteine and increasing hepatic levels of cysteine and glutathione in BPA-treated rats. Overall, this study's results provided new insights into the role and mechanism of metformin in BPA-induced liver injury in rats.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2020
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IF 5.774
Longqian Xu,Linghui Zhao,Yunfeng Mao,Zhen Zhou,Deli Wu
Copper-iron bimetallic material shows a high reactive activity in dioxygen activation processes (DOAs) but presents a significant challenge for enhancing superoxide radical ( • O 2 − ) generation. In this study, a practical strategy was developed to enhance • O 2 − generation for BPA degradation using a zeolite-supported Cu-Fe bimetallic system (called Cu/Fe@zeolite), which was simply prepared by impregnation method. The results verified that the Cu(I) regeneration at the zeolite surface contributes • O 2 − generation and the H 2 O 2 that is further generated induces • OH production via a further Fenton reaction. In the reaction process, the initial generation of • O 2 − was primarily enhanced by the Cu(I) loaded onto the zeolite surface and the adsorbed BPA was easily degraded by the •OH. Under optimal operating conditions (i.e., Cu/Fe@zeolite = 3 g/L, Cu:Fe = 1:2, pH = 5, t = 120 min), it was found that 87% of BPA can be removed from wastewater. It is also important to note that the weak alkali buffering property of zeolite not only provides BPA adsorption sites under acidic conditions but also accelerates the precipitation efficiency for metallic ions and reduced the adverse effect of metallic residue on the effluent quality.
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