JOURNAL OF THE AMERICAN CERAMIC SOCIETY
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2023
·Vol. 106
·期 7
·4089-4102
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IF 3.9
Peng Zhao,Yuanhui Gao,Guogang Xu,Enliang Zhang,Lulu Liu,Shaowei Jin
In this experiment, a novel catalytic ceramic membrane (CCM) with spherical Cu 1.4 Mn 1.6 O 4 material loading was prepared through hydrothermal in situ growth method. The synergistic effects of membrane separation and catalytic ozonation on membrane antipollution and degradation of micro-pollutants were systematically investigated. The results indicated that the degradation efficiency of bisphenol A by CCMs reached 85.7% with a stable normalized flux of 0.90 under the operating conditions of [O 3 ] = 4 g/h, transmembrane pressure = 0.2 bar, and pH = 6. In addition, the results showed that the composite bimetallic oxides have good stability by measuring the leaching concentration of metal ions during the catalytic process. This study provides a promising strategy for in situ growth of catalytically active composite bimetallic oxides on the surfaces of ceramic membrane and for mitigation of membrane fouling complex water treatment.
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Jingyu Zhang,Yan Wang,Mei Hong,Bin Peng,Chunyang Bao,Xiaoling Xu,Die Li,Jing Chen,Bingyu Wang,Qiang Zhang
As a classical advanced oxidation technology, the Fenton reaction is often criticized for having a narrow pH window, difficult recovery of catalysts, and generating iron-containing sludge. Furthermore, traditional Fenton reaction was also limited in treating high salinity wastewater. In this work, a ferrocene-containing resin is prepared and used as the heterogeneous catalyst for a Fenton-like reaction to treat different organic pollutants wastewaters in high salinity conditions under a wide pH range. Using ascorbic acid as a reducing agent, the Fenton-like reaction can degrade different organic pollutants such as methylene blue, bisphenol A, bisphenol S, tetracyclines, and 4-nitrophenol within 10 min in high salinity conditions (500 mmol/L) at a wide range of pH values from acidic to basic. In mechanism investigation, singlet oxygen and superoxide radicals were identified as the primary reactive oxygen species. It was straightforward to recover the resin from water, and the degradation ratio exceeded 99% in five consecutive experiments. Such a Fenton-like reaction could also efficiently regenerate the resins to restore their adsorption capacity without using acid, base, or organic solvents.
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MICROCHIMICA ACTA
·
2023
·Vol. 190
·期 4
·1-9
·
IF 5.7
Tu Xinman,Deng Lamei,Ren Boyuan,Xu Zihan,Zhang Li
A conventional colorimetric method based on CuS-catalyzed H 2 O 2 is improved by a dual-modification strategy and employed for thioglycolic acid (TGA) determination. The doping of Co(II) can enhance ion exchange efficiency. Meanwhile, the modification of g-C 3 N 4 can increase specific surface area and decrease unspecific aggregation. The constructed g-C 3 N 4 /Co-CuS nanocomposite exhibited a favorable catalytic feature. A Michaelis constant (K m ) value of 0.02 mM has been achieved, which is 1/160 of those of CuS and horseradish peroxidase (HRP). The g-C 3 N 4 /Co-CuS displays a rapid color response in 3 min and resulted in a stable measurable signal within 10 min. In the determination procedure, the sulfhydryl contained in TGA is capable of preventing TMB oxidation via competing the · OH produced by catalysis and caused a color distinction that is related to the TGA amount. The distinctions of absorbance (λ max = 652 nm) of different concentrations of TGA are recorded. Linearity is obtained in the ranges of 2.5 – 20 µM and 20 – 160 µM, and the LOD is 0.14 µM. In the real sample assays of perm agent and Qianhu lake water, the recoveries were 96.70 – 106.84% and 100.21 – 101.90%, respectively. This demonstrates that the proposed dual-modification strategy for CuS contributes to highly efficient and convenient determination of TGA in daily cosmetics and water analysis. Graphical Abstract
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 27
·71088-71102
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IF 5.8
Fan Xinfei,Liu Na,Yang Jia,Yu Yueling,Xu Yuanlu,Song Chengwen,Liu Yanming
Persulfate activation is emerged as an alternative applied in environment remediation, but it is still a great challenge to develop highly active catalysts for efficient degradation of organic pollutants. Herein, a heterogeneous iron-based catalyst with dual-active sites was synthesized by embedding Fe nanoparticles (FeNPs) onto the nitrogen-doped carbon, which was used to activate peroxymonosulfate (PMS) for antibiotics decomposition. The systematic investigation indicated the optimal catalyst exhibited a significant and stable degradation efficiency of sulfamethoxazole (SMX), in which the SMX can be completely removed in 30 min even after 5 cycle tests. Such satisfactory performance was mainly attributed to the successful construction of electron-deficient C centers and electron-rich Fe centers via the short C-Fe bonds. These short C-Fe bonds accelerated electrons to shuttle from SMX molecules to electron-rich Fe centers with a low transmission resistance and short transmission distance, enabling Fe (III) to receive electrons to promote the regeneration of Fe (II) for durable and efficient PMS activation during SMX degradation. Meanwhile, the N-doped defects in the carbon also provided reactive bridges that accelerated the electron transfer between FeNPs and PMS, ensuring the synergistic effects toward Fe (II)/Fe (III) cycle to some extent. The quenching tests and electron paramagnetic resonance (EPR) indicated O 2 ·− and 1 O 2 were the dominant active species during the SMX decomposition. As a result, this work provides an innovative method to construct a high-performance catalyst to active sulfate for organic contaminant degradation.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
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
·
2023
·
IF 13.6
Liwei Yang,Fashan Yang,Heng Zhang,Hongyu Zhou,Mengfan Luo,Yunmei Liu,Chuanliang Zhao,Lu Zheng,Bo Lai
At present, the potential mechanism of manganese oxide (MnO 2 ) activation of PI and the key active sites of PI activation are still unclear and controversial. To this end, three different crystal forms of MnO 2 were prepared in this study and used to activate PI to degrade pollutants. The results showed that different crystal types of MnO 2 showed different catalytic abilities, and the order was γ-MnO 2 > α-MnO 2 > β-MnO 2 . Through quenching experiments, EPR tests, Raman experiments and in situ electrochemical experiments, it has been confirmed that electron transfer-mediated non-free radical process is the main mechanism of pollutant degradation , in which the active substance is the highly active metastable intermediate complex (MnO 2 /PI*). Hydroxyl radical (HO • ), superoxide radical (O 2 •− ), singlet oxygen ( 1 O 2 ) and iodine radical (IO 3 • ) did not participate in pollutant degradation. The quantitative structure-activity relationship analysis confirmed that the catalytic performance of MnO 2 was highly positively correlated with the surface Mn(IV) content, which indicated that the surface Mn(IV) site was the main active site. Overall, this study will be of great help to the design and application of manganese dioxide activation for periodate degradation of pollutants.
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Yukun Yang,Xiaoxing Zeng,Yu Tian,Xiaomin Wang,Xu Jing,Ligang Yu,Baoqing Bai,Jinhua Zhang,Shu Qin
A universal design of turn-on fluorescent aptasensor based on aptamer functionalized gold nanoparticles (AuNPs) and luminescent metal–organic frameworks (LMOFs) complex (AuNPs-Apt/NH 2 -MIL-125(Ti)) was realized for bisphenol A (BPA) detection. LMOF NH 2 -MIL-125(Ti) was prepared using facial hydrothermal method. BPA aptamer functionalized AuNPs were prepared and adsorbed on the surface of NH 2 -MIL-125(Ti) to obtain platform of the fluorescent aptasensor. The fabrication process, sensing performance and applicability of the proposed aptasensor were characterized and investigated carefully. Linear detection range of the constructed aptasensor was from 1 × 10 –9 mol L –1 to 1 × 10 –4 mol L –1 with good selectivity, repeatability, stability and reproducibility under optimal experimental conditions. Meanwhile, the fluorescent aptasensor was successfully utilized for BPA detection in real samples with the recoveries of 95.80%-103.12%. The proposed aptasensor based on AuNPs-Apt/NH 2 -MIL-125(Ti) holds significant potential for BPA detection in environmental and food samples, promoting the construction and application of LMOFs-based aptasensor.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Baokang Xu,Xiao Zhang,Yue Zhang,Shiwen Wang,Peng Yu,Yongjun Sun,Xi Li,Yanhua Xu
The nonradical pathway selectively oxidizes pollutants with less interference from environmental factors, which can effectively improve the environmental suitability of peroxymonosulfate (PMS) activation. Herein, a Co-doped nanotubular carbon nitride catalyst (Co-CNNT) based on CoN x sites was constructed for stable and efficient PMS activation with a better specific surface area, number of CoN x sites, and electron transfer capability than Co-doped lamellar carbon nitride catalyst (Co-CN). Co-CNNT improved PMS utilization efficiency (∼50%) and enhanced the contribution of the electron transfer pathway to tetracycline (TET) degradation. The enhanced ability of Co-CNNT to adsorb PMS leads to Co-CNNT–PMS* generated by PMS at the CoN x site, which raises the Co-CNNT surface potential and allows PMS to be activated in a manner that captured electrons. Thus, the Co-CNNT/PMS system could effectively destroy electron-rich or low-potential pollutants within 24 min. The stronger environmental adaptability allows it to maintain catalytic activity in complex aqueous matrices, achieving effective oxidation of diluted tetracycline-based pharmaceutical wastewater. This paper reveals the effects of carbon nitride morphology control strategies on the properties of CoN x active sites and PMS activation mechanisms, providing new insights into the induction of nonradical PMS activation pathways.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Zixuan Li,Ziyi Yang,Qinghong Shi,Yan Sun
Environmentally widespread endocrine-disrupting chemicals, such as bisphenol A (BPA), have posed a risk to living things. Laccase, a kind of oxidoreductase, can effectively catalyze the degradation of phenolic compounds like BPA. Herein, a defective metal-organic framework (dPCN-224) with BPA adsorption capability was synthesized and used for laccase immobilization. The material was extensively characterized and successful immobilization of laccase via hydrophobic interaction was confirmed. The immobilization reached an enzyme loading density of 80 mg/g onto dPCN-224 and the laccase@dPCN-224 showed high activity recovery (90.0% vs. free laccase) and increased thermostability, pH tolerance, and organic co-solvent resistance over the free enzyme. Moreover, at various concentrations (0.5–20 mg/L), the BPA removal efficiencies of laccase@dPCN-224 were 3.3–5.0 times higher than those of free laccase due to the cooperative effect of adsorption and enzymatic degradation. The BPA bound on laccase@dPCN-224 could be almost completely biodegraded by adding 0.5 mM of electro-mediator (2,2′-azino-bis (3-ethylbenzothiazoline-6-sulfonic acid)). In addition, after five consecutive batch cycles, the BPA removal efficiency of laccase@dPCN-224 kept as high as 98.1% at 5 mg/L BPA. Taken together, the results proved the potential of laccase@dPCN-224 for applications in addressing environmental BPA pollutions.
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WATER RESEARCH
·
2023
·
IF 12.8
Mengfan Luo,Heng Zhang,Yang Shi,Jia Zhao,Can Feng,Jialong Yin,Yang Liu,Peng Zhou,Zhaokun Xiong,Bo Lai
Advanced oxidation technologies based on periodate (PI, IO 4 − ) have garnered significant attention in water decontamination. In this work, we found that electrochemical activation using graphite electrodes (E-GP) can significantly accelerate the degradation of micropollutants by PI. The E-GP/PI system achieved almost complete removal of bisphenol A (BPA) within 15 min, exhibited unprecedented pH tolerance ranging from pH 3.0 to 9.0, and showed more than 90% BPA depletion after 20 h of continuous operation. Additionally, the E-GP/PI system can realize the stoichiometric transformation of PI into iodate, dramatically decreasing the formation of iodinated disinfection by-products. Mechanistic studies confirmed that singlet oxygen ( 1 O 2 ) is the primary reactive oxygen species in the E-GP/PI system. A comprehensive evaluation of the oxidation kinetics of 1 O 2 with 15 phenolic compounds revealed a dual descriptor model based on quantitative structure−activity relationship (QSAR) analysis. The model corroborates that pollutants exhibiting strong electron-donating capabilities and high p K a values are more susceptible to attack by 1 O 2 through a proton transfer mechanism. The unique selectivity induced by 1 O 2 in the E-GP/PI system allows it to exhibit strong resistance to aqueous matrices. Thus, this study demonstrates a green system for the sustainable and effective elimination of pollutants, while providing mechanistic insights into the selective oxidation behaviour of 1 O 2 .
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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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HIGH PERFORMANCE POLYMERS
·
2023
·
IF 2.1
Slimane Abdous,Mehdi Derradji,Zineb Mekhalif,Karim Khiari,Oussama Mehelli,Younes Bourenane Cherif
Given their substantial neutron capture cross-section, extreme hardness, and high chemical and thermal stability, boron-based materials are widely used as building blocks to protect against highly ionizing radiations such as gamma rays and neutrons. Indeed, uncontrolled nuclear radiation exposure can be highly hazardous to radiation workers and the general public. In this sense, this work presents an extensive study and experimental evaluation of the nuclear shielding features of boron carbide (B4C) based nanocomposite, where bisphenol-A based polybenzoxazine (BA-PBz) was used as matrix. The latter was used for its wide range of interesting properties that overcome some of the shortcomings of conventional phenolic resins. A two-pot synthesis process was adopted for the synthesis of (BA-Bz) monomer. Moreover, the boron carbide nanoparticles were treated with a silane (KH-560) coupling agent in order to improve the intramolecular interactions with the polymeric matrix. The neutron shielding studies were carried out at the Nuclear Research reactor of Algeria NUR. The results showed that the developed boron carbide-based nanocomposite exhibits intriguing shielding performances and good thermal stability. The highest performances were obtained at a B4C concentration of 5. wt %, where the macroscopic cross section was found to be (Σ = 3.3878 cm−1) with a screening ratio of (S = 97.78%).
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