ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Jinxin Li,Dan Zhong,Yiru Chen,Kefei Li,Wencheng Ma,Shaobo Zhang,Jingna Zhang,Aoshuang Sun,Haijiao Xie
Coal pyrolysis wastewater (CPW) contained all kinds of toxic and harmful components, which would seriously threaten the natural environment and human health. However, the traditional advanced oxidation processes frequently failed to remove phenolic substances. An A 2 BO 4 -type perovskite (La 2 CuO 4 ) was successfully synthesized through sol-gel process and first applied in the treatment of CPW. More than 90% of 3, 5-dimethylphenol (DMP) was removed within 200 min at neutral conditions. Moreover, La 2 CuO 4 also displayed excellent catalytic activity and stability in the actual CPW treatment process. Results demonstrated that DMP was removed through the attack of ∙OH, ∙O 2 − and 1 O 2 in La 2 CuO 4 /H 2 O 2 system. The La 2 CuO 4 were more favorable for H 2 O 2 activation and have a lower adsorption energy than LaFeO 3 . XPS of fresh and spent La 2 CuO 4 illustrated that the decomposition of hydrogen peroxide (H 2 O 2 ) was mainly due to the redox cycle between surface copper and oxygen species. Moreover, the possible degradation pathway of DMP was deduced by identifying degradation products and analyzing density functional theory (DFT) calculations. This research provided a novel strategy for the development of perovskite-based catalytic materials on the treatment of practical CPW.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
PubMed
高影响因子
WATER AIR AND SOIL POLLUTION
·
2024
·Vol. 235
·期 5
·1-14
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IF 3.8
Zhou Rui,Zou Congyang,Wang Yong,Zhou Zhuyou,Liu Menghe,Ji Yufeng
One 3D Cu-based metal–organic frameworks (Cu-MOFs) was prepared by hydrothermal method as a catalyst for activating persulfate to degrade tetracycline. The degradation efficiency of TC was investigated under various conditions including catalyst dosage, pH, and persulfate concentration. The effects of these factors on the degradation efficiency were examined and discussed in detail. Cu-MOFs/PS catalytic systems can degrade 96% of TC under suitable conditions. The quenching experiments showed that there are both free radical and non-free radical pathways in TC degradation, with singlet-line substitution of oxygen playing a major role. The stability of the material structure was explored through cyclic experiments. The degradation pathway of TC was investigated through the analysis of intermediate products. Additionally, the toxicity of these intermediate products was evaluated using toxicity analysis software.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Yihao Li,Lu Jiang,Rui Wang,Pingxiao Wu,Juan Liu,Shanshan Yang,Jiahao Liang,Guining Lu,Nengwu Zhu
In this paper, Phenol , 4-Chlorophenol (4-CP), 2,4-Dichlorophenol (2,4-DCP) and 2,4,6-Trichlorophenol (2,4,6-TCP) were selected as model pollutants to explore the oxidant mechanism by ferrate (Fe(VI)). The reactions between ferrate (1000 μM) and four phenolic compounds (100 μM) were conformed to the second-order reaction kinetics at pH 9.2, and the order of k obs followed as: k 4-CP (129 M −1 s −1 ) > k 2,4-DCP (96 M −1 s −1 ) > k 2,4,6-TCP (44 M −1 s −1 ) > k Phenol (12 M −1 s −1 ). Meanwhile, the degradation rates of all four compounds by Fe(VI) increased with increased pH (3.1–9.2). A total of 14 degradation products were identified by Liquid chromatography-Time-of-Flight-Mass Spectrometry (LC-TOF-MS), and two pathways including hydroxylation of benzene ring and substitution of chlorine atom were proposed. Hydroxyl radicals , played a vital role during the degradation of phenolic compounds. Moreover, density functional theory calculations were used to explore the degradation mechanisms. The results showed that the hydroxyl radical was more favorable to substitute chlorine atom than hydrogen atom , and the substitution on ortho-position was more favorable than para-position for all four compounds. The findings of this study could greatly improve our understanding on the degradation mechanism of chlorophenol-like compounds by Fe(VI) for environmental remediation.
研究领域:
环境科学
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化学
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PubMed
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2012
·
IF 2.234
Huan Liu,Zi-en Fu,Kai Xu,Hua-lun Cai,Xin Liu,Ming-Cai Chen
A novel Schiff-base liquid crystal diepoxide polymer was prepared via a thermal copolymerization of a Schiff-base epoxy monomer ( PBMBA ) with a diamine co-monomer (MDA). We first proposed that specific effects of highly conjugated Schiff-base moiety on thermal properties of the Schiff-base epoxy polymer ( PBMBA /MDA). Thermal degradation behavior of the polymer was characterized using thermogravimetric analysis (TGA) under nitrogen and under air, respectively. Thermogravimetric data obtained from TGA under nitrogen and under air reveal that PBMBA /MDA exhibits higher thermal stability compared with bisphenol-A type epoxy polymer (DGEBA/MDA) and other mesogene-containing epoxy polymer. It is worth pointing out that the outstanding residual char value for the Schiff-base epoxy polymers had been rarely reported. For thermal degradation mechanism of PBMBA /MDA under nitrogen, thermogravimetric analysis/infrared spectrometry (TG-IR) were used to investigate volatile components, and scanning electron microscopy/energy dispersive spectroscopy (SEM/EDS) was used to explore morphologies and chemical components of the residual char. The effects of calcination temperature and calcination time on evolution of morphologies and chemical components of the residual char have been studied. It is proposed that the highly π-conjugated Schiff-base moiety is not only involved in a formation of intramolecular hydrogen bonding increasing the onset thermal degradation temperature ( T d ), but also possesses an effective charring ability retarding a further degradation of polymers. Due to the presence of the specific effects, the thermal stability of the Schiff-base epoxy is improved.
研究领域:
材料科学
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高分子化学
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 37
·15908-15918
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IF 3.288
Xiuna Yu,Zhixiang Liu,Yemei Wang,Hongyu Luo,Xu Tang
Insights into active sites and charge transport behavior are challenging topics for fabricating composite photocatalysts and investigating their photocatalytic degradation reaction mechanisms. Herein, novel composites comprising biomass charcoal and graphitic carbon nitride (CN) were fabricated via facial alkali catalysis and thermal condensation of corncob and melamine precursors. By fine-tuning the calcination temperature, the carbonization temperature of corncob-derived biomass charcoal was controlled, which had a great influence on the optimal photocatalytic activity of C–CN-600, which was 90% of the degradation activity of 2-mercaptobenzothiazole (MBT), and about 2-fold higher than that of pure CN. The corncob not only acts as a precursor for biomass charcoal, but can also prevent the agglomeration of CN at high temperature. Moreover, the charge carrier lifetime, visible light absorption and surface area are also revealed in detail by systematic characterization. In addition, the intermediate products of MBT, the degradation reaction pathway, and the mechanism over C–CN are revealed in depth.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Chunyan Yang,Hua Chai,Peng Xu,Peng Wang,Xiaojing Wang,Tianyao Shen,Qingzhu Zheng,Guangshan Zhang
Atrazine (ATZ), as a widely used s-triazine herbicide, has persistence and biological toxicity in the environment. Photocatalytic technique is considered as sustainable and promising strategy for the degradation of emerging organic pollutants. Thus, 3D/2D Bi 2 WO 6 /g-C 3 N 4 heterojunction photocatalysts were synthesized via one-step hydrothermal method for ATZ degradation. The Bi 2 WO 6 /g-C 3 N 4 -0.15 exhibited 99.96% removal efficiency for ATZ and the rate constant was approximately 25, 4.8 and 10 times greater than the rate constants of Bi 2 WO 6 , g-C 3 N 4 and “Bi 2 WO 6 + g-C 3 N 4 ”, respectively. The influence of synthesis reaction factors of Bi 2 WO 6 /g-C 3 N 4 and various environmental factors including catalyst dosage, ATZ concentration, pH, common anions and HA on photocatalytic property of Bi 2 WO 6 /g-C 3 N 4 were also investigated. The radical-quenching experiments proved that holes (h + ), 1 O 2 and O 2 – played pivotal roles in ATZ degradation in Bi 2 WO 6 /g-C 3 N 4 photocatalytic system. The ATZ degradation pathway involved dealkylation, alkyl hydroxylation, alkyl oxidation, dechlorination-hydroxylation and deamination-hydroxylation reactions, which was proposed by HPLC–MS/MS results and density functional theory (DFT) analysis. Moreover, quantitative structure–activity relationship (QSAR) evaluation showed that the ecotoxicity of many intermediates declined compared with ATZ. The 3D/2D Bi 2 WO 6 /g-C 3 N 4 heterojunction exhibited excellent photostability and pH adaptability, showing efficient practicality in the removal of refractory organic pollutants in wastewater.
研究领域:
环境科学
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材料科学
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化学工程
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分析化学
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 37
·14829-14840
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IF 3.069
Jianhui Li,Quan Zhou,Fan Yang,Lijie Wu,Wenying Li,Ruipeng Ren,Yongkang Lv
The binary BiOBr/BiOI composite photocatalysts with different molar ratios obtained via a simple one-step solvothermal method were investigated by using XRD, Raman spectroscopy, SEM, EDS, TEM, HR-TEM, BET, UV-vis DRS and PL. The degradation efficiency of uniform flower-like BiOBr/BiOI (3 : 1) is best when the samples were used to degrade RhB solution under visible light irradiation, which is attributed to its uniform particle distribution and the largest specific surface area of 44.21 m2 g−1. Compared with the previously synthesized BiOBr/BiOI, the morphology and specific surface area of BiOBr/BiOI (3 : 1) have obvious advantages. The influence factors (pH, NO3−, Cl− and HCO3−) on the photocatalytic performance of BiOBr/BiOI (3 : 1) were explored. The recycling experiments demonstrate that BiOBr/BiOI (3 : 1) composite maintains high photocatalytic activity after eight recycling experiments, and its crystal structure and morphology do not change. In addition, a possible degradation mechanism was also ascertained by radical capture experiments, EPR and semiconductor structure analysis. All results suggest that the uniform flower-like BiOBr/BiOI (3 : 1) composite with high photocatalytic degradation efficiency, excellent recyclability and stability has promising application potential for the photocatalytic degradation of organic compounds in wastewater.
研究领域:
材料科学
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环境科学
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化学
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Zishang Tian,Qi Zhao,Xingchen Liu,Yingxiong Wang,Jie Zhao,Yuqi Wang,Xianglin Hou
Aromatic polyimide (PI) is characterized by rigid chains and strong interchain interactions, resulting in poor solubility and non-melting of polymers, so chemical recovery of PI is challenging. Herein, ethylenediamine (EDA) was successfully used for the aminolysis of PI on the surface of flexible printed circuit boards (FPCBs). The PI can be completely degraded at 50 °C for 40 min at a revolution speed of 200 rpm, and the epoxy adhesive and flexible copper clad laminate sheet were separated by simple filtration. The degradation mechanism of PI was proposed and verified by the density functional theory (DFT) method. Intermolecular hydrogen bonding and the vicinal amino moiety of EDA play an important role in activating nucleophiles. DFT calculations show that the formation of the six-membered ring transition state is the rate-determining step during the breaking of the amide bonds. The Gibbs activation energy and the Gibbs reaction energy are 22.90 and 11.73 kcal/mol, respectively. This study provides guidance for the degradation of PI and the recovery of FPCBs.
研究领域:
材料科学
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化学工程
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环境科学
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DOI
高影响因子
RSC Advances
·
2019
·Vol. 9
·期 41
·23545-23553
·
IF 3.049
Jianhui Li,Fan Yang,Quan Zhou,Lijie Wu,Wenying Li,Ruipeng Ren,Yongkang Lv
The ternary magnetic Fe3O4/BiOBr/BiOI (x : 3 : 1) photocatalysts were successfully synthesized by a facile solvothermal method. The samples were characterized by XRD, SEM, EDS, ICP-AES, XPS, UV-vis DRS, PL and VSM. Nitrogen-containing dye RhB was used as a degradation substrate to evaluate the photocatalytic degradation activities of the samples. The photocatalytic performance of Fe3O4/BiOBr/BiOI (0.4 : 3 : 1) is superior to other Fe3O4/BiOBr/BiOI (x : 3 : 1). Compared with binary magnetic Fe3O4/BiOBr (0.5 : 1) prepared in our previous work, the Fe3O4/BiOBr/BiOI (0.4 : 3 : 1) has obvious advantages in photocatalytic activity and adsorption capacity. And the specific surface area (48.30 m2 g−1) is much larger than that of the previous report (Fe3O4/BiOBr/BiOI (0.5 : 2 : 2)) synthesized by a co-precipitation method. Besides, after 25 s of magnetic field, Fe3O4/BiOBr/BiOI (0.4 : 3 : 1) can be rapidly separated from water. After eight recycling cycles, the magnetic properties, photocatalytic activity, crystallization and morphology of the Fe3O4/BiOBr/BiOI (0.4 : 3 : 1) catalyst remain good. The possible photocatalytic degradation mechanism of RhB under Fe3O4/BiOBr/BiOI (0.4 : 3 : 1) photocatalyst was also proposed. The results indicate that the ternary magnetic Fe3O4/BiOBr/BiOI (0.4 : 3 : 1) composite with high photocatalytic degradation efficiency, good magnetic separation performance and excellent recyclability and stability has potential application prospect in wastewater.
研究领域:
环境科学
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材料科学
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化学
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DOI
PubMed
高影响因子
JOURNAL OF THERMAL ANALYSIS AND CALORIMETRY
·
2023
·Vol. 148
·期 10
·4211-4221
·
IF 4.4
Dai Shuming,Song Ping,Jiao Ziyue,Cheng Yi,Shang Jingzhao,Leng Xuefei,Wei Zhiyong,Li Yang
A series of bisphenol A-based polyarylates was synthesized by using 2,2-bis (4-hydroxyphenyl) propane (BPA), terephthaloyl dichloride (TPC), and isophthaloyl dichloride (IPC) as raw materials and p-tert-butylphenol as a capping agent through interfacial polymerization to investigate the effect of end group structure on polymer properties. And the polymer films could be obtained by solvent casting method. The successful introduction of p-tert-butylphenol into the backbone adjusted molecular masses and achieved a regulable improvement of the polymer’s thermal properties. The thermal mass loss 5% temperature of the polymers raised above 470 °C, which indicated the thermal properties were broadly in line with that of the commercial product U-100. Besides, the addition of capping agent also improved the light transmission of the polymers and the transmittance reached above 83% at a wavelength of 450 nm. In addition, the thermal degradation mechanism of polyarylate and U-100 was investigated by simultaneous thermal analysis (STA)-IR and Py/GC–MS. It was discovered that PAR decomposed thermally at their end groups and ester groups first, followed by the breakage of their carbon–carbon bonds, which coincided with U-100’s thermal degradation mechanism. The thermal degradation mechanism of bisphenol A-based polyarylates was proposed. Graphical abstract
研究领域:
高分子科学
·
材料科学
·
热分析
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DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 51
·40726-40736
·
IF 3.84
Zhi Zhu,Ziyang Lu,Xiaoxu Zhao,Yongsheng Yan,Weidong Shi,Dandan Wang,Lili Yang,Xue Lin,Zhoufa Hua,Yang Liu
In the present work, based on Fe3O4/g-C3N4 as the support, 2-mercaptobenzothiazole (MBT) as the template molecule, and pyrrole as the functional monomer, we synthesized magnetic conductive imprinted photocatalysts (MCIPs) that were significantly efficient and stable through a suspension polymerization method. Moreover, the MCIPs not only exhibited a higher photodegradation capacity for MBT under visible light irradiation, but also possessed good selectivity. The specific surface areas of the resultant MCIPs were approximately four times that of pure g-C3N4. Furthermore, the results indicated that h+ was the major reactive species in the photocatalytic reaction system. The photodegradation mechanism was also discussed by analyzing the mass spectrum (MS), and the results demonstrated that MBT was degraded to H2O, CO2 and other small molecules, step by step. In addition, after five cycles, the MCIPs still showed high photocatalytic efficiency, indicating that the as-prepared MCIPs had excellent photochemical stability and good prospects for application in water treatment.
研究领域:
环境科学
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材料科学
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化学
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产品关联
DOI
高影响因子
ENVIRONMENTAL TECHNOLOGY
·
2021
·
IF 3.247
Xiaoman Li,Longsheng Yi,Qinglin Zhu,Lihua Zhao,Yuanhong Xu,Miao Liu,Tao Liu,Qian Wu
In this study, coal fly ash supported MnO2 (CFA@MnO2) was synthesized as heterocatalyst for the activation of peroxymonosulfate to degrade Acid Red 73 (AR73). The synthesized catalyst was characterized by X-Ray Fluorescence Spectrometer (XRF), X-ray powder diffraction (XRD), Scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS) and Brunauer–Emmett–Teller (BET). The composite of CFA@MnO2 possesses a large surface area of 74.59 m2/g. In the catalytic experiment, CFA@MnO2 exhibits excellent catalytic performance with 99.13% AR73 removed within 40 min with a high kinetic rate constant of 0.124 min−1, 5.49 times higher than that of pure MnO2. The operating parameters of CFA@MnO2-based fenton catalytic system were discussed, including MnO2 loading, solution pH, PMS dosage and temperature. The catalyst maintained a relatively high removal rate (>85%) over 5 cycles and degradation intermediates are detected on the catalyst surface after cycled via XPS analysis. The degradation mechanism was investigated by quenching experiments and Electron Paramagnetic Resonance technology. The surface-bound ·OH and SO4·− are considered as the main active radicals in the degradation process. The composite of CFA@MnO2 provides a low-cost and efficient alternative for the catalytic oxidation of organic pollutants.
研究领域:
环境科学
·
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子