CHEMOSPHERE
·
2021
·
IF 7.086
Qing Zhao,Xiao Zhang,Dezhi Huang,Long Chen,Shuxin Li,Jean-Marc Chovelon,Lei Zhou,Guangli Xiu
Cu(II) is generally considered to be a poor activator for PMS decomposition, thus the potential impact of trace Cu(II) on PMS induced oxidation of typical pollutants is always overlooked. In this study, we reported that trace Cu(II) could significantly promote PMS induced degradation of four selected sulfonamide antibiotics (SAs), namely, sulfamehoxazole (SMX), sulfathiazole (STZ), sulfamerazine (SMZ), and sulfamonomethoxine (SMM). Different from conventional PMS-induced oxidation process, high-valent Cu(III) was ascertained as the primary reactive intermediate for SAs degradation, which was confirmed by raman tests and electron paramagnetic resonance (EPR). High concentrations of Cu(II) or PMS were beneficial to degradation of the selected contaminants. In PMS/Cu(II) oxidation system, all the selected SAs could undergo several different degradation pathways including continuous oxidation of aniline group, hydroxylation and S–N bond cleavage. In particular, for six-membered SAs, such as SMZ and SMM, a SO 2 extrusion pathway was also detected. The potential mechanism for Cu(III) formation was also proposed, which was believed to be highly related to the nature of the SAs. Hydroxylamine-SAs (N 4 –OH–SAs), generated from direct PMS oxidation of SAs, was deduced as the “promoter” for the whole oxidation process. And the generation of Cu(III) was likely to proceed through the interaction between PMS and Cu(I), which possibly derived from the reduction of Cu(II) by N 4 –OH–SAs. The results obtained in this study validated the contribution of Cu(III) to the elimination of pollutants and expanded our understanding of the oxidation process of PMS in the presence of trace amounts of Cu(II).
研究领域:
环境化学
·
水处理
·
污染物降解
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
·
2022
·
IF 5.089
Xiao-Chao Chen,Lin Guo,Guang-Hui Shi,Kai-Chun Zhao,Yong Lu,Ye Liu
Carbon dioxide (CO 2 ) was found to serve as a novel and green catalyst for the first time in N -formylation of amines with N, N -dimethylformamide (DMF), wherein only the aliphatic amines were applicable to afford the formamides in the yield of 71∼95%. The isotope labeling experiment with DMF- d 7 indicated that the N -formyl group in the formylated product was originated from DMF rather than CO 2 . The control experiments and the in situ high-pressure FT-IR spectra demonstrated that the formation of the carbamate salt of cyclohexylammonium cyclohexylcarbamate ( A ) derived from the reaction of CO 2 with cyclohexylamine was the driving force for this reaction. Accordingly, the mechanism of CO 2 -catalyed N -formylation of aliphatic amines with DMF was proposed, involving the formation of carbamate salt intermediate with enhanced nucleophilicity in anion in favor of the attack on carbonyl-group of DMF.
研究领域:
有机化学
·
绿色化学
✓ 已验证
DOI
高影响因子
C-Journal of Carbon Research
·
2024
·Vol. 10
·期 3
·62
·
IF 3.9
Xuexin Yuan,Qiqi Zhou,Yu Chen,Hai-Jian Yang,Qingqing Jiang,Juncheng Hu,Cun-Yue Guo
In the present work, inexpensive and commercially available diethyltriamine pentaacetic acid (DTPA) was used as an initiator to catalyze the N-formylation reaction of CO2with amines via the construction of C-N bonds in the presence of xanthone as the photosensitizer and PhSiH3as the reducing agent. After a systematic study of various factors, the optimal conditions for the photocatalytic reaction were obtained: 2.5 mmol of amine, 2.5 mmol of PhSiH3, 10 mol% of DTPA, 20 mol% of xanthone, 1 mL of dimethylsulfoxide (DMSO), atmospheric pressure, and 35 W UV lamp irradiation for 48 h. Under the optimal conditions, the catalyst system afforded high performance for the N-formylation of amines (primary and secondary amines) and CO2, and the yields of the N-formylated products of dialkylamines were above 70%. Further studies exhibit that the catalytic system has a wide scope of substrate applications. For various alicyclic secondary amines, heterocyclic secondary amines, aliphatic primary amines, and aromatic primary amines, the corresponding N-formylation products can be obtained efficiently. In addition, the catalyst can be recycled by simple precipitation and filtration. After five cycles of recycling, there was no significant change in the catalytic and structural properties of DTPA. Finally, a possible reaction mechanism is proposed.
研究领域:
化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Antibiotics-Basel
·
2022
·Vol. 11
·期 1
·51
·
IF 5.222
Xiaoming Su,Hao Lv,Jianyu Gong,Man Zhou
The oxidative mineralization of sulfanilamide drugs (SAs) using micro-size zero-valent iron (mZVI) cooperated with a citric acid buffer solution was evaluated. In this study SM2, SMX, and SD could be removed at 66%, 89%, and 83%, respectively, in a 0.5% Bi/mZVI+CA+NaCA system within 2 h. Based on our analysis, the produced ·OH could be ascribed from the complexation between citrate iron (Fe(II)[Cit]−) and the generated H2O2resulting from the activation of O2on the mZVI surface in the Bi/mZVI+CA+NaCA system, further inducing the mineralization of antibiotics. The related possible degradation pathways were proposed. Two similar degradation pathways of SM2, SMX, and SD in the mixed liquid, including hydroxylation and SO2extrusion, were solved. Meanwhile, there was an additional proposed degradation pathway for SMX to be degraded more effectively, as reflected in the opening of the N-O bond on the benzene ring. Therefore, this work provides an experimental basis and theoretical support for the efficient treatment of antibiotic wastewater in real industry by using an iron-based method.Keywords:sulfanilamide drugs;Bi/mZVI;antibiotic;oxidative degradation
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
·
2022
·
IF 5.089
Yanwei Cao,Dilong Chen,Yaowei Wang,Huibing Shi,Baolin Feng,Chungu Xia,Yuxiao Ding,Lin He
The development of new application scenarios for the red mud, a huge by-product from the aluminum manufacture, has become urgent because of the increasingly stringent demands of environmental protection. Herein, a very simple and sustainable approach to the design of a synergistic catalytic system for the direct oxidative cross-coupling of alcohols and amines to (un)symmetric imines by physically mixing MnO x and red mud is presented. With the catalysis of active red mud, the synthesis of imines over MnO x can achieve an excellent (>98%) yield at 60 °C, air as oxidant for 8 h Without this catalysis, the imine yield reaches only 25%. The red mud clearly assists the reaction, resulting in a 4 ∼ 10-folds higher increase over reactions using only MnO x . From detailed experiments and characterizations, the synergistic effects of the extraordinary performance of this catalytic system were confirmed to be a combination of the reactivity of MnO x in the oxidation of alcohols and the enhancement by the active red mud in the condensation of aldehydes and amines. This work demonstrates a facile strategy for revival of the hazardous red mud. It could turn “waste” into wealth and greatly promote the catalytic applications of red mud.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Food Chemistry-X
·
2024
·
IF 6.5
Qian Han,Min Yang,Zexin Zhang,Xinwen Bai,Xiuying Liu,Zhenhua Qin,Wei Zhang,Pingping Wang,Lijie Zhu,Zaixi Shu,Xuepeng Li
In this study, amine vapor-sensitive films with ratiometric fluorescence attributes were developed. The pH-sensitive fluorescein 8-hydroxypyrene-1,3,6-trisulfonic acid trisodium salt (HPTS) and its tetraphenylethylene derivative (TPB) were selected as ratiometric indicators and incorporated into a polyvinyl alcohol (PVA) matrix to produce HPTS/TPB-PVA films. The films responded well to amine vapors, and the interference of aromatic vapors did not substantially affect the fluorescence signals of the films. Under UV light at a wavelength of 365 nm, the fluorescence of the films changed from dark pink to light pink and finally to yellow when the freshness of the fish was visually checked during storage. In addition, the color difference values of the films showed a positive correlation with the total volatile basic nitrogen (TVB-N), ranging from 12.7 to 24.8 mg/100 g at 25 °C and 8.4 to 25.6 mg/100 g at 4 °C, respectively. This indicates that fluorescent films have good potential for quantifying fish freshness in the near future when connected to an automatic data processing system based on color differences.
研究领域:
食品科学
·
生物传感
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CATALYSIS COMMUNICATIONS
·
2014
·
IF 3.32
Qian Han,Xingquan Xiong,Sizhong Li
An efficient, green and scale-up synthesis of amides from esters and amines has been developed using Ru-MACHO as a readily available catalyst. A diverse range of amides were obtained in moderate to excellent yields (55–98%). Furthermore, when the scale of the amidation reaction was increased to 240.0 mmol, the desired amide still could be obtained in high yield (48.2 g of N -benzylbenzamide, 95%).
研究领域:
有机化学
·
催化化学
✓ 已验证
DOI
高影响因子
Sustainability
·
2023
·Vol. 15
·期 17
·13279
·
IF 3.9
Ke Li,Miaomiao Chen,Lei Chen,Songying Zhao,Wencong Xue,Yanchao Han
In this study, a novel Fe3O4/Ag3PO4/g-C3N4magnetic composite photocatalyst was successfully synthesized, tailored specifically for the visible light-driven photocatalytic degradation of sulfonamide antibiotics, more precisely, sulfamethazine (SMZ). To analyze the fabricated samples, characterization techniques such as X-ray diffraction (XRD), scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FT-IR), photoluminescence spectroscopy (PL), and UV-vis diffuse reflectance spectra (UV-vis) were systematically employed. The composite showcased efficient visible-light absorption and charge separation, with its peak photocatalytic performance recorded at a solution pH value of 6.0. Significantly, the Fe3O4/Ag3PO4/g-C3N4magnetic composite photocatalyst displayed excellent stability and recyclability, consistently maintaining a high degradation efficiency of over 97% even after five consecutive cycles. Further experimentation with radical scavengers confirmed a significant decrease in photocatalytic activity, establishing that superoxide radicals (•O2−) and photo-generated holes (h+) are the primary active species during the degradation of SMZ. Overall, it provides a crucial understanding regarding the photocatalytic decomposition of sulfonamide antibiotics using magnetic composite photocatalysts. It also emphasizes the promising potential of the Fe3O4/Ag3PO4/g-C3N4composite for tangible applications in environmental remediation.Keywords:visible light;photocatalysis;Fe3O4/Ag3PO4/g-C3N4;sulfonamide
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL MONITORING AND ASSESSMENT
·
2024
·Vol. 196
·期 10
·1-16
·
IF 2.9
Xu Xiaojian,Yang Chao,Zou Li,Leng Jun,Wang Ning,Zhang Jing
This work examined the occurrence characteristics and ecological risks of 31 antibiotics across five classes and seven ARGs in the surface waters of Gaoyou Lake. A total of 27 antibiotics, spanning four classes, were detected in the surface waters of Gaoyou Lake, with an overall concentration ranging from 57.5 to 114 ng/L and an average of 78.8 ng/L. Sulfonamide antibiotics exhibited the highest average concentration at 32.7 ng/L. Spatial analysis revealed that antibiotic concentration levels in the western region of the lake were higher than those in other areas. Similarly, ARGs were most abundant in this area, with sulfonamide ARGs demonstrating a notably higher mean abundance than other ARGs. Correlation analysis revealed strong positive associations between sul1 and several antibiotics, including sulfadimidine, sulfamethoxazole, ciprofloxacin, lincomycin, clindamycin, erythromycin, and intl1 ( P < 0.05), with intra-group correlations among sulfonamide ARGs exceeding those between different ARG groups. Ecological risk assessment indicated that erythromycin and sulfamethoxazole presented medium risks, whereas roxithromycin, azithromycin, and lincomycin were associated with low risks to aquatic organisms. The ecological risk proportions across monitoring sites were primarily low (10.6%) and moderate (16.7%), with no high-risk areas identified and 72.7% presenting no risk. The cumulative ecological risk quotient (RQ cum ) suggested a medium-risk level at all surveyed sites.
研究领域:
环境科学
·
微生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL COMMUNICATIONS
·
2011
·Vol. 48
·期 14
·2024-2026
·
IF 5.787
Jian Gao,Qing-Wen Song,Liang-Nian He,Zhen-Zhen Yang,Xiao-Yong Dou
An iron(III)-catalyzed three-component coupling reaction of alkynes, CH2Cl2 and amines was developed for facile synthesis of propargylamines. Preliminary mechanism investigation using in situFT-IR reveals that the crucial Fe-acetylide intermediate could be formed through C–H bond activation of alkynes thanks to cooperative effect of FeCl3 and 1,1,3,3-tetramethylguanidine.
研究领域:
有机化学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Shan Huang,Qicong Song,Weiwei Hu,Bin Yuan,Junwen Liu,Bin Jiang,Wei Li,Caihong Wu,Fan Jiang,Wei Chen,Xinming Wang,Min Shao
Atmospheric amines have attracted increasing attention due to their significant impact on new particle formation, particle hygroscopicity and particle optical properties . In this study, four low-molecule-weight amines were detected from PM 2.5 filter samples collected at an urban site of Pearl River Delta (PRD) region of China in 2018 autumn. During the campaign, the mass concentrations of ambient particulate methylamine (MA, CH 3 NH 2 ), dimethylamine (DMA, (CH 3 ) 2 NH), trimethylamine (TMA, (CH 3 ) 3 N), and diethylamine (DEA, (C 2 H 5 ) 2 NH) were quantified at daily or 12-h resolution using an optimized Ion Chromatograph (IC) method. The total measured amine concentration was 297 ± 209 ng/m 3 , which can account for 0.76 ± 0.33% of PM 2.5 mass concentrations. The particulate amines in PRD urban area were dominated by MA (243 ± 179 ng/m 3 ), accounting for over 80% of total amines, then followed by DMA (49 ± 30 ng/m 3 , 16.5%), TMA (4 ± 2 ng/m 3 ) and DEA (1 ± 1 ng/m 3 ). Based on the correlation analysis, MA and DMA mainly presented as nitrate and sulfate salts. We speculate the amines tend to react with gas-phase HNO 3 or particle-phase nitrate to form particulate amine salts via local process in Guangzhou. As the relative humidity (RH) increased, enhanced partitioning of amine towards the particle phase was observed. Using approach of multiple linear regression, 71% of the particulate amines in PRD urban site could be explained by acid-base process and the rest by primary emissions from combustion sources (29%).
研究领域:
环境科学
·
大气化学
✓ 已验证
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2019
·
IF 5.108
Yiping Tai,Nora Fung-Yee Tam,Weifeng Ruan,Yufen Yang,Yang Yang,Ran Tao,Jingfan Zhang
Wetland plants are proven to perform well in water treatment . However, the phytoremediation capability of wetland plants for antibiotics, especially the uptake and metabolism involved in vivo, is poorly understood. In this study, we investigated the removal, uptake, and specific metabolism by Canna indica and Iris pseudacorus of five sulfonamides (SAs) using hydroponic experiments for seven days. The removal of SAs ranged from 15.2% to 98.4% in the planted groups, whereas that in the unplanted control group was much lower (12.6%–39.9%). The accumulation of SAs in plants was in a concentration-dependent manner via an active process and is not a major removal mechanism (constituted 0.31%–3.62% of the total removal load in plant system). The results also showed differences in the removal and accumulation by plant species of SAs. The acetyl conjugates (N-acetyl SA) were formed, which significantly enhanced the uptake of SAs ( P < 0.001) except sulfapyridine. The concentrations of N-acetyl SA accounted for only 0.4%–23.8% of the total SAs distribution in plants, suggesting the involvement of other metabolism pathways. Methylation and oxidation metabolites were identified in plant tissues and no SA-induced growth stress occurred, revealing that antibiotic metabolism in vivo should be associated with the ability of wetland plants to accumulate antibiotic and tolerate antibiotic stress.
研究领域:
环境科学
·
植物学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）