CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ronghao Wu,Qu Zhang,Chao Xue,Zuliang Chen
17beta-estradiol (E2) is classified as an endocrine disruptor and it poses a significant threat to the environment. Despite our previous work on the preparation of green-reduced graphene immobilized Ochrobactrum sp. FJ1(FJ1@rGO) to achieve high efficiency in removing E2, the functions of strain FJ1 and rGO, as well as their removal mechanism of E2, remain not well understood. In this study, FJ1@rGO was used to remove E2 to comprehend the removal mechanism where efficiency was found to be 93.74% after 10 days of removal compared to only rGO (43.82%). This indicated that E2 degradation was based on the integration of adsorption using rGO and biodegradation through strain FJ1, as evidenced by HPLC-UV. Additionally, results confirmed that the E2 removal process by FJ1@rGO conforms to first-order degradation kinetics and pseudo-second-order kinetics, further demonstrating the synergistic effect of physical adsorption and biodegradation. LC-Q/TOF-MS analysis identified the primary degradation products as estrone (E1), 4-OH-E1, and catechol. Combining characterization analysis, rGO facilitates the transfer of electrons between cells and E2, improving the strain's tolerance of environmental changes. Finally, the assessment of various wastewaters showed that the removal efficiency was 99.76%, 96.89%, and 78.09%, respectively. Overall, the mechanism by FJ1@rGO to remove E2 was proposed here, providing new insights into green and sustainable technology for treating E2 in wastewater.
研究领域:
环境科学
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微生物学
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产品关联
DOI
高影响因子
AAPS PHARMSCITECH
·
2017
·Vol. 18
·期 8
·2889-2897
·
IF 2.451
Xiong Hui,Fu Jinping,Sun Hanjing,Wang Enfu,Ding Yunhui,Ren Guobin,Jing Qiufang,Ren Fuzheng
Micro-particles of 17β-estradiol (ED) were prepared with polyvinylpyrrolidone (PVP) by in situ pH-dependent solubility technique. Products were characterized using multiple instruments, and molecular interactions between ED and PVP were explored. Powder X-ray diffraction and thermal analysis revealed crystalline ED in the micro-particles is hemihydrated. PVP was also present in the micro-particles. Laser particle size analysis and scanning electron microscopy revealed thin slice morphology, which might have resulted from the influence of PVP. Moreover, the results of contact angle, specific surface area, and dynamic vapor sorption showed that the surface properties of products were improved. These physicochemical properties of the micro-particles resulted in an obvious improvement in dissolution rate. Fourier transform infrared spectroscopy and 1 H nuclear magnetic resonance revealed hydrogen bonding between ED and PVP. A method was established for the preparation of micro-particles through the addition of PVP during the reaction process.
研究领域:
药剂学
·
物理化学
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DOI
高影响因子
ENVIRONMENTAL POLLUTION
·
2020
·
IF 6.793
Kai Sun,Xing Cheng,Jialin Yu,Luojian Chen,Jiajun Wei,Wenjun Chen,Jun Wang,Shunyao Li,Qingzhu Liu,Youbin Si
Estrogens, which are extensive in the eco-environments, are a category of high-toxic emerging contaminants that induce metabolic disorders and even carcinogenic risks in wildlife and humans. Here we investigate whether fungus-secreted laccase can be used as a green catalyst to eliminate a representative estrogen, 17 β -estradiol (E2). A white-rot fungus Trametes hirsuta La-7 with high laccase-productivity, was isolated from pig manure-contaminated soil. Extracellular laccase activity expressed by strain La-7 was 65.4 U·mL −1 for a 3 d inoculation under the optimal fermentation parameters. The concentrated-crude laccase from Trametes hirsuta La-7 (CC- Th Lac) was capable of effectively metabolizing E2 at pH 4–6, and the apparent pseudo first-order reaction rate constant and half-life values were respectively 0.027–0.055 min −1 and 25.86–12.67 min ( R 2 > 0.98). The mass measurement of high-resolution mass spectrometry in combination with 13 C-isotope labeling identified that the main by-products of E2 metabolism were dimers, trimers , and tetramers, which are consistent with radical-driven C–C and/or C–O–C covalent coupling pathway, involving the initial enzymatic production of phenoxy radical intermediates and then the successive oxidative-oligomerization of radical intermediates. The formation of oligomers dramatically reduced the estrogenic activity of E2. Additionally, CC- Th Lac also exhibited high-efficiency metabolism capability toward E2 in the natural water and pig manure, with more than 94.4% and 91.0% of E2 having been metabolized, respectively. These findings provide a broad prospect for the clean biotechnological applications of Trametes hirsuta La-7 in estrogen-contaminated ecosystems.
研究领域:
环境生物学
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生物化学
·
生态学
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DOI
PubMed
高影响因子
Environmental Science-Processes & Impacts
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2019
·Vol. 22
·期 1
·197-206
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IF 2.688
Changwei Li,Xianwang Kong,Lihua Lan,Musa Abubakar Tadda,Dezhao Liu
17β-estradiol (E2) ubiquitously exists in various water bodies with long-term endocrine-disrupting and carcinogenic impacts on wildlife even at the trace level of ng L−1. However, it remains unclear how easy-to-degrade carbon sources alter E2 biodegradation patterns. In this study, E2 biodegradation by Sphingomonas sp. MCCC 1A06484 was investigated with regard to alternative carbon sources. Results showed that the bacterium preferentially utilized glucose, sodium succinate and sodium acetate over E2. Interestingly, the presence of these preferred nutrients increased the E2 removal efficiency by 20.1%. Furthermore, a positive relation (p < 0.05) between the utilization of total organic carbon (TOC) and E2 was found. Using intracellular metabolomics by UHPLC-QTOF-MS, 11 up-regulated and 35 down-regulated metabolites (variable importance > 1, p < 0.05) were identified in the bacterium when cultivated with E2 under various carbon and nitrogen backgrounds. The E2 exposure contributed to metabolism changes of lipid, nucleotide, carbohydrate, amino acid and membrane transport, which were considered to play roles in the E2 metabolism. The up-regulated phosphatidylcholine might act as an indicator during the bacterial degradation of E2. Generally, this study contributes to an in-depth understanding of E2 biodegradation in complex environments with multiple carbon and nitrogen sources.
研究领域:
环境科学
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微生物学
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DOI
PubMed
高影响因子
Science of Advanced Materials
·
2019
·Vol. 11
·期 1
·105-111
·
IF 1.158
Di Huang,Long Yanju,Luo Lijun,Li Lingxin,Zhang Sifeng,Wang Lulu,Jiang Fengzhi
N-doped Bi2O3 with hierarchical structure was synthesized using precipitation/calcination method. In this method, ethylenediamine was used as both the nitrogen source and morphology controller besides the P123 triblock copolymer as main structure directing agent,
to control the texture and morphology of the catalyst. The microstructure and chemical composition of N-doped Bi2O3 photocatalyst were characterized with XRD, XPS, SEM-EDS, DR UV-vis, and N2 physisorption. The prepared hierarchical N-doped Bi2O3
was used for the photocatalytic degradation of 17β-estradiol (E2) under visible light. The absorption edge of prepared N doped Bi2O3 appeared an obvious red shift comparing with pure phase Bi2O3. This would help photocatalyst make full
use of light source to degrade E2. Under the same conditions of the photocatalytic reaction, the rate constant of degradation of E2 over N-doped Bi2O3 was 6.3 times of that obtained over Bi2O3. The stability of N-doped Bi2O3
and the mechanism of the photocatalytic degradation of E2 under visible light were studied.
研究领域:
环境科学
·
材料科学
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DOI
高影响因子
CHEMOSPHERE
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2017
·
IF 4.208
Cong Li,Feilong Dong,John C. Crittenden,Feng Luo,Xinbo Chen,Taotao Zhao
The kinetics and mechanisms of 17β-estradiol (E2) chlorination in water distribution systems (WDS) were studied. We examined the impacts of different factors, including pH, temperature, humic acid concentration and type, and flow velocity. The experimental results showed that the rate constants in beaker tests and WDS were described by a pseudo-first-order model. pH had the greatest impact on E2 chlorination in the beaker tests. However, temperature had the greatest impact on E2 chlorination in WDS. Mechanistic analysis of E2 chlorination showed that chlorine attacked E2 in three stages: 1) halogenation of the aromatic ring, 2) cleavage of the benzene moiety and chlorine or bromine substitution formation, and 3) formation of trihalomethanes (THMs) and halogenated acetic acids (HAAs) from phenolic intermediates through benzene ring opening with chlorine and/or bromine substitution of hydrogen on the carbon atoms. In the third stage, the concentrations of THMs and HAAs increased rapidly.
研究领域:
环境科学
·
生物学
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DOI
PubMed
高影响因子
ENVIRONMENT INTERNATIONAL
·
2024
·
IF 10.3
Xuemin Qi,Ziyan Niu,Shenghua Xiao,Michael Gatheru Waigi,Hui Lin,Kai Sun
Global-scale crop contamination with environmental estrogens has posed a huge risk to agri-food safety and human health. Laccase is regarded as an unexceptionable biocatalyst for regulating pollution and expediting humification, but the knowledge of estrogen bioremediation and C storage strengthened by laccase-driven rhizosphere humification (LDRH) remains largely unknown. Herein, a greenhouse microcosm was performed to explore the migration and fate of 17 β -estradiol (E2) in water-wheat ( Triticum aestivum L.) matrices by LDRH. Compared to the non-added laccase, the pseudo-first-order decay rate constants of E2 in the rhizosphere solution after 10 and 50 μM exposures by LDRH increased from 0.03 and 0.02 h −1 to 0.36 and 0.09 h −1 , respectively. Furthermore, LDRH conferred higher yield, polymerizability, O-containing groups, and functional-C signals in the humified precipitates, because it accelerated the formation of highly complex precipitates by radical-controlled continuous polymerization. In particular, not only did LDRH mitigate the phytotoxicity of E2, but it also diminished the metabolic load of E2 in wheat tissues. This was attributed to the rapid attenuation of E2 in the rhizosphere solution during LDRH, which limited E2 uptake and accumulation in each subcellular fraction of the wheat roots and shoots. Although several typical intermediate products such as estrone, estriol, and E2 oligomers were detected in roots, only small-molecule species were found in shoots, evidencing that the polymeric products of E2 were unable to be translocated acropetally due to the vast hydrophobicity and biounavailability. For the first time, our study highlights a novel, eco-friendly, and sustainable candidate for increasing the low-C treatment of organics in rhizosphere microenvironments and alleviating the potential risks of estrogenic contaminants in agroenvironments.
研究领域:
环境科学
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植物学
·
土壤生物学
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DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Weiwei Yu,Shuo Yang,Banghao Du,Zhi Zhang,Mingyuan Xie,Yao Chen,Chenju Zhao,Xiangyu Chen,Qi Li
17β-Estradiol (17β-E2) as a non-conventional pollutant with high damage, the effective removal of 17β-E2 had been studied wildly. In recent years, nano materials application enabled the rapid removal of 17β-E2. Nano zero valent iron (nZVI) as one of the most widely used nano materials could also be used to degrade 17β-E2. But, the degradation performance of nZVI was limited by oxidation and aggregation. Therefore, this study explored the degradation mechanisms of 17β-E2 by nZVI and the enhancement mechanisms of nZVI by citrate. Firstly, 17β-E2 could be effectively degraded under acidic conditions without the addition of citrate. Citrate had protective effect on nZVI, so the degradation efficiency in neutral condition and degradation rate at all pH values of 17β-E2 were enhanced greatly in nZVI-citrate system. 17β-E2 degradation was mainly about group change and cleavage of ring A, as well as dominated by O 2 − ▪ and O H ∙ in the absence and presence of citrate. The formation of dimers and trimers proved the existence of laccase-like reaction during the 17β-E2 degradation process by nZVI. In nZVI-citrate system, the laccase-like reaction was replaced by specific cross-coupling of 17β-E2, E1, and citrate. Overall, the study proved that citrate could enhance the degradation of 17β-E2 by nZVI.
研究领域:
环境科学
·
生物化学
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DOI
高影响因子
ENVIRONMENTAL POLLUTION
·
2018
·
IF 4.358
Siyuan Wang,Xinghao Wang,Chenguang Li,Xinxin Xu,Zhongbo Wei,Zunyao Wang,Ruijuan Qu
This paper evaluates the UV photodegradation of 17β-estradiol (E2) on silica gel and in natural soil with different soil components. Silica gel was chosen as a stable and pure support to simulate the photochemical behavior of E2 on the surface of natural soil. Ultraviolet light, rather than visible light, was confirmed to play a decisive role in the photodegradation of E2 on silica gel. The effect of three soil components, including humic acid (HA), inorganic salts, and relative humidity (RH), on the photochemical behavior of E2 on silica gel or soil under UV irradiation was then evaluated. Two HA concentrations (10 and 20 mg g −1 ) and three salts (ferric sulfate, copper sulfate and sodium carbonate) were observed to obviously inhibit the degradation of E2 on silica gel. Interestingly, nitrate was found to obviously improve the removal efficiency of E2. Both too-dry and too-wet conditions obviously reduced the removal rate of E2, and the optimum relative humidity (RH) value was found to be approximately about 35% (30 °C). Furthermore, twenty intermediate products and two major pathways were proposed to describe the transformation processes of E2 treated by UV irradiation, among which oligomers were found to be the major intermediate products before complete mineralization. The efficient UV removal of E2 on silica gel and natural soil suggested a feasible strategy to remediate E2 contaminated soil.
研究领域:
环境科学
·
毒理学
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DOI
PubMed
高影响因子
ANALYTICA CHIMICA ACTA
·
2024
·
IF 5.7
Wenrui Hu,Hang Ao,Ziyi Lv,Wencheng Xiao,Wei Li,Jianping Lei,Jie Wu,Huangxian Ju
Background Chemiluminescence (CL) bioassay is one of the most advanced and used detection method in clinical diagnosis and biomedical research because of the advantages of low background, easy operation, and wide-field imaging without a light source or microscope. The luminol/hydrogen peroxide/horseradish peroxidase (luminol/H 2 O 2 /HRP) system is the most popular CL system, but its application in high-throughput imaging detection is challenged due to its low luminescence efficiency and flash-type emission which is difficult in ensuring the reproducibility and consistency of detection results. Results We reported a glow-type CL system of luminol@CD/H 2 O 2 /HRP by using a supramolecular enhancer of cyclodextrin (CD). This luminol@CD/H 2 O 2 /HRP system exhibited a luminescence lifetime of 41 min for sensitive and accurate imaging analysis. The long-lasting CL emission was attributed to the formation of a 1:1 host–guest complex between luminol and CD, which could stabilize the emitter and effectively reduce nonradiative relaxation. The formation of luminol@CD complex was determined through NMR experiments and theoretical analysis. Under optimum conditions, the luminol@CD/H 2 O 2 /HRP system showed higher sensitivity and much better precision than classical luminol/H 2 O 2 /HRP system for imaging detection of HRP. Especially, this glow-type luminol@CD/H 2 O 2 /HRP system realized CL imaging of microwell arrays on microfluidic chips. In addition, the luminol@CD/H 2 O 2 /HRP system was successfully applied for point-of-care detection of 17 β- estradiol based on a competitive mechanism of host–guest recognition. Significance An efficient CL system is crucial for obtaining reproducible and consistent results for accurate detection. Our luminol@CD/H 2 O 2 /HRP system emitted strong and persistent luminescence, resulting in reliability and efficiency at both CL macroscopic and microscopic imaging detection. We expected the luminol@CD/H 2 O 2 /HRP CL system to be applied in various detection fields.
研究领域:
分析化学
·
生物医学工程
·
临床诊断
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHROMATOGRAPHY B-ANALYTICAL TECHNOLOGIES IN THE BIOMEDICAL AND LIFE SCIENCES
·
2024
·
IF 2.8
Jun Zhang,Ze-hua Liu,Ke-meng Zhao,Zhi Dang,Yun Liu,Yu Liu
This work for the first time reported the complete transformation of 17β-estradiol (E2) to estrone (E1) by unknown wild-type enzyme present in the widely used commercial arylsulfatase derived from Helix pomatia . It was found that acetate could effectively inhibit the unknown enzyme with a half inhibitory concentration (IC 50 ) of 140.9 μM, while phosphate and citrate showed no inhibition. Since the buffer solutions with phosphate and citrate have been used in the enzymatic hydrolysis of natural estrogen conjugates for decades, the transformation of E2 to E1 likely occurred during such procedure, inevitably leading to overestimated E1, but underestimated E2. It was further suggested that acetate should be used to prevent this undesirable transformation during the enzymatic hydrolysis of natural estrogen conjugates.
研究领域:
生物化学
·
环境科学
·
医学
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产品关联
DOI
PubMed
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2025
·
IF 4.6
Yinjia Zhao,Xufang Hu,Chengyu Li,Jing Hu,Tianran Yuan,Yanxiong Liu,Qiue Cao,Shiyu Feng,Liyan Zheng
17β-estradiol (E2) is a crucial estrogen that significantly influences reproductive biological processes and the development of associated diseases, highlighting the need for effective detection methods. Here, we propose a magnetic hierarchical porous material (Mag MOF@COF-Apt) through the in situ growth of a TAPB-DMTP-COF layer on a magnetic Fe-MOF core for the selective recognition and surface-enhanced Raman scattering (SERS) analysis of E2. The Mag MOF@COF-Apt features the inherent SERS-enhancing properties of Mag MOFs. Furthermore, the COF layer establishes a gap between E2 and the Mag MOF, enhancing SERS activity through the on-shell-isolated effect. Additionally, the topological structure of the COF on the MOF provides a high surface area platform for more affinity sites, and its expanded porous structure facilitates size-exclusion of interferents. Finally, E2 aptamer functionalization equips this heterojunction with the capability for the selective capture of E2. Through these multiple synergistic effects, the Mag MOF@COF-Apt assisted E2 profiling features good sensitivity (detection limit of 110.14 nmol L −1 ), strong tolerance to protein (40 mg mL −1 BSA, 40 mg mL −1 HSA) and salt (40 mg mL −1 NaCl) interference, high signal reproducibility (RSD = 7.29 %) and reusability over four cycles. The effectiveness of Mag MOF@COF-Apt based profiling was validated by successful E2 detection in human serum. This work is anticipated to advance MOF/COF hybrid substrates for SERS, providing an effective tool for E2 analysis.
研究领域:
分析化学
·
生物医学工程
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）