ACS Applied Materials & Interfaces
·
2024
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IF 8.3
Shengnan Hu,Hanzhu Kong,Yuting Sun,Ronghui Wu,Jing Xu,Ming Guo
Biological enzyme-driven degradation of environmental pollutants has attracted widespread attention because it is ecofriendly and highly efficient. Immobilized enzyme technology has emerged as a promising technique in enzymology that addresses the limitations associated with free enzymes. Traditional solid-loaded enzyme substrates are often affected by blockages and restricted substrate accessibility. In this study, we synthesized an efficient heterogeneous pepsin catalyst, named PEP@M-MIL100(Fe), by covalently combining carboxylated ferrite structural expanded metal–organic frameworks with pepsin. This catalyst demonstrated excellent environmental adaptability and remarkable catalytic degradation capabilities. Notably, it rapidly degraded the persistent microplastic pollutant diisononyl phthalate (DINP) within just 150 min, with a removal efficiency of up to 95.88%. Impressively, even after 10 consecutive uses, the catalyst maintained its high performance. We proposed an innovative steady-state heterogeneous enzyme-catalyzed degradation mechanism, i.e., diffusion (D)–absorption (A)–binding (B)–reaction (R)–degradation (D)–link mechanism, which emphasizes the influence of substrate diffusion rates in this process. This work presents the first successful application of pepsin to DINP degradation and offers a sustainable and effective approach for addressing contemporary pollution challenges.
研究领域:
环境科学
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酶学
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材料科学
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污染控制
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ning Lu,Junzhuo Cai,Baoling Niu,Ye Zhou,Guohua Zhao
Endowing traditional photocatalysis with selectivity for a class of characteristic pollutants is important in environmental science. Using PAEs-TiO 2 as a selective photocatalyst, 302.5 μg L −1 of 11 phthalic esters (PAEs) were preferentially removed to 4.94 μg L −1 in the presence of 10 mg L −1 of natural organic matter via specific hydrogen bonds or cation-π interactions. Further, degradation of PAEs is a lower risk pathway for PAEs-TiO 2 . The in-situ photocatalytic electron paramagnetic resonance initially revealed that PAEs-TiO 2 facilitated the ring opening and mineralization of PAEs, resulting in nearly 100 % detoxification. In actual wastewater, PAEs were not detected after treatment with PAEs-TiO 2 . Further, the energy cost was reduced by 48.1 %, reaching discharge standard. This study offers new sights into selective photocatalysis of a class of pollutants with similar molecular structure.
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
Toxicology Research
·
2022
·Vol. 11
·期 5
·863-871
·
IF 2.68
Xia Ling-Zi,Jiang Ming-Zhe,Liu Li-Lan,Wu Yi,Zhang Yi-Lin,Yang Li-Xia,Shen Xin-Yue,Zhang Qiu-Yu,Lin Min,Gao Hai-Tao
Humans are increasingly exposed to ubiquitous phthalates (PEs), e.g. butyl benzyl phthalate (BBP), dibutyl phthalate (DBP), and di(2-ethylhexyl) phthalate (DEHP), which are widely used plasticizers in polymer products. This study was aimed to investigate the effect of phytochemical quercetin (Que) on hepatotoxicity caused by the mixture of the 3 commonly used PEs (MPEs), and further to explore the underlying mechanism. Forty male Sprague–Dawley rats were randomly divided into control group, MPEs group, and MPEs combined Que at Low-, Median-, and High-dose groups; rats in MPEs group were orally administered with 900 mg/kg/d MPEs, whereas rats in MPEs combined Que groups were simultaneously treated with 900 mg/kg/d MPEs and respectively 10, 30, and 90 mg/kg/d Que. The intervention last 30 days. Compared with control group, serum ALT, AST, LDH and AKP, and hepatic MDA, SOD, CAT and GPx were significantly increased, whereas, serum albumin and total protein were significantly decreased in MPEs group (P < 0.05); hepatic histopathological observation showed numerous inflammatory cells infiltration, hepatocyte ballooning degeneration, and numerous residual erythrocytes in the central vein in MPEs group. Western-blot analysis showed that hepatic Keap1 was downregulated, whereas Nrf2 and HO-1 were upregulated in MPEs group (P < 0.05). However, the alterations of these parameters were alleviated in MPEs combined Que at Median- and High-dose groups. The results indicated that MPEs-induced hepatic oxidative stress, and caused hepatic injuries; whereas, Que inhibited MPEs’ hepatotoxicity, which might relate to Que’s ability of quenching free radicals directly, and restored the regulation of Nrf2 signaling pathway.
研究领域:
毒理学
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药理学
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分子生物学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Yinghua Yan,Yujie Lu,Baichun Wang,Yiqian Gao,Lingling Zhao,Hongze Liang,Dapeng Wu
The development of covalent organic framework (COF)-derived materials with additional functions and applications is highly desired. In this work, a unique COF-functionalized hydrophilic magnetic nanosphere (Fe3O4@PDA@TbBd) with Fe3O4 as a magnetic core, polydopamine (PDA) as a hydrophilic middle layer, and TbBd as an outer COF shell was facilely prepared as a novel hydrophilic platform for efficient detection of phthalic acid esters (PAEs). The resultant Fe3O4@PDA@TbBd nanosphere displayed strong magnetic response, high surface area, and good hydrophilicity. Accordingly, the newly synthesized COF exhibited great potential in phthalate analysis with a wide linearity (50–8000 ng/mL), good recovery (92.3–98.9%), a low limit of detection (0.0025–0.01 ng/mL), and a small relative standard deviation (for intraday less than 4.6% and for interday less than 6.8%). More excitingly, the new COF was applied to analyze nine PAEs in the human plasma sample. This work opens up new avenues for the development and application of functionalized COF-derived materials.
研究领域:
材料科学
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分析化学
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纳米技术
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产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2020
·
IF 5.778
Xiaotong Gu,Ning Qin,Guangfeng Wei,Yiqiong Hu,Ya-nan Zhang,Guohua Zhao
It is stubborn to remove the lowly concentrated phthalic acid esters (PAEs) that usually coexist with other highly concentrated but low-toxic pollutants in municipal sewage. Herein, we report a novel strategy for completely removing the PAEs over a bi-functional {001}TiO 2 surface (with highly exposed {001} facet), which not only serve as functional sites to specifically adsorb the target PAEs pollutants, but also contribute to an enhanced oxidation ability. The adsorption behavior of PAEs on {001}TiO 2 is analyzed deeply through kinetic experiments combining with in situ ATR-FTIR spectroscopy and theoretical calculations. The results reveal that the adsorption capacities of PAEs on {001}TiO 2 are about 4–5 times higher than that on TiO 2 , both of which follow the pseudo-second-order and Langmuir model. This is mainly attributed to the interfacial Lewis Acid-Base Pair between {001} facet Ti 5c sites and C O of PAEs. Benefitting from the specific adsorption capability toward target pollutant and enhanced oxidation ability of {001} facets, nearly 100% of DMP or DEP in simulated wastewater can be eliminated by {001}TiO 2 within 2 h illumination, and the relevant degradation rate constants ( k ) (3.67 h −1 for DMP and 2.19 h −1 for DEP) are 5.73 and 3.08 folds higher than that of pure TiO 2 , respectively. In the application of municipal wastewater , nearly 76% of DMP and 85% DEP can be eliminated by {001}TiO 2 within 2 h illumination, which are nearly 3–6 fold higher than that of pure TiO 2 .
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
Journal of Food Measurement and Characterization
·
2023
·Vol. 17
·期 6
·6168-6179
·
IF 3.4
Xiang Gang,Li Wenzhuo,Nong Qiuxiang,Zhang Cuizhong,Zhang Zhengfa,Lian Huan,Peng Jinyun,Jiang Yufen,Tan Yiqiu,Sun Jing
Conjugated microporous polymers (CMPs) have been widely used in various fields as a new class of porous materials. In this study, a quinoxaline-based CMP (BQP-CMP) was prepared and used as the coating in SPME for the extraction and enrichment of nine phthalate esters (PAEs) in juice, soya sauce, cooking wine, and blended edible oil samples. Several parameters affecting solid-phase microextraction (SPME) were optimized. The feasibility of the developed method was verified using real samples, which showed low LODs (0.014–0.032 µg L −1 ), wide linearities (0.05–50 µg L −1 ), good repeatability (2.8–6.6%), and a long service life. The real liquid samples were successfully analyzed using this proposed method and spiked recoveries of 70.16–96.36% were obtained. Moreover, the interaction model and binding energies between BQP-CMP and the PAEs were explored using molecular docking. Satisfactory extraction efficiency was achieved owing to the high specific surface area (601.62 m 2 g −1 ), high hydrophobicity, and the conjugated planar structural unit distribution of BQP-CMP. This study demonstrates that BQP-CMP is excellent as a rapid and sensitive analysis material for PAEs at trace levels in various types of samples and that CMP materials are also excellent candidates for SPME coatings.
研究领域:
分析化学
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食品科学
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产品关联
DOI
高影响因子
CRYSTAL GROWTH & DESIGN
·
2025
·
IF 3.4
Zhonghua Li,Songgu Wu,Junbo Gong
The influence of halogen-atom substitution for a dimethyl isophthalate compound on the polymorphic behavior and isostructurality property was explored in this paper. Sublimation was demonstrated to exhibit remarkable advantages. Specifically, two polymorphs (Form I and Form II) of dimethyl 5-bromoisophthalate and two polymorphs (Form A and Form B) of dimethyl 5-iodoisophthalate were discovered for the first time. Moreover, the corresponding single crystals suitable for crystal structure determination were also successfully harvested within a few hours. More interestingly, the crystal packing similarities between the stable Form II and metastable Form A were established with the evaluation of quantitative analysis tools. The success in achieving the regulation of luminescence emission with the changes of crystal packing patterns, molecular conformations, and interactions via halogen substitution will provide some inspiration for the development of novel flexible optical solid-state systems in the future.
研究领域:
材料科学
·
晶体学
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Ning Wang,Nan Zhang,Mei-Ling Sun,Yan Sun,Qing-Yu Dong,Yu Wang,Zeng-Tian Gu,Hai-Tao Ding,Qi-Long Qin,Yong Jiang,Xiu-Lan Chen,Yu-Zhong Zhang,Chao Gao,Chun-Yang Li
Phthalate esters (PAEs) are emerging hazardous and toxic chemicals that are extensively used as plasticizers or additives. Diethyl phthalate (DEP) and dimethyl phthalate (DMP), two kinds of PAEs, have been listed as the priority pollutants by many countries. PAE hydrolases are the most effective enzymes in PAE degradation, among which family IV esterases are predominate. However, only a few PAE hydrolases have been characterized, and as far as we know, no crystal structure of any PAE hydrolases of the family IV esterases is available to date. HylD1 is a PAE hydrolase of the family IV esterases, which can degrade DMP and DEP. Here, the recombinant HylD1 was characterized. HylD1 maintained a dimer in solution, and functioned under a relatively wide pH range. The crystal structures of HylD1 and its complex with monoethyl phthalate were solved. Residues involved in substrate binding were identified. The catalytic mechanism of HylD1 mediated by the catalytic triad Ser140-Asp231-His261 was further proposed. The hylD1 gene is widely distributed in different environments, suggesting its important role in PAEs degradation. This study provides a better understanding of PAEs hydrolysis , and lays out favorable bases for the rational design of highly-efficient PAEs degradation enzymes for industrial applications in future.
研究领域:
环境科学
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生物化学
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酶学
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结构生物学
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2019
·
IF 7.149
Wei Guo,Jian Han,Shengmin Wu,Xiongjie Shi,Qiangwei Wang,Bingsheng Zhou
Bis(2-ethylhexyl)-2,3,4,5-tetrabromophthalate (TBPH) is a ubiquitous environmental contaminant, but its toxicity is not fully understood. Accordingly, we investigated the effects of TBPH and its metabolite, mono-(2-ethyhexyl)tetrabromophthalate (TBMEHP), on lipid metabolism using a zebrafish model. The molecular docking study revealed that TBPH and TBMEHP bind to zebrafish peroxisome proliferator-activated receptor γ (PPARγ), with binding energies similar to rosiglitazone, a PPARγ agonist. Zebrafish embryos 0.75 hpf were exposed to TBPH (0.2–2000 nM) or TBMEHP (0.2–2000 nM) until 72 hpf, and their effects on PPARγ-mediated lipid metabolism were evaluated. Significant regional DNA demethylation of the PPARγ promoter was observed in the larvae at 72 hpf. Demethylation of the PPARγ promoter accompanied by upregulation of tet1 and tet2 transcription caused upregulation of PPARγ transcription and certain downstream genes involved in lipid lipolysis, transport, and metabolism. The triglyceride and total cholesterol concentrations in the larvae were significantly reduced following exposure to TBPH or TBMEHP. Furthermore, significant increases in the whole ATP content and locomotor activity in the 120 hpf larvae were observed. The overall results suggest that both TBPH and TBMEHP affect methylation of the PPARγ promoter, subsequently influencing larvae lipid metabolism via the PPARγ signaling pathway and disrupting energy homeostasis.
研究领域:
环境毒理学
·
分子生物学
·
发育生物学
·
表观遗传学
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产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2024
·
IF 11.4
Huan-yu Tao,Jianghong Shi,Jiawei Zhang,Hui Ge,Xiaowei Liu,Xiao-yan Li
The city-river-reservoir system is an important system for safeguarding drinking water. Phthalic acid esters (PAEs) are emerging contaminants in drinking water sources that are gaining attention, and they could pose risks to human health and aquatic organisms. In this study, field studies that lasted four years were conducted to analyze the concentrations, spatial-temporal distribution, and removal effects of six PAEs. The total concentrations of the Σ6PAEs in the water and sediment samples were 0.2–7.4 μg L −1 (mean: 1.3 μg L −1 ) and 9.2–9594.1 ng g −1 (mean: 847.5 ng g −1 ), respectively. Di-n-butyl phthalate (DBP) and, bis(2-ethylhexyl) phthalate (DEHP) were the predominant congeners, accounting for 57.2 % in the water samples and 94.1 % in the sediment samples. The urban area contributed 72 % of the PAEs in the system. A significant removal effect of PAEs was observed in the wetland, with a removal rate of 40.2 %. The partitioning of PAEs between the water and sediment was attributed to the removal of dimethyl phthalate and diethyl phthalate that occurred during the water phase, while the removal of DBP and DEHP primarily occurred during the sediment phase. The ecological risk calculation based on the sensitivity distribution model indicated that DBP (HQ water = 0.19, HQ sediment = 0.46) and DEHP (HQ water = 0.20, HQ sediment = 0.13) possessed moderate risks according to some water and sediment samples. The ecological projects were verified to be effective engineering strategies to reduce ecological risk in the drinking water source.
研究领域:
环境科学
·
生态学
·
公共卫生
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产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Qingfeng Dong,Yaqi Dai,Weiting Wang,Yanli Ma,Li Li
In this research, the carvacrol (CAR) loaded cellulose acetate phthalate (CAP) /shellac (SH) films were prepared via electrostatic repulsion strategy and casting method. The CAP/SH-CAR films demonstrated excellent tensile strength , while also exhibiting good UV light barrier and thermal stability . The results showed that the addition of CAR significantly improved the barrier of the CAP film to water vapor and oxygen permeability. When the addition amount of CAR was 0.9 % (w/w) with respect to CAP content, the CAP/SH-CAR films exhibited good antibacterial activity and effectively reduced the growth of S. aureus and E. coli by approximately 47.9 % and 50.9 %, respectively. The presence of SH improved the retention rate of CAR in CAP/SH-CAR films, with the retention rate ranging from 45.2 to 56.8 %. Finally, the CAP/SH-CAR films were applied to preserve the mackerel fillets, indicating that the rate of freshness deterioration had been delayed and showing a good freshness preservation effect. Therefore, the CAP/SH-CAR films have the potential to be used as food packaging materials.
研究领域:
食品科学
·
材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Peng Zhou,Xiaowei Huo,Jing Zhang,Yang Liu,Feng Cheng,Xin Cheng,Yunqi Wang,Yongli Zhang
Hydroxylated fullerene (fullerenol) has gained increasing attention in the field of water environment remediation based on its intrinsic properties of photosensitivity and high water solubility. In this work, C 60 fullerenol was added to the Fe(III)/PMS process to enhance diethyl phthalate (DEP) degradation both with and without visible light. The DEP removal ratio was increased from 2.2% to 58.8% with the addition of fullerenol at 60 min in dark condition, and the removal of DEP was completely achieved within 50 min under visible light irradiation. Mechanism investigation shows that carboxyl and carbonyl were formed via keto-enol isomerization at acid condition, resulting in the formation of open-cage fullerenol. The open-cage fullerenol can act as complex agent and electron donor to enhance oxidizing capability of the Fe(III)/PMS process by promoting Fe(III)/Fe(II) cycles. Competitive radical capture tests by electron spin resonance (ESR) and radical quenching analysis demonstrate that hydroxyl radical and sulfate radical were primarily responsible for DEP removal, but not superoxide radical and singlet oxygen. The DEP removal in the F/Fe(III)/PMS process is more efficiency at initial pH ranging from 2.1 to 4.9. Moreover, the DEP degradation route was proposed involving the generation of various intermediary products. This study provides a novel method for the application of fullerene derivatives on environment remediation by combining with metal catalyzed advanced oxidation processes.
研究领域:
环境科学
·
化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）