ADVANCED FUNCTIONAL MATERIALS
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2026
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IF 19.9
Yifan Lai,Xuejiao J. Gao,Zhenxiang Li,Yuxin Wan,Ning Yue,Weili Zhang,Xin Zhao,Rongxin Su,Xing Lu,Jiangjiexing Wu
Achieving enzyme-like substrate selectivity in nanozymes remains a critical challenge that restricts their analytical reliability in practical sensing. Inspired by the nanoconfined active pockets of metalloenzymes, we engineered amino acid-modulated MIL-101(Fe) nanozymes to tailor substrate discrimination and elucidate the distinct regulatory roles of individual amino acids. Among the four amino acids investigated (cysteine (Cys), histidine (His), aspartic acid (Asp), and proline (Pro)), Cys-MIL-101(Fe) introduces the most pronounced spatial gating effect by refining pore microenvironments, thereby achieving substantially enhanced substrate selectivity despite reduced catalytic activity. In contrast, His modification affords the highest catalytic activity but only moderate discrimination capability, while Asp and Pro cause limited modulation. Further sensing results demonstrate that Cys-MIL-101(Fe) affords up to a tenfold improvement in pesticide differentiation relative to the pristine MOF, whereas the His-modified analogue provides only a fivefold enhancement. These results reveal that different amino acids exert distinct influences on the activity-selectivity balance of nanozymes and show that, in multi-target analytic discrimination, selectivity can provide an additional and sometimes dominant contribution to sensing performance. This work establishes a new paradigm for selectivity-oriented nanozyme engineering, demonstrating that sacrificing activity can, counterintuitively, improve analytical precision.
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Sustainable Chemistry and Pharmacy
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2026
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IF 6.7
Xuehui Chen,Xianzhao Zhang,Fengmao Liu,Yufei Dong
The integration of hydrochar with advanced oxidation processes (AOPs) offers a green and efficient approach to water pollutant treatment. However, the real-world use of hydrochar is obstructed by the stringent preparation conditions typically required. This study introduces acidic deep eutectic solvents (DES) to replace water, enabling atmospheric-pressure hydrochar conversion at 150°C and overcoming the high temperature/pressure limitations of conventional hydrothermal carbonization (HTC), while also providing effective active sites for hydrochar-activated AOPs. Hydrochar was prepared from corn stover at atmospheric pressure and 150°C. For an aqueous fomesafen solution with a starting concentration of 40 mg/L, 0.3 g/L hydrochar catalyzed 5 mmol/L sodium persulfate, achieving a degradation and removal rate exceeding 80% in 100 min. The acidity of DES was found to positively correlate with the catalytic performance of the prepared hydrochar. In addition, key factors influencing the performance of hydrochar-based AOPs were investigated. Potential degradation mechanisms were also proposed.
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ENVIRONMENTAL POLLUTION
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2023
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IF 8.9
Guoqiang Zhao,Jing Zhou,Yanning Tian,Qifeng Chen,Dongmei Mao,Jianchun Zhu,Xing Huang
Fomesafen is a diphenyl ether herbicide used to control the growth of broadleaf weeds in bean fields. The persistence, phytotoxicity, and negative impact on crop rotation associated with this herbicide have led to an increasing concern about the buildup of fomesafen residues in agricultural soils . The exigent matter of treatment and remediation of soils contaminated with fomesafen has surfaced. Nevertheless, the degradation pathway of fomesafen in soil remains nebulous. In this study, Bacillus sp. Za was utilized to degrade fomesafen residues in black and yellow brown soils. Fomesafen's degradation rate by strain Za in black soil reached 74.4%, and in yellow brown soil was 69.2% within 30 days. Twelve intermediate metabolites of fomesafen were identified in different soils, with nine metabolites present in black soil and eight found in yellow brown soil. Subsequently, the degradation pathway of fomesafen within these two soils was inferred. The dynamic change process of soil bacterial community structure in the degradation of fomesafen by strain Za was analyzed. The results showed that strain Za potentially facilitate the restoration of bacterial community diversity and richness in soil samples treated with fomesafen, and there were significant differences in species composition at phylum and genus levels between these two soils. However, both soils shared a dominant phylum and genus, Actinobacteriota, Proteoobacteria, Firmicutes and Chloroflexi dominated in two soils, with a high relative abundance of Sphingomonas and Bacillus . Moreover, an intermediate metabolite acetaminophen degrading bacterium, designated as Pseudomonas sp. YXA-1, was isolated from yellow brown soil. When strain YXA-1 was employed in tandem with strain Za to remediate fomesafen contaminated soil, the degradation rate of fomesafen markedly increased. Overall, this study furnishes crucial insights into the degradation pathway of fomesafen in soil, and presents bacterial strain resources potentially beneficial for soil remediation in circumstances of fomesafen contamination.
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FOOD CHEMISTRY
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2023
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IF 8.8
Ning Yue,Jiangjiexing Wu,Wei Qi,Rongxin Su
Despite the potential of nanozymes combined with sensor arrays for discriminating multiple pesticides simultaneously, they have few practical pesticide sensing uses due to the limited performance of existing nanozymes and the complexity of their preparation. Here, agricultural waste is utilized for the facile synthesis of high-performance biochar nanozymes and the fabrication of biochar nanozyme sensor arrays. The production of autogenous N-doped biochars with abundant surface functional groups and good peroxidase-like activities is achieved with different types of algae. High-performance biochar nanozyme sensor arrays can discriminate pesticides in a concentration range from 1 to 500 μM and in real samples from soil, lake water, seawater, apples, cucumbers, peaches, tomatoes and cabbages. Furthermore, pesticides can be quantified down to 1 μM. The development of high-performance nanozyme sensor arrays based on waste conversion could be a step toward pesticide discrimination and detection, which would improve human and environmental safety.
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JOURNAL OF MOLECULAR STRUCTURE
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2019
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IF 2.12
Xue Dong,Leng Wang,Ruirui Feng,Zhaoyang Ren,Li Zhang,Huizhe Lu
The long residual period and toxicity of fomesafen makes it accumulating in the environment as environmental pollutant . Bovine serum albumin (BSA) plays an indispensable role in the binding, trans -mission, distribution and efficacy of fomesafen in vivo . Thereby, we studied the interaction of fomesafen and BSA by spectroscopic methods and molecular simulation. Spectroscopic measurements reveal that static quenching is the predominant quenching mechanism, resulting in the forming of BSA-fomesafen. The thermodynamic results manifest that hydrophobic force is the major factor. We have found an active pocket around Trp-213 based on competitive binding of fomesafen and warfarin. The model optimized by MD is the ultimately identified model reflecting real situation, from which we can find that the interactions of BSA-fomesafen depend mainly on the contribution of hydrophobic residues. Compared with the models before and after MD, we have found that aqueous solution is an indispensable condition for the emergence of significant hydrophobic interaction in this system. The free energy and energy decomposition measured by the MD simulations indicate that the interaction is spontaneous and Trp-213 has great contributions to the formation of BSA-fomesafen system. In summary, our results have pro-vided meaningful reference to assess the biological toxicity risk of fomesafen.
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INTERNATIONAL JOURNAL OF ENVIRONMENTAL ANALYTICAL CHEMISTRY
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2018
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IF 1.372
Yanfang Zhao,Lubin Xu
In this work, a low-cost melamine-formaldehyde polymer with large-surface-area mesoporous structure was prepared and applied as an efficient solid sorbent for pre-concentration of five kinds of chlorinated herbicides including fomesafen, atrazine, pyrithiobac-sodium, benazolin and acifluorfene from water samples. Extraction parameters such as pH of the sample solution, amount of mesoporous melamine-formaldehyde polymer (mMFP), extraction time, type of desorption solv-ent and volume of the sample were systematically investigated. Combining dispersive solid-phase extraction with high-performance liquid chromatography (HPLC), the detection limits (S/N = 3) of the five herbicides were ranged from 0.04 to 0.18 μg L−1 with good linearity (R2 ≥ 0.9908). Then the tap water and river water samples were analysed by the developed method, and the obtained results indicated that this method provides acceptable recoveries and precisions. mMFP can be prepared through one-pot catalyst-free polymerisation from low-cost starting materials, so that they could be easily scaled up for the sample pre-treatment and have the powerful potentiality in purification of contaminated water.
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Frontiers in Environmental Science
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2024
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IF 3.3
Ma Rong,Yu Shuangshuang,Li Yafang,Lin Yan,Ma Xiaodong
Background: With the growing use of nitrogen-containing pesticides in agriculture, their residues in the environment have raised significant public health concerns.Objective: This study aimed to develop a novel PPy-DBSA/IT-SPME coating to enhance the detection efficiency of polar nitrogen-containing pesticides in water matrices.Methods: The preparation conditions were optimized, including pyrrole concentration at 7.0 mol/L, DBSA concentration at 0.014 mol/L, oxidant concentration at 0.35 mol/L, and a coating cycle repeated 10 times. High-performance liquid chromatography-tandem mass spectrometry (HPLC-MS/MS) was employed for detection.Results: The novel coating effectively adsorbed 19 different categories of polar nitrogen-containing pesticides, including sulfonylureas, triazolopyrimidines, diphenyl ether herbicides, benzoylurea insecticides, and phenylurea herbicides, with unadsorbed rates below 10%. The analytical method achieved an average recovery rate of 61.92% to 115.21%, with an RSD below 5.0%. Detection and quantification limits ranged from 0.012 to 0.524 μg/L and 0.127 to 5.243 μg/L, respectively.Conclusion: The developed method is green, efficient, simple, and cost-effective. It offers an environmentally friendly and user-friendly approach for the detection of polar nitrogen-containing pesticide residues, demonstrating good recovery and precision. This method holds potential for wide application in environmental monitoring and food safety.
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JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Zhimin Liu,Weijun Wang,Yibo Geng,Yuting Zhang,Xuan Gao,Junfeng Xu,Xiaolu Liu
The accumulation of polyethylene microplastic (PE-MPs) in soil can significantly impact plant quality and yield, as well as affect human health and food chain cycles. Therefore, developing rapid and effective detection methods is crucial. In this study, traditional machine learning (ML) and H2O automated machine learning (H2O AutoML) were utilized to offer a powerful framework for detecting PE-MPs (0.1 %, 1 %, and 2 % by dry soil weight) and the co-contamination of PE-MPs and fomesafen (a common herbicide) in soil. The development of the framework was based on the results of the metabolic reprogramming of soybean plants. Our study stated that traditional ML exhibits lower accuracy due to the challenges associated with optimizing complex parameters. H2O AutoML can accurately distinguish between clean soil and contaminated soil. Notably, H2O AutoML can detect PE-MPs as low as 0.1 % (with 100 % accuracy) and co-contamination of PE-MPs and fomesafen (with 90 % accuracy) in soil. The VIP and SHAP analyses of the H2O AutoML showed that PE-MPs and the co-contamination of PE-MPs and fomesafen significantly interfered with the antioxidant system and energy regulation of soybean. We hope this study can provide a reliable scientific basis for sustainable development of the environment.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Ning Yue,Yifan Lai,Jiangjiexing Wu,Qiaochu Zhang,Wei Qi,Rongxin Su
Biosensors provide simple, rapid and sensitive detection of a wide range of analytes. Recently, they have been widely used for the rapid detection of pesticides, which makes up for the shortcomings of traditional detection methods. However, the catalytic activity of some nanozymes is not satisfactory in practical applications, limiting the performance of biosensors. Further development of highly active and stable nanozymes is conducive to improving the sensitivity of the sensors and expanding their application in practical detection. Herein we simulated the amino acid microenvironment of natural enzymes and synthesized His-MIL-101(Fe)-X with different histidine (His) modification amounts (X = 0, 25%, 50%, 75%) by regulating the ratio of histidine and terephthalic acid ligands using a one-step solvothermal method. With increasing histidine doping, the peroxidase-like activity of His-MIL-101(Fe)-X was gradually enhanced, and the sensing performance of the sensor arrays constructed by combining His-MIL-101(Fe)-X with three peroxidase substrates was also gradually improved, with a 25-fold increase in detection limit. The His-MIL-101(Fe)-75% sensor array was not only able to accurately discriminate five pesticides in the range of 2-100 μM, but also to quantitatively identify different concentrations of pesticides. Moreover, the His-MIL-101(Fe)-75% sensor array showed good anti-interference capability and was able to discriminate five pesticides at only 2 μM in soil, lake water, seawater, and apple samples, as well as quantitatively detecting diafenthiuron, which has great potential for practical application.
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ACS Applied Materials & Interfaces
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2024
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IF 8.3
Jiale Lin,Cai Shen,Yongfa Cheng,Oi-Ming Lai,Chin-Ping Tan,Worawan Panpipat,Ling-Zhi Cheong
The stimulus-responsive regulation of enzyme catalytic activity and selectivity provides a new opportunity to extend the functionality and efficiency of immobilized enzymes. This work aims to design and synthesize a thermo-switchable enzyme@MOF for size-selective biocatalysis and biosensing through the immobilization of Candida rugosa lipase (CRL) within ZIF-8 functionalized with thermally responsive polymer, poly(N-isopropylacrylamide) (PNIPAM) (CRL@ZIF-8-PNIPAM). Unlike free CRL, which does not demonstrate substrate selectivity, we can reversibly tune the pore size of the ZIF-8-PNIPAM nanostructures (open pores or blocked pores) through temperature stimulus and subsequently modulate the substrate selectivity of CRL@ZIF-8-PNIPAM. CRL@ZIF-8-PNIPAM had the highest hydrolytic activity for small molecules (12 mM p-nitrophenol/mg protein/min, 4-nitrophenyl butyrate (p-NP Be)) and the lowest hydrolytic activity for large molecules (0.16 mM p-nitrophenol/mg protein/min, 4-nitrophenyl palmitate (p-NP P)). In addition, CRL@ZIF-8-PNIPAM demonstrated thermo-switchable behavior for large molecules (p-NP P). The p-NP P hydrolytic activity of CRL@ZIF-8-PNIPAM was significantly lower at 40 °C (blocked pores) than at 27 °C (open pores). However, the transition of blocked pores and open pores is a gradual process that resulted in a delay in the “thermo-switchable” catalytic behavior of CRL@ZIF-8-PNIPAM during thermal cycling. CRL@ZIF-8-PNIPAM was also successfully used for the fabrication of electrochemical biosensors for the selective biosensing of pesticides with different molecular sizes.
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Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Kuo Liu,Yulin Wu,Lining Zheng,Xian Wu,Hao Zhang
Microbial remediation is an eco-friendly and cost-effective approach to mitigate the environmental risks caused by fomesafen (FSA) and lead (Pb). In this study, a novel strain, Acidovorax temporans LK1, was isolated and demonstrated the ability to degrade 97.5 % of FSA within 2 d. Strain LK1 achieved simultaneous removal rates of 68.6 % for FSA and 38.4 % for Pb within 48 h. The effectiveness of strain LK1 in addressing FSA and Pb co-contamination was further validated by flow cytometry and energy-dispersive spectroscopy (EDS). Analysis of the degradation products revealed potential FSA degradation pathways, including nitro reduction, S-N bond cleavage, C-N bond cleavage, and ether bond cleavage. Over 21 d, strain LK1 removed more than 70 % of FSA and 40 % of Pb from the soil, significantly reducing the combined pollution stress on sweet corn and demonstrating its high efficacy under real-world conditions. Metabolomic analysis revealed that strain LK1 employed a series of metabolic reactions to maintain the intracellular metabolic balance, enabling efficient FSA degradation. These findings highlight the significant potential of strain LK1 for bioremediation, offering a novel solution for addressing the agricultural challenges associated with FSA and Pb co-contamination.
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