Materials Chemistry Frontiers
·
2023
·Vol. 7
·期 14
·2896-2905
·
IF 7
Ke-Xin Li,Guo-Wei Guan,Ling-Min Pei,Qing-Yuan Yang
Since peroxidases have potential applications as biocatalysts, it is important to improve their usefulness. Traditional “semiconductor photocatalyst + peroxidase” catalytic cascade systems are inspired by nature's photosynthesis and provide the basis for maintaining the optimal stability and reactivity of the peroxidase enzyme. However, inherent fragility, non-recyclability, and low catalytic efficiency still limit their industrial application. In this work, we present a new generation of photoperoxidase catalytic platform, g-C3N4/PDI-HRP@ZIF-90 (graphite carbon nitride; PDI: perylene diimide; and HRP: horseradish peroxidase), for efficient photo-peroxidase catalysis. This new composite catalyst was created by introducing a rationally designed metal–organic framework (ZIF-90) in situ as a dual “modulator” for the “semiconductor photocatalyst + peroxidase” catalytic cascade system, which is highly applicable to industrial applications. In situ introduced modulators of ZIF-90 not only significantly increase the electron transfer rate but also significantly improve enzyme stability, cyclability, and molecular transfer rates between photoenzyme catalytic systems through spatial confinement. The new catalytic system (semiconductor + MOF + peroxidase) is capable of responding to a cascade catalytic reaction with wavelengths > 420 nm and is resistant to a catalytic environment at pH = 3. This work outlines a versatile and effective strategy to use the properties of MOFs to improve two major drawbacks of the efficient industrial use of peroxidases (inefficiency and poor stability), paving the way for efficient green biomanufacturing industrialization using peroxidases.
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AMB Express
·
2018
·Vol. 8
·期 1
·1-16
·
IF 1.719
Duan Zihong,Shen Rui,Liu Binjie,Yao Mengwei,Jia Rong
Irpex lacteus F17 is well-known for its ability to degrade recalcitrant aromatic pollutants, which mainly results from the action of the manganese peroxidase (MnP) that it is able to produce. Recently, the genome sequencing and annotation of this strain provided comprehensive picture of the ligninolytic peroxidase gene family. In addition to revealing the presence of 13 MnPs, genes for five dye-decolorizing peroxidases (DyPs) were also discovered in the I. lacteus F17 genome, which are unrelated to the fungal class II peroxidases. In the present study, amino acid sequences of five DyPs and 13 MnPs, representing two different families of heme peroxidases, were analyzed. Of these, two enzymes, a DyP (Il-DyP4) and a MnP (Il-MnP6) were expressed respectively in Escherichia coli, and were characterized by comparing their molecular models, substrate specificities, and catalytic features. The results showed that Il-DyP4 possessed a higher catalytic efficiency for some representative substrates, and a stronger decolorizing ability to a wide range of synthetic dyes in acidic conditions. Based on electrochemical measurements, Il-DyP4 was found to have a high redox potential of 27 mV at pH 3.5, which was superior to that of Il-MnP6 (− 75 mV), thereby contributing to its ability to oxidize high redox potential substrates, such as veratryl alcohol and polymeric dye Poly R-478. The results highlighted the potential of Il-DyP4 for use in industrial and environmental applications.
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AICHE JOURNAL
·
2024
·
IF 3.5
Xue-Li Cao,Tian Tian,Yong Bai,Chun Cui,Cong Luo,Jiang-Shan Xing,Chuan-Yu Chen,Lili Zhao,Shi-Peng Sun
Traditional nanofiltration membranes often struggle to maintain stability in harsh environments due to issues like swelling, chemical bond dissociation, and polymer chain creep. Fluoropolymers like poly(ethylene-chlorotrifluoroethylene) (ECTFE) are promising substrate candidates for broad-spectrum corrosion-resistant nanofiltration (CRNF) membranes, but their solvent insolubility and hydrophobicity present significant processing challenges. This study harnesses the electrospinnability and abundant reactive sites of polyvinyl alcohol to create a reactive site-bridged nanofibrous network. This network provides reactive sites to decorate the hydrophobic ECTFE substrate and bridges the molecular selective layer through aldolization, Schiff base reactions, and esterification. The resulting robust thin-film nanofibrous composite membranes exhibit high rejection rates for small molecular dyes under a variety of harsh conditions, including exposure to 10 wt% H 2 SO 4 , 1 M NaOH, ethanol, N , N -dimethylformamide, N -methylpyrrolidone, and 80°C solutions. This work paves the way for designing next-generation broad-spectrum CRNF membranes, enhancing their applicability in diverse harsh environments.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2024
·
IF 3.7
Yuhang Wei,Qingpeng Zhu,Weiwei Xie,Xinyue Wang,Song Li,Zhiming Chen
Efficient and convenient treatment of industrial dyeing wastewater is of a great significance to guarantee human and animal health. This work presented the enhanced catalytic activity at pH 3.0 of laccase immobilized on amino-functionalized ZnFe 2 O 4 nanoparticles (ZnFe 2 O 4 -laccase) and its application for degradation of textile dyes. Due to the existence of a large number of oxygen vacancies on the surface of the ZnFe 2 O 4 nanoparticles, negative ions accumulated on the magnetic carriers, which resulted in a harsh optimal pH value of the ZnFe 2 O 4 -laccase. Laccase activity assays revealed that the ZnFe 2 O 4 -laccase possessed superior pH and thermal stabilities, excellent reusability, and noticeable organic solvent tolerance. Meanwhile, the ZnFe 2 O 4 -laccase presented efficient and sustainable degradation of high concentrations of textile dyes. The initial decoloration efficiencies of malachite green (MG), brilliant green (BG), azophloxine, crystal violet (CV), reactive blue 19 (RB19) and procion red MX-5B were approximately 99.1%, 95.0%, 93.3%, 87.4%, 86.1% and 85.3%, respectively. After 10 consecutive reuses, the degradation rates of the textile dyes still maintained about 98.2%, 92.5%, 83.2%, 81.5%, 79.8% and 65.9%, respectively. The excellent dye degradation properties indicate that the ZnFe 2 O 4 -laccase has a technical application in high concentrations of dyestuffs treatment.
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RSC Advances
·
2014
·Vol. 4
·期 13
·6500-6507
·
IF 3.708
Zhujian Huang,Pingxiao Wu,Hailing Li,Wen Li,Yajie Zhu,Nengwu Zhu
A series of La and Ce doped hydroxyl FeAl intercalated montmorillonite (FeAl-Mt) were prepared by a co-intercalation method for catalytic oxidation of Reactive Blue 19 (RB19) by a heterogeneous photo Fenton process under natural sunlight irradiation. The physicochemical properties of the obtained catalysts were deciphered by X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, X-ray photoelectron spectroscopy (XPS), X-ray absorption fine structure (XAFS) and UV-vis diffuse reflectance spectroscopy (DRS). The results showed that Ce or La doped FeAl Keggin polyoxocations were intercalated into the gallery of montmorillonite and the physicochemical properties of intercalated FeAl Keggin polyoxocations were mildly changed after Ce or La doping, resulting in defects and lattice vacancies. The doping of Ce or La could effectively improve the catalytic performance of FeAl-Mt measured by heterogeneous photo Fenton degradation of RB19 catalyzed by the obtained products. The synergistic effect between the doped element and FeAl intercalated montmorillonite played a crucial role in the enhancement of heterogeneous catalytic activity under natural sunlight irradiation.
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RESEARCH ON CHEMICAL INTERMEDIATES
·
2024
·
IF 2.8
Fu Xiaolei,He Yan,Guo Zhulei,Chen Mingfan,Du Wenlong,Zeng Yuqin,Yuan Dingzhong,Na Bing
In this work, we designed and synthesized two novel bi-heteroatom functionalized hyper-crosslinked porous polymers (HCP-CT and HCP-CF) through a simple one-step Friedel–Crafts alkylation reaction. The resulted polymers N/S bi-heteroatom functionalized polymer HCP-CT and N/O bi-heteroatom functionalized polymer HCP-CF both have good adsorption property for organic dyes such as methyl orange (MO) and methylene blue (MB) in aqueous solution due to its rich pore structure, high specific surface area and rich-heteroatoms of pore surface. It is worth mentioned that the maximum adsorption capacity ( q max ) of cationic dye MB by the porous polymer HCP-CT at room temperature was reached up to 1571.46 mg/g, which is much higher than that of most reported porous materials. Furthermore, the adsorption capacity of HCP-CT for the cationic dye MB was more than seven times that of the anionic dye MO ( q max = 212.77 mg/g). Also, the polymer HCP-CF for the MB adsorption capacity ( q max = 352.11 mg/g) was more than twice higher than that of anionic dye MO ( q max = 131.75 mg/g). The above trends may be because of the stronger electrostatic interaction between the negatively charged N-S/O bi-heteroatom of HCP-CT and HCP-CF with the cationic dye MB than that of MO. In addition, the removal percentage of polymers HCP-CT and HCP-CF still remained above 80% after five adsorption–desorption cycles. Hence, this work may provide a convenient synthetic route to develop a novel hyper-crosslinked polymer with high capacity for the entrapment of dyes from aqueous solution.
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Nano Research
·
2024
·
IF 9.5
Zhang Kai,Dai Yu,Shi Yongli,Zhang Zhaoxin,Li Linji,Zhang Xiaojin,Xia Fan
Nanofilms that can fast permeate solvents and accurately sieve molecules are of significant importance for separation. A promising strategy is to align the inner cavities of macrocycles into the channels within nanofilms, and control the channel size by selecting the macrocycles. However, the channels outside the macrocycles are ignored. Here, we prepare nanofilms with hydrophobic channels (cyclodextrin inner cavity) and hydrophilic channels (cyclodextrin outer space) through interfacial polymerization of azobenzene-4,4′-dicarbonyl dichloride and amino-functionalized β-cyclodextrin. By utilizing the significant geometric changes caused by the photoisomerization of azobenzene, nanofilms with adjustable hydrophilic channel sizes were obtained. Our nanofilms have high permeability to polar and non-polar solvents, and can distinguish molecules with almost the same molecular weight but different shapes. This work expands the development of next-generation nanofilms generated through interfacial polymerization by incorporating rational molecular design.
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LWT-FOOD SCIENCE AND TECHNOLOGY
·
2024
·
IF 6
Huimin Shao,Xiaoyun Su,Yaru Wang,Jie Zhang,Tao Tu,Xiaolu Wang,Huoqing Huang,Bin Yao,Huiying Luo,Xing Qin
Mycotoxins are widely present from cereal crops to food products, posing a significant risk to food safety and causing serious health and economic losses. Therefore, it is imperative to develop a sustainable and efficient detoxification strategy to address mycotoxin contamination. Herein, a dye-decolorizing peroxidase, Ba DyP, from the white-rot fungus Bjerkandera adusta was successfully expressed as a soluble form in Escherichia coli with the help of molecular chaperones. Purified recombinant Ba DyP could efficiently degrade multiple mycotoxins including aflatoxin B 1 , zearalenone, and deoxynivalenol in the presence of mediators such as Mn 2+ or 1-HBT. Meanwhile, their degradation products were identified using UPLC-MS/MS, including AFB 1 -diol, AFQ 1 , 15-OH-ZEN, HZEN, and C 15 H 18 O 8 . Furthermore, cell survival tests exhibited a significant reduction in the biological toxicity of these degradation products. These findings indicate that the use of dye-decolorizing peroxidase could be a promising approach for the effective removal of multiple mycotoxins in cereal crops and food products.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Zhipeng Zhang,Jie Chen,Yan Ke,Xi Du,Xiaoqun Qiu,Liming Zhou,Yugao Zhang,Minghui Qiu,Jing Guo,Xu Jiang,Lu Shao
The treatment and reuse of high-salinity dyeing wastewater remains a critical challenge in the cotton textile industry, where lamellar graphene oxide (GO) membranes show significant potentials but are limited by permselectivity and stability of their channels. Herein, the porous covalent organic framework nanosheets (CONs) incorporated GO (GO/CON) membranes with engineered separation nanochannels were fabricated by a continuous rod-coating strategy using Mayer bars. Specifically, the incorporation of porous TpPa-SO 3 H nanosheets into GO membranes enhanced membrane permeability and dye/salt selectivity, attributed to the introduction of additional porous channels and the strengthened electrostatic properties from CONs. This GO/CON membrane exhibits exceptional durability during continuous cross-flow operations exceeding 300 h in high-salinity dyeing wastewater. Furthermore, the high-salinity permeate was successfully reused for dyeing cotton fabrics, producing textiles with minimal color differences, thereby demonstrating both environmental sustainability and economic viability for practical industrial applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Haowen Li,Huiwen Feng,Kai Wang,Yingjie Zhang,Jun Ma,Dan Song,Xiao Sui
Two-dimensional covalent organic frameworks (2D COFs) membranes have well-ordered nanochannels for selective molecular sieving. One-dimensional (1D) materials have been proposed to link the loosely packed COFs nanosheet for enhancing the separation performance of COFs membranes. However, it remains unclear how the enhancement arises. Herein, we demonstrate the role of 1D materials in modulating the microstructure and interlayer force of 2D COFs membranes. The optimized composite membrane, assembled from 2D COFs and chitosan exhibits a 75% enhancement in permeance without sacrificing selectivity towards different dyes. Our results show that the interaction forces between COFs and 1D materials are directly correlated to the transport nanochannels. When the interaction forces are stronger, the microstructure is more densely packed. Meanwhile, the shielding effect of 1D materials on the intrinsic channels of 2D COFs is more significant, resulting in narrow transport channels for mass transfer. In contrast, the weaker interaction forces prevent the excessive shrinkage of nanochannels, facilitating fast mass transfer and maintaining the high molecular selectivity. The work unravels the interaction forces between 2D COFs and 1D materials leading to the shaping of mass transfer nanochannels, offering a new perspective for the advancement of COFs membrane for nanofiltration.
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JOURNAL OF MOLECULAR LIQUIDS
·
2024
·
IF 5.3
Jialu Bo,Baoli Shi
Obtaining the interaction between two substances in liquid through their molecular structures can promote the design and preparation of new functional materials. When multiple types of intermolecular forces coexist, whether the contribution terms generated by each type of intermolecular force have the same scaling factor is a key consideration. In this paper, an empirical equation for calculating the total intermolecular interaction is proposed. The required molecular property parameters for calculation can be obtained through quantum–chemical calculation. For the experiments of removing eight ionic dyes in water by using corn cobs as adsorbents, linear correlation was found between the removal percentage and the total interaction calculated from the proposed equation. When the scaling factors of polar and hydrogen bond interaction terms are 1, the scaling factor of dispersion force interaction term in the equation is greater than 2.5.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-10
·
IF 15.7
Lin Jiuyang,Yu Zijian,Chen Tianci,Huang Junming,Chen Lianxin,Li Jiangjing,Li Xuewei,Huang Xiaolei,Luo Jianquan,Ang Elisa Yun Mei,Toh William,Wang Peng Cheng,Ng Teng Yong,Seo Dong Han,Zhao Shuaifei,Zhong Kuo,Xie Ming,Ye Wenyuan,Van der Bruggen Bart,Wan Yinhua
During the synthesis of dyes, desalination of high-salinity dye-containing waste liquor is a critical premise for high-quality, clean dye production. Conventional membrane processes, such as electrodialysis, nanofiltration and ultrafiltration, are inevitably subjected to serious membrane fouling, deteriorating the dye/salt fractionation efficacy. Integrating the technical merits of electrodialysis and pressure-driven membrane separation, we devise an electro-driven filtration process using a tight ultrafiltration membrane as alternative to conventional anion exchange membrane for rapid anion transfer, in view of dye desalination and purification. By employing a sub-4 nanometer tight ultrafiltration membrane as anion conducting membrane, the electro-driven filtration process achieves 98.15% desalination efficiency and 99.66% dye recovery for one-step fractionation of reactive dye and NaCl salt, markedly outperforming the system using commercial anion exchange membranes. Notably, the electro-driven filtration system displays a consistently high and stable fractionation performance for dyes and salts with unprecedentedly low membrane fouling through an eight-cycle continuous operation. Our results demonstrate that the electro-driven filtration process using nanoporous membranes as high-performance anion conducting membranes shows a critical potential in fractionation of organic dyes and inorganic salts, unlocking the proof of concept of nanoporous membranes in electro-driven application.
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