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JOURNAL OF CONTROLLED RELEASE · 2023 · IF 10.8

Employing single valency polyphenol to prepare metal-phenolic network antitumor reagents through FeOOH assistance

Mengsi Zhang,Lu Wang,Hao Jin,Nan Zhao,Yi Liu,Shijie Lan,Shuwei Liu,Hao Zhang

Metal-phenolic networks (MPNs) have been conventionally formed by the coordination of metal ions and polyphenols, which can responsively release metal ions and polyphenols under the trigger of tumor microenvironment (TME), showing high potential in the field of antitumor. However, MPNs are mainly limited to multi-valency polyphenols, and the unavailability of single valency polyphenols greatly hinders their applications even though they have excellent antitumor activity . Herein, we demonstrate a FeOOH assisted preparation method for MPNs antitumor reagent by introducing the complexes of Fe 3+ , H 2 O and polyphenol (Fe(H 2 O) x -polyphenol y ) in the preparation process, which overcomes the shortage of single valency polyphenols. Taking apigenin (Ap) as an example, Fe(H 2 O) x -Ap y complexes are foremost formed, in which the Fe(H 2 O) x is capable of hydrolyzing to generate FeOOH, thus producing Fe 3+ -Ap networks-coated FeOOH nanoparticles ( [email protected] NPs). Under the stimulation of the TME, [email protected] NPs could release Fe 2+ and Ap, realizing ferroptosis and apoptosis for tumor combination therapy. In addition, FeOOH can shorten transverse relaxation time, acting as a T 2 -weighted magnetic resonance imaging contrast agent . The current efforts provide an alternative strategy for constructing MPNs by exploiting single valency polyphenols, which strengthens the potential of MPNs in antitumor applications.

研究领域: 纳米技术 · 癌症研究 · 材料科学 · 生物医学工程
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ACS Applied Materials & Interfaces · 2016 · IF 7.145

Polyphenol Coating as an Interlayer for Thin-Film Composite Membranes with Enhanced Nanofiltration Performance

Xi Zhang,Yan Lv,Hao-Cheng Yang,Yong Du,Zhi-Kang Xu

Thin-film composite (TFC) nanofiltration membranes are prepared via interfacial polymerization with a polyphenol coating as an interlayer for the thin and smooth polyamide selective layer. The polyphenol interlayer is simply fabricated by the codeposition of tannic acid and diethylenetriamine without changing the surface morphology of the polysulfone ultrafiltration substrate. An interfacial polymerization is conducted from piperazidine and trimesoyl chloride on the polyphenol interlayer to construct the polyamide selective layer. The as-prepared TFC nanofiltration membranes show nearly tripled fold of water permeation flux as compared with those prepared at the same condition without an interlayer. They also exhibit a high rejection to Na2SO4 (>98%) because the thin and defect-free polyamide selective layer is formed on the polyphenol interlayer. These nanofiltration properties have high reproducibility, which means the TFC nanofiltration membranes are suitable for scale-up industrial applications.

研究领域: 材料科学 · 环境工程
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JOURNAL OF MEMBRANE SCIENCE · 2018 · IF 6.578

Metal-polyphenol coordination networks: Towards engineering of antifouling hybrid membranes via in situ assembly

Xueting Zhao,Ning Jia,Lijuan Cheng,Lifen Liu,Congjie Gao

Metal-polyphenol coordination networks have been actively explored as a facile, rapid and green platform for developing materials. In this study, novel antifouling hybrid membranes are successfully prepared via in situ assembling metal-polyphenol coordination networks and are proposed for oil/water separation application. Based on the coordination-driven cross-linking and assembling of Ti IV and TA within polyvinylidene fluoride (PVDF) membrane matrix, TA-Ti coordination networks are successfully introduced and uniformly distributed in the as-prepared PVDF/TA-Ti membranes. The effects of the embedded TA-Ti coordination networks on both surface morphologies and pore structures of PVDF/TA-Ti membranes are investigated. The surface chemical compositions of PVDF/TA-Ti membranes are analyzed by energy-dispersive X-ray (EDX) and Fourier transform infrared spectroscopy (FTIR). The water contact angle analysis and DSC study on bound water content reveal the outstanding hydration capability of PVDF/TA-Ti membranes, indicating the higher underwater superoleophobicity and antifouling property of PVDF/TA-Ti membranes. The as-prepared PVDF/TA-Ti membranes exhibit remarkably improved antifouling performance with the flux recover ability increased to a maximum level about 100% for the filtration of oil-in-water emulsions. Overall, this study highlights the promising antifouling potential of TA-Ti coordination networks in designing antifouling membranes, and proposes a facile in situ hybridization method for preparing antifouling membranes derived from versatile metal-polyphenol coordination networks.

研究领域: 材料科学 · 化学工程 · 环境工程
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ACS Sustainable Chemistry & Engineering · 2024 · IF 7.1

A Spider-like Polyphenol–Metal Dendrimer Chrome-Free Tanning Agent for Sustainable Leather Manufacturing

Sijie Yu,Taotao Qiang,Ruilong Li,Fangfang Dong,Xiaonan Ruan,Yihao Wei,Longfang Ren

To solve the problem of chrome pollution in the leather industry from the source, based on the large end-group functionality and strong designability of the dendrimer, a series of phenolic hydroxyl-terminated dendrimers (Gx-GA) were synthesized. Then, Gx-GA complexed with Al3+ to construct different generations of chrome-free tanning agents (Gx-GA-Al) with polyphenol–metal network (MPN) structures. It can take advantage of its branched structure to form multipoint and multiform cross-linking with leather collagen fibers, thus giving leather excellent physical and chemical properties. The results showed that the shrinkage temperature (Ts) of leather tanned with the first generation of chrome-free tanning agents (G1-GA-Al) reached 87.2 °C, which was 17.6 °C higher than that of 8% aluminum-tanned leather. The tensile strength and elongation at break increased by 26.5 and 60.8%, and the fastness to washing was also greater than 99%. The antibacterial rates against Staphylococcus aureus and Escherichia coli reached 99.9 and 98.7%, respectively. Moreover, leather tanned by Gx-GA-Al also had a good thickening effect, fullness, and softness. The degradation rate of Gx-GA-Al-tanned leather under natural conditions was much higher than that of chrome-tanned leather. Treated tanning wastewater was used in agricultural irrigation, and results showed that the growth of crops was accelerated. Therefore, the construction of Gx-GA-Al avoided the pollution of chrome from the source and endowed leather with better tanning properties. This study provides a new strategy for sustainable leather manufacturing.

CAS / MDL: 25952-53-8
研究领域: 材料科学 · 环境科学 · 化学工程 · 可持续发展
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POLYMER · 2024 · IF 4.1

A self-cleaning biocatalytic membrane with adjusted polyphenol deposition for edible oil-water separation

Bo Zhang,Qingzhe Mao,Wenchong He,Rongqing Zhou,Chongde Wu,Nicolas Hengl,Frederic Pignon,Yao Jin

Catechol-amine co-deposition membranes have garnered significant interest in enzyme immobilization, yet the deposited coating leads to excessive mass transfer resistance, negatively impacting membrane filtration performance. This work adjusts polyphenol deposition by utilizing the co-deposition structure with tannic acid (TA) and 3-aminopropyltriethoxysilane (APTES) with glycerol to enhance the filtration capability while maintaining enzyme activity. The glycerol addition has brought in a structural transition from dense nanosphere stacking to the loose flaky structure of greater bulkiness. Consequently, the resulting membrane showed a 69 % of permeability improvement along with improved enzyme activity post-adjustment. In oil-water separation cycle tests, the biocatalytic membrane enabled the clarification of oil emulsions and facilitates offline self-cleaning, maintaining high permeability and recovery even after five cycles of heavy oil (4 g/L) filtration, showing great application potential in edible oil-water separation. The biocatalytic membrane of this work, derived from biomass and characterized by its facile preparation and minimal mass transfer resistance, presents a promising avenue for the integration of biocatalysis with filtration technologies within industrial production processes.

CAS / MDL: 1492-30-4
研究领域: 生物技术 · 材料科学 · 环境工程
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LWT-FOOD SCIENCE AND TECHNOLOGY · 2021 · IF 4.952

Assembly of zein–polyphenol conjugates via carbodiimide method: Evaluation of physicochemical and functional properties

Yanan Xu,Zihao Wei,Changhu Xue,Qingrong Huang

Recently, the carbodiimide-mediated coupling method has attracted the attention of some scholars in the food field for its safety and high efficiency. In this study, the carbodiimide method was utilized to assemble zein–polyphenol conjugates innovatively. The covalent insertion of polyphenols to zein was confirmed by the increase of molecular weight and the reduction of nucleophilic groups. Chlorogenic acid (CGA) as well as Gallic acid (GA) were selected as polyphenol models, and the total phenolic content of zein–CGA conjugate and zein–GA conjugate reached 71 mg/g and 43 mg/g, individually. Afterwards, the structural and chemical characteristics between zein–polyphenol conjugates and physical mixtures were compared. Scanning electron microscopy (SEM) indicated that zein–polyphenol conjugates formed regularly shaped spheres with small particle sizes. Compared with control zein and physical mixtures, zein–polyphenol conjugates demonstrated better solubility and dispersibility, higher thermal stability as well as lower surface hydrophobicity. In terms of antioxidant capacity, zein–GA conjugate showed higher scavenging abilities of ABTS and DPPH free radicals than zein–CGA conjugate. The present research developed a new approach to fabricating zein–polyphenol conjugates that can be applied in the food industry as functional additives or materials for delivery systems.

CAS / MDL: 327-97-9
研究领域: 食品科学 · 材料科学 · 化学
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Journal of Food Measurement and Characterization · 2020 ·Vol. 14 ·期 4 ·2134-2144 · IF 1.648

Effective removal of heavy metals with amino-functionalized silica gel in tea polyphenol extracts

Huang Xin,Wang Li,Chen Jingyu,Jiang Chengyu,Wu Shijia,Wang Hongxin

Tea polyphenols (TPPs), as the most important functional component in tea extract, are easily contaminated by many heavy metals during tea processing, transportation and storage. TPPs with heavy metals can cause serious health problems and economic losses. In this study, to efficiently remove heavy metals from TPPs without affecting their active compounds and antioxidant functions, we prepared the amino-functionalized modified silica gel (AFSG) to remove Pb, Cu and Cd from TPPs, and determined removal rate of heavy metals, total polyphenolic content (TPC) and antioxidant activity of TPPs before and after adsorption. The static adsorption experiments showed that the adsorption isotherms were consistent with Langmuir model, in which the maximum sorption capacities of Pb, Cu and Cd were 140.23, 100.75 and 48.03 mg/g (25 °C, pH 5.0), respectively. Compared with before adsorption, the contents of Pb, Cu and Cd in 3 TPPs samples decreased significantly after adsorption on AFSG column (p < 0.01). However, the TPC and antioxidant capacity of the 3 TPPs samples had no significant effect before and after adsorption (p > 0.05). Meanwhile, the desorption and regeneration experiment showed that after 6 times of cyclic adsorption, the removal ability of Pb, Cu and Cd in TPPs by AFSG column could still reach 98.1%, 99.59% and 99.78%, respectively. Therefore, these results suggested that AFSG column could effectively remove heavy metals from TPPs without affecting the TPC and its antioxidant activity, it has potential applications in the removal and detection of heavy metals in TPPs.

CAS / MDL: 919-30-2 112926-00-8
研究领域: 食品科学 · 环境科学
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POLYMER TESTING · 2020 · IF 3.275

Hydrophobic octadecylamine-polyphenol film coated slow released urea via one-step spraying co-deposition

Meizhou Sun,Heling Guo,Jiliang Zheng,Yu Wang,Xinghuan Liu,Qian Li,Rongjie Wang,Xin Jia

Polymer coated fertilizer has been designed for gradual release of nutritional content of fertilizer to improve the utilization efficiency. However, the better slow release property of the coated fertilizer and simplified preparation process are still a huge challenge. The hydrophobic ODA-polyphenol film coated urea was prepared by one-step spraying for excellent nutrient release performance. Octadecylamine (ODA) was used to modify poly(tannic acid) (PTA) and poly(pyrogallol) (PPG) coating on substrates and prepare the hydrophobic ODA-PTA and ODA-PPG coated urea granules. The nutrient release rate of ODA-PTA and ODA-PPG coated fertilizers was much slower than PTA and PPG coated fertilizers in water and soil. The N release longevities of ODA-PTA coated fertilizers will be extended from 2 h to 30 days compared with PTA coated fertilizers. Moreover, pot experiments showed that coated fertilizer could effectively promote plant growth. This work will provide one-step spraying co-deposition approach to fabricate hydrophobic ODA-polyphenol film coated urea to improve the N release longevity, which can shine a light on the development of new slow release fertilizers (SRFs).

研究领域: 农业科学 · 材料科学
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JOURNAL OF MEMBRANE SCIENCE · 2021 · IF 8.742

Polyphenol-engineered superwetting membranes with wrinkled microspherical organizations for high-efficient oil/water separation

Xueting Zhao,Youyou Lan,Jiefeng Pan,Ruoxi Wang,Tingyuan Wang,Lifen Liu

Superwetting membranes, especially superhydrophilic and underwater superoleophobic membranes, are promising functional materials for oily wastewater treatment . Most superwetting membranes are charactered by micro-porous membranes with hierarchical morphology and hydrophilic composition. However, challenges still remain to synthesize superwetting membranes directly via phase separation that can overcome the limitations of the inherent features of the substrate and the need of multistep post-processing procedures. In this study, a facile strategy is reported to fabricate superwetting membranes via combining multiple polyphenol-mediated complexation with nonsolvent-induced phase separation (MPMC-NIPS). The metal-phenolic gelation networks (MPgNs) are formed within membrane matrix by in situ complexation in the casting solution, and followed by the interfacial complexation of F127-phenolic hydrogen-bonding networks (FPhNs) during the coagulation process. The MPgNs create surface structures with wrinkled microspherical organizations, and the FPhNs facilitate surface hydrophilicity. The resulting specific hierarchical wrinkled and hydrophilic surface architectures endow the membranes with superhydrophilicity and underwater superoleophobicity. The as-prepared PVDF/TA-Ti-SF127 membrane exhibits excellent emulsion permeation flux up to 6265 L m -2  h -1 bar -1 with high separation efficiency of over 99.6% and superior antifouling performance. This study highlights a promising and facile route to design superwetting membranes with tailored hierarchical wrinkled surface morphology for high-efficient oil-in-water emulsion separation, which contributes to the on-demand design and construction of micro-porous superwetting membranes.

研究领域: 材料科学 · 环境工程 · 化学工程
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Drug Delivery and Translational Research · 2023 · IF 5.4

Metal-polyphenol microgels for oral delivery of puerarin to alleviate the onset of diabetes

Li Si-hui,Li Yan-fei,Wu Di,Xu Yu,Yan Hui-jia,Hu Jiang-Ning

Puerarin (Pue) is a naturally bioactive compound with many potential functions in regulating blood glucose and lipid metabolism. However, the low bioavailability and rapid elimination in vivo limit the application of Pue in diabetic treatment. Here, we developed a metal-polyphenol-functionalized microgel to effectively deliver Pue in vivo and eventually alleviate the onset of diabetes. Pue was initially encapsulated in alginate beads through electrospray technology, and further immersed in Fe 3+ and tannic acid solution from tannic acid (TA)–iron (Fe) coatings (TF). These constructed Pue@SA-TF microgels exhibited uniform spheres with an average size of 367.89 ± 18.74 µm and high encapsulation efficiency of Pue with 61.16 ± 1.39%. In vivo experiments proved that compared with free Pue and microgels without TF coatings, the biological distribution of Pue@SA-TF microgels specifically accumulated in the small intestine, prolonged the retention time of Pue, and achieved a high effectiveness in vivo. Anti-diabetic experimental results showed that Pue@SA-TF microgels significantly improved the levels of blood glucose, blood lipid, and oxidative stress in diabetic mice. Meanwhile, histopathological observations indicated that Pue@SA-TF microgels could significantly alleviate the damage to the liver, kidney, and pancreas in diabetic mice. Our study provided an effective strategy for oral delivery of Pue and achieved high anti-diabetic efficacy. Graphical Abstract

CAS / MDL: 9005-38-3
研究领域: 药学 · 生物医学工程 · 糖尿病研究 · 药物递送系统
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Photothermal enhanced polyphenol-based nanofibers ameliorate catalytic efficiency of ferroptosis for synergistic tumor therapy

Kai Sun,Jiaying Yu,Jinzhong Hu,Wanxiang Yang,Xianfeng Chu,Lucheng Chen,Xiongwei Deng,Baiwang Sun,Zhifei Wang

Ferroptosis is an emerging antitumor treatment modality with the superiority for evading apoptotic cell death pathway. However, how to elevate catalytic efficacy of Fe 2+ -mediated Fenton reaction and efficiently elicit ferroptosis remain enormously challenging. Herein, inspired by hyperthermia-enhanced Fenton reaction kinetics, we firstly designed iron-polyphenol-aspirin-coordinated nanochelates for photothermal-enhanced ferroptosis antitumor immunotherapy. Specifically, we modulated optimal mass feeding ratio of gallic acid (GA), aspirin (ASA), Fe (II) and polyvinylpyrrolidone (PVP) to construct novel nanofibrous GA-ASA-Fe (II) metalchelates named GAFs. The variations in size and structure allowed the nanomedicines to avoid the risk of premature renal clearance in vivo, compared with the reported ultrasmall GA-Fe (II) nanocomplexes (GFs). Under NIR laser irradiation, GAFs could constantly amplify toxic hydroxyl radicals ( OH) generation and deplete excessive GSH to induce more accumulation of lethal lipid peroxidation (LPO), thereby triggering ferroptosis pathway in vitro and in vivo. Besides, the introduction of ASA could inhibit cyclooxygenase-2 (COX-2) and prostaglandin E 2 (PGE 2 ), in combination with photothermal-enhanced ferroptosis tumor therapy to induce immunogenic cell death (ICD), promote maturation of dendritic cells (DCs) and activate cytotoxic T cells for synergistic antitumor immunotherapy. GAFs with laser irradiation exhibited the capacity of inhibition of pulmonary metastasis. This work presented a strategy for incorporating small molecule immunomodulator into the metal-polyphenolic coordination to ameliorate its deficiencies, thereby inspiring a new design concept for tumor treatment.

研究领域: 癌症治疗 · 纳米技术 · 药学 · 免疫学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2023 · IF 8.2

A polyphenol and ε-polylysine functionalized bacterial cellulose/PVA multifunctional hydrogel for wound healing

Xiaotong Yi,Jinmei He,Xinjing Wei,Hongbin Li,Xingyuan Liu,Feng Cheng

Hydrogels for wound dressings have recently attracted considerable attention in the field of biomedical materials. Developing hydrogel dressings with multiple functions, including good antibacterial, mechanical and adhesive properties, to enhance wound regeneration is significant for clinical applications. To this end, a novel hydrogel wound dressing (PB-EPL/ [email protected] ) was developed, which was prepared by incorporating bacterial cellulose (BC) modified with tannic acid and ε-polylysine (EPL) into a PVA and borax matrix through a simple method without introducing any other chemical reagents. The hydrogel exhibited good adhesion (8.8 ± 0.2 kPa) to porcine skin, and the mechanical properties were significantly improved after adding BC. Meanwhile, it showed good inhibition against Escherichia coli , Staphylococcus aureus and Methicillin-resistant Staphylococcus aureus (84.1 ± 2.6 %, 86.0 ± 2.3 % and 80.7 ± 4.5 %) in vitro and Methicillin-resistant Staphylococcus aureus (MRSA) in vivo without the use of antibiotics, ensuring that the process of wound repair with a sterile environment. The hydrogel also presented good cytocompatibility and biocompatibility and could achieve hemostasis within 120 s. The in vivo experiments indicated that hydrogel could not only instantly complete hemostasis of the injured liver models but also obviously promote wound healing in a full-thickness skin. Furthermore, the hydrogel accelerated wound healing process by reducing inflammation promoting collagen deposition compared with commercial Tegaderm™ films. Therefore, the hydrogel is a promising high-end dressing material for wound hemostasis and repair for to enhance the wound healing.

研究领域: 生物医学材料 · 组织工程 · 伤口愈合 · 材料科学
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