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Acta Biomaterialia · 2022 · IF 10.633

Inflammatory environment-adaptive patterned surface for spatiotemporal immunomodulation of macrophages

Yilun Luo,Peiqi Yuan,Sentao Hu,Hanwen Wang,Haiqi Zhang,Lie Ma

Designing biomaterials with precise immunomodulation can help to decipher the dynamic interactions between macrophages and biomaterials to match the tissue healing process. Although some advanced stimuli-responsive immunomodulatory biomaterials were reported for cell dynamic modulation, while most triggers need external stimuli by manual intervention, there would be the inevitable errors and uncertainties. Thus, developing immunomodulatory biomaterials with adaptive abilities, which can recognize the inflammation signals, change their properties spatiotemporally under the microenvironment triggers, and provide feedback to realize macrophages modulation in different healing stages, has become a promising strategy. In this work, we developed an inflammation-adaptive Arg-Gly-Asp (RGD) -patterned surface for spatiotemporal immunomodulation of macrophage. We fabricated a methacrylated hyaluronic acid (MA-HA) hydrogel with thiol-functionalized RGD-patterned surface by employing photolithography technology. Then, thiol-functionalized RGD contained ROS-cleavable linker was filled the remaining sites and consequently, a dynamic surface with temporary homogeneous RGD was obtained. Under the overproduction of ROS by the inflammation-activated macrophages, the linker was cleaved, and the homogeneous RGD surface was transformed to the RGD patterned surface, which triggered elongation of macrophages and consequently the upregulated expressions of arginase-1, IL-10 and TNF-β1, indicating the polarization toward to anti-inflammatory phenotype. Developing inflammatory environment-adaptive surface for spatiotemporal modulation of macrophages polarization provides a precise and smart strategy for the healing-matched immunomodulation to facilitate healing outcomes. Statement of significance Designing biomaterials with precise immunomodulation can help to decipher the dynamic interactions between macrophages and biomaterials to match tissue repair process. Some immunomodulatory biomaterials were reported for cell dynamic modulation, while most triggers need external manual intervention. Thus, we developed an immunomodulatory biomaterial with inflammation-adaptive patterned surface, which can recognize abnormal signals and change its properties spatiotemporally under the microenvironment triggers, and provide feedback to realize macrophages modulation in different stages. The dynamic surface can adapt to the changes of microenvironment and dynamically to match the cell behavior and tissue healing process on demand without external manual intervention. Additionally, the surface achieves the balance of macrophages with pro- and anti-inflammatory phenotypes in the tissue repair process.

研究领域: 生物材料 · 免疫学 · 组织工程 · 生物医学工程
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JOURNAL OF HAZARDOUS MATERIALS · 2020 · IF 9.038

Carbon nitride-doped melamine-silver adsorbents with peroxidase-like catalysis and visible-light photocatalysis: Colorimetric detection and detoxification removal of total mercury

Mengyuan Yin,Yuqi Wan,Shuai Li,Xiaoting Zhao,Wenwen Zhang,Yun Zhang,Hua Wang

Mesoporous melamine-silver (MA-Ag) nanocomposites doped with carbon nitride quantum dots (CN QDs ) were fabricated simply by the controlled supramolecular self-assembly. It was discovered that the resulting nanoflower-like CN QDs @MA-Ag nanocomposites could exhibit the peroxidase-like catalysis, which could be specifically enhanced by Hg 2+ by forming [email protected] alloys. A double catalysis-based colorimetric method was thereby developed for the fast detecting of Hg 2+ and Hg 0 in wastewater samples, with the levels down to 0.050 nM and 18.3 nM, respectively. Moreover, strong visible-light-driven photocatalysis of the nanocomposites was demonstrated for oxidizing Hg 0 into Hg 2+ through photocatalytic H 2 O 2 production so as to realize the detoxification of Hg 0 in the environmental wastewater. Besides, the fabricated mesoporous CN QDs @MA-Ag nanocomposites with large specific surface areas might facilitate the high Hg adsorption through the powerful MA-Hg chelate interaction, showing the efficient adsorption and/or removal of total Hg. The catalysis-selective colorimetric analysis and photocatalysis-based detoxification removal of total mercury may promise for wide applications in the environmental monitoring and wastewater treatment of toxic heavy metals of mercury.

研究领域: 环境科学 · 纳米技术 · 分析化学 · 材料科学 · 废水处理
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JOURNAL OF CHEMICAL AND ENGINEERING DATA · 2020 · IF 2.369

Solubility of Zaltoprofen in Five Binary Solvents at Various Temperatures: Data Determination and Thermodynamic Modeling

Renren Sun,Yameng Wan,Haixia He,Jiao Sha,Tao Li,Baozeng Ren

The solubility of zaltoprofen in binary {2-methoxyethanol (ME) + ethyl acetate (EAC)/ethanol (ET), 2-ethoxyethanol (EE) + ethyl acetate (EAC)} from 278.15 to 323.15 K and 1,4-dioxane (Diox) + ethyl acetate (EAC)/ethanol (ET) from 288.15 to 323.15 K was determined using the dynamic method under 0.1 MPa. The Hansen solubility parameter provided a reasonable explanation for the dissolution behavior of zaltoprofen. Three new crystal forms appeared during the dissolution process. Then, the Jouyban–Acree model, the Jouyban–Acree–van’t Hoff model, the Jouyban–Acree–Apelblat model, the Sun model, and the Ma model closely correlated with the measured solubility data. As a result, the Ma model and the Sun model provided better fitting. The basic data could provide support for industrial design and purification optimization process of zaltoprofen.

研究领域: 药物化学 · 物理化学 · 热力学
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Nano Research · 2018 ·Vol. 11 ·期 8 ·4245-4264 · IF 7.994

Stimuli-responsive gel-micelles with flexible modulation of drug release for maximized antitumor efficacy

Aouameur Djamila,Cheng Hao,Opoku-Damoah Yaw,Sun Bo,Dong Qiuling,Han Yue,Zhou Jianping,Ding Yang

Engineered stimuli-responsive drug delivery devices hold vast promise in biological applications for disease treatment due to their maximized therapeutic efficacy. In this study, a novel, stably cross-linked, and pH-sensitive biodegradable gel-micelle was constructed with amphiphilic conjugates of trimethylene dipiperidine-methacrylic anhydride-hyaluronic acid-stearylamine (TMDP-MA-HA-SA, TMHS) to improve tumor-targeting with flexible intracellular delivery of paclitaxel (PTX).The cross-linked methacrylate bonds significantly improved the biostability of TMHS gel-micelle (~ 200 nm) over the non-cross-linked under physiological conditions, while hyaluronic acid plays an important role in active tumor targetability. The gradual degradation of cross-linked hyaluronic acid shell was triggered by the concentrated hyaluronidase. Meanwhile, under acidic conditions (pH < 6.5), the tertiary amines of pH-sensitive TMDP moieties were protonated and thereby solubilized the gel-micellar core-portions. The resultant pH-triggered inner-core spaces rapidly prompted PTX release in the presence of multiple cytosolic enzymes that mainly degraded the remaining hydrophobic stearylamine core. During the in vitro cytotoxicity assay, PTX-loaded TMHS gel-micelles (CLTMHSPTX) revealed anticancer efficacy against human hepatocellular carcinoma HepG2 cells with IC 50 of 1.42 μg/mL (PTX concentration), significantly lower than other groups. In parallel, the in vivo anti-tumor efficacy of CL TMHS PTX gel-micelles against BALB/c xenograft tumor animal model demonstrated the greater tumor growth inhibition capacity of 72.06%, compared to other treatment groups at a safe concentration. Consequently, the cross-linked and stimuli-responsive CL TMHS PTX gel-micelles hold a great potential for flexible modulation of intracellular delivery of hydrophobic anticancer drugs with maximized antitumor efficacy.

研究领域: 药学 · 生物医学工程 · 癌症研究
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Strategies for controlling gas evolution reactions to boost the divergent paired electrochemical upgrading of furfural in acidic environment

Xinxin Li,Linchuan Cong,Yupeng Wu,Nan Lin,Fangbing Liu,Deyuan Xin,Fuyu Han,Jin Yang,Weitong Chen,Haibo Lin

Electrochemical methods for catalytic furfural conversion have drawn significant interest in both academic and industrial research communities. Paired electrocatalytic conversion has been identified as a promising strategy for reducing energy consumption and promoting carbon neutrality. To optimize product distribution and conversion efficiency, we have developed a divergent paired electrochemical upgrading approach for furfural in acidic environments, with a focus on prioritizing strong gas evolution reactions and product transformations. The high electrocatalytic activity of CuSn/CuF@Cu prepared by electrodeposition can effectively inhibit the hydrogen evolution. The performance of the electrocatalysts and the pathways of electrocatalytic hydrogenation (ECH) of furfural to 2-methylfuran (MF) were investigated by combination of experiments and the density functional theory (DFT) calculations. A stable Ti/PbO 2 electrode with high oxygen evolution overpotential was prepared for anodic electrocatalytic oxidation (ECO) and the product transformation route was described. The conversion of furfural to maleic acid (MA) and MF in acidic environment was successfully achieved. In the paired electrosynthesis system, the electrons generated from anodic ECO of furfural are utilized in valuable and controllable cathodic ECH. It significantly and continuously reduces the power cost associated with renewable energy sources and further promotes the development of biomass electrochemical conversion.

研究领域: 电化学 · 催化 · 可再生能源 · 生物质转化 · 材料科学
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BIOCHEMICAL ENGINEERING JOURNAL · 2021 · IF 3.978

Low modification of PETase enhances its activity toward degrading PET: Effect of conjugate monomer property

Kun Chen,Mingqin Quan,Xiaoyan Dong,Qinghong Shi,Yan Sun

Polyethylene terephthalate is one of the most widely used synthetic plastics. The accumulation of abandoned PET has brought an environmental problem. A recently reported PET hydrolase , PETase, displays an efficient decomposition to PET. Herein, we synthesized four PETase conjugates by modifying four types of monomers onto PETase, which were hydrophobic tert-butyl methacrylate (TBMA), hydrophilic hydroxyethyl methacrylate (HEMA), positively charged 2-(dimethylamino)ethyl methacrylate (DMAEMA), and negatively charged methacrylic acid (MA). Despite the low modification with an average number of 3–5 monomers on each enzyme molecule, all the PETase conjugates exhibited improved enzyme activity , and thermal and pH stability. Particularly, the catalytic efficiency ( k cat / K m ) of TBMA-/DMAEMA-PETase toward bis-2(hydroxyethyl) terephthalate (BHET) increased 1.4 and 1.6-fold as compared with PETase. Characterizations by fluorescence and circular dichroism spectroscopy unraveled that the modification induced the structural transformations, including compact overall structure and opened substrate-binding pocket, which were in favor of the enhanced catalytic performance. Biodegradation against PET films by TBMA-/DMAEMA-PETase were 4.69 and 3.26-fold higher than PETase. The different catalytic performances of the enzyme conjugates for BHET and PET are considered due to the different interactions of the conjugates with the different substrates. The work demonstrated that the low modifications with hydrophobic and hydrophilic monomers were both effective in improving the catalytic performance toward PET degradation, especially for the hydrophobic and positively charged monomers.

研究领域: 生物技术 · 环境科学 · 酶学 · 材料科学
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Polymers · 2024 ·Vol. 16 ·期 11 ·1570 · IF 4.7

Surface Reconstruction of Silicone-Based Amphiphilic Polymers for Mitigating Marine Biofouling

Chuanying Wei,Yan Zhang,Zhen Tang,Changan Zhang,Jianhua Wu,Bo Wu

Poly(dimethylsiloxane) (PDMS) coatings are considered to be environmentally friendly antifouling coatings. However, the presence of hydrophobic surfaces can enhance the adhesion rate of proteins, bacteria and microalgae, posing a challenge for biofouling removal. In this study, hydrophilic polymer chains were synthesised from methyl methacrylate (MMA), Poly(ethylene glycol) methyl ether methacrylate (PEG-MA) and 3-(trimethoxysilyl) propyl methacrylate (TPMA). The crosslinking reaction between TPMA and PDMS results in the formation of a silicone-based amphiphilic co-network with surface reconstruction properties. The hydrophilic and hydrophobic domains are covalently bonded by condensation reactions, while the hydrophilic polymers migrate under water to induce surface reconstruction and form hydrogen bonds with water molecules to form a dense hydrated layer. This design effectively mitigates the adhesion of proteins, bacteria, algae and other marine organisms to the coating. The antifouling performance of the coatings was evaluated by assessing their adhesion rates to proteins (BSA-FITC), bacteria (B. subtilisandP. ruthenica) and algae (P. tricornutum). The results show that the amphiphilic co-network coating (e.g., P-AM-15) exhibits excellent antifouling properties against protein, bacterial and microalgal fouling. Furthermore, an overall assessment of its antifouling performance and stability was conducted in the East China Sea from 16 May to 12 September 2023, which showed that this silicon-based amphiphilic co-network coating remained intact with almost no marine organisms adhering to it. This study provides a novel approach for the development of high-performance silicone-based antifouling coatings.

研究领域: 材料科学 · 海洋生物学 · 化学工程 · 环境科学
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Journal of Materials Chemistry A · 2024 ·Vol. 12 ·期 45 ·31500-31507 · IF 10.7

An ultrathin phase-inversion induced co-assembly separator for high-performance lithium-metal batteries

Yuying Wang,Fanjun Guo,Mengzhen Zhou,Qian Wu,Tao You,Zhengxiang Zhong,Jiankun Yang,Li Liu,Yudong Huang,Mingqiang Wang

Lithium metal batteries (LMBs) have been regarded as promising electrochemical energy storage systems due to the high theoretical specific capacity of metallic lithium. However, the uncontrolled growth of lithium dendrites, stemming from uneven lithium deposition, poses a significant challenge to their practical implementation. To tackle this issue, an ultra-thin composite separator, consisting of octamethacryloyloxy sesquioxane (MA–POSS), methacryloyloxy trimethoxysilane grafted holey graphene oxide (MPS–HGO), and aramid nanofibers (ANF), was prepared through a combination of phase transition-induced co-assembly and in situ polymerization techniques. Experiments indicate that the composite separator, with a thickness of only 3.8 μm, exhibits exceptional mechanical properties, specifically a tensile strength of 104 ± 5.1 MPa and a modulus of 3.23 ± 0.2 GPa, due to extensive hydrogen bonding and π–π interactions between the HGO sheets and ANF. Furthermore, benefiting from the synergistic effect of the abundant pores in MPS–HGO and the inhibition of stacking through the copolymerization of MPS–HGO and MA–POSS, the composite separator also demonstrates good electrolyte infiltration and a high lithium-ion transport number (tLi+ = 0.87), which not only acts as a physical obstacle but also efficiently regulates Li-ion transport to hinder irregular dendritic growth. The simultaneous regulation of Li-ion transport and mitigation of dendrite growth resulted in a long cycle life for Li|Li cells without dendrite deposition after 1500 cycles at a high current density of 5 mA cm−2. Moreover, the LiFePO4 (LFP)|Li battery with the composite separator displayed a capacity of 154 mA h g−1, a coulombic efficiency of 99%, and a high capacity retention of 99.6% after 250 cycles at 0.5C (85.7% after 1000 cycles at 2C). This work provides a promising new approach to fabricating high-performance lithium battery separators.

研究领域: 材料科学 · 电化学 · 储能技术
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Frontiers in Molecular Biosciences · 2021 · IF 5.246

Mitomycin C Inhibits Esophageal Fibrosis by Regulating Cell Apoptosis and Autophagy via lncRNA-ATB and miR-200b

Zhang Yin,Wang Qinge,Xu Yuping,Sun Jing,Ding Yanbo,Wang Li,Chen Bingfang,Sun Kewen,Chen Jianping

Benign esophageal strictures (BESs) frequently results from esophageal fibrosis. The transformation of fibroblasts into fibrocyte is an important cause of fibrosis. The treatment of fibrosis is challenging. Some previous studies have indicated the antifibrotic effect of mitomycin C (MMC). However, the mechanism of action of MMC and its optimal dose for treatment remains unclear. In the present study, the role of MMC in fighting fibrosis and its mechanism was investigated. Human esophageal fibroblast cells (HEFs)were treated without or with MMC, at 2, 5, 10 μg/ml, combining with mimic lncRNA-ATB, miR-200b inhibitor, rapamycin (RAPA), and 3-Methyladenine (3-MA). The cell viability, and cell apoptosis were evaluated. In addition, expression of apoptosis related proteins (caspase8 and caspase3), autophagy related proteins (LC3II and ATG5) and fibrosis related proteins (α-SMA collagen-1 and TGF-β) were also evaluated. Furthermore, autophagosome was observed by transmission electron microscope. Results showed that the expression of lncRNA-ATB was down-regulated and miR-200b was up-regulated after treated with MMC. And MMC induced cell apoptosis and inhibited cell autophagy. On the other hand, RAPA, mimic lncRNA-ATB and miR-200b inhibitor reduced fibrogenic effect of MMC on HEFs. Collectively, this study suggests that MMC inhibited esophageal fibrosis by regulating cell apoptosis and autophagy via downregulating lncRNA-ATB and upregulating miR-200b.

CAS / MDL: 5142-23-4 53123-88-9
研究领域: 药理学 · 分子生物学 · 细胞生物学 · 病理学
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PHYTOMEDICINE · 2022 · IF 6.656

Folium Hibisci Mutabilis extract, a potent autophagy enhancer, exhibits neuroprotective properties in multiple models of neurodegenerative diseases

Chang-Long He,Yong Tang,Xue Chen,Tao Long,Yan-Ni He,Jing Wei,Jian-Ming Wu,Cai Lan,Lu Yu,Fei-Hong Huang,Cong-Wei Gu,Jian Liu,Chong-Lin Yu,Vincent Kam-Wai Wong,Betty Yuen-Kwan Law,Da-Lian Qin,An-Guo Wu,Xiao-Gang Zhou

Background Protein aggregates are considered key pathological features in neurodegenerative diseases (NDs). The induction of autophagy can effectively promote the clearance of ND-related misfolded proteins. Objective In this study, we aimed to screen natural autophagy enhancers from traditional Chinese medicines (TCMs) presenting potent neuroprotective potential in multiple ND models. Methods The autophagy enhancers were broadly screened in our established herbal extract library using the transgenic Caenorhabditis elegans ( C. elegans ) DA2123 strain. The neuroprotective effects of the identified autophagy enhancers were evaluated in multiple C. elegans ND models by measuring Aβ-, Tau-, α-synuclein-, and polyQ40-induced pathologies. In addition, PC-12 cells and 3 × Tg-AD mice were employed to further validate the neuroprotective ability of the identified autophagy enhancers, both in vitro and in vivo . Furthermore, RNAi bacteria and autophagy inhibitors were used to evaluate whether the observed effects of the identified autophagy enhancers were mediated by the autophagy-activated pathway. Results The ethanol extract of Folium Hibisci Mutabilis (FHME) was found to significantly increase GFP::LGG-1-positive puncta in the DA2123 worms. FHME treatment markedly inhibited Aβ , α-synuclein, and polyQ40, as well as prolonging the lifespan and improving the behaviors of C. elegans , while siRNA targeting four key autophagy genes partly abrogated the protective roles of FHME in C. elegans . Additionally, FHME decreased the expression of AD-related proteins and restored cell viability in PC-12 cells, which were canceled by cotreatment with 3-methyladenine (3-MA) or bafilomycin A1 (Baf). Moreover, FHME ameliorated AD-like cognitive impairment and pathology, as well as activating autophagy in 3 × Tg-AD mice. Conclusion FHME was successfully screened from our natural product library as a potent autophagy enhancer that exhibits a neuroprotective effect in multiple ND models across species through the induction of autophagy. These findings offer a new and reliable strategy for screening autophagy inducers, as well as providing evidence that FHME may serve as a possible therapeutic agent for NDs.

CAS / MDL: 458-37-7 59-92-7
研究领域: 神经科学 · 药理学 · 中药 · 自噬研究 · 神经退行性疾病
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Enzyme induced polymer degradation as a pathway to create microbial habitats for biomanufacturing intensification

Wei Cheng,Huilin Wen,Haixia Shen,Chenwei Fu,Erkuang Miao,Dongbao Li,Xiaoqiang Chen,Chi Hu,Ziyi Yu

Polymer hydrogels are instrumental in cell immobilization for biomanufacturing, yet traditional hydrogel bioreactors often compromise cell viability, function, and mass transfer. This results in uncontrolled microbial proliferation and significant cell leakage, thereby impeding the continuous production of high-value products. To address these challenges, we introduce an innovative liquid microcavity technique employing a blend of Gelatin-methacryloyl (Gel-MA) and Pluronic F127diacrylate (F127-DA) for precision bioprinting, followed by selective enzymatic digestion of gelatin to create microbial habitats. Through tailoring of the hydrogel’s pore structure and integration of diverse networks, our approach facilitates controlled nutrient transfer, efficient waste removal, and stable mechanical support, all while maintaining a leak-free suspension culture of microorganisms. We validated the effectiveness of our method by fabricating yeast-infused Three-dimensional (3D) lattice constructs, successfully achieving continuous fermentation of glucose into ethanol in a flow reactor with minimal efficiency reduction (≥90 % yield) over five cycles. This research not only confronts the spatial limitations inherent in hydrogel-based systems but also demonstrates a foundational potential for revolutionary change in biomanufacturing practices.

研究领域: 生物技术 · 材料科学 · 生物工程 · 微生物学 · 化学工程
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