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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Novel Positively Charged Metal-Coordinated Nanofiltration Membrane for Lithium Recovery

Li Wang,Danyal Rehman,Peng-Fei Sun,Akshay Deshmukh,Liyuan Zhang,Qi Han,Zhe Yang,Zhongying Wang,Hee-Deung Park,John H. Lienhard,Chuyang Y. Tang

Nanofiltration (NF) with high water flux and precise separation performance with high Li+/Mg2+ selectivity is ideal for lithium brine recovery. However, conventional polyamide-based commercial NF membranes are ineffective in lithium recovery processes due to their undesired Li+/Mg2+ selectivity. In addition, they are constrained by the water permeance selectivity trade-off, which means that a highly permeable membrane often has lower selectivity. In this study, we developed a novel nonpolyamide NF membrane based on metal-coordinated structure, which exhibits simultaneously improved water permeance and Li+/Mg2+ selectivity. Specifically, the optimized Cu–m-phenylenediamine (MPD) membrane demonstrated a high water permeance of 16.2 ± 2.7 LMH/bar and a high Li+/Mg2+ selectivity of 8.0 ± 1.0, which surpassed the trade-off of permeance selectivity. Meanwhile, the existence of copper in the Cu–MPD membrane further enhanced anti-biofouling property and the metal-coordinated nanofiltration membrane possesses a pH-responsive property. Finally, a transport model based on the Nernst–Planck equations has been developed to fit the water flux and rejection of uncharged solutes to the experiments conducted. The model had a deviation below 2% for all experiments performed and suggested an average pore radius of 1.25 nm with a porosity of 21% for the Cu–MPD membrane. Overall, our study provides an exciting approach for fabricating a nonpolyamide high-performance nanofiltration membrane in the context of lithium recovery.

研究领域: 材料科学 · 环境工程 · 化学工程
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JOURNAL OF MEMBRANE SCIENCE · 2024 · IF 8.4

Multi-functional nanofibrous membrane with antibacterial property for highly effective capture of PM0.3 and hydrogen sulfide

Guangyao Wang,Zhuoran Feng,Lin Sun,Miao Wang,Yulu Li,Lanling Xiu,Yueguang Fang,Junwei Ye

In order to reduce the possible harm caused by air pollution, including particulate matters (PM), harmful gases and airborne pathogens, high-efficiency air filtration materials are attracting more and more attention. Therefore, multifunctional materials that can filter these pollutants and kill pathogenic bacteria simultaneously are urgently desired. Herein, a copper-coordinated nanofibrous membrane, named PAN-P-Cu, was successfully prepared based on polyacrylonitrile (PAN) nanofibers grafted polyethyleneimine (PEI) by electrospinning and coordination assembly method. The PAN-P-Cu showed high filtration efficiency (99.9%) towards PM 0.3 under an airflow velocity of 5.3 cm s −1 and high filtration efficiency (99.94%) towards PM 10 , respectively. Importantly, used membrane could be regenerated by a simple washing process. Moreover, PAN-P-Cu possessed removal property of 60 mg g −1 for hydrogen sulfide through the occurrence of chemical reactions. Furthermore, the PAN-P-Cu also exhibited excellent antibacterial activities against Escherichia coli and Staphylococcus aureus (>99.99%). This work may provide new insights on designing high-performance and multi-functional air filtration materials for public health protection in complicated environments.

研究领域: 材料科学 · 环境科学 · 生物医学
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JOURNAL OF ENZYME INHIBITION AND MEDICINAL CHEMISTRY · 2020 · IF 4.673

Functionality study of chalcone-hydroxypyridinone hybrids as tyrosinase inhibitors and influence on anti-tyrosinase activity

L. Ravithej Singh,Yu-Lin Chen,Yuan-Yuan Xie,Wei Xia,Xing-Wen Gong,Robert C. Hider,Tao Zhou

In an attempt to synthesise new tyrosinase inhibitors, we designed and synthesised a series of chalcone-hydroxypyridinone hybrids as potential tyrosinase inhibitors adopting strategic modifications of kojic acid. All the newly synthesised compounds were characterised by NMR and mass spectrometry. Initial screening of the target compounds demonstrated that compounds 1a, 1d, and 1n had relatively strong inhibitory activities against tyrosinase monophenolase, with IC50 values of 3.07 ± 0.85, 2.25 ± 0.8 and 2.75 ± 1.19 μM, respectively. The inhibitory activity against monophenolase was 6- to 8-fold higher than that of kojic acid. Compounds 1a, 1d, and 1n also showed inhibition of diphenolase, with IC50 values of 17.05 ± 0.07, 11.70 ± 0.03 and 19.3 ± 0.28 μM, respectively. The inhibition kinetics of diphenolase indicates that compounds 1a and 1d induce reversible inhibition on tyrosinase. Finally, we found that copper coordination should be one of the important inhibitory mechanism of these compounds in tyrosinase.

研究领域: 药物化学 · 生物化学
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ACS Applied Materials & Interfaces · 2017 · IF 7.504

Multicopper Laccase Mimicking Nanozymes with Nucleotides as Ligands

Hao Liang,Feifei Lin,Zijie Zhang,Biwu Liu,Shuhui Jiang,Qipeng Yuan,Juewen Liu

Using nanomaterials to achieve functional enzyme mimics (nanozymes) is attractive for both applied and fundamental research. Laccases are multicopper oxidases highly important for biotechnology and environmental remediation. In this work, we report an exceptionally simple yet functional laccase mimic based on guanosine monophosphate (GMP) coordinated copper. It forms an amorphous metal–organic framework (MOF) material. The ratio of copper and GMP is 3:4 as determined by isothermal titration calorimetry. It has excellent laccase-like activity and converts a diverse range of phenol containing substrates such as hydroquinone, naphthol, catechol and epinephrine. Comparative work shows that the activity is originated from guanosine coordination instead of phosphate binding in GMP. Cu2+ is required and cannot be substituted by other metal ions. At the same mass concentration, the Cu/GMP nanozyme has a higher Vmax and similar Km compared to the protein laccase. To achieve the same catalytic efficiency, the cost of the Gu/GMP is ∼2400-fold lower than that of laccase. The Cu/GMP is much more stable at extreme pH, high salt, high temperature and for long-term storage. This is one of the first laccase-mimicking nanozymes, which will find important applications in analytical chemistry, environmental protection, and biotechnology.

研究领域: 生物技术 · 环境修复 · 分析化学 · 纳米材料 · 酶模拟
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ACS Applied Materials & Interfaces · 2025 · IF 8.2

Cystine-Modified Lignin–Copper Coordination Nanocarriers Improve the Therapeutic Efficacy of Tyrosine Kinase Inhibition via Cuproptosis

Shiyao Song,Xingfeng Qiu,Shaoqing Huang,Huixuan Tian,Ruihan Pu,Jingyi Huang,Jiayin Su,Yan-Lai Tang,Libin Huang,Xuequn Luo,Weiling He,Qingfeng Ni,Weijing Zhang

The clinical application of tyrosine kinase inhibitors (TKIs) is rapidly growing and has emerged as a cornerstone in the treatment of both solid tumors and hematologic malignancies. However, resistance to TKI targets and disease progression remain inevitable. Nanocarrier-mediated delivery has emerged as a promising strategy to overcome the limitations of the TKI application. We utilized the facile modification of lignin polyhydroxyl groups to synthesize cystine-grafted lignin–copper coordinated nanoparticles for TKI delivery via the Mannich reaction. The materials exhibited a stable, uniform morphology and effectively encapsulated and delivered a variety of TKI inhibitors. Moreover, we optimized the fabrication process and found that the material could release the encapsulated drug in response to both pH and GSH. These nanoparticles significantly enhanced the therapeutic activity of TKIs both in vitro and in vivo through cuproptosis while demonstrating good biosafety. We propose a novel strategy for the targeted delivery of TKI inhibitors by combining cuproptosis with modified lignin. This approach not only offers new strategies for the clinical application of TKIs but also provides novel insights and inspiration for the modified use of lignin.

研究领域: 药学 · 材料科学 · 肿瘤学 · 纳米技术 · 分子生物学
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-10 · IF 14.7

Substituent tuning of Cu coordination polymers enables carbon-efficient CO2 electroreduction to multi-carbon products

Deng Huiying,Liu Tingting,Zhao Wenshan,Wang Jundong,Zhang Yuesheng,Zhang Shuzhen,Yang Yu,Yang Chao,Teng Wenzhi,Chen Zhuo,Zheng Gengfeng,Li Fengwang,Su Yaqiong,Hui Jingshu,Wang Yuhang

CO 2 electroreduction is a potential pathway to achieve net-zero emissions in the chemical industry. Yet, CO 2 loss, resulting from (bi)carbonate formation, renders the process energy-intensive. Acidic environments can address the issue but at the expense of compromised product Faradaic efficiencies (FEs), particularly for multi-carbon (C 2+ ) products, as rapid diffusion and migration of protons (H + ) favors competing H 2 and CO production. Here, we present a strategy of tuning the 2-position substituent length on benzimidazole (BIM)-based copper (Cu) coordination polymer (CuCP) precatalyst – to enhance CO 2 reduction to C 2+ products in acidic environments. Lengthening the substituent from H to nonyl enhances H + diffusion retardation and decreases Cu-Cu coordination numbers (CNs), favoring further reduction of CO. This leads to a nearly 24× enhancement of selectivity towards CO hydrogenation and C-C coupling at 60 mA cm −2 . We report the highest C 2+ product FE of more than 70% at 260 mA cm −2 on pentyl-CuCP and demonstrate a CO 2 -to-C 2+ single-pass conversion (SPC) of ~54% at 180 mA cm −2 using pentyl-CuCP in zero-gap electrolyzers.

CAS / MDL: 298-14-6
研究领域: 化学 · 材料科学 · 电化学 · 可持续能源
✓ 已验证 产品关联 DOI PubMed 高影响因子
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Journal of Food Measurement and Characterization · 2024 ·Vol. 18 ·期 5 ·3344-3352 · IF 2.9

Wool keratin-based colorimetric detection of organophosphorus pesticides via a multi-enzyme cascade reaction

Cao Mengrui,Xu Yiwei,Jia Xupeng,He Baoshan,Ren Wenjie,Wei Min,Suo Zhiguang,Jin Huali,Zhao Wenhong

A simple and sensitive colorimetric method for organophosphorus pesticides (Ops) detection was proposed via a multi-enzyme cascade reaction. The coordination compound of wool keratin and Cu (WK-Cu) was synthesized by self-assembly and used as a key catalyst in the cascade reaction. The enzymatic kinetics curve was established to explore the catalytic property, and the obtained K m and V max proved that WK-Cu has a good peroxidase-like activity. Ops could inhibit acetylcholinesterase activity and trigger the multienzyme cascades process, resulting in an amplified response signal. The key conditions were optimized, such as enzyme-linked reaction time and the concentration of each reactant in Ops detection. The detection range of phoxim was 10-1000 µg/L with a detection limit of 2.31 µg/L. Compared with other colorimetric detections, the proposed method exhibited a wider detection range and a relatively lower detection limit. In addition, this colorimetric method showed good universality and anti-interference ability for the analysis of phoxim in apple, cabbage and cauliflower samples. Owing to these merits, the proposed method has a good application prospect in Ops detection.

研究领域: 分析化学 · 环境科学 · 生物化学 · 酶学 · 材料科学
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DYES AND PIGMENTS · 2023 · IF 4.5

Highly sensitive and selective colorimetric and fluorescent dual-readout assay for the analysis of spermine, spermidine and cysteine

Zekun Shi,Yongning Wu,Xue Zhang,Yanyan Gao,Luqin Qiao,Qin Hou,Minglin Wang

Fluorescent cuprous iodide (CuI)-based coordination polymers (CuI-CPs) were widely used in the sensor field for high selectivity and sensitivity. Here, a new CuI-CP fluorescent probe was fabricated for the detection of spermine, spermidine and cysteine with dual-mode, which was capable of both convenient colorimetric analysis and ratiometric fluorescent detection. The fluorescence of CuI-CP solution was quenched and the solution changed from white to purple upon addition of spermine or spermidine, while the solution changed from white to yellow for cysteine. This probe exhibited selective, sensitive, rapid and linear response to spermine, spermidine and cysteine with a limit of detection of 0.57, 1.06 and 1.18 μM, respectively. Furthermore, cellulose acetate was used as the matrix to fabricate intelligent fluorescent film for real-time and visual monitoring the freshness of pork samples based on distinct fluorescence changes under UV light. This work realized a rapid, efficient, and profitable method for visually evaluating food quality.

研究领域: 分析化学 · 材料科学 · 食品科学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Polymerized Network-Based Artificial Peroxisome Reprogramming Macrophages for Photoacoustic Imaging-Guided Treatment of Rheumatoid Arthritis

Liyun Wang,Lingyan Zhang,Fan Chen,Qian Li,Bihui Zhu,Yuanjiao Tang,Zhengbao Yang,Chong Cheng,Li Qiu,Lang Ma

Artificial peroxisomes (AP) with enzyme-mimetic catalytic activity and recruitment ability have drawn a great deal of attention in fabricating protocell systems for scavenging reactive oxygen species (ROS), modulating the inflammatory microenvironment, and reprogramming macrophages, which is of great potential in treating inflammatory diseases such as rheumatoid arthritis (RA). Herein, a macrophage membrane-cloaked Cu-coordinated polyphthalocyanine-based AP (CuAP) is prepared with a macrocyclic conjugated polymerized network and embedded Cu-single atomic active center, which mimics the catalytic activity and coordination environment of natural superoxide dismutase and catalase, possesses the inflammatory recruitment ability of macrophages, and performs photoacoustic imaging (PAI)-guided treatment. The results of both in vitro cellular and in vivo animal experiments demonstrated that the CuAP under ultrasound and microbubbles could efficiently scavenge excess ROS in cells and tissues, modulate microenvironmental inflammatory cytokines such as interleukin-1β, tumor necrosis factor-α, and arginase-1, and reprogram macrophages by polarization of M1 (proinflammatory phenotype) to M2 (anti-inflammatory phenotype). We believe this study offers a proof of concept for engineering multifaceted AP and a promising approach for a PAI-guided treatment platform for RA.

研究领域: 生物医学工程 · 纳米技术 · 免疫学 · 诊疗学 · 炎症研究
✓ 已验证 产品关联 DOI PubMed 高影响因子
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Pharmaceutics · 2024 ·Vol. 16 ·期 4 ·512 · IF 4.9

Polydopamine-Modified Copper Coordination Mesoporous Silica Nanoparticles Loaded with Disulfiram for Synergistic Chemo-Photothermal Therapy

Junhong Ling,Yingying Cai,Haozhan Feng,Zhen Liu,Xiao-kun Ouyang

Disulfiram (DSF) degrades to diethyldithiocarbamate (DTC) in vivo and coordinates with copper ions to form CuET, which has higher antitumor activity. In this study, DSF@CuMSN-PDA nanoparticles were prepared using mesoporous silica with copper ions, DSF as a carrier, and polydopamine (PDA) as a gate system. The nanoparticles selectively released CuET into tumor tissue by taking advantage of the tumor microenvironment, where PDA could be degraded. The release ratio reached 79.17% at pH 5.0, indicating pH-responsive drug release from the nanoparticles. The PDA-gated system provided the nanoparticles with unique photothermal conversion performance and significantly improved antitumor efficiency. In vivo, antitumor experiments showed that the designed DSF@CuMSN-PDA nanoparticles combined with near-infrared light (808 nm, 1 W/cm2) irradiation effectively inhibited tumor growth in HCT116 cells by harnessing the combined potential of chemotherapy and photothermal therapy; a synergistic effect was achieved. Taken together, these results suggest that the designed DSF@CuMSN-PDA construct can be employed as a promising candidate for combined chemo-photothermal therapy.

研究领域: 纳米技术 · 药学 · 生物医学工程 · 癌症研究 · 治疗诊断学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Nanoscale coordination polymer-coated microneedle patches against bacterial biofilm infection via hypoxia-enhanced copper ion interference therapy

Xinwei Fu,Shan Du,Jie Liang,Bo Wang,Yingqi Liu,Yunlong Yu,Liqun Xu,Peng Xue,Bin Wang,Yuejun Kang

Ion interference therapy (IIT) represents an intervention strategy aimed at modulating the intracellular distribution of functional ions to mitigate bacterial biofilm infections (BBI). However, bacteria tend to activate protective pathways to alleviate the damage induced by ion interference under stress conditions, substantially diminishing the long-term therapeutic efficacy of IIT. Herein, we proposed an antibiofilm strategy of the photodynamic therapy (PDT)-mediated hypoxia-enhanced copper ion interference therapy (PHCIIT). The double-layered microneedles (CuIA@SCC MN) were synthesized by integrating the novel copper-coordinated polymeric nanorods (CuIA NRs) with sodium copper chlorophyllin (SCC) on the surface of hydrogel microneedles. Compared to conventional copper ion therapy, treatment with CuIA@SCC MN resulted in the PDT-mediated hypoxic microenvironment, enhancing the copper toxicity by inhibiting the protective mechanisms of bacteria, including down-regulation of multicopper oxidase activity and the enhanced accumulation of monovalent copper ions. Furthermore, the sustained release of therapeutic copper ions from CuIA NRs within the micro-acidic biofilm would further aggravate copper overload. The efficacy of the PHCIIT strategy was validated using diabetic wounds infected with E. coli biofilm. Following PHCIIT intervention, macrophages in the infected tissues exhibited polarization towards the M2-like phenotype, which could expedite wound healing. It is believed that the PHCIIT-based strategy is highly significant in advancing conventional IIT.

研究领域: 生物医学工程 · 微生物学 · 材料科学 · 治疗学 · 伤口愈合
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JOURNAL OF NANOBIOTECHNOLOGY · 2024 ·Vol. 22 ·期 1 ·1-19 · IF 10.6

Copper-coordination driven brain-targeting nanoassembly for efficient glioblastoma multiforme immunotherapy by cuproptosis-mediated tumor immune microenvironment reprogramming

Chen Yang,Tian Hailong,Zhang Xiaodian,Nice Edouard C.,Huang Canhua,Zhang Haiyuan,Zheng Shaojiang

Limited drug accumulation and an immunosuppressive microenvironment are the major bottlenecks in the treatment of glioblastoma multiforme (GBM). Herein, we report a copper-coordination driven brain-targeting nanoassembly (TCe6@Cu/TP5 NPs) for site-specific delivery of therapeutic agents and efficient immunotherapy by activating the cGAS-STING pathway and downregulating the expression of PD-L1. To achieve this, the mitochondria-targeting triphenylphosphorus (TPP) was linked to photosensitizer Chlorin e6 (Ce6) to form TPP-Ce6 (TCe6), which was then self-assembled with copper ions and thymopentin (TP5) to obtain TCe6@Cu/TP5 NPs. This nanoassembly effectively accumulated in tumor sites through the copper transport mechanism. Meanwhile, TCe6@Cu/TP5 could induce mitochondrial impairment by photodynamic therapy (PDT) mediated reactive oxygen species (ROS) accumulation and Cu 2+ triggered cuproptosis, resulting in evoking the AMP-activated protein kinase (AMPK) pathway to degrade PD-L1, and activating the cGAS-STING pathway to enhance anti-tumor immunity. Moreover, TP5 significantly promoted the proliferation and differentiation of dendritic cells (DCs) and T lymphocytes to further amplify the cancer immunity cycle. Collectively, our TCe6@Cu/TP5 NPs effectively facilitate drug accumulation and activate systemic antitumor immunity in vitro and in vivo, providing an innovative solution across the BBB that potentiates GBM immunotherapy. Graphical

研究领域: 癌症研究 · 纳米技术 · 免疫学 · 神经科学
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