Journal of Inorganic and Organometallic Polymers and Materials
·
2023
·Vol. 33
·期 10
·3237-3246
·
IF 4
Zhu Xiaokang,Wang Xiuwu,Zhou Guiyang,Yin Hong,Qi Dongming,Deng Hangjun,Chen Tao
The preparation of polymer-metal complex is an effective way to achieve the bifunctionality of polymer and metal. In this study, temperature-sensitive polymer was synthesized from triethylene glycol methyl ether methacrylate (MEO 2 MA) and methacrylic acid N-hydroxysuccinimide ester (NMS) monomers via reversible addition-fragmentation chain transfer (RAFT) polymerization. 6-Aminohexanoic acid was introduced into the temperature-sensitive polymer using an activated ester strategy to obtain branched carboxyl-containing polymers. The carboxyl group in the polymer was coordinated with Fe(III), resulting in temperature-sensitive polymer-based iron complexes. The obtained iron complexes were used as homogeneous catalysts in the Fenton oxidation. Where, 97% and 96% decolorization of rhodamine B (RhB) and methylene blue (MB) could be achieved within 2 h for P(COOH 10 - co -MEO 2 MA 41 )-Fe 3+ , and the catalytic activities increased with the increase of the COOH content of polymer. In addition, the recycling of the catalyst can be achieved by the heating-centrifugal precipitation method using the temperature-sensitive nature of the polymer. Graphical Abstract
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Aisha Kanwal,Bassam Saif,Arif Muhammad,Wei Liu,Jiangtao Liu,Hao Ren,Peng Yang,Zhongli Lei
The construction of biomimetic nanozymes with efficient catalytic activities, low costs, and robust stability is fundamentally challenging but practically meaningful for biomedicine, immunoassays, catalysis, and environmental applications. Herein, we present a facile one-step strategy to fabricate a hemoglobin–gold nanoparticle (Hb–AuNP) catalytic system by using hemoglobin (Hb) as an efficient stabilizer and reducing agent. Remarkably, the Hb–AuNPs exhibit good dispersion and high catalytic stability under harsh conditions (temperature, pH, and storage time), which can ensure the long-term application properties of this catalytic system. Combining AuNPs with Hb for reactive oxygen species regulation resulted in 12-fold enhancements in catalytic activity compared with natural horseradish peroxidase (HRP). Further, the Hb–AuNPs exhibit a high glucose, H2O2, and ascorbic acid sensing performance with an unprecedented combination of a low detection limit and a rapid speed. This colorimetric method based on Hb–AuNPs was also effectively used to measure the levels of glucose and ascorbic acid in real samples.The current work comes up with new ideas for making gold-based biomimetic nanozymes that are both highly effective and stable. It also has interesting potential uses in biosensors and biomimetic catalysis.
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INTERNATIONAL JOURNAL OF PHARMACEUTICS
·
2023
·
IF 5.8
Yang Wang,Wenhui Zha,Ji Wang,Shuo Dong,Chao Liu,Yuhao Jiang,Xinsong Li
Chemodynamic therapy (CDT) has emerged as a powerful tumor treatment option by inducing the imbalance of redox homeostasis in cancer cells. Nevertheless, the therapeutic outcomes were greatly limited because of insufficient endogenous H 2 O 2 and upregulated cellular antioxidant defense in the tumor microenvironment (TME). Herein, a liposome-incorporated in-situ alginate hydrogel locoregional treatment strategy was developed, which involves using hemin-loaded artesunate dimer liposomes (HAD-LP) as redox-triggered self-amplified C-center free radical nanogenerator to enhance CDT. First, HAD-LP based on artesunate dimer glycerophosphocholine (ART-GPC) was prepared by a thin film method. Their spherical structure was manifested by dynamic light scattering (DLS) and transmission electron microscope (TEM). The generation of C-center free radicals from HAD-LP was carefully evaluated by using methylene blue (MB) degradation method. The results suggested that the hemin was reduced to heme under the action of glutathione (GSH), which could catalyze the breakage of endoperoxide of ART-GPC derived dihydroartemisinin (DHA) to generate toxic C-centered free radicals in a H 2 O 2 and pH-independent manner. Moreover, the change of intracellular GSH and free radical level was monitored through ultraviolet spectroscopy and confocal laser scanning microscope (CLSM). It was revealed that the hemin reduction induced GSH depletion and elevated free radical level, disrupting cellular redox homeostasis. After co-incubation with MDA-MB-231 or 4 T1 cells, HAD-LP was found to be highly cytotoxic. In order to prolong retention and improve antitumor efficacy, HAD-LP was mixed with alginate and injected intratumorally into 4 T1 tumor bearing mice. The injected HAD-LP and alginate mixture formed in-situ hydrogel and achieved best antitumor effect with the growth inhibition rate of 72.6%. Together, the hemin-loaded artesunate dimer liposome-incorporated alginate hydrogel possessed effective antitumor activity through redox-triggered C-center free radical generation induced apoptosis in a H 2 O 2 and pH-independent manner, which might be a promising candidate in the application of chemodynamic anti-tumor therapy.
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MOLECULAR PHARMACEUTICS
·
2023
·
IF 4.9
Zhaomin Tang,Shuting Jiang,Wanlan Tang,Qian He,Huangzhao Wei,Chengyu Jin,Shuai Wang,Hui Zhang
Chemodynamic therapy (CDT) that involves the use of Fenton catalysts to convert endogenous hydrogen peroxide (H2O2) to hydroxyl radicals (·OH) constitutes a promising strategy for cancer therapy; however, insufficient endogenous H2O2 and glutathione (GSH) overexpression render its efficiency unsatisfactory. Herein, we present an intelligent nanocatalyst that comprises copper peroxide nanodots and DOX-loaded mesoporous silica nanoparticles (MSNs) (DOX@MSN@CuO2) and can self-supply exogenous H2O2 and respond to specific tumor microenvironments (TME). Following endocytosis into tumor cells, DOX@MSN@CuO2 initially decomposes into Cu2+ and exogenous H2O2 in the weakly acidic TME. Subsequently, Cu2+ reacts with high GSH concentrations, thereby inducing GSH depletion and reducing Cu2+ to Cu+ Next, the generated Cu+ undergoes Fenton-like reactions with exogenous H2O2 to accelerate toxic ·OH production, which exhibits a rapid reaction rate and is responsible for tumor cell apoptosis, thereby enhancing CDT. Furthermore, the successful delivery of DOX from the MSNs achieves chemotherapy and CDT integration. Thus, this excellent strategy can resolve the problem of insufficient CDT efficacy due to limited H2O2 and GSH overexpression. Integrating H2O2 self-supply and GSH deletion enhances CDT, and DOX-induced chemotherapy endows DOX@MSN@CuO2 with effective tumor growth-inhibiting properties alongside minimal side effects in vivo.
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TALANTA
·
2023
·
IF 6.1
Weiquan Wang,Yunpeng Xu,Jie Hou,Zhixin Li,Fang Luo,De He,Zhenyu Lin
Hyaluronidase (HAase) is a potential tumor biomarker for diseases of the digestive tract and nervous system, the development of simple and sensitive techniques for HAase determination is urgent needed. Gold nanorods (Au NRs) can be etched by H 2 O 2 with high efficiency and display color changing. In this work, a HAase-responsive hydrogel system had been designed and the amount of H 2 O 2 spilled from the system had a close relationship with the amount of HAase, then the spilled H 2 O 2 had been applied to etch Au NRs. The color change of the solution was used to realize semi-quantitative determination of HAase. Furthermore, the longitudinal peak shift of Au NRs had a linear correlation with the concentration of HAase in the range of 10–60 U/mL (within 40 min) and the limit of detection (LOD) was 3.8 U/mL (S/N = 3), which can be used to realize accurate quantitative analysis of HAase. The proposed method has been applied to monitor HAase in serum of pancreatic cancer patients with satisfied results.
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MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 12
·1-11
·
IF 6.408
Wang Jing,Xu Wei,Zhou Lin,Zhang Tianqi,Yang Na,Wang Min,Luo Xuemei,Jin Lu,Zhu Huaijun,Ge Weihong
The peroxidase-like activity of MXene@Fe 3 O 4 nanocomposites and the relevant colorimetric application have been investigated for the first time. According to a kinetic study, MXene@Fe 3 O 4 nanocomposites displayed higher peroxidase activity than their individual components, and the catalytic process followed a ping-pong mechanism. The improved peroxidase-like activity of the MXene@Fe 3 O 4 nanocomposites was obtained due to the synergetic impact of the Fe 3 O 4 and MXene phases, the huge ion-accessible interface, and quick electron transfer channels in the nanocomposites. In the presence of hydrogen peroxide (H 2 O 2 ), the MXene@Fe 3 O 4 nanocomposites can catalyze the reaction of the colorless substrate 3, 3, 5, 5-tetramethylbenzidine (TMB) into oxidized TMB which revealed a blue color at 652 nm. After the introduction of glutathione (GSH), the blue color was gradually fading owing to the hydroxyl radical scavenging effect of glutathione. A colorimetric detection platform based on the peroxidase-like activity of the MXene@Fe 3 O 4 nanocomposites was developed for H 2 O 2 and GSH with a detection limit of 0.4 μM and 0.5 μM, respectively. The calibration plot for glutathione detection is calculated by absorbance difference at 652 nm, which ranged from 0.5 to 10 μM with a detection limit of 0.2 μM. The recoveries of GSH with different concentrations ranged from 93.76 to 108.50% and the relative standard deviation from 0.30 to 5.96%. This work significantly extends the application of MXene@Fe 3 O 4 nanocomposites in the construction of colorimetric sensors and reveals a satisfactory result in real sample analysis. Graphical Abstract
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MACROMOLECULAR MATERIALS AND ENGINEERING
·
2022
·Vol. 308
·期 4
·2200541
·
IF 4.402
Lin Qi,Yong Huang,Zheng Liu,Yulin Jiang,Meixuan Du,Limin Liu,Ganjun Feng,Yubao Li,Li Zhang
Skin is highly susceptible to foreign pathogens when damaged. Infections usually lead to serious damage to wounds and hinder wound healing, which results in nonhealing and inflammation of the wounds. Herein, a kind of fibrous membrane incorporated with calcium peroxide nanoparticles (n-CaO 2 ) is fabricated by electrospinning the polymer blend solution of polycaprolactone and gelatin. The obtained membranes show a randomly distributed nanofibrous structure with n-CaO 2 particles embedded in each fiber. Such a structure endows the membranes with medium hydrophilicity and improves blood clotting in comparison with the commonly used gauze, while the loading of n-CaO 2 achieves the in situ generation and rapid release of hydrogen peroxide (H 2 O 2 ), enabling FM-10 to display a robust bacteria inhibition of over 90% elimination to E. coli . The in vitro cytocompatibility experiment on the fibrous membranes demonstrates low cytotoxicity to L929 fibroblasts. The in vivo assessment indicates that the fibrous membranes can distinctly accelerate the wound healing, of which FM-5 exhibits the highest wound closure rate (>95%) after 14 days. This study provides a versatile approach, simply by varying the loading dosage of n-CaO 2 into fiber matrix, to fulfill different functions to meet the multiple needs of wound care.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Suzhou Xu,Can Liu,Xuping Jiang,Xinyu Wang,Shijin Zhang,Yanting Zhang,Qingguo Wang,Weiling Xiong,Jing Zhang
The performance and mechanisms of a titanium carbide (Ti 3 C 2 ) MXene modified Fe 3+ /hydrogen peroxide (H 2 O 2 ) system were compared in detail under dark and visible light conditions, with a new mechanism proposed for the reaction and reduction of MXene by Fe 3+ . Using Bisphenol A (BPA) as the target pollutant, the degradation of BPA by the Fe 3+ /H 2 O 2 system was improved after adding MXene in the dark, and the degradation rate of BPA was ≥ 95 % within 12.5 min under visible light, six times higher than that in the dark. Fe 2+ was ascertained to be the effective component responsible for H 2 O 2 activation to produce ·OH. SEM , XPS, ICP, XRD, and FTIR spectroscopy , analyses show that MXene and Fe 3+ form a complex, and then MXene reacts with Fe 3+ by breaking the Ti–C bonding to accelerate the Fe 3+ /Fe 2+ cycle. MXene uses photogenerated electrons to promote this reaction under visible light. In addition, quenching experiments and electron spin resonance spectroscopy results show that ·OH and O 2 •− are the main reactive oxygen species under visible light, while ·OH is the main active species in the dark. MXene thus effectively uses O 2 to form O 2 •− under visible light and promotes the Fe 3+ /Fe 2+ cycle. This study provides a theoretical basis for the combination of visible light catalysis and the advanced oxidation process of a Ti 3 C 2 MXene.
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Science China-Materials
·
2022
·Vol. 66
·期 3
·1053-1061
·
IF 8.64
Wang Junxia,Guo Changliang,Jiang Yong,Wan Jiafeng,Zheng Bing,Li Yuxin,Jiang Baojiang
Hydrogen peroxide is an environment-friendly reactive oxygen species and a significant green oxidant. However, the highly efficient and sustainable production of H 2 O 2 remains a challenge. Herein, we demonstrated a state-of-the-art photocatalytic method for H 2 O 2 production using an optimal tubular graphic carbon nitride (TCN)/ZnIn 2 S 4 (ZIS) heterojunction. Within 3 h, a H 2 O 2 production rate of 2.77 mmol g −1 h −1 was achieved by the TCN/ZIS heterojunction, which is 3.4- and 23.1-fold higher than that obtained by its individual TCN and ZIS components, respectively. Experimental results showed that the excellent photoactivity of TCN/ZIS is mainly due to the formation of heterojunction, which improves the charge separation ability and thereby promotes the proton-coupled electron transfer by initially reducing O 2 to ·O 2 − and subsequently generating H 2 O 2 . This work has developed an efficient and green strategy for H 2 O 2 production with scientific and practical value for environmental remediation.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Lidong Wang,Xiaohan Guo,Qingying Ye,Juanjuan Qi,Ping Li,Fei Yan
Dimethyl sulfoxide (DMSO) is a widely used solvent in many industries. The biodegradation of DMSO is difficult, resulting in large amounts volatile and noxious compounds emitted into the atmosphere, including dimethylsulfide, methyl mercaptan, and H2S. Therefore, it is necessary to deal with DMSO-containing wastewater using chemical methods. Here, supported niobia catalysts were prepared and characterized, and their catalytic performances was evaluated by the oxidative degradation of DMSO via H2O2 activation. The product of DMSO oxidation is dimethylsulfone which is a biodegradable and environmentally benign compound. The most active catalyst, 20%Nb2O5/SiO2, can remove 178.6 mmol/L DMSO within 2 h at 25 °C following a pseudo-first-order reaction. EPR spectroscopic studies and scavenging experiments confirms that O2•– and 1O2 are the active species for DMSO degradation. Although the catalytic activity of Nb2O5/SiO2 drops significantly after use, its reusability improved conspicuously after calcination, and the catalyst can be reused for 5 times with an 82.2% DMSO conversion.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Dongliang Wang,Yuxiao Li,Shaogang Hu,Jingping Hu,Huijie Hou,Bingchuan Liu,Han Zheng,Xi Luo,Haixiao Li
Electro-Fenton (EF) has shown great advantages in the effecient degradation of recalcitrant organic pollutants through in situ generation of •OH, and the main limitations on system performance are the efficiencies of H 2 O 2 activation and Fe 2+ regeneration. In this research, a triple-cathode EF system with a microbial fuel cell (MFC) cathode for the acceleration of Fe 2+ regeneration, a gas diffusion electrode for H 2 O 2 production and a stainless steel mesh (SSM) for electro-activation of H 2 O 2 was designed for efficient degradation of organic pollutants. The triple-cathode EF exhibited improved removal rate for recalcitrant organic pollutants with an average electricity consumption of 18.2 kWh Kg −1 TOC for Rhodamine B degradation, and the dosage of Fe 2+ could be reduced to 0.1 mM due to better utilization of H 2 O 2 and inhibition of parasitic reactions. Electrochemical characterization and theoretical calculation revealed that both one-electron reduction and H*-mediated activation contributed to the electro-activation of H 2 O 2 on SSM. This work demonstrates a novel construction and feasible approach for efficient EF with low cost.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 30
·14510-14516
·
IF 3.925
Yunxian Zhang,Yongyu Pang,Dong Xia,Guoliang Chai
As a successful alternative to the complex and dangerous anthraquinone process, a simple and safe method for the efficient preparation of hydrogen peroxide is to use the electrochemical two-electron oxygen reduction reaction (2e− ORR) process. Herein, we report a facile approach to achieving metal-free nitrogen-doped carbon material electrocatalysts (N-CMCs) using cheap and easily available raw materials, which also have an excellent electrochemical 2e− ORR catalytic performance and selectivity for hydrogen peroxide (H2O2). The as-fabricated nitrogen-doped carbon material electrocatalysts (named as N-CMC-1 : 5) deliver the high H2O2 selectivity of over 80% in a wide potential range from 0.30 to 0.70 V vs. RHE, where the highest H2O2 selectivity can reach 81.4% at 0.42 V vs. RHE. X-ray photoelectron spectroscopy and electrochemical analyses reveal that the content of pyrrolic-N in the catalysts has a positive effect on the 2e− ORR activity. When the catalyst contains more pyrrolic-N, the catalyst demonstrates a better 2e− ORR performance and H2O2 selectivity in alkaline medium, as well as the long-term stability of the catalyst.
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