ACS Applied Bio Materials
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2019
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IF 0
Ying Zhang,Hongyue Zhang,Xiang Qin,Chen Yang,Zhiqiang Wang,Yingxue Jin
Targeted delivery of photosensitizer for antitumor photodynamic therapy has received much attention recently. In this research, a multitargeting graphene oxide (GO) nanosystem (GFFP-TPPa) was fabricated based on the magnetically targeted nano-Fe3O4, active targeted folic acid (FA), and mitochondria-targeted triphenylphosphine, aiming to provide an effective drug delivery system of photosensitizer for improved photodynamic therapy against human tumor. The effective photosensitizer release from GFFP-TPPa under mild acidic pH condition (such as tumor microenvironment) suggested our designed nanosystem could reduce cutaneous phototoxicity of nanoparticles (NPs) in normal cells environment, which was further verified by the observation that the fluorescence of GFFP-TPPa was significantly quenched compared with free PPa. Research of cellular morphological variation, uptaking test, and intracellular single oxygen detection has validated the effectiveness of GFFP-TPPa NPs against tumor cells and potential fluorescence imaging function. Moreover, GFFP-TPPa NPs have excellent superparamagnetic properties and FA-targeted property of NPs, which was verified by the tumor cellular uptake of GFFP-TPPa. Finally, the precise deliver of photosensitizer to mitochondria has been proved by Mito-Tracker Green organelle localization. Our research indicated that the fabricated nanosystem could be applied conveniently for PDT based on multitargetability.
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ENERGY & FUELS
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2019
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IF 3.021
Kaiyu Zhang,Guodong Zhang,Zhuojing Li,Jirui Hou
Low pH fracturing fluids, such as the transition metal cross-linked guar derivative, can reduce the formation damage caused by clay swelling and fines migration in hydraulic fracturing treatments. However, a major disadvantage of the fluids is the uncontrollable rapid viscosity development, especially cross-linking under a pH below 3.0. In this paper, a novel delayed organic zirconium cross-linker with lactate and ethylene glycol as ligands was designed to overcome the shortcoming. Carboxymethyl hydroxypropyl guar (CMHPG), which results in a low gel residue after breaking, was used as the polymer at low concentration. The impact of gelation parameters on the properties of zirconium-CMHPG gel system was systematically investigated using a Sydansk bottle-testing method combined with a controlled stress rheometer. Desirable gelation time delay with agreeable rheological performance could be obtained by optimizing the polymer and cross-linker concentrations even at a pH as low as 2.0. Uniformly and compactly generated 3D network microstructures could firmly lock the free water within the gel, which further improved the thermostability and acid-resistance of the system. Meanwhile, the structures could also maintain the viscoelasticity of the fluid at a high level to ensure the efficient transportation of the proppants. Proppant settling and gel breaking tests demonstrated that the low pH and low polymer concentration gel system generated fewer insoluble residues with an uncompromised suspension performance. Moreover, the formation damage evaluation revealed that the low pH fracturing fluid system produced a better return permeability than the high pH system.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Huike Dong,Guanghua Lu,Xiaoping Wang,Peng Zhang,Haohan Yang,Zhenhua Yan,Jianchao Liu,Runren Jiang
Perfluorooctanoic acid (PFOA) is widely distributed in nature, particularly in aquatic environments. Its bioaccumulation and toxicity in aquatic organisms can be affected by both the chemical status of PFOA in water and the physiology of the organism. However, research on the patterns of these effects is scarce. In this study, we investigated the influence of aqueous pH (pH 6, acidic; pH 7.5, neutral; pH 9, basic) and fish sex on PFOA uptake, clearance, and biochemical effects in crucian carp ( C. auratus ) using flow-through exposure. In the 17-d kinetic experiment, PFOA bioaccumulation adhered to a uniform first-order model in which PFOA uptake rates from water to blood and liver in acidic conditions were faster than those in other conditions, indicating possible acidic pH influence on PFOA uptake. PFOA clearance rates in these compartments of males were slower than in females, which was attributed to the notably stronger expression of Oat2 (organic anion transporter 2, responsible for reabsorption) in the kidneys of males. Similar responses were observed for peroxisome proliferation-related biomarkers at different pH levels and in different sexes. These biochemical responses were driven by the internal concentrations of PFOA. The inhibition acetylcholinesterase activity in the fish brain was closely linked to changes in P-glycoprotein content, demonstrating a protective relationship. Collectively, an aqueous pH lower than 7.5 might affect the uptake of PFOA by fish. The clearance discrepancies between the sexes highlight the importance of anion carriers for ionizable organic compounds in aquatic organisms.
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Yinxue Li,Hongru Shang,Yongna Cao,Chunhui Yang,Yujie Feng,Yanling Yu
This study aimed to investigate the degree of contribution of adsorption mechanisms of sulfamethoxazole (SMX) on corncob - derived biochar CC800 through competition experiments. The SMX adsorption was governed by diverse mechanisms under different pH, resulting in high pH dependent adsorption of SMX on biochar. The adsorption of SMX on CC800 in the presence of ions was evaluated, demonstrating that the ion exchange mechanism had a weak effect on the adsorption. The intense competitiveness of SMX structural analogs verified π + –π electron donor-acceptor (EDA) effect was the dominant adsorption mechanism of SMX on CC800 at low pH, and the negative charge-assisted hydrogen bond (CAHB) was critical to the adsorption at high pH. The adsorption mechanisms contribution of SMX on CC800 were further quantified. The SMX adsorption on CC800 was mainly controlled by 51% pore filling and 43% π + –π EDA effect in the acid region, 62% pore filling mechanism and 25% (−)CAHB mechanism in the alkalic region, and less than 5% of hydrophobic interaction and ion exchange. Consequently, the above mechanisms provided a theoretical basis for biochar application to remove sulfonamide antibiotics and other similar organic contaminants and targeted design of biochar products. Also, this quantification method can be extended to quantify the adsorption mechanisms between other antibiotics or organics and biochar adsorbent materials by selecting suitable adsorption competitors.
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ChemNanoMat
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2022
·Vol. 8
·期 12
·e202200424
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IF 3.82
Lihui Yuwen,Yue Zhang,Huayu Xiao,Hang Xiao,Xiao Li,Wenjing Yang,Zhaoxia Yang,Heng Dong,Lianhui Wang
Graphical FeOCl nanodots were prepared by a ball-milling method and used as novel Fenton agents. Glutathione/pH dual-responsive polymer nanoparticles were synthesized by co-polymerization of acrylic acid and 3-methacrylamido dopamine with a cross-linker containing disulfide bonds, which can load FeOCl nanodots and doxorubicin to form a multifunctional nanoplatform for efficient chemodynamic therapy/chemotherapy. Chemodynamic therapy (CDT) based on the Fenton reaction has been considered as a promising solution for the treatment of tumors. However, the limited therapeutic efficacy and lack of responsive release of Fenton agents still hinder the further application of CDT. To this end, we designed a disulfide bond (−S−S−) cross-linked polymer nanoparticles (poly(AA-co-DMA), PAD) to load FeOCl nanodots (FeOCl NDs) and doxorubicin (DOX) with the surface coating of bovine serum albumin (BSA) to prepare glutathione (GSH)/pH-responsive PAD-FeOCl/DOX@BSA nanoparticles (PFDB). In the tumor microenvironment (TME) with abundant GSH and acidic pH, the −S−S− bond in PFDB can be reduced and the linkage between the polymer chains is broken down, which facilitates the controlled release of FeOCl NDs and DOX. Both in vitro and in vivo experimental results showed that PFDB can serve as a GSH/pH-responsive nanoagent for the effective killing of 4T1 tumor cells by combined CDT/chemotherapy. This study provides a promising TME-responsive nanoagent with dual therapeutic modes for the effective treatment of tumors.
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CARBOHYDRATE POLYMERS
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2022
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IF 10.723
Zexiang Zheng,Xing Yang,Yifan Zhang,Weiqiang Zu,Minna Wen,Taisheng Liu,Changren Zhou,Lihua Li
To achieve the pH-responsive release of metformin in tumor acidic microenvironment, we prepared OHA-Met by covalently grafting metformin (Met) onto oxidized hyaluronic acid (OHA) through imine bonds, and then prepared carboxymethyl chitosan (CMCS)/OHA-Met drug loaded hydrogels. The CMCS/OHA-Met hydrogels showed the in-situ injection performance. At pH = 7.4, the cumulative release rate of metformin from CMCS/OHA-Met20 hydrogel was 42.7 ± 2.6 % in 6 h, and the release tended to balance after 72 h. At pH = 5.5, the release kept constant and the cumulative release rate was 79.3 ± 4.7 % at 6 h, showing good pH-responsive behavior. Metformin induced apoptosis of MCF-7 cells through the caspase 3/PARP pathway. CMCS/OHA-Met20 hydrogel could effectively kill MCF-7 cells, while reducing the cytotoxicity of free metformin to L929 cells. In vivo breast cancer recurrence experiments showed CMCS/OHA-Met20 hydrogel could achieve local injection and pH-responsive smart drug delivery at the tumor resection site, inhibiting breast cancer recurrence. Compared with direct administration, CMCS/OHA-Met20 hydrogel reduced the metformin dosage, frequency of administration and systemic side effects.
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高影响因子
PEST MANAGEMENT SCIENCE
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2022
·Vol. 79
·期 3
·969-979
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IF 4.462
Linhuai Li,Jun Cen,Lingling Huang,Ling Luo,Guangqi Jiang
BACKGROUND The development of stimulus-responsive and photothermally controlled-release microcapsule pesticide delivery systems is a promising solution to enhance the effective utilization and minimize the excessive use of pesticides in agriculture. RESULTS In this study, an AVM@CS@TA-Fe microcapsule pesticide delivery system was developed using avermectin as the model drug, chitosan and tannic acid as the wall materials, and tannic acid–Fe complex layer as the photothermal agent. The optical microscope, scanning electron microscope, transmission electron microscope, and Fourier-transform infrared spectroscope were used to characterize the prepared microcapsule. The slow-release, UV-shielding, photothermal performance, and nematicidal activity of the microcapsule were systematically investigated. The results showed that the system exhibited excellent pH-responsive and photothermal-sensitive performances. In addition, the UV-shielding performance of the delivery system was improved. The photothermal conversion efficiency ( η ) of the system under the irradiation of near-infrared (NIR) light was determined to be 14.18%. Moreover, the nematicidal activities of the system against pine wood nematode and Aphelenchoides besseyi were greatly increased under the irradiation of light-emitting diode (LED) simulated sunlight. CONCLUSION The release of the pesticide-active substances in such a pesticide delivery system could be effectively regulated with the irradiation of NIR light or LED-simulated sunlight. Thus, the developed pesticide delivery system may have broad application prospects in modern agriculture fields. © 2022 Society of Chemical Industry.
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高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
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2019
·Vol. 25
·期 10
·2637-2644
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IF 5.16
Yanqiang Li,Huiyong Huang,Siru Chen,Chao Wang,Tingli Ma
Graphical Doped to reduce : FeN x -decorated carbon nanotubes are prepared by utilizing ZnO nanowires as a sacrificial template and Fe–polydopamine (Fe–PDA) complex as metal and carbon sources (see figure). The evaporation of Zn at high temperature results in a high surface area of the carbon nanotubes, and the FeN x species contribute greatly to the oxygen reduction reaction activity of the catalyst. It is of increasing importance to develop highly active and economical oxygen reduction reaction (ORR) electrocatalysts, which have great significance for the large-scale implementation of various energy conversion systems, including metal–air batteries and fuel cells. Herein, a novel method to synthesize FeN x -decorated carbon nanotubes as a high-efficiency ORR catalyst, by utilizing ZnO nanowires as a sacrificial template and a Fe–polydopamine complex as metal and carbon sources, is reported. The obtained catalyst shows great potential for replacing Pt/C as the ORR catalyst under various pH conditions, from alkaline to acidic electrolytes. The high conductivity, large surface area of the carbon nanotube, and highly active FeN x species contributed greatly to the high performance of the catalyst. The work presented herein paves a new way for the synthesis of 1D porous nanomaterials for a broad range of energy-related applications.
研究领域:
材料科学
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电化学
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能源技术
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Materials Science & Engineering C-Materials for Biological Applications
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2016
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IF 3.42
Lei Wang,Xiaodong Yang,Xiuli Chen,Yuping Zhou,Xiaodan Lu,Chenggong Yan,Yikai Xu,Ruiyuan Liu,Jinqing Qu
A novel fluorescence probe 1 based on triphenylamine was synthesized and characterized by NMR, IR, high resolution mass spectrometry and elemental analysis. Its fluorescence was quenched when pH below 2. There was a linear relationship between the fluorescence intensity and pH value ranged from 2 to 7. And its fluorescence emission was reversibility in acidic and alkaline solution. Furthermore, it exhibited remarkable selectivity and high sensitivity to Fe 3 + and was able to detect Fe 3 + in aqueous solution with low detection limit of 0.511 μM. Job plot showed that the binding stoichiometry of 1 with Fe 3 + was 1:1. Further observations of 1 H NMR titration suggested that coordination interaction between Fe 3 + and nitrogen atom on C N bond promoted the intramolecular charge transfer (ICT) or energy transfer process causing fluorescence quenching. Additionally, 1 was also able to be applied for detecting Fe 3 + in living cell and bioimaging.
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SENSORS AND ACTUATORS B-CHEMICAL
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2018
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IF 5.667
Shuai Yue,Xiao-Ting Sun,Yue Wang,Wen-Shu Zhang,Zhang-Run Xu
Surface-enhanced Raman scattering (SERS) spectroscopy is an ultrasensitive analytical technique with high specificity, making it an ideal candidate for therapeutic drug monitoring. However, SERS measurement of drugs in biological samples is inevitably affected by the proteins adsorbed nonspecifically on metal nanoparticles, so the drugs usually require separation before SERS detection. In this work, semipermeable alginate microparticles containing gold nanoparticles were fabricated via a centrifugal microfluidic chip, and served as a reliable substrate for SERS detection of 6-thioguanine in serum without protein removal. In comparison with the conventional microfluidic methods using oil for droplet generation, this oil-free method can fabricate more clean and versatile microparticles. The microparticles were characterized by size/charge selectivity and pH response, which effectively improved anti-interference ability and SERS sensitivity for 6-thioguanine detection in serum. The microparticles were further endowed with magnetic property and SERS activity simultaneously by forming Janus structures embedded with magnetic nanoparticles and gold nanoparticles separately in independent hemispheres, which was convenient for manipulation in SERS detection. More broadly, the microparticles are potentially applicable for SERS detection of other small molecules in complex real samples.
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Arabian Journal of Chemistry
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2023
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IF 6
Fulong Cheng,Yinian Wang,Yuting Fan,Dan Huang,Jie Pan,Wei Li
Biochar-based adsorbents for phosphate removal from wastewater has gained increasing attention and achieved significant progress. However, there is still much room for the enhancement on adsorption performance in terms of removal rate, adsorption capacity and pH application range. Herein, novel Ca-Al-La modified biochar adsorbents in this study were synthesized for enhancing phosphate adsorption in wastewater. The synthesis parameters of adsorbents were optimized by using the response surface methodology (RSM). The Ca-Al-La modified biochar adsorbent synthesized under the optimal conditions (CAL-MBC) exhibited superior adsorption capability towards phosphate. Specifically, CAL-MBC achieved a rapid removal rate to reach the adsorption equilibrium within 1 h, a maximum phosphate adsorption capacity of 152.9 mg/g, and excellent pH stability within a broad pH range of 3.0–11.0. The adsorption mechanisms involving electrostatic interaction, precipitation and inner-sphere complexation via ligand exchange were responsible for the excellent adsorption performance of phosphate on CAL-MBC. This study verifies CAL-MBC as a promising metal modified biochar adsorbent to enhance phosphate removal from wastewater.
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CHEMICAL ENGINEERING JOURNAL
·
2026
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IF 12.5
Xiaohan Guo,Yanfang Liu,Hongxiang Zhu,Xiaohui Yu,Feng Shi,Qinqin Liu,Qiang Liu,Ying Xu
Asp donates electrons to reprogram Fe O clusters of MIL-53(Fe). • This electronic switch redirects dominant ROS from •OH to •O 2 − . • The mechanism enables neutral-pH POD-like activity of MIL-53(Fe)@Asp. • The Asp-modified nanozyme integrates with GOX for cascade glucose sensing. MIL-53(Fe) exhibits peroxidase-like activity only under acidic conditions, limiting its biosensing applications. We overcome this by using aspartic acid (Asp) as a structure-directing agent to modify MIL-53(Fe) (MIL-53(Fe)@Asp) via hydrothermal synthesis followed by Asp coordination. Unlike conventional pH-reduction strategies, Asp modification does not alter bulk pH but induces intrinsic electronic restructuring of Fe O clusters, as confirmed by increased Fe 3+ /Fe 2+ ratio and introduction of N → Fe coordination (XPS). At pH 6.9, the TMB-based activity of MIL-53(Fe)@Asp is 27-fold higher than that of pristine MIL-53(Fe). Steady-state kinetics show favorable Km values (TMB 0.27 mM, H 2 O 2 1.38 mM) at neutral pH. Mechanistic studies (ROS identification, EPR, band structure, DFT) reveal that Asp exerts an electron-donating effect that reprograms the electron distribution of Fe O clusters, activating the otherwise inactive MIL-53(Fe) framework at neutral pH and diversifying the catalytic pathways to include a less pH-dependent •O 2 − route alongside the partially maintained •OH pathway. This pathway diversification enables efficient neutral-pH peroxidase-like catalysis, with •O 2 − as the dominant pathway. Leveraging this, we construct a cascade nanoplatform (MIL-53(Fe)@Asp@GOX) integrating glucose oxidase, which exhibits excellent cascade activity at neutral pH. The method is applied to glucose detection in blood and saliva, demonstrating good linearity, precision, selectivity, and recovery. The glucose concentrations determined by our sensor correlated well with those obtained using a commercial assay kit. Notably, the limit of detection for glucose in saliva reaches 2.08 μM, offering a promising route toward non-invasive glucose sensing. This work establishes a design principle for creating pH-adaptive catalytic microenvironments in Fe-MOFs through electronic restructuring and pathway diversification, overcoming a long-standing limitation of MIL-53(Fe) for biomedical applications. Download: Download high-res image (111KB) Download: Download full-size image
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