Your browser doesn't support javascript.
loading
: 20 | 50 | 100
1 - 20 de 175
1.
J Hazard Mater ; 470: 134198, 2024 May 15.
Article En | MEDLINE | ID: mdl-38608582

A novel Ag3PO4/ZnWO4-modified graphite felt electrode (AZW@GF) was prepared by drop coating method and applied to photoelectrocatalytic removal of harmful algae. Results showed that approximately 99.21% of chlorophyll a and 91.57% of Microcystin-LR (MCLR) were degraded by the AZW@GF-Pt photoelectrocatalytic system under the optimal operating conditions with a rate constant of 0.02617 min-1 and 0.01416 min-1, respectively. The calculated synergistic coefficient of photoelectrocatalytic algal removal and MC-LR degradation by the AZW@GF-Pt system was both larger than 1.9. In addition, the experiments of quenching experiments and electron spin resonance (ESR) revealed that the photoelectrocatalytic reaction mainly generated •OH and •O2- for algal removal and MC-LR degradation. Furthermore, the potential pathway for photoelectrocatalytic degradation of MC-LR was proposed. Finally, the photoelectrocatalytic cycle algae removal experiments were carried out on AZW@GF electrode, which was found to maintain the algae removal efficiency at about 91% after three cycles of use, indicating that the photoelectrocatalysis of AZW@GF electrode is an effective emergency algae removal technology.


Electrodes , Graphite , Marine Toxins , Microcystins , Silver Compounds , Graphite/chemistry , Graphite/radiation effects , Microcystins/chemistry , Microcystins/isolation & purification , Catalysis , Silver Compounds/chemistry , Phosphates/chemistry , Oxides/chemistry , Electrochemical Techniques , Tungsten/chemistry , Chlorophyll A/chemistry , Zinc/chemistry , Water Purification/methods , Chlorophyll/chemistry , Photochemical Processes , Harmful Algal Bloom
2.
Environ Res ; 251(Pt 2): 118672, 2024 Jun 15.
Article En | MEDLINE | ID: mdl-38508360

A series of TiO2 - based photocatalysts have been prepared by the incorporation of 10 wt% of various carbon-based nanomaterials as modifying agents to titania. More specifically, commercial TiO2 P25 was modified through a wet impregnation approach with methanol with four different carbon nanostructures: single-walled carbon nanotubes (SWCNTs), partially reduced graphene oxide (prGO), graphite (GI), and graphitic carbon nitride (gCN). Characterization results (XPS and Raman) anticipate the occurrence of important interfacial phenomena, preferentially for samples TiO2/SWCNT and TiO2/prGO, with a binding energy displacement in the Ti 2p contribution of 1.35 eV and 1.54 eV, respectively. These findings could be associated with an improved electron-hole mobility at the carbon/oxide interface. Importantly, these two samples constitute the most promising photocatalysts for Rhodamine B (RhB) photodegradation, with nearly 100% conversion in less than 2 h. These promising results must be associated with intrinsic physicochemical changes at the formed heterojunction structure and the potential dual-role of the composites able to adsorb and degrade RhB simultaneously. Cyclability tests confirm the improved performance of the composites (e.g., TiO2/SWCNT, 100% degradation in 1 h) due to the combined adsorption/degradation ability, although the regeneration after several cycles is not complete due to partial blocking of the inner cavities in the carbon nanotubes by non-reacted RhB. Under these reaction conditions, Rhodamine-B xanthene dye degrades via the de-ethylation route.


Nanotubes, Carbon , Titanium , Titanium/chemistry , Catalysis , Nanotubes, Carbon/chemistry , Rhodamines/chemistry , Photolysis , Carbon/chemistry , Photochemical Processes , Graphite/chemistry , Graphite/radiation effects
3.
Chemosphere ; 353: 141544, 2024 Apr.
Article En | MEDLINE | ID: mdl-38408573

Meeting societal demand for potable water supply remains one of the prioritized challenges faced in the modern era. The anthropogenic intervention has led to a dire situation threatening ecological balance and human health. There is an inevitable need for the development of new technologies and innovations in existing technologies for water treatment. Photocatalytic Membrane technology, encompassing the merits of membrane filtration and photocatalytic degradation has evolved as a potential and reliable technology for sustainable water treatment. Innovations in photocatalytic materials and membrane fabrication techniques can lead to the goal of commercialization of membrane water treatment technology. Herein, we demonstrate the potential of graphitic carbon nitride (g-C3N4) and its functionalized analog as photocatalytic membranes for sustainable water treatment. g-C3N4 and Tetracarboxyphenylporphyrin sensitized g-C3N4 (g-C3N4/TCPP) was introduced onto commercial nylon membrane surface via a layer-by-layer (LBL) assembly method using chitosan and sodium salt of polystyrene sulphonic acid as polyelectrolytes. The fabricated membranes were characterized to ensure the integration of the photocatalysts. The performance of the membranes for water treatment was assessed by selecting some common dyes as model pollutants. The modified membranes exhibited excellent flux recovery and could afford high rejection rates upon irradiation indicating the prospects for sustainable filtration.


Graphite , Water Purification , Humans , Graphite/radiation effects , Nitrogen Compounds , Water Purification/methods , Catalysis
4.
J Mater Chem B ; 10(2): 306-320, 2022 01 05.
Article En | MEDLINE | ID: mdl-34935023

Poor tumor selectivity, low stability and quenched fluorescence are the main challenges to be overcome for nanomedicine, and are mainly caused by the dissociation of the nanostructure and aggregation of chromophores in the biological environment. Herein, covalently connected nanoparticles RGD-graphene-phthalocyanine (RGD-GO-SiPc) were constructed based on RGD peptide, silicon phthalocyanine (SiPc) and graphene oxide (GO) via a conjugation reaction for fluorescence imaging-guided cancer-targeted combinatorial phototherapy. The prepared RGD-GO-SiPc exhibited supreme biological stability, high-contrast fluorescence imaging, significantly enhanced NIR absorption, high photothermal conversion efficiency (25.6%), greatly improved cancer-targeting capability, and synergistic photodynamic (PDT) and photothermal therapy (PTT) efficacy along with low toxicity. Both in vitro and in vivo biological studies showed that RGD-GO-SiPc is a kind of promising multifunctional nanomedicine for fluorescence imaging-guided combined photothermal and photodynamic therapy with dual active/passive tumor-targeting properties.


Antineoplastic Agents/therapeutic use , Fluorescent Dyes/therapeutic use , Nanocomposites/therapeutic use , Neoplasms/drug therapy , Animals , Antineoplastic Agents/chemistry , Antineoplastic Agents/radiation effects , Cell Line, Tumor , Female , Fluorescent Dyes/chemistry , Fluorescent Dyes/radiation effects , Graphite/chemistry , Graphite/radiation effects , Graphite/therapeutic use , HEK293 Cells , Humans , Isoindoles/chemistry , Isoindoles/radiation effects , Isoindoles/therapeutic use , Light , Mice , Nanocomposites/chemistry , Nanocomposites/radiation effects , Nanoparticles/chemistry , Nanoparticles/radiation effects , Nanoparticles/therapeutic use , Neoplasms/diagnostic imaging , Neoplasms/metabolism , Oligopeptides/chemistry , Optical Imaging , Photochemotherapy , Photosensitizing Agents/chemistry , Photosensitizing Agents/radiation effects , Photosensitizing Agents/therapeutic use , Phototherapy , Singlet Oxygen/metabolism
5.
J Mater Chem B ; 9(47): 9734-9743, 2021 12 08.
Article En | MEDLINE | ID: mdl-34787633

Non-chemotherapeutic tumour treatment has received extensive attention due to its having fewer side effects as compared to chemotherapy. However, nanomaterials-based non-chemotherapy still faces limitations such as poor targeting and low retention. Therefore, a Schiff base cross-linked hydrogel was designed and prepared using aldehyde-modified polyethylene glycol (PEG) and carboxymethyl chitosan (CMC). This hydrogel has good injectable and self-healing properties and can carry graphene oxide (GO) as a photothermal agent and needle-like nano-hydroxyapatite (HAP) as a tumour inhibitor. Combined with tumour proliferation inhibition therapy and photothermal therapy, the nanocomposite hydrogel system can avoid the side effects of chemotherapy and improve the accuracy of tumour treatment. The PEG-CMC/HAP/GO nanocomposite hydrogel system has a porous structure, good injectability and self-healing properties to meet the mechanical requirements. In vitro cell characterization showed that GO is phototoxic to tumour cells, HAP can inhibit the proliferation of tumour cells, the nanocomposite hydrogel remained in the tumour site, and the encapsulated GO and HAP did not transfer to the normal site and cause cell damage. In the in vivo investigation, the breast cancer tumour-bearing mice, the model animals for tumour treatment, were treated with an intratumoral injection of the PEG-CMC/HAP/GO nanocomposite hydrogel. This functional self-healing hydrogel loaded with GO and HAP effectively inhibited tumour cell proliferation and realized the synergistic effect of photothermal therapy, which is expected to become a new effective treatment approach for tumours.


Antineoplastic Agents/therapeutic use , Breast Neoplasms/drug therapy , Durapatite/therapeutic use , Graphite/therapeutic use , Hydrogels/chemistry , Nanocomposites/chemistry , Animals , Cell Line, Tumor , Cell Proliferation/drug effects , Chitosan/analogs & derivatives , Chitosan/chemistry , Graphite/radiation effects , Infrared Rays , Male , Mice , Mice, Inbred BALB C , Mice, Nude , NIH 3T3 Cells , Photothermal Therapy , Polyethylene Glycols/chemistry
6.
ACS Appl Mater Interfaces ; 13(40): 47327-47340, 2021 Oct 13.
Article En | MEDLINE | ID: mdl-34587454

In this work, we developed the first 3D-printed polyetheretherketone (PEEK)-based bone scaffold with multi-functions targeting challenging bone diseases such as osteosarcoma and osteomyelitis. A 3D-printed PEEK/graphene nanocomposite scaffold was deposited with a drug-laden (antibiotics and/or anti-cancer drugs) hydroxyapatite coating. The graphene nanosheets within the scaffold served as effective photothermal agents that endowed the scaffold with on-demand photothermal conversion function under near-infrared laser irradiation. The bioactive hydroxyapatite coating significantly boosted the stem cell proliferation in vitro and promoted new bone growth in vivo. The presence of antibiotics and anti-cancer drugs enabled eradication of drug-resistant bacteria and ablation of osteosarcoma cancer cells, the treatment efficacy of which can be further enhanced by on-demand laser-induced heating. The promising results demonstrate the strong potential of our multi-functional scaffold in applications such as bone defect repair and multimodal treatment of osteosarcoma and osteomyelitis.


Anti-Bacterial Agents/therapeutic use , Antineoplastic Agents/therapeutic use , Benzophenones/chemistry , Osteomyelitis/drug therapy , Osteosarcoma/drug therapy , Polymers/chemistry , Tissue Scaffolds/chemistry , Animals , Anti-Bacterial Agents/radiation effects , Antineoplastic Agents/radiation effects , Bone Regeneration/drug effects , Cell Line, Tumor , Cell Proliferation/drug effects , Cisplatin/therapeutic use , Combined Modality Therapy , Durapatite/chemistry , Durapatite/therapeutic use , Graphite/chemistry , Graphite/radiation effects , Graphite/therapeutic use , Humans , Infrared Rays , Male , Mice, Inbred BALB C , Mice, Nude , Nanocomposites/chemistry , Nanocomposites/radiation effects , Nanocomposites/therapeutic use , Photothermal Therapy , Printing, Three-Dimensional , Quaternary Ammonium Compounds/therapeutic use , Rats, Sprague-Dawley
7.
ACS Appl Mater Interfaces ; 13(34): 40278-40289, 2021 Sep 01.
Article En | MEDLINE | ID: mdl-34424666

It is hard to achieve safe, effective, and minimally invasive therapies on myocardial infarction (MI) via conventional treatments. To address this challenge, a vascular endothelial growth factor (VEGF)-loaded and near-infrared (NIR)-triggered self-unfolding graphene oxide (GO)-poly(vinyl alcohol) (PVA) microneedle (MN) patch was designed and fabricated to treat MI through a minimally invasive surgery (MIS). The folded MN patch can be easily placed into the chest cavity through a small cut (4 mm) and quickly recover to its original shape with 10 s of irradiation of NIR light (1.5 W/cm2, beam diameter = 0.5 cm), thanks to its excellent shape memory effect and fast shape recovery ability. Meanwhile, the unfolded MN patch can be readily punctured into the heart and wrap the heart tightly, thanks to its sufficient mechanical strength and adjustable morphological structure, thus ensuring a high fixation strength to withstand the high-frequency pulsation of the heart. In addition, the prepared MN patch has low cytotoxicity and controllable and sustainable release of VEGF. More importantly, the MN patch can effectively promote neovascularization, reduce myocardial fibrosis, and restore cardiac function, which indicates its promising application prospects in MIS.


Drug Delivery Systems/instrumentation , Myocardial Infarction/drug therapy , Needles , Vascular Endothelial Growth Factor A/therapeutic use , Animals , Cell Line , Drug Delivery Systems/methods , Drug Liberation , Graphite/chemistry , Graphite/radiation effects , Infrared Rays , Male , Mice , Polyvinyl Alcohol/chemistry , Polyvinyl Alcohol/radiation effects , Rats , Vascular Endothelial Growth Factor A/chemistry
8.
J Inorg Biochem ; 223: 111558, 2021 10.
Article En | MEDLINE | ID: mdl-34329998

Photo-chemotherapy (PCT) reveals great potential in hepatocellular carcinoma (HCC) treatment, therefore the construct of smart PCT nano-agents with high photothermal conversion efficiency and accurate drug delivery is of great significant. Herein, a novel hybrid nanomaterial MGO-TCA-FA has been designed and constructed by grafting the triformyl cholic acid (TCA) and folic acid (FA) on the surface of Fe3O4 modified graphene oxide (MGO). The doxorubicin hydrochloride (DOX) as a model drug could be effectively loaded on the MGO-TCA-FA via hydrogen bonding and π-π stacking (the drug loading amount was 1040 mg/g). The formed MGO-TCA-FA@DOX has been developed to be an effective PCT nanoplatform with the advantages of multiple-targeted drug delivery, near-infrared light (NIR) and pH triggered drug release, and photothermal conversion efficiency. In vitro experiments showed that compared with other cancer cells and normal liver cells, MGO-TCA-FA@DOX could specifically target liver cancer cells and presented significant killing ability to liver cancer cells. More importantly, in vivo experiments indicated that PCT synergistic therapy (MGO-TCA-FA@DOX) revealed the best tumor inhibition (the tumor inhibition rate was about 85%) compared with chemotherapy and photothermal therapy alone. Thus, this study supplied a viable multiple-targeted PCT nano-agent for chemo-photothermal combination therapy of liver cancer.


Antineoplastic Agents/therapeutic use , Drug Carriers/therapeutic use , Graphite/therapeutic use , Liver Neoplasms/drug therapy , Nanocomposites/therapeutic use , Animals , Antineoplastic Agents/chemistry , Antineoplastic Agents/pharmacokinetics , Antineoplastic Agents/radiation effects , Cell Line, Tumor , Cholic Acids/chemistry , Combined Modality Therapy/methods , Doxorubicin/chemistry , Doxorubicin/pharmacokinetics , Doxorubicin/therapeutic use , Drug Carriers/chemistry , Drug Carriers/radiation effects , Drug Liberation , Drug Therapy , Ferrosoferric Oxide/chemistry , Folic Acid/chemistry , Graphite/chemistry , Graphite/radiation effects , Humans , Infrared Rays , Magnetic Phenomena , Mice, Inbred BALB C , Nanocomposites/chemistry , Nanocomposites/radiation effects , Photothermal Therapy
9.
ACS Appl Mater Interfaces ; 13(26): 31066-31076, 2021 Jul 07.
Article En | MEDLINE | ID: mdl-34137247

The serious problem of pharmaceutical and personal care product pollution places great pressure on aquatic environments and human health. Herein, a novel coating photocatalyst was synthesized by adhering Ag-AgCl/WO3/g-C3N4 (AWC) nanoparticles on a polydopamine (PDA)-modified melamine sponge (MS) through a facile layer-by-layer assembly method to degrade trimethoprim (TMP). The formed PDA coating was used for the anchoring of nanoparticles, photothermal conversion, and hydrophilic modification. TMP (99.9%; 4 mg/L) was removed in 90 min by the photocatalyst coating (AWC/PDA/MS) under visible light via a synergistic photocatalytic-photothermal performance route. The stability and reusability of the AWC/PDA/MS have been proved by cyclic experiments, in which the removal efficiency of TMP was still more than 90% after five consecutive cycles with a very little mass loss. Quantitative structure-activity relationship analysis revealed that the ecotoxicities of the generated intermediates were lower than those of TMP. Furthermore, the solution matrix effects on the photocatalytic removal efficiency were investigated, and the results revealed that the AWC/PDA/MS still maintained excellent photocatalytic degradation efficiency in several actual water and simulated water matrices. This work develops recyclable photocatalysts for the potential application in the field of water remediation.


Nanoparticles/chemistry , Trimethoprim/chemistry , Catalysis/drug effects , Graphite/chemistry , Graphite/radiation effects , Indoles/chemistry , Indoles/radiation effects , Light , Nanoparticles/radiation effects , Nitrogen Compounds/chemistry , Nitrogen Compounds/radiation effects , Oxides/chemistry , Oxides/radiation effects , Polymers/chemistry , Polymers/radiation effects , Silver/chemistry , Silver/radiation effects , Silver Compounds/chemistry , Silver Compounds/radiation effects , Temperature , Triazines/chemistry , Triazines/radiation effects , Tungsten/chemistry , Tungsten/radiation effects , Water Purification/methods
10.
Carbohydr Polym ; 268: 118235, 2021 Sep 15.
Article En | MEDLINE | ID: mdl-34127218

In-depth understanding of interfacial property is the key to guiding the synthesis of biomass composites with desired performance. However, the exploration is of great challenge due to limitations of experimental techniques in locating hydrogen, requiring large/good crystals and detecting a weak interaction like van der Waals (vdW). Herein, we experimentally and computationally investigated the composite cellulose/zinc oxide/g-C3N4. Hydrothermal synthesis afforded cellulose/ZnO, and then fabricated the ternary composite by adding g-C3N4 under ultrasonic condition. Three components are found to co-exist in the composite, and the ZnO nanoparticle is attaching to cellulose and coupling with g-C3N4. These experimental findings were corroborated by relativistic DFT calculations. The interfacial coupling is elaborated as contributions of dative bonds, hydrogen bonds and vdW interaction. The vdW is increased by a factor of 4.23 in the ZnO/g-C3N4 interface. This improves electron-hole separation and offers prospective application of the composite in photocatalysis, antibacteria and gas sensing.


Cellulose/chemistry , Graphite/chemistry , Nanocomposites/chemistry , Nitrogen Compounds/chemistry , Zinc Oxide/chemistry , Catalysis/radiation effects , Cellulose/radiation effects , Density Functional Theory , Graphite/radiation effects , Light , Models, Chemical , Nanocomposites/radiation effects , Nitrogen Compounds/radiation effects , Static Electricity , Zinc Oxide/radiation effects
11.
Phys Chem Chem Phys ; 23(5): 3351-3360, 2021 Feb 07.
Article En | MEDLINE | ID: mdl-33502403

The development of photocatalysts with high catalytic activity that are capable of full utilization of solar energy is a challenge in the field of photocatalysis. Accordingly, in the present study, an efficient Z-scheme cage-structured Co9S8/g-C3N4 (c-CSCN) photocatalyst was constructed for the degradation of tetracycline antibiotics under visible-light irradiation. The Z-scheme charge-transfer mechanism accelerates the separation of photogenerated charge carriers and effectively improves photocatalytic activity. Moreover, c-CSCN has a hollow structure, allowing light to be reflected multiple times inside the cavity, thereby effectively improving the utilisation efficiency of solar energy. As a result, the photocatalytic activity of c-CSCN is 1.5-, 2.5-, and 5.8-times higher than those of sheet-type Co9S8/g-C3N4 (s-CSCN), c-Co9S8, and g-C3N4, respectively, for the degradation of tetracycline. c-CSCN maintains favourable photocatalytic activity over five consecutive degradation cycles, demonstrating its excellent stability. In addition, c-CSCN performs efficient tetracycline removal in different water substrates. Moreover, c-CSCN exhibits excellent ability to remove tetracycline under direct natural sunlight. This work fully demonstrates that c-CSCN has high catalytic activity and the potential for practical application as a wastewater treatment material.


Anti-Bacterial Agents/chemistry , Cobalt/chemistry , Graphite/chemistry , Nitrogen Compounds/chemistry , Sulfides/chemistry , Tetracycline/chemistry , Water Pollutants, Chemical/chemistry , Catalysis/radiation effects , Cobalt/radiation effects , Graphite/radiation effects , Light , Models, Chemical , Nitrogen Compounds/radiation effects , Sulfides/radiation effects
12.
Chemistry ; 27(9): 3085-3090, 2021 Feb 10.
Article En | MEDLINE | ID: mdl-33263935

Universal access to clean water has been a global ambition over the years. Photocatalytic water disinfection through advanced oxidation processes has been regarded as one of the promising methods for breaking down microbials. The forefront of this research focuses on the application of metal-free photocatalysts for disinfection to prevent secondary pollution. Graphitic carbon nitride (g-C3 N4 ) has achieved instant attention as a metal-free and visible-light-responsive photocatalyst for various energy and environmental applications. However, the photocatalytic efficiency of g-C3 N4 is still affected by its rapid charge recombination and sluggish electron-transfer kinetics. In this contribution, two-dimensionally protonated g-C3 N4 was employed as metal-free photocatalyst for water treatment and demonstrated 100 % of Escherichia coli within 4 h under irradiation with a 23 W light bulb. The introduction of protonation can modulate the surface charge of g-C3 N4 ; this enhances its conductivity and provides a "highway" for the delocalization of electrons. This work highlights the potential of conjugated polymers in antibacterial application.


Disinfection/methods , Escherichia coli/chemistry , Escherichia coli/radiation effects , Graphite/chemistry , Graphite/radiation effects , Light , Microbial Viability/radiation effects , Nitrogen Compounds/chemistry , Nitrogen Compounds/radiation effects , Protons , Catalysis/radiation effects , Electrons , Graphite/pharmacology , Microbial Viability/drug effects , Nitrogen Compounds/pharmacology , Photochemistry
13.
ACS Appl Mater Interfaces ; 12(51): 56924-56934, 2020 Dec 23.
Article En | MEDLINE | ID: mdl-33317266

The use of polyetheretherketone (PEEK) has grown exponentially in the biomedical field in recent decades because of its outstanding biomechanical properties. However, its lack of bioactivity/osteointegration remains an unresolved issue toward its wide use in orthopedic applications. In this work, graphene nanosheets have been incorporated into PEEK to obtain multifunctional nanocomposites. Because of the formation of an electrical percolation network and the π-π* conjugation between graphene and PEEK, the resulting composites have achieved 12 orders of magnitude enhancement in their electrical conductivity and thereby enabled electrophoretic deposition of a bioactive/antibacterial coating consisting of stearyltrimethylammonium chloride-modified hydroxyapatite. The coated composite implant shows significant boosting of bone marrow mesenchymal stem cell proliferation in vitro. In addition, the strong photothermal conversion effect of the graphene nanofillers has enabled laser-induced heating of our nanocomposite implants, where the temperature of the implant can reach 45 °C in 150 s. The unique multifunctionality of the implant has also been demonstrated for photothermal applications such as enhancing bacterial eradication and tumor cell inhibition, as well as bone tissue regeneration in vivo. The results suggest the strong potential of our multifunctional implant in bone repair applications as well as multimodal therapy of challenging bone diseases such as osteosarcoma and osteomyelitis.


Bone Regeneration/drug effects , Coated Materials, Biocompatible/pharmacology , Graphite/chemistry , Ketones/chemistry , Nanocomposites/chemistry , Polyethylene Glycols/chemistry , Animals , Anti-Bacterial Agents/pharmacology , Benzophenones , Cell Line, Tumor , Cell Proliferation/drug effects , Coated Materials, Biocompatible/chemistry , Coated Materials, Biocompatible/radiation effects , Durapatite/pharmacology , Electric Conductivity , Escherichia coli/drug effects , Female , Graphite/radiation effects , Humans , Infrared Rays , Ketones/radiation effects , Mesenchymal Stem Cells/drug effects , Mice, Inbred BALB C , Nanocomposites/radiation effects , Neoplasms/drug therapy , Osseointegration/drug effects , Photothermal Therapy/methods , Polyethylene Glycols/radiation effects , Polymers , Quaternary Ammonium Compounds/pharmacology , Staphylococcus aureus/drug effects , Xenograft Model Antitumor Assays
14.
ACS Appl Mater Interfaces ; 12(51): 57410-57420, 2020 Dec 23.
Article En | MEDLINE | ID: mdl-33289538

The development of intelligent and multifunctional hydrogels having photothermal properties, good mechanical properties, sustained drug release abilities with low burst release, antibacterial properties, and biocompatibility is highly desirable in the biomaterial field. Herein, mesoporous polydopamine (MPDA) nanoparticles wrapped with graphene oxide (GO) were physically cross-linked in cellulose nanofibril (CNF) hydrogel to obtain a novel MPDA@GO/CNF composite hydrogel for controllable drug release. MPDA nanoparticles exhibited a high drug loading ratio (up to 35 wt %) for tetracycline hydrochloride (TH). GO was used to encapsulate MPDA nanoparticles for extending the drug release time and reinforcing the physical strength of the obtained hydrogel. The mechanical strength of the as-fabricated MPDA@GO/CNF composite hydrogel was five times greater compared to that of the pure CNF hydrogel. Drug release experiments demonstrated that burst release behavior was significantly reduced by adding MPDA@GO. The drug release time of the MPDA@GO/CNF composite hydrogel was 3 times and 7.2 times longer than that of the polydopamine/CNF hydrogel and pure CNF hydrogel, respectively. The sustained and controlled drug release behaviors of the composite hydrogel were highly dependent on the proportion of MPDA and GO. Moreover, the rate of drug release could be accelerated by near-infrared (NIR) light irradiation and pH value change. The drug release kinetics of the as-prepared composite hydrogel was well described by the Korsmeyer-Peppas model, and the drug release mechanism of TH from the composite hydrogel was anomalous transport. Importantly, this carefully designed MPDA@GO/CNF composite hydrogel showed good biocompatibility through an in vitro cytotoxicity test. In particular, the toxicity of GO was well shielded by the CNF hydrogel. Therefore, this novel MPDA@GO/CNF composite hydrogel with an encapsulation structure for controllable drug release and toxicity shielding of GO could be used as a very promising controlled drug delivery carrier, which may have potential applications for chemical and physical therapies.


Cellulose/chemistry , Drug Carriers/chemistry , Graphite/chemistry , Hydrogels/chemistry , Indoles/chemistry , Nanofibers/chemistry , Polymers/chemistry , Cellulose/radiation effects , Cellulose/toxicity , Delayed-Action Preparations/chemistry , Delayed-Action Preparations/radiation effects , Delayed-Action Preparations/toxicity , Drug Carriers/radiation effects , Drug Carriers/toxicity , Drug Liberation/radiation effects , Graphite/radiation effects , Graphite/toxicity , Human Umbilical Vein Endothelial Cells , Humans , Hydrogels/radiation effects , Hydrogels/toxicity , Indoles/radiation effects , Indoles/toxicity , Infrared Rays , Nanofibers/radiation effects , Nanofibers/toxicity , Polymers/radiation effects , Polymers/toxicity , Tetracycline/chemistry
15.
J Mater Chem B ; 8(36): 8294-8304, 2020 09 23.
Article En | MEDLINE | ID: mdl-32785373

Highly efficient photoactive antimicrobial coatings were obtained using zinc oxide-reduced graphene oxide nanocomposites (ZnO-rGO). Their remarkable antibacterial activity and high stability demonstrated their potential use for photoactive biocide surfaces. The ZnO-rGO nanocomposites were prepared by the sol-gel technique to create photocatalytic surfaces by spin-coating. The coatings were deeply characterised and several tests were performed to assess the antibacterial mechanisms. rGO was homogeneously distributed as thin sheets decorated with ZnO nanoparticles. The surface roughness and the hydrophobicity increased with the incorporation of graphene. The ZnO-rGO coatings exhibited high activity against the Gram-positive bacterium Staphylococcus aureus. The 1 wt% rGO coated surfaces showed the highest antibacterial effect in only a few minutes of illumination with up to 5-log reduction in colony forming units, which remained essentially free of bacterial colonization and biofilm formation. We demonstrated that these coatings impaired the bacterial cells due to cell membrane damage and intracellular oxidative stress produced by the photogenerated reactive-oxygen species (ROS). The enhancement of the ZnO photocatalytic performance upon rGO incorporation is due to the increased detected generation of hydroxyl radicals, attributed to the reduction of electron-hole pair recombination. This intimate contact between both components also conveyed stability against zinc leaching and improved the coating adhesion.


Anti-Bacterial Agents/pharmacology , Graphite/pharmacology , Nanocomposites/chemistry , Zinc Oxide/pharmacology , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/radiation effects , Graphite/chemistry , Graphite/radiation effects , Light , Materials Testing , Microbial Sensitivity Tests , Nanocomposites/radiation effects , Staphylococcus aureus/drug effects , Zinc Oxide/chemistry , Zinc Oxide/radiation effects
16.
Anal Chim Acta ; 1125: 299-307, 2020 Aug 15.
Article En | MEDLINE | ID: mdl-32674777

As a broad-spectrum tetracycline antibiotic, the overuse of oxytetracycline (OTC) causes antibiotics residues in the environment and seriously threats to human health owing to effective antibacterial properties. Thus, it is particularly important to design a photoelectrochemical (PEC) aptasensor to detect OTC with excellent performance. Herein, we developed a selective and stable PEC aptasensor of OTC on the basis of Co3O4 nanoparticles (Co3O4 NPs)/graphitic carbon nitride (g-CN) heterojunction, used as PEC active materials. The Co3O4 NPs were successfully grown on the g-CN via grinding and calcining mixture of Co3O4 precursors and bulk g-CN. The Co3O4/g-CN heterojunction with improved light utilization and promoted electrons/holes separation capability can exhibit higher PEC signal than that of g-CN. In order to implement the purpose of specific recognition, OTC-aptamer was introduced into modified electrode to construct highly selective PEC aptasensor for OTC determination, which can possess wide linear range (0.01-500 nM) with low detection limit (3.5 pM, S/N = 3). This PEC aptasensor platform with excellent selectivity and high stability can provide a practical application in the field of water monitoring.


Aptamers, Nucleotide/chemistry , Biosensing Techniques/methods , Electrochemical Techniques/methods , Metal Nanoparticles/chemistry , Oxytetracycline/analysis , Photochemistry/methods , Base Sequence , Cobalt/chemistry , Cobalt/radiation effects , Graphite/chemistry , Graphite/radiation effects , Light , Limit of Detection , Metal Nanoparticles/radiation effects , Nitrogen Compounds/chemistry , Nitrogen Compounds/radiation effects , Oxides/chemistry , Oxides/radiation effects , Oxytetracycline/chemistry , Reproducibility of Results , Rivers/chemistry , Water Pollutants, Chemical/analysis , Water Pollutants, Chemical/chemistry
17.
Molecules ; 25(13)2020 Jun 30.
Article En | MEDLINE | ID: mdl-32630005

In this paper, we report the preparation of a new composite (TiO2/SiO2/γ-Fe2O3/rGO) with a high photocatalytic efficiency. The properties of the composite were examined by different analyses, including X-ray diffraction (XRD), field emission scanning electron microscope (FE-SEM), photoluminescence (PL), UV-Visible light diffuse reflectance spectroscopy, Fourier transform infrared spectroscopy (FTIR), Raman, vibrating-sample magnetometer (VSM), and nitrogen gas physisorption (BET) studies. The photocatalytic efficiency of the proposed composite was evaluated by the degradation of methylene blue under UV and visible light, and the results were compared with titanium dioxide (TiO2), where degradation increased from 30% to 84% and 4% to 66% under UV and visible light, respectively. The significant increase in photocatalytic activity may be explained by the higher adsorption of dye on the surface of the composite and the higher separation and transfer of charge carriers, which in turn promote active sites and photocatalytic efficiency.


Ferric Compounds/chemistry , Graphite/chemistry , Magnetics , Photochemistry , Silicon Dioxide/chemistry , Titanium/chemistry , Catalysis , Ferric Compounds/radiation effects , Graphite/radiation effects , Light , Photoelectron Spectroscopy , Silicon Dioxide/radiation effects , Titanium/radiation effects , Ultraviolet Rays
18.
Mikrochim Acta ; 187(8): 449, 2020 07 16.
Article En | MEDLINE | ID: mdl-32676680

Graphitic carbon nitride (g-C3N4) as an outstanding photoresponsive nanomaterial has been widely used in biosensing. Other than the conventional single channel sensing mode, a triple-channel sensing array was developed for high discrimination of proteins based on the photoresponsive g-C3N4. Besides the photoluminescence and Rayleigh light scattering features of g-C3N4, we exploit the new photosensitive colorimetry of g-C3N4 as the third channel optical input. The triple-channel optical behavior of g-C3N4 can be synchronously changed after interaction with the protein, resulting in the distinct response patterns related to each specific protein. Such a triple-channel sensing array is demonstrated for highly discriminative and precise identification of nine proteins (hemoglobin, trypsin, lysozyme, cytochrome c, horseradish peroxidase, transferrin, human serum albumin, pepsin, and myoglobin) at 1 µM concentration levels with 100% accuracy. It also can discriminate proteins being present at different concentration and protein mixtures with different content ratios. The practicability of this sensor array is validated by high accuracy identification of nine proteins in human urine samples. This indicates that the array has a great potential in terms of analyzing biological fluids. Graphic abstract .


Graphite/chemistry , Nanostructures/chemistry , Nitrogen Compounds/chemistry , Proteins/analysis , Armoracia/enzymology , Colorimetry/methods , Graphite/radiation effects , Humans , Light , Nanostructures/radiation effects , Nitrogen Compounds/radiation effects , Urine/chemistry
19.
Toxicol Mech Methods ; 30(7): 508-525, 2020 Sep.
Article En | MEDLINE | ID: mdl-32375587

Pathogenic microorganism delays wound-healing process by causing infection. In recent years, researchers have developed various kinds of photo-active nanomaterials with enhanced antibacterial properties. This work focus on the preparation of graphene oxide and TiO2 nanocomposites (GO/TiO2) as a visible light-induced high efficiency antibacterial material. The hydrothermal method was used for the synthesis of GO/TiO2 nanocomposites at 180 oC for 3 h with different loading percentages of GO (10, 20, 30, 40 and 50 wt. %). The systematic characterization tools including X-ray diffraction analysis, FT-IR, UV-vis, Raman and TEM which were used to understand the physicochemical properties of the prepared GO/TiO2 nanocomposites. Furthermore, GO/TiO2 nanocomposites were used as photocatalytic active materials against wound infection-causing bacteria in the presence of visible light irradiation. The possible antibacterial mechanism under presence and absence of light were depicted. The antibacterial mechanism of the GO/TiO2 nanocomposite was investigated on wound infection-causing bacteria such as Staphylococcus aureus, Pseudomonas aeruginosa, Escherichia coli, and Enterococcus faecalis. The high hemocompatibility and the cellular biocompatibility of the nanocomposite aids in using it for wound-healing application. Overall, the results suggest that the GO/TiO2 nanocomposite could be developed as a photo-active nanomaterial against pathogenic microorganisms that are present in wound.


Anti-Bacterial Agents/pharmacology , Bacteria/drug effects , Graphite/pharmacology , Nanocomposites , Titanium/pharmacology , Wound Healing/drug effects , Wound Infection/drug therapy , Animals , Anti-Bacterial Agents/radiation effects , Anti-Bacterial Agents/toxicity , Bacteria/genetics , Bacteria/growth & development , Biofilms/drug effects , Biofilms/growth & development , Cell Survival/drug effects , DNA Damage , DNA, Bacterial/drug effects , DNA, Bacterial/genetics , Graphite/radiation effects , Graphite/toxicity , Hemolysis/drug effects , Humans , Mice , Microbial Viability/drug effects , NIH 3T3 Cells , Oxidative Stress/drug effects , Photochemical Processes , Titanium/radiation effects , Titanium/toxicity , Wound Infection/microbiology
20.
ACS Appl Mater Interfaces ; 12(21): 23677-23688, 2020 May 27.
Article En | MEDLINE | ID: mdl-32380825

As a newly emerging treatment strategy for many diseases, hydrogen therapy has attracted a lot of attention because of its excellent biosafety. However, the high diffusivity and low solubility of hydrogen make it difficult to accumulate in local lesions. Herein, we develop a H2 self-generation nanoplatform by in situ water splitting driven by near-infrared (NIR) laser. In this work, core-shell nanoparticles (CSNPs) of NaGdF4:Yb,Tm/g-C3N4/Cu3P (UCC) nanocomposites as core encapsulated with zeolitic imidazolate framework-8 (ZIF-8) modified with folic acid as shell are designed and synthesized. Due to the acid-responsive ZIF-8 shell, enhanced permeability and retention (EPR) effect, and folate receptor-mediated endocytosis, CSNPs are selectively captured by tumor cells. Upon 980 nm laser irradiation, CSNPs exhibit a high production capacity of H2 and active oxygen species (ROS), as well as an appropriate photothermal conversion temperature. Furthermore, rising temperature increases the Fenton reaction rate of Cu(I) with H2O2 and strengthens the curative effect of chemodynamic therapy (CDT). The excess glutathione (GSH) in tumor microenvironment (TME) can deplete positive holes produced in the valence band of g-C3N4 in the g-C3N4/Cu3P Z-scheme heterojunction. GSH also can reduce Cu(II) to Cu(I), ensuring a continuous Fenton reaction. Thus, a NIR-driven H2 production nanoplatform is constructed for H2-mediated cascade-amplifying multimodal synergetic therapy.


Anti-Inflammatory Agents/therapeutic use , Antineoplastic Agents/therapeutic use , Hydrogen/therapeutic use , Nanoparticles/therapeutic use , Neoplasms/drug therapy , Water/chemistry , Animals , Anti-Inflammatory Agents/chemistry , Antineoplastic Agents/chemistry , Antineoplastic Agents/radiation effects , Cell Line, Tumor , Copper/chemistry , Copper/radiation effects , Fluorides/chemistry , Fluorides/radiation effects , Gadolinium/chemistry , Gadolinium/radiation effects , Graphite/chemistry , Graphite/radiation effects , Humans , Hydrogen/chemistry , Hyperthermia, Induced/methods , Infrared Rays , Lasers , Mice , Nanoparticles/chemistry , Nanoparticles/radiation effects , Nitrogen Compounds/chemistry , Nitrogen Compounds/radiation effects , Photochemotherapy/methods , Reactive Oxygen Species/metabolism , Thulium/chemistry , Thulium/radiation effects , Ytterbium/chemistry , Ytterbium/radiation effects
...