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1.
Nanoscale ; 15(46): 18550-18570, 2023 Nov 30.
Article in English | MEDLINE | ID: mdl-37962424

ABSTRACT

Nanotechnology brings hope for targeted drug delivery. However, most current drug delivery systems use passive delivery strategies with limited therapeutic efficiency. Over the past two decades, research on micro/nanomotors (MNMs) has flourished in the biomedical field. Compared with other driven methods, light-driven MNMs have the advantages of being reversible, simple to control, clean, and efficient. Under light irradiation, the MNMs can overcome several barriers in the body and show great potential in the treatment of various diseases, such as tumors, and gastrointestinal, cardiovascular and cerebrovascular diseases. Herein, the classification and mechanism of light-driven MNMs are introduced briefly. Subsequently, the applications of light-driven MNMs in overcoming physiological and pathological barriers in the past five years are highlighted. Finally, the future prospects and challenges of light-driven MNMs are discussed as well. This review will provide inspiration and direction for light-driven MNMs to overcome biological barriers in vivo and promote the clinical application of light-driven MNMs in the biomedical field.


Subject(s)
Nanostructures , Neoplasms , Humans , Nanostructures/radiation effects , Nanotechnology/methods , Drug Delivery Systems , Neoplasms/diagnosis , Neoplasms/drug therapy
2.
Adv Sci (Weinh) ; 10(25): e2301854, 2023 09.
Article in English | MEDLINE | ID: mdl-37386797

ABSTRACT

Optoelectronic biointerfaces have gained significant interest for wireless and electrical control of neurons. Three-dimentional (3D) pseudocapacitive nanomaterials with large surface areas and interconnected porous structures have great potential for optoelectronic biointerfaces that can fulfill the requirement of high electrode-electrolyte capacitance to effectively transduce light into stimulating ionic currents. In this study, the integration of 3D manganese dioxide (MnO2 ) nanoflowers into flexible optoelectronic biointerfaces for safe and efficient photostimulation of neurons is demonstrated. MnO2 nanoflowers are grown via chemical bath deposition on the return electrode, which has a MnO2 seed layer deposited via cyclic voltammetry. They facilitate a high interfacial capacitance (larger than 10 mF cm-2 ) and photogenerated charge density (over 20 µC cm-2 ) under low light intensity (1 mW mm-2 ). MnO2 nanoflowers induce safe capacitive currents with reversible Faradaic reactions and do not cause any toxicity on hippocampal neurons in vitro, making them a promising material for biointerfacing with electrogenic cells. Patch-clamp electrophysiology is recorded in the whole-cell configuration of hippocampal neurons, and the optoelectronic biointerfaces trigger repetitive and rapid firing of action potentials in response to light pulse trains. This study points out the potential of electrochemically-deposited 3D pseudocapacitive nanomaterials as a robust building block for optoelectronic control of neurons.


Subject(s)
Electrochemistry , Light , Manganese Compounds , Nanostructures , Neurons , Oxides , Action Potentials/radiation effects , Electric Capacitance , Electrochemistry/methods , Electrodes , Electrolytes/chemistry , Electrolytes/radiation effects , Electrophysiology , Hippocampus/cytology , Manganese Compounds/chemistry , Nanostructures/adverse effects , Nanostructures/chemistry , Nanostructures/radiation effects , Neurons/metabolism , Neurons/radiation effects , Oxides/chemistry , Patch-Clamp Techniques , Photic Stimulation , Wireless Technology , Humans , Animals , Rats
3.
Int J Biol Macromol ; 245: 125577, 2023 Aug 01.
Article in English | MEDLINE | ID: mdl-37379944

ABSTRACT

In this study, graphene oxide/N-halamine nanocomposite was synthesized through Pickering miniemulsion polymerization, which was then coated on cotton surface. The modified cotton exhibited excellent superhydrophobicity, which could effectively prevent microbial infestation and reduce the probability of hydrolysis of active chlorine, with virtually no active chlorine released in water after 72 h. Deposition of reduced graphene oxide nanosheets endowed cotton with ultraviolet-blocking properties, attributing to enhanced UV adsorption and long UV paths. Moreover, encapsulation of polymeric N-halamine resulted in improved UV stability, thus extending the life of N-halamine-based agents. After 24 h of irradiation, 85 % of original biocidal component (active chlorine content) was retained, and approximately 97 % of initial chlorine could be regenerated. Modified cotton has been proven to be an effective oxidizing material against organic pollutants and a potential antimicrobial substance. Inoculated bacteria were completely killed after 1 and 10 min of contact time, respectively. An innovative and simple scheme for determination of active chlorine content was also devised, and real-time inspection of bactericidal activity could be achieved to assure antimicrobial sustainability. Moreover, this method could be utilized to evaluate hazard classification of microbial contamination in different locations, thus broadening the application scope of N-halamine-based cotton fabrics.


Subject(s)
Amines , Anti-Bacterial Agents , Cotton Fiber , Gossypium , Latex , Nanostructures , Polymerization , Amines/chemistry , Amines/radiation effects , Anti-Bacterial Agents/chemical synthesis , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/radiation effects , Biofilms/drug effects , Chlorine/chemistry , Coloring Agents , Cotton Fiber/microbiology , Cotton Fiber/radiation effects , Disinfectants/chemistry , Disinfectants/radiation effects , Electric Conductivity , Equipment Contamination/prevention & control , Gossypium/chemistry , Gossypium/microbiology , Graphite/chemistry , Halogenation , Hydrophobic and Hydrophilic Interactions , Latex/chemistry , Latex/radiation effects , Nanostructures/chemistry , Nanostructures/radiation effects , Particle Size , Spectroscopy, Fourier Transform Infrared , Textile Industry/methods , Ultraviolet Rays , Water/chemistry
4.
J Mater Chem B ; 10(2): 204-213, 2022 01 05.
Article in English | MEDLINE | ID: mdl-34935026

ABSTRACT

The treatment of melanoma requires not only the elimination of skin cancer cells but also skin regeneration to heal defects. To achieve this goal, a bifunctional composite scaffold of poly(DL-lactic-co-glycolic acid) (PLGA), collagen and black phosphorus nanosheets (BPNSs) was prepared by hybridizing a BPNS-embedded collagen sponge with a PLGA knitted mesh. The composite mesh increased the temperature under near-infrared laser irradiation. The incorporation of BPNSs provided the PLGA-collagen-BPNS composite mesh with excellent photothermal properties for the photothermal ablation of melanoma cells both in vitro and in vivo. The PLGA-collagen-BPNS composite mesh had high mechanical strength for easy handling. The PLGA-collagen-BPNS composite mesh facilitated the proliferation of fibroblasts, promoted the expression of angiogenesis-related genes and the genes of components of the extracellular matrix for skin tissue regeneration. The high mechanical strength, photothermal ablation capability and skin tissue regeneration effects demonstrate that the bifunctional PLGA-collagen-BPNS composite mesh is a versatile and effective platform for the treatment of melanoma and the regeneration of skin defects.


Subject(s)
Antineoplastic Agents/therapeutic use , Melanoma/drug therapy , Phosphorus/therapeutic use , Regeneration/drug effects , Skin Physiological Phenomena/drug effects , Tissue Scaffolds/chemistry , Animals , Antineoplastic Agents/chemistry , Antineoplastic Agents/radiation effects , Cell Line, Tumor , Collagen/chemistry , Female , Humans , Infrared Rays , Mice, Inbred BALB C , Mice, Nude , Nanostructures/chemistry , Nanostructures/radiation effects , Nanostructures/therapeutic use , Phosphorus/chemistry , Phosphorus/radiation effects , Photothermal Therapy/methods , Polylactic Acid-Polyglycolic Acid Copolymer/chemistry , Tissue Engineering/methods
5.
Int J Mol Sci ; 22(23)2021 Nov 29.
Article in English | MEDLINE | ID: mdl-34884744

ABSTRACT

Cellulose materials and products are frequently affected by environmental factors such as light, temperature, and humidity. Simulated UV irradiation, heat, and moisture exposure were comprehensively used to characterize changes in cellulose nanopaper (NP) tensile properties. For the preparation of NP, high-purity cellulose from old, unused filter paper waste was used. Lignin and xylan were used as sustainable green interface engineering modifiers for NP due to their structural compatibility, low price, nontoxic nature, and abundance as a by-product of biomass processing, as well as their ability to protect cellulose fibers from UV irradiation. Nanofibrillated cellulose (NFC) suspension was obtained by microfluidizing cellulose suspension, and NP was produced by casting films from water suspensions. The use of filler from 1 to 30 wt% significantly altered NP properties. All nanopapers were tested for their sensitivity to water humidity, which reduced mechanical properties from 10 to 40% depending on the saturation level. Xylan addition showed a significant increase in the specific elastic modulus and specific strength by 1.4- and 2.8-fold, respectively. Xylan-containing NPs had remarkable resistance to UV irradiation, retaining 50 to 90% of their initial properties. Lignin-modified NPs resulted in a decreased mechanical performance due to the particle structure of the filler and the agglomeration process, but it was compensated by good property retention and enhanced elongation. The UV oxidation process of the NP interface was studied with UV-Vis and FTIR spectroscopy, which showed that the degradation of lignin and xylan preserves a cellulose fiber structure. Scanning electron microscopy images revealed the structural formation of the interface and supplemented understanding of UV aging impact on the surface and penetration depth in the cross-section. The ability to overcome premature aging in environmental factors can significantly benefit the wide adaption of NP in food packaging and functional applications.


Subject(s)
Cellulose/chemistry , Lignin/chemistry , Nanostructures/chemistry , Xylans/chemistry , Materials Testing , Nanostructures/radiation effects
6.
ACS Appl Mater Interfaces ; 13(41): 49482-49489, 2021 Oct 20.
Article in English | MEDLINE | ID: mdl-34636536

ABSTRACT

Although organic artificial enzymes have been reported as biomimetic oxidation catalysts and are widely used for colorimetric biosensors, developing organic artificial enzymes with high enzymatic activity is still a challenge. Two-dimensional (2D) covalent organic frameworks (COFs) have shown superior potential in biocatalysts because of their periodic π-π arrays, tunable pore size and structure, large surface area, and thermal stability. The interconnection of electron acceptor and donor building blocks in the 2D conjugated COF skeleton can lead to narrower band gaps and efficient charge separation and transportation and thus is helpful to improve catalytic activity. Herein, a donor-acceptor 2D COF was synthesized using tetrakis(4-aminophenyl)pyrene (Py) as an electron donor and thieno[3,2-b]thiophene-2,5-dicarbaldehyde (TT) as an electron acceptor. Under visible light irradiation, the donor-acceptor 2D COF exhibited superior enzymatic catalytic activity, which could catalyze the oxidation of chromogenic substrates such as 3,3',5,5'-tetramethylbenzidine (TMB) by the formation of superoxide radicals and holes. Based on the above property, the photoactivated donor-acceptor 2D COF with enzyme-like catalytic properties was designed as a robust colorimetric probe for cheap, highly sensitive, and rapid colorimetric detection of glutathione (GSH); the corresponding linear range of GSH was 0.4-60 µM, and the limit of detection was 0.225 µM. This study not only presents the construction of COF-based light-activated nanozymes for environmentally friendly colorimetric detection of GSH but also provides a smart strategy for improving nanozyme activity.


Subject(s)
Glutathione/blood , Metal-Organic Frameworks/chemistry , Nanostructures/chemistry , Benzidines/chemistry , Catalysis/radiation effects , Chromogenic Compounds/chemistry , Colorimetry/methods , Density Functional Theory , Glutathione/chemistry , Humans , Light , Limit of Detection , Metal-Organic Frameworks/chemical synthesis , Metal-Organic Frameworks/radiation effects , Models, Chemical , Nanostructures/radiation effects , Oxidation-Reduction , Pyrenes/chemical synthesis , Pyrenes/chemistry , Pyrenes/radiation effects , Thiophenes/chemical synthesis , Thiophenes/chemistry , Thiophenes/radiation effects
7.
ACS Appl Mater Interfaces ; 13(36): 43414-43425, 2021 Sep 15.
Article in English | MEDLINE | ID: mdl-34472827

ABSTRACT

Two-dimensional material titanium carbide (Ti3C2Tx MXene) has been widely used for building diverse functional materials; however, the disadvantages of unsatisfactory yield and low concentration during the preparation process generally limit its large-scale promotion. In the present work, an MXene dispersion with enhanced yield (90%), high concentration (45 mg/mL), and excellent dispersibility was successfully prepared. Subsequently, the active MXene nanosheets were effectively in situ deposition onto the silk fiber by means of dip-coating, relying on van der Waals forces and hydrogen bonds. The obtained MXene-decorated silk fabric (MXene@silk) exhibits satisfactory electrical conductivity (170 mS/cm), excellent photothermal and electrothermal conversion properties, especially dual-drive energy conversion, rapid thermal responses, and long-term functional stability. Furthermore, UV protection factor of the fabric, and its antibacterial efficiency against Gram-negative Escherichia coli (E. coli) within 20 min of contact reach over 110 and 99%, respectively, demonstrating remarkable UV resistance and rapid photothermal antibacterial ability. Meanwhile, the fabric of MXene@silk still retains the original characteristics of breathability, softness, and skin-friendly properties compared to the untreated. The multifunctional fabric constructed through a facile and high-yield strategy shows a noticeable potential applying to smart textiles to meet people's multipurpose needs in the future.


Subject(s)
Anti-Bacterial Agents/pharmacology , Nanostructures/chemistry , Silk/chemistry , Textiles , Wearable Electronic Devices , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/radiation effects , Electric Conductivity , Escherichia coli/drug effects , Heating , Light , Nanostructures/radiation effects , Silk/radiation effects , Textiles/radiation effects , Titanium/chemistry , Titanium/pharmacology , Titanium/radiation effects
8.
ACS Appl Mater Interfaces ; 13(37): 43855-43867, 2021 Sep 22.
Article in English | MEDLINE | ID: mdl-34494809

ABSTRACT

Black phosphorus (BP) nanosheet is easily oxidized by oxygen and water under ambient environment, thus, reliable BP passivation techniques for biomedical applications is urgently needed. A simple and applicable passivation strategy for biomedical applications was established by encapsulating BP nanosheet into zeolitic imidazole framework-8 (ZIF-8). The resulted BP nanosheet in ZIF-8 (BP@ZIF-8) shows not only satisfied chemical stability in both water and phosphate buffered saline (PBS), but also excellent biocompatibility. Notably, BP nanosheet endows the prepared BP@ZIF-8 with prominent photothermal conversion efficiency (31.90%). Besides passivation BP, ZIF-8 provides the BP@ZIF-8 with high drug loading amount (1353.3 mg g-1). Moreover, the loaded drug can be controlled release by pH stimuli. Both in vitro and in vivo researches verified the resulted BP@ZIF-8 an ideal candidate for tumor multimodal treatments.


Subject(s)
Antineoplastic Agents/therapeutic use , Drug Carriers/chemistry , Metal-Organic Frameworks/chemistry , Nanostructures/chemistry , Neoplasms/drug therapy , Phosphorus/chemistry , Animals , Antineoplastic Agents/chemistry , Cell Line, Tumor , Combined Modality Therapy , Doxorubicin/chemistry , Doxorubicin/therapeutic use , Drug Carriers/radiation effects , Drug Carriers/toxicity , Drug Liberation , Drug Therapy , Female , Humans , Hydrogen-Ion Concentration , Infrared Rays , Metal-Organic Frameworks/radiation effects , Metal-Organic Frameworks/toxicity , Mice , Nanostructures/radiation effects , Nanostructures/toxicity , Phosphorus/radiation effects , Phosphorus/toxicity , Photothermal Therapy
9.
J Am Chem Soc ; 143(36): 14635-14645, 2021 09 15.
Article in English | MEDLINE | ID: mdl-34410692

ABSTRACT

Antibodies are recognition molecules that can bind to diverse targets ranging from pathogens to small analytes with high binding affinity and specificity, making them widely employed for sensing and therapy. However, antibodies have limitations of low stability, long production time, short shelf life, and high cost. Here, we report a facile approach for the design of luminescent artificial antibodies with nonbiological polymeric recognition phases for the sensitive detection, rapid identification, and effective inactivation of pathogenic bacteria. Transition-metal dichalcogenide (TMD) nanosheets with a neutral dextran phase at the interfaces selectively recognized S. aureus, whereas the nanosheets bearing a carboxymethylated dextran phase selectively recognized E. coli O157:H7 with high binding affinity. The bacterial binding sites recognized by the artificial antibodies were thoroughly identified by experiments and molecular dynamics simulations, revealing the significance of their multivalent interactions with the bacterial membrane components for selective recognition. The luminescent WS2 artificial antibodies could rapidly detect the bacteria at a single copy from human serum without any purification and amplification. Moreover, the MoSe2 artificial antibodies selectively killed the pathogenic bacteria in the wounds of infected mice under light irradiation, leading to effective wound healing. This work demonstrates the potential of TMD artificial antibodies as an alternative to antibodies for sensing and therapy.


Subject(s)
Anti-Bacterial Agents/therapeutic use , Escherichia coli Infections/drug therapy , Luminescent Agents/therapeutic use , Nanostructures/therapeutic use , Animals , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/radiation effects , Dextrans/chemistry , Escherichia coli O157/drug effects , Escherichia coli O157/isolation & purification , Light , Luminescent Agents/chemistry , Luminescent Agents/radiation effects , Mice , Molecular Dynamics Simulation , Molybdenum/chemistry , Molybdenum/radiation effects , Molybdenum/therapeutic use , Nanostructures/chemistry , Nanostructures/radiation effects , Photothermal Therapy , Selenium Compounds/chemistry , Selenium Compounds/radiation effects , Selenium Compounds/therapeutic use , Skin/microbiology , Spectrum Analysis, Raman , Staphylococcus aureus/drug effects , Staphylococcus aureus/isolation & purification , Sulfides/chemistry , Sulfides/radiation effects , Sulfides/therapeutic use , Tungsten Compounds/chemistry , Tungsten Compounds/radiation effects , Tungsten Compounds/therapeutic use , Wound Healing/drug effects
10.
Carbohydr Polym ; 271: 118386, 2021 Nov 01.
Article in English | MEDLINE | ID: mdl-34364585

ABSTRACT

A series of fluorescent nanocomplexes of carboxymethyl cellulose (CMC)/Terbium (Tb)- Europium (Eu) were successfully synthesized without introducing a second ligand. By adjusting the concentration of the coordinated ions, these nanocomplexes exhibit favorably visibly tunable luminescence properties with colors being able to change from green to red. The XPS analysis demonstrates the formation Tb(III)-O2- and Eu(III)-O2- between OH and COO- in CMC and Tb3+ or Eu3+ ions, which is advantage for light absorption by UV-Vis spectroscopy and fluorescence spectroscopy. The ligand CMC plays a role in coordinating with terbium and europium ions, but also serves as an energy donor to these metal ions by antenna effect. Moreover, the energy transfer also occurred from terbium ions to europium ions in CMC matrix, which is responsible for the tunable luminescence properties of these complexes.


Subject(s)
Coordination Complexes/chemistry , Luminescent Agents/chemistry , Nanostructures/chemistry , Carboxymethylcellulose Sodium/chemistry , Coordination Complexes/radiation effects , Energy Transfer , Europium/chemistry , Europium/radiation effects , Ligands , Light , Luminescence , Luminescent Agents/radiation effects , Nanostructures/radiation effects , Terbium/chemistry , Terbium/radiation effects
11.
ACS Appl Mater Interfaces ; 13(28): 32690-32702, 2021 Jul 21.
Article in English | MEDLINE | ID: mdl-34229434

ABSTRACT

The synergistic nanotheranostics of reactive oxygen species (ROS) augment or phototherapy has been a promising method within synergistic oncotherapy. However, it is still hindered by sophisticated design and fabrication, lack of a multimodal synergistic effect, and hypoxia-associated poor photodynamic therapy (PDT) efficacy. Herein, a kind of porous shuttle-shape platinum (IV) methylene blue (Mb) coordination polymer nanotheranostics-loaded 10-hydroxycamptothecin (CPT) is fabricated to address the abovementioned limitations. Our nanoreactors possess spatiotemporally controlled O2 self-supply, self-sufficient singlet oxygen (1O2), and outstanding photothermal effect. Once they are taken up by tumor cells, nanoreactors as a cascade catalyst can efficiently catalyze degradation of the endogenous hydrogen peroxide (H2O2) into O2 to alleviate tumor hypoxia. The production of O2 can ensure enhanced PDT. Subsequently, under both stimuli of external red light irradiation and internal lysosomal acidity, nanoreactors can achieve the on-demand release of CPT to augment in situ mitochondrial ROS and highly efficient tumor ablation via phototherapy. Moreover, under the guidance of near-infrared (NIR) fluorescent imaging, our nanoreactors exhibit strongly synergistic potency for treatment of hypoxic tumors while reducing damages against normal tissues and organs. Collectively, shuttle-shape platinum-coordinated nanoreactors with augmented ROS capacity and enhanced phototherapy efficiency can be regarded as a novel tumor theranostic agent and further promote the research of synergistic oncotherapy.


Subject(s)
Antineoplastic Agents/therapeutic use , Camptothecin/analogs & derivatives , Drug Carriers/chemistry , Nanostructures/chemistry , Neoplasms/drug therapy , Tumor Hypoxia/drug effects , Animals , Antineoplastic Agents/chemistry , Camptothecin/chemistry , Camptothecin/therapeutic use , Catalysis/radiation effects , Cell Line, Tumor , Drug Carriers/radiation effects , Drug Liberation , Female , Humans , Hydrogen Peroxide/chemistry , Hydrogen Peroxide/metabolism , Light , Methylene Blue/analogs & derivatives , Methylene Blue/radiation effects , Mice, Inbred BALB C , Nanostructures/radiation effects , Neoplasms/metabolism , Oxygen/metabolism , Photosensitizing Agents/chemistry , Photosensitizing Agents/therapeutic use , Photothermal Therapy , Platinum/chemistry , Platinum/radiation effects , Polymers/chemical synthesis , Polymers/chemistry , Polymers/radiation effects , Porosity , Singlet Oxygen/metabolism , Theranostic Nanomedicine
12.
ACS Appl Mater Interfaces ; 13(26): 30274-30283, 2021 Jul 07.
Article in English | MEDLINE | ID: mdl-34170100

ABSTRACT

In this work, an iron self-boosting polymer nanoenzyme was prepared by using pyrrole-3-carboxylic acid as a monomer and iron as an oxidizing agent via a simple and one-step method [hereafter referred to as FePPy nanoparticles (NPs)]. In fact, researchers previously paid negligible attention on the iron element during the polymerization reaction of polypyrrole, thus the intrinsically catalytic functions and enzymatic activities of the high iron content (wt %: 21.11%) are ignored and not fully explored. As expected, results demonstrate that the as-synthesized FePPy NPs can decompose H2O2 to generate hydroxyl radicals (•OH) which exhibit enzyme characteristics, further inducing a nonapoptotic ferroptosis pathway. Moreover, the nanoenzyme shows impressive photothermal properties which can accelerate the Fenton reactions to enhance ferroptosis. The combined photothermal and ferroptosis therapy of FePPy NPs was found to have high efficacy. With the properties of easy synthesis, high efficacy, and good biocompatibility, the FePPy NPs are considered as potential agents for cancer treatments.


Subject(s)
Antineoplastic Agents/therapeutic use , Ferroptosis/drug effects , Nanostructures/therapeutic use , Neoplasms/drug therapy , Photosensitizing Agents/therapeutic use , Animals , Antineoplastic Agents/chemistry , Antineoplastic Agents/radiation effects , Carboxylic Acids/chemistry , Carboxylic Acids/radiation effects , Carboxylic Acids/therapeutic use , Catalysis , Female , HeLa Cells , Humans , Hydrogen Peroxide/chemistry , Hydroxyl Radical/metabolism , Iron/chemistry , Iron/radiation effects , Light , Mice, Inbred BALB C , Mice, Nude , Nanostructures/chemistry , Nanostructures/radiation effects , Photosensitizing Agents/chemistry , Photosensitizing Agents/radiation effects , Photothermal Therapy , Polymers/chemistry , Polymers/radiation effects , Polymers/therapeutic use , Pyrroles/chemistry , Pyrroles/radiation effects , Pyrroles/therapeutic use , Temperature
13.
Chem Asian J ; 16(14): 1979-1987, 2021 Jul 19.
Article in English | MEDLINE | ID: mdl-34058080

ABSTRACT

Water oxidation is a bottleneck in artificial photosynthesis that impedes its practicality for solar energy conversion and utilization. It is highly desired to significantly improve the efficacy of the existing catalysts or to rationally design new catalysts with improved performance. We report a novel conjugated and sulfone containing polyimide as a metal-free photocatalyst synthesized via a two-step method: (i) synthesis of precursor poly(amic acid) (PAA) (ii) solvothermal synthesis of polyimide through thermal imidization. The synthesis of the polyimide photocatalyst was demonstrated by the amide linkage in the FTIR spectrum. The obtained photocatalyst was semicrystalline in nature and possessed sheet-like morphology as illustrated by the diffraction pattern and the electron micrographic images, respectively. The thermogravimetric analysis of the polyimide nanosheets validated a thermally stable structure. The DFT calculations were performed which showed a suitable HOMO band position, favorable for water oxidation. The photoelectrocatalytic (PEC) performance of the polyimide nanosheets evaluated by studying water oxidation reaction without any sacrificial agent under 1-SUN showed enhanced PEC performance and good stability towards water oxidation at 0 V versus SCE.


Subject(s)
Nanostructures/chemistry , Naphthalimides/chemistry , Polymers/chemistry , Sulfones/chemistry , Water/chemistry , Catalysis/radiation effects , Density Functional Theory , Light , Models, Chemical , Nanostructures/radiation effects , Naphthalimides/radiation effects , Oxidation-Reduction , Polymers/radiation effects , Sulfones/radiation effects
14.
Dalton Trans ; 50(19): 6598-6619, 2021 May 18.
Article in English | MEDLINE | ID: mdl-33899890

ABSTRACT

MoS2 nanosheets were developed by undertaking the liquid-phase exfoliation of bulk counterparts. In order to enhance its photocatalytic properties, the host material was doped with p-type transition metals (i.e., Ag, Co, Bi, and Zr). The hydrothermal technique was used to produce samples doped with 7.5 wt% transition metals (TM). X-ray diffraction detected the existence of 2H-phase by mirroring its reflection at 2θ ∼ 14°, while the peak distribution revealed the degree of exfoliation in samples. Low PL intensities indicated a lower recombination of electron-hole pairs, as corroborated by a high degree of photocatalytic action. Raman analysis was undertaken to identify molecular vibrations. The A1g mode in Raman spectra consistently showed a blueshift in all samples and the E12g mode was only slightly affected, which is evidence of the p-type doping in the MoS2 nanosheets. In the XPS spectrum, two characteristic peaks of Mo 3d appeared at 229.87 and 233.03 eV assigned to Mo-3d5/2 and Mo-3d3/2, respectively. Furthermore, a microstructural examination with HR-TEM and FESEM divulged a thin-layered structure of MoS2 consisting of flat, gently curved or twisted nanosheets. Diverse morphologies were observed with a non-uniform distribution of the dopant. Photocatalytic action of the TM-doped products effectively degraded methylene blue (MB) concentrations of up to 94 percent (for Ag-MoS2). The synergistic effect of doped MoS2 nanosheets against S. aureus in comparison to E. coli bacteria was also evaluated. The efficacy % age improved from (0-31.7%) and (23.5-55.2%) against E. coli, and (0-34.2%) and (8.3-69.23%) against S. aureus. Moreover, results from first principles calculations indicate that substitutional doping of TM atoms is indeed advantageous. Theoretical calculations confirmed that doping with Ag, Co, Bi, and Zr leads to a decrease in the band gap to a certain degree, in which the conduction band edge shifts toward lower energy, while the valence band shifts closer to the high energy end. It can be concluded that Ag, Co, and Bi impurities can lead to beneficial p-type doping in MoS2 monolayered structures. With regards to doping with Zr, the acceptor levels are formed above the edge of the valence band, revealing an introduction of the p-type character.


Subject(s)
Anti-Bacterial Agents , Disulfides , Nanostructures , Transition Elements , Anti-Bacterial Agents/administration & dosage , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/radiation effects , Catalysis , Disulfides/administration & dosage , Disulfides/chemistry , Disulfides/radiation effects , Escherichia coli/drug effects , Escherichia coli/growth & development , Light , Methylene Blue/chemistry , Microscopy, Electron, Scanning , Microscopy, Electron, Transmission , Nanostructures/administration & dosage , Nanostructures/chemistry , Nanostructures/radiation effects , Nanostructures/ultrastructure , Staphylococcus aureus/drug effects , Staphylococcus aureus/growth & development , Transition Elements/administration & dosage , Transition Elements/chemistry , Transition Elements/radiation effects
15.
Chemistry ; 27(2): 778-784, 2021 Jan 07.
Article in English | MEDLINE | ID: mdl-33063405

ABSTRACT

Stimuli-responsive switching molecules have been widely investigated for the purpose of the mechanical control of biomolecules. Recently developed arylazopyrazole (AAP) shows photoisomerization activity, displaying a faster response to light-induced conformational changes and unique absorption spectral properties compared with those of conventionally used azobenzene. Herein, it is demonstrated that AAP can be used as a photoswitching molecule to control photoinduced assembly and disassembly of DNA origami nanostructures. An AAP-modified DNA origami has been designed and constructed. It is observed that the repeated assembly and disassembly of AAP-modified X-shaped DNA origami and hexagonal origami with complementary strands can be achieved by alternating UV and visible-light irradiation. Closed and linear assemblies of AAP-modified X-shaped origami were successfully formed by photoirradiation, and more than 1 µm linear assemblies were formed. Finally, it is shown that the two photoswitches, AAP and azobenzene, can be used in tandem to independently control different assembly configurations by using different irradiation wavelengths. AAP can extend the variety of available wavelengths of photoswitches and stably result in the assembly and disassembly of various DNA origami nanostructures.


Subject(s)
DNA/chemistry , DNA/radiation effects , Light , Nanostructures/chemistry , Nanostructures/radiation effects , Nucleic Acid Conformation/radiation effects , Photochemical Processes/radiation effects
16.
ACS Appl Mater Interfaces ; 13(1): 1105-1113, 2021 Jan 13.
Article in English | MEDLINE | ID: mdl-33332080

ABSTRACT

Silicon (Si) is a highly abundant, environmentally benign, and durable material and is the most popular semiconductor material; and it is used for the field enhancement of dielectric materials. Porous Si (PSi) exhibits high functionality due to its specific structure. However, the field enhancement of PSi has not been clarified sufficiently. Herein, we present the field enhancement of PSi by the fluorescence intensity enhancement of a dye molecule. The raw material used for producing PSi was rice husk, a biomass material. A nanocoral structure, consisting of spheroidal structures on the surface of PSi, was observed when PSi was subjected to chemical processes and pulsed laser melting, and it demonstrated large field enhancement with an enhancement factor (EF) of up to 545. Confocal microscopy was used for EF mapping of samples before and after laser melting, and the maps were superimposed on nanoscale scanning electron microscope images to highlight the EF effect as a function of microstructure. Nanocoral Si with high EF values were also evaluated by analyzing the porosity from gas adsorption measurements. Nanocoral Si was responsible for the high EF, according to thermodynamic calculations and agreement between experimental and calculation results as determined by Mie scattering theory.


Subject(s)
Nanostructures/chemistry , Silicon/chemistry , Fluorescent Dyes/chemistry , Fluorescent Dyes/radiation effects , Freezing , Gentian Violet/chemistry , Gentian Violet/radiation effects , Light , Models, Chemical , Nanostructures/radiation effects , Oryza/chemistry , Porosity , Silicon/radiation effects
17.
Int J Mol Sci ; 21(22)2020 Nov 21.
Article in English | MEDLINE | ID: mdl-33233379

ABSTRACT

Polypyrrole one-dimensional nanostructures (nanotubes, nanobelts and nanofibers) were prepared using three various dyes (Methyl Orange, Methylene Blue and Eriochrome Black T). Their high electrical conductivity (from 17.1 to 60.9 S cm-1), good thermal stability (in the range from 25 to 150 °C) and resistivity against ageing (half-time of electrical conductivity around 80 days and better) were used in preparation of lightweight and flexible composites with silicone for electromagnetic interference shielding in the C-band region (5.85-8.2 GHz). The nanostructures' morphology and chemical structure were characterized by scanning electron microscopy, Brunauer-Emmett-Teller specific surface measurement and attenuated total reflection Fourier-transform infrared spectroscopy. DC electrical conductivity was measured using the Van der Pauw method. Complex permittivity and AC electrical conductivity of respective silicone composites were calculated from the measured scattering parameters. The relationships between structure, electrical properties and shielding efficiency were studied. It was found that 2 mm-thick silicone composites of polypyrrole nanotubes and nanobelts shield almost 80% of incident radiation in the C-band at very low loading of conductive filler in the silicone (5% w/w). Resulting lightweight and flexible polypyrrole composites exhibit promising properties for shielding of electromagnetic interference in sensitive biological and electronic systems.


Subject(s)
Electromagnetic Radiation , Nanostructures/chemistry , Polymers/chemistry , Pyrroles/chemistry , Silicones/chemistry , Azo Compounds/chemistry , Methylene Blue/chemistry , Microscopy, Electron, Scanning , Nanofibers/chemistry , Nanofibers/radiation effects , Nanostructures/radiation effects , Nanostructures/ultrastructure , Nanotubes/chemistry , Nanotubes/radiation effects , Nanotubes/ultrastructure , Polymers/radiation effects , Pyrroles/radiation effects , Silicones/radiation effects
18.
J Mater Chem B ; 8(36): 8323-8336, 2020 09 23.
Article in English | MEDLINE | ID: mdl-32793936

ABSTRACT

Exploiting two-dimensional nanomaterials as photo-based theranostic agents is promising for the highly efficient ablation of deep-tissue-buried tumors. However, they are limited by their poor absorption in the second near-infrared-light (NIR-II) bio-window (1000-1300 nm) and intrinsic nonbiodegradability. Herein, defect-rich sulfur-doped Ni(OH)2 (S-Ni(OH)2) nanosheets decorated with bovine serum albumin (BSA) as a novel theranostic agent is developed, which can accomplish multimodal-imaging-guided photothermal ablation of mouse cancers in the NIR-II bio-window. Sulfur doping extends the absorption spectra of Ni(OH)2 nanosheets from the visible to NIR-II bio-window, affording highly efficient photothermal conversion (58.20% for 1064 nm), entailing it to become an excellent contrast agent for photoacoustic imaging. Further, because of their intrinsic paramagnetic property, they can be applied for magnetic resonance imaging. Owing to the abundant defective sites in S-Ni(OH)2 nanosheets, they exhibit response to the tumor microenvironment, resulting in effective biodegradation and excretion from the body. In vivo toxicity experiments indicated that S-Ni(OH)2-BSA NSs delivered no appreciable toxicity and good biocompatibility. This work provides an avenue for the rational design of effective theranostics agents.


Subject(s)
Antineoplastic Agents/therapeutic use , Hydroxides/therapeutic use , Nanostructures/therapeutic use , Neoplasms/diagnostic imaging , Neoplasms/drug therapy , Nickel/therapeutic use , Tumor Microenvironment/drug effects , Animals , Antineoplastic Agents/chemistry , Antineoplastic Agents/pharmacokinetics , Cattle , Female , HeLa Cells , Humans , Hydroxides/chemistry , Hydroxides/pharmacokinetics , Hydroxides/radiation effects , Infrared Rays , Mice, Inbred ICR , Multimodal Imaging , Nanostructures/chemistry , Nanostructures/radiation effects , Nickel/chemistry , Nickel/pharmacokinetics , Nickel/radiation effects , Photothermal Therapy , Serum Albumin, Bovine/chemistry , Serum Albumin, Bovine/pharmacokinetics , Serum Albumin, Bovine/therapeutic use , Sulfur/chemistry , Sulfur/pharmacokinetics , Sulfur/radiation effects , Sulfur/therapeutic use , Theranostic Nanomedicine
19.
ACS Sens ; 5(9): 2663-2678, 2020 09 25.
Article in English | MEDLINE | ID: mdl-32786383

ABSTRACT

The global sanitary crisis caused by the emergence of the respiratory virus SARS-CoV-2 and the COVID-19 outbreak has revealed the urgent need for rapid, accurate, and affordable diagnostic tests to broadly and massively monitor the population in order to properly manage and control the spread of the pandemic. Current diagnostic techniques essentially rely on polymerase chain reaction (PCR) tests, which provide the required sensitivity and specificity. However, its relatively long time-to-result, including sample transport to a specialized laboratory, delays massive detection. Rapid lateral flow tests (both antigen and serological tests) are a remarkable alternative for rapid point-of-care diagnostics, but they exhibit critical limitations as they do not always achieve the required sensitivity for reliable diagnostics and surveillance. Next-generation diagnostic tools capable of overcoming all the above limitations are in demand, and optical biosensors are an excellent option to surpass such critical issues. Label-free nanophotonic biosensors offer high sensitivity and operational robustness with an enormous potential for integration in compact autonomous devices to be delivered out-of-the-lab at the point-of-care (POC). Taking the current COVID-19 pandemic as a critical case scenario, we provide an overview of the diagnostic techniques for respiratory viruses and analyze how nanophotonic biosensors can contribute to improving such diagnostics. We review the ongoing published work using this biosensor technology for intact virus detection, nucleic acid detection or serological tests, and the key factors for bringing nanophotonic POC biosensors to accurate and effective COVID-19 diagnosis on the short term.


Subject(s)
Betacoronavirus , Coronavirus Infections/diagnosis , Nanostructures/chemistry , Pneumonia, Viral/diagnosis , Surface Plasmon Resonance/methods , Antigens, Viral/analysis , Betacoronavirus/chemistry , Betacoronavirus/isolation & purification , COVID-19 , COVID-19 Testing , Clinical Laboratory Techniques , Genome, Viral , Humans , Immunoassay/methods , Nanostructures/radiation effects , Pandemics , SARS-CoV-2 , Serologic Tests/methods
20.
Mikrochim Acta ; 187(8): 449, 2020 07 16.
Article in English | MEDLINE | ID: mdl-32676680

ABSTRACT

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 .


Subject(s)
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
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