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A green and economical methodology to fabricate carbon-based materials with suitable pore size distributions is needed to achieve rapid electrolyte diffusion and improve the performance of supercapacitors. Here, a method combining in situ templates with self-activation and self-doping is proposed. By variation of the molar ratio of magnesium folate and potassium folate, the pore size distribution was effectively adjusted. The optimal carbon materials (Kx) have a high specific surface area (1021-1676 m2 g-1) and hierarchical pore structure, which significantly promotes its excellent capacitive properties. Notably, K2 shows an excellent mass specific capacitance of 233 F g-1 at 0.1 A g-1. It still retained 113 F g-1 at 55 A g-1. The assembled symmetric supercapacitor exhibited an outstanding cyclic stability. It maintains 100% capacitance after 100â¯000 cycles at 10 A g-1. The symmetric supercapacitor demonstrated a maximum power density of 99.8 kW kg-1. This study focuses on the preparation of layered pore structures to provide insights into the sustainable design of carbon materials.
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The preparation of porous carbon is constrained by the extensive use and detrimental impact of activators and dopants. Therefore, developing green and efficient strategies that leverage the intrinsic properties and pretreatment of the materials to achieve self-activation and self-doping is particularly crucial for porous carbon materials. Herein, potassium histidine was utilized as the molecular salt precursor, attaining the efficient and streamlined preparation of porous carbon through a one-step carbonization process that enables self-activation, self-doping, and self-templating. More interestingly, the carbonization temperature significantly impacts the porous structure of the molecular salt precursors, the properties of the heteroatoms, and electrochemical performance. The designed electrodes exhibit high accessibility to electrolyte ions and effective ion-electron transport channels. Therefore, the optimal carbon material (KHis800) has an excellent mass-specific capacitance of 305.2 F g-1 at 0.2 A g-1, and a high capacitance retention rate of 115.6% (50,000 cycles at 5 A g-1). Notably, KHis800 also shows a maximum energy density of 19.6 Wh kg-1. This research is dedicated to exploring a more efficient preparation method for porous carbon material via molecular salts, offering insights for the sustainable development of carbon materials.
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The hierarchical porous carbon-based materials derived from biomass are beneficial for the enhancement of electrochemical performances in supercapacitors. Herein, we report the fabrication of nitrogen-doped 3D flower-like hierarchical porous carbon (NPC) assembled by nanosheets using a mixture of urea, ZnCl2, and starch via a low-temperature hydrothermal reaction and high-temperature carbonization process. As a consequence, the optimized mass ratio for the mixture is 2:2:2 and the temperature is 700 °C. The NPC structures are capable of electron transport and ion diffusion owing to their high specific surface area (1498.4 m2 g-1) and rich heteroatoms. Thereby, the resultant NPC electrodes display excellent capacitive performance, with a high specific capacitance of 249.7 F g-1 at 1.0 A g-1 and good cycling stability. Remarkably, this implies a superior energy density of 42.98 Wh kg-1 with a power density of 7500 W kg-1 in organic electrolyte for the symmetrical supercapacitor. This result verifies the good performance of as-synthesized carbon materials in capacitive energy storage applications, which is inseparable from the hierarchical porous features of the materials.
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N, O Co-Doped porous carbon materials are promising electrode materials for supercapacitors. However, it is still a challenge to prepare high capacitance performance N, O Co-Doped porous carbon materials with balanced pore structure. In this work, a simple chemical blowing method was developed to produce hierarchal porous carbon materials with Zn(NO3)2·6H2O and Fe(NO3)3·9H2O as the foaming agents and precursors of dual templates. Soybean protein isolate served as a self-doping carbon source. The amount of Fe(NO3)3·9H2O influenced the microstructure, element content and capacitance performance of the obtained porous carbon materials. The optimized sample CZnFe-5 with the addition of 5% Fe(NO3)3·9H2O displayed the best capacitance performance. The specific capacitance reached 271 F g-1 at 0.2 A g-1 and retained 133 F g-1 at 100 A g-1. The CZnFe-5//CZnFe-5 symmetric supercapacitors delivered a maximum energy density of 16.83 Wh kg-1 and good stability with capacitance retention of 86.33% after 40,000 cycles tests at 50 A g-1. The symmetric supercapacitors exhibited potential applications in lighting LED bulbs with a voltage of 3 V. This work provides a new strategy for the synthesis of hierarchical porous carbon materials for supercapacitors from low-cost biomass products.
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Self-supporting electrode materials with the advantages of a simple operation process and the avoidance of the use any binders are promising candidates for supercapacitors. In this work, carbon-based self-supporting electrode materials with nanosheets grown on Al foil were prepared by combining hydrothermal reaction and the one-step chemical vapor deposition method. The effect of the concentration of the reaction solution on the structures as well as the electrochemical performance of the prepared samples were studied. With the increase in concentration, the nanosheets of the samples became dense and compact. The CNS-120 obtained from a 120 mmol zinc nitrate aqueous solution exhibited excellent electrochemical performance. The CNS-120 displayed the highest areal capacitance of 6.82 mF cm-2 at the current density of 0.01 mA cm-2. Moreover, the CNS-120 exhibited outstanding rate performance with an areal capacitance of 3.07 mF cm-2 at 2 mA cm-2 and good cyclic stability with a capacitance retention of 96.35% after 5000 cycles. Besides, the CNS-120 possessed an energy density of 5.9 µWh cm-2 at a power density of 25 µW cm-2 and still achieved 0.3 µWh cm-2 at 4204 µW cm-2. This work provides simple methods to prepared carbon-based self-supporting materials with low-cost Al foil and demonstrates their potential for realistic application of supercapacitors.
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Araceae , Carbono , Capacitância Elétrica , Eletrodos , GasesRESUMO
The simple design of a high-energy-density device with high-mass-loading electrode has attracted much attention but is challenging. Manganese oxide (MnO2 ) with its low cost and excellent electrochemical performance shows high potential for practical application in this regard. Hence, the high-mass-loading of the MnO2 electrode with wood-derived carbon (WC) as the current collector is reported through a convenient hydrothermal reaction for high-energy-density devices. Benefiting from the high-mass-loading of the MnO2 electrode (WC@MnO2 -20, ≈14.1 mg cm-2 ) and abundant active sites on the surface of the WC hierarchically porous structure, the WC@MnO2 -20 electrode shows remarkable high-rate performance of areal/specific capacitance ≈1.56 F cm-2 /45 F g-1 , compared to the WC electrode even at the high density of 20 mA cm-2 . Furthermore, the obtained symmetric supercapacitor exhibits high areal/specific capacitances of 3.62 F cm-2 and 87 F g-1 at 1.0 mA cm-2 and high energy densities of 0.502 mWh cm-2 /12.2 Wh kg-1 with capacitance retention of 75.2% after 10 000 long-term cycles at 20 mA cm-2 . This result sheds light on a feasible design strategy for high-energy-density supercapacitors with the appropriate mass loading of active materials and low-tortuosity structural design while also encouraging further investigation into electrochemical storage.
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For the proliferation of the supercapacitor technology, it is essential to attain superior areal and volumetric performance. Nevertheless, maintaining stable areal/volumetric capacitance and rate capability, especially for thick electrodes, remains a fundamental challenge. Here, for the first time, a rationally designed porous monolithic electrode is reported with high thickness of 800 µm (46.74 mg cm-2 , with high areal mass loading of NiCo2 S4 6.9 mg cm-2 ) in which redox-active Ag nanoparticles and NiCo2 S4 nanosheets are sequentially decorated on highly conductive wood-derived carbon (WC) substrates. The hierarchically assembled WC@Ag@NiCo2 S4 electrode exhibits outstanding areal capacitance of 6.09 F cm-2 and long-term stability of 84.5% up to 10 000 cycles, as well as exceptional rate capability at 50 mA cm-2 . The asymmetric cell with an anode of WC@Ag and a cathode of WC@Ag@NiCo2 S4 delivers areal/volumetric energy density of 0.59 mWh cm-2 /3.93 mWh cm-3 , which is much-improved performance compared to those of most reported thick electrodes at the same scale. Theoretical calculations verify that the enhanced performance could be attributed to the decreased adsorption energy of OH- and the down-shifted d-band of Ag atoms, which can accelerate the electron transport and ion transfer.
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A facile one-pot hydrothermal approach for synthesizing water-dispersed nitrogen and sulfur doped carbon dots (NS-CDs) with high luminescence quantum yield was explored, using cysteine and tryptophan as precursors. The NS-CDs were characterized by means of FT-IR spectroscopy, XRD, TEM, etc. It was found that the absolute photoluminescence quantum yield (QY) of the NS-CDs determined with an integrating sphere can reach up to 73%, with an average decay time of 17.06 ns. Electrochemiluminescence (ECL) behaviors and mechanisms of the NS-CDs/K2S2O8 coreactant system were investigated. When the working electrode was modified with the prepared NS-CDs, the ECL efficiency of the NS-CDs with K2S2O8 was 24%, relative to Ru(bpy)3Cl2/K2S2O8. This work shows great potential for the NS-CDs to be used in bioanalytical applications.
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Carbono , Pontos Quânticos , Aminoácidos , Nitrogênio , Espectroscopia de Infravermelho com Transformada de Fourier , Enxofre , ÁguaRESUMO
In the electrochemiluminescence (ECL) field, most reported luminophores were focused on high-triggering potential and short wavelength, which was adverse for the ECL theory study and application at low potentials. Perylene diimide derivatives could emit near-infrared (NIR) ECL at low-triggering potential; however, they are always highly aggregated into a microrod structure and stacked together, which largely limited their application in biological fields such as bio-sensing and bio-imaging. To overcome these obstacles, we designed a novel perylene diimide molecule, namely N,N'-dicaproate sodium-3,4,9,10-perylenedicarboximide (PDI-COONa). This molecule self-assembled into a two-dimensional network nanostructure, which largely decreased the aggregation degree of PDI molecules and provided solid bases for designing lowly-aggregated PDI molecules. Also, the formed nanoluminophore produced strong emission at -0.26 V with an NIR wavelength 700 nm, which should be due to the excited J-type PDI-COO- dimers. Moreover, this network nanoluminophore well-dispersed on graphene oxide (GO) as an ECL nanomaterial to label secondary antibodies and fabricate a sandwiched immunosensor for alpha-fetoprotein (AFP) detection between 0 and -0.6 V. This immunosensor showed a wider linear response for AFP ranging from 0.1 fg mL-1 to 1 µg mL-1 with a low detection limit 0.0353 fg mL-1 compared with other immunosensors based on PDI microrod-modified GO ECL materials. The fabricated immunosensor also showed good feasibility in human serum samples.
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Técnicas Biossensoriais , Perileno , Técnicas Eletroquímicas , Humanos , Imunoensaio , Limite de Detecção , Medições LuminescentesRESUMO
Artificial lighting sources are one of the most important technological developments for our modern lives; the search for cost-effective and efficient luminophores is therefore crucial to a sustainable future. Graphene quantum dots (GQDs) are carbon-based nanomaterials that exhibit exceptional optical and electronic properties, making them a prime candidate for a luminophore in a light-emitting device. Nitrogen-doped GQDs fabricated from a facile top-down electrochemical exfoliation process with a nitrogen-containing electrolyte in this report showed strong photoluminescent emission at 450â nm, and electrogenerated chemiluminescence at 660â nm in the presence of benzoyl peroxide as a coreactant. When introduced into solid-state light-emitting electrochemical cells, for the first time, the GQDs displayed a broad white emission centered at 610â nm, corresponding to Commision Internationale de l'eclairage (CIE) colour coordinates of (0.38, 0.36).
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A facile and cost-efficient hydrothermal and lyophilization two-step strategy has been developed to prepare three-dimensional (3D) SnO2/rGO composites as NO2 gas sensor. In the present study, two different metal salt precursors (Sn(2+) and Sn(4+)) were used to prepare the 3D porous composites. It was found that the products prepared from different tin salts exhibited different sensing performance for NO2 detection. The scanning electron microscopy and transmission electron microscopy characterizations clearly show the macroporous 3D hybrids, nanoporous structure of reduce graphene oxide (rGO), and the supported SnO2 nanocrystals with an average size of 2-7 nm. The specific surface area and porosity properties of the 3D mesoporous composites were analyzed by Braunauer-Emmett-Teller method. The results showed that the SnO2/rGO composite synthesized from Sn(4+) precursor (SnO2/rGO-4) has large surface area (441.9 m(2)/g), which is beneficial for its application as a gas sensing material. The gas sensing platform fabricated from the SnO2/rGO-4 composite exhibited a good linearity for NO2 detection, and the limit of detection was calculated to be as low as about 2 ppm at low temperature. The present work demonstrates that the 3D mesoporous SnO2/rGO composites with extremely large surface area and stable nanostructure are excellent candidate materials for gas sensing.
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Metal oxide materials have been widely used as gas-sensing platforms, and their sensing performances are largely dependent on the morphology and surface structure. Here, freestanding flower-like Co3O4 nanostructures supported on three-dimensional (3D) carbon foam (Co3O4@CF) were successfully synthesized by a facile and low-cost hydrothermal route and annealing procedure. The morphology and structure of the nanocomposites were studied by X-ray diffraction, X-ray photoelectron spectroscopy, energy-dispersive spectroscopy, and scanning electron microscopy (SEM). The SEM characterizations showed that the skeleton of the porous carbon foam was fully covered by flower-like Co3O4 nanostructures. Moreover, each Co3O4 nanoflower is composed of densely packed nanoneedles with a length of ~10 µm, which can largely enhance the surface area (about 286.117 m(2)/g) for ethanol sensing. Gas sensor based on the as-synthesized 3D Co3O4@CF nanostructures was fabricated to study the sensing performance for ethanol at a temperature range from 180 to 360 °C. Due to the 3D porous structure and the improvement in sensing surface/interface, the Co3O4@CF nanostructure exhibited enhanced sensing performance for ethanol detection with low resistance, fast response and recovery time, high sensitivity, and limit of detection as low as 15 ppm at 320 °C. The present study shows that such novel 3D metal oxide/carbon hybrid nanostructures are promising platforms for gas sensing.
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Carbono/química , Cobalto/química , Etanol/análise , Gases/química , Nanoestruturas , Óxidos/química , Microscopia Eletrônica de Varredura , PorosidadeRESUMO
Hydrogen sulfide (H2S) is a toxic contaminant and has great influence on many physiological processes. Due to various pathophysiological roles and environmental pollution problems, it is necessary to construct and develop simple and portable monitoring sensors for the precise detection of H2S. Herein, we developed a smartphone-adapted dual-mode detection platform by integrating the colorimetric and photothermal imaging analysis into a metal-organic framework-based chip (ZIF-8/Cu). Due to the nanoconfinement effect of ZIF-8, small-sized plasmonic CuS could be in-situ formed during the detection procedure of H2S and endowed the chips with excellent photothermal properties. By constructing a smartphone-adapted photothermal imager, the metal-organic framework-based chip could achieve a portable photothermal imaging analysis of H2S. Moreover, as the formed CuS was a good peroxidase-like nanozyme, the chips could also be used to trigger the enzymic catalytic reaction toward the chromogenic reaction of 3,3',5,5'-tetramethylbenzidine (TMB)-H2O2, thus providing another colorimetric sensing mode by using a smartphone App. In this smartphone-adapted visualization platform, the portable chemosensors could simultaneously achieve double detection modes at one electrode, which provided a new pathway for the accurate detection of H2S and circumvented the false-positive or negative errors during the detection process. Besides, by using the finite difference time domain (FDTD) simulation method, the in-depth mechanism, including the plasmonic effect and spatial electromagnetic field distribution, was explored to provide a possible reason for the excellent sensing performance of the dual-mode visualization platform. This work provides a new insight into the construction of the accurate, portable and smart sensing platform in the visual screening of H2S.
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Estruturas Metalorgânicas , Smartphone , Peróxido de Hidrogênio , Catálise , ColorimetriaRESUMO
With the rapid development of the Internet of Things, nanogenerator as a green energy collection technology has attracted great attention in various fields. Specifically, the natural renewable nanocellulose as a raw material can significantly improve the environmental friendliness of the nanocellulose-based nanogenerators, which also makes the nanocellulose based nanogenerators expected to further develop in areas such as wearable devices and sensor networks. This paper mainly reports the application of nanocellulose in nanogenerator, focusing on the sensor. The types, sources and preparation methods of nanocellulose are briefly introduced. At the same time, the special structure of nanocellulose highlights the advantages of nanocellulose in nanogenerators. Then, the application of nanocellulose-based nanogenerators in sensors is introduced. Finally, the future development prospects and shortcomings of this nanogenerator are discussed.
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Internet , Dispositivos Eletrônicos Vestíveis , TecnologiaRESUMO
Exploration of greatly efficient and steady non-noble oxygen evolution reaction (OER) electrocatalysts is of great significance in improving the overall efficiency of energy density systems such as regenerative fuel cells, water electrolyzes, and metal-air batteries. Herein, inspired by hierarchical 3D porous structures with open microchannels of natural wood, CoO@NiFe LDH sandwich-like nanosheets were anchored on the carbonized wood (CW) via electrodeposition and calcination strategies. The strong interactions between CoO nanosheets and NiFe LDH nanosheets endow CoO@NiFe LDH/CW electrocatalyst with high catalytic properties toward the OER comparable to CoO/CW and NiFe LDH/CW. The optimized CoO@NiFe LDH/CW electrocatalyst demonstrates good OER catalytic performance with an overpotential of 230â mV at 100â mA cm-2. This work presents an innovative approach to utilize renewable resources for constructing advanced free-standing catalysts.
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The flexible and self-healing supercapacitors (SCs) are considered to be promising smart energy storage devices. Nevertheless, the SCs integrated with flexibility, lightweight, pattern editability, self-healing capabilities and desirable electrochemical properties remain a challenge. Herein, an all-in-one self-healing SC fabricated with the free-standing hybrid film (TCMP) composed of the 2,2,6,6-tetramethylpiperidin-1-yloxy-oxidized cellulose nanofibers (TOCNs) carried carbon nanotubes (CNTs), manganese dioxide (MnO2) and polyaniline (PANI) as the electrode, polyvinyl alcohol/sulfuric acid (PVA/H2SO4) gel as the electrolyte and dynamically cross-linked cellulose nanofibers/PVA/sodium tetraborate decahydrate (CNF/PB) hydrogel as the self-healing electrode matrix is developed. The TCMP film electrodes are fabricated through a facile in-situ polymerization of MnO2 and PANI in TOCNs-dispersed CNTs composite networks, exhibiting lightweight, high electrical conductivity, flexibility, pattern editability and excellent electrochemical properties. Benefited from the hierarchically porous structure and high mechanical properties of TOCNs, excellent electrical conductivity of CNTs and the desirable synergistic effect of pseudocapacitance induced by MnO2 and PANI, the assembled SC with an interdigital structure demonstrated a high areal capacitance of 1108 mF cm-2 at 2 mA cm-2, large areal energy density of 153.7 µWh cm-2 at 1101.7 µW cm-2. A satisfactory bending cycle performance (capacitance retention up to 95 % after 200 bending deformations) and self-healing characteristics (â¼90 % capacitance retention after 10 cut/repair cycles) are demonstrated for the TCMP-based symmetric SC, delivering a feasible strategy for electrochemical energy storage devices with excellent performance, designable patterns and desirable safe lifespan.
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Fluorescent composites have widespread applications in many aspects. Wood-derived cellulose is a renewable, easily processed and biodegradable, and cellulose-based fluorescent composites are highly favored for in different fields. However, the existing cellulose-based fluorescent composites still have many urgent problems to be solved, such as unstable luminescence properties and easy shedding of luminescent substances, and the development of their practical applications is still a formidable challenge. Herein, a green and mild strategy for the in-situ controllable synthesis of cellulose-based fluorescent composites membrane (CFM) was developed. Firstly, delignified wood (DW) was modified with citric acid, and then lanthanide ions were introduced on modified DW through coordinated covalent bonds. Additionally, the luminescence mechanism of CFM is proposed. CFMs show adjustable color for decorative and light conversion and can be accurately identified for data protection, which increases the high value-added of cellulose-based composites. The stable luminescent properties were maintained after sonication for 30 min or solvent immersion for three months. Therefore, this work presents a new approach for the synthesis of CFM, which provides an environment-friendly strategy for manufacturing cellulose-based fluorescent materials, which is significant for the subsequent development of environment-friendly composites for anti-counterfeiting and decorative applications.
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Inspired by creatures, abundant stimulus-responsive hydrogel actuators with diverse functionalities have been manufactured for applications in soft robotics. However, constructing a shape memory and self-sensing bilayer hydrogel actuator with high mechanical strength and strong interfacial bonding still remains a challenge. Herein, a novel bilayer hydrogel with a stimulus-responsive TEMPO-oxidized cellulose nanofibers/poly(N-isopropylacrylamide) (TOCN/PNIPAM) layer and a non-responsive TOCN/polyacrylamide (TOCN/PAM) layer is proposed as a thermosensitive actuator. TOCNs as a nano-reinforced phase provide a high mechanical strength and endow the hydrogel actuator with a strong interfacial bonding. Due to the incorporation of TOCNs, the TOCN/PNIPAM hydrogel exhibits a high compressive strength (~89.2 kPa), elongation at break (~170.7 %) and tensile strength (~24.0 kPa). The prepared PNIPAM/TOCN/PAM hydrogel actuator performs the roles of an encapsulation, jack, temperature-controlled fluid valve and temperature-control manipulator. The incorporation of Fe3+ further endows the bilayer hydrogel actuator with a synergistic performance of shape memory and temperature-driven, which can be used as a temperature-responsive switch to detect ambient temperature. The PNIPAM/TOCN/PAM-Fe3+ conductive hydrogel can be assembled into a flexible sensor and generate sensing signals when driven by temperature changes to achieve real-time feedback. This research may lead to new insights into the design and manufacturing of intelligent flexible soft robots.
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Antibiotics are commonly used to treat bacterial infections, but the misuse and abuse of antibiotics have given rise to a severe problem of the drug resistance of bacteria. Solving this problem has been a vitally important task in the modern medical arena. Antibacterial peptide (AMPs) has become a promising candidate drug to replace antibiotics because of their broad-spectrum antibacterial activity and their difficulty in making bacteria resistant. However, its wider clinical application is limited by the shortcomings of high cytotoxicity and low antibacterial efficiency. In this paper, we constructed an antibacterial peptide (Cu-GGH-KKLRKIAFK, abbreviated as Cu-GGH-AMP) with a DNA cleavage function. The peptide has two functional regions, the C-terminal antibacterial peptide PaDBS1R6F10 (KKLRLKIAFK) and the N-terminal Cu-GGH complex. PaDBS1R6F10 is a unique antibacterial peptide, which shows lower tendency to produce bacterial resistance than traditional antibiotics. Cu-GGG complexes are formed by chelating Cu with the classical amino terminal Cu (II)- and Ni (II) -Binding (ATCUN) motif GGH. In the presence of ascorbic acid, Cu-GGH can efficiently catalyze the oxidative cleavage of bacterial DNA, thus playing a synergistic antibacterial role with antibacterial peptides. The in vitro and in vivo experiments demonstrated this functionalized antibacterial peptide possesses excellent antibacterial and anti-skin infection capability, as well as the activity of promoting wound healing.
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Anti-Infecciosos , Desinfecção , Clivagem do DNA , Cobre/farmacologia , Cobre/química , Peptídeos/farmacologia , Peptídeos/química , Antibacterianos/farmacologia , Antibacterianos/química , BactériasRESUMO
Efficient and spatiotemporally controllable cleavage of deoxyribonucleic acid (DNA) is of great significance for both disease treatment (e.g. tumour, bacterial infection, etc) and molecular biology applications (e.g. gene editing). The recently developed light-induced cleavage strategy based on catalytic nanoparticles has been regarded as a promising strategy for DNA controllable cleavage. Although the regulation based on orthogonal light in biomedical applications holds more significant advantages than that based on single light, nanoparticle-mediated DNA cleavage based on orthogonal light has yet to be reported. In this article, for the first time, we demonstrated an orthogonal light-regulated nanosystem for efficient and spatiotemporal DNA cleavage. In this strategy, tungsten oxide (WO3) nanoparticles with photochromic properties were used as nano-antennae to convert the photoenergy from the orthogonal visible light (405 nm) and near-infrared light (808 nm) into chemical energy for DNA cleavage. We verified that only the orthogonal light can trigger high cleavage efficiency on different types of DNA. Moreover, such an orthogonal light-response nano-system can not only induce significant apoptosis of tumour cells, but also effectively eliminate bacterial biofilms.