RESUMO
Infectious bacterial biofilms are recalcitrant to most antibiotics compared to their planktonic version, and the lack of appropriate therapeutic strategies for mitigating them poses a serious threat to clinical treatment. A ternary heterojunction material derived from a Bi-based perovskite-TiO2 hybrid and a [Ru(2,2'-bpy)2(4,4'-dicarboxy-2,2'-bpy)]2+ (2,2'-bpy, 2,2'-bipyridyl) as a photosensitizer (RuPS) is developed. This hybrid material is found to be capable of generating reactive oxygen species (ROS)/reactive nitrogen species (RNS) upon solar light irradiation. The aligned band edges and effective exciton dynamics between multisite heterojunctions are established by steady-state/time-resolved optical and other spectroscopic studies. Proposed mechanistic pathways for the photocatalytic generation of ROS/RNS are rationalized based on a cascade-redox processes arising from three catalytic centers. These ROS/RNS are utilized to demonstrate a proof-of-concept in treating two elusive bacterial biofilms while maintaining a high level of biocompatibility (IC50 > 1 mg/mL). The in situ generation of radical species (ROS/RNS) upon photoirradiation is established with EPR spectroscopic measurements and colorimetric assays. Experimental results showed improved efficacy toward biofilm inactivation of the ternary heterojunction material as compared to their individual/binary counterparts under solar light irradiation. The multisite heterojunction formation helped with better exciton delocalization for an efficient catalytic biofilm inactivation. This was rationalized based on the favorable exciton dissociation followed by the onset of multiple oxidation and reduction sites in the ternary heterojunction. This together with exceptional photoelectric features of lead-free halide perovskites outlines a proof-of-principle demonstration in biomedical optoelectronics addressing multimodal antibiofilm/antimicrobial modality.
Assuntos
Biofilmes , Bismuto , Bismuto/farmacologia , Bismuto/química , Espécies Reativas de OxigênioRESUMO
Turning the carrier dynamics in heterojunction photocatalysts is a direct and effective strategy for improving the solar energy conversion efficiency of photocatalysts. Herein, we report a ternary CdS@MoS2-Co3O4 multiheterojunction photocatalyst consisting of the p-n junction of MoS2-Co3O4 and the type-I junction of CdS@MoS2, wherein MoS2 located at the frontier between CdS and Co3O4 acts as an intermediate bridge. The type-I junction allows the directional transfer of photoinduced charge from CdS to MoS2, suppressing the photocorrosion of CdS. Notably, the single-particle photoluminescence technique demonstrates the sequential one-direction hole transfer from MoS2 to Co3O4 aroused by the p-n junction, resulting in a long-lifetime charge separation in the carrier lifetime (54-58 ns). Compared to the bare CdS and type-I CdS@MoS2, the CdS@MoS2-Co3O4 photocatalyst affords a 347-fold and 3.5-fold enhancement of the H2 evolution rate, a quantum efficiency of 28.6% at 450 nm, and a 20 h of long-term stability. This work provides a new understanding of the rational regulation of the charge-transfer mechanism of type-I systems by constructing multiheterojunction photocatalysts.
RESUMO
In this research, a novel ternary multi-heterojunction Bi2O3/Bi2O2CO3/(BiO)4CO3(OH)2 photocatalyst is fabricated via submerged DC electrical arc discharge in urea solution. FT-IR, XRD, EDS and PL results confirm the formation of Bi2O3/Bi2O2CO3/(BiO)4CO3(OH)2 multi-heterojunction. Formation of nanoflake morphology is revealed by FE-SEM and TEM images. The optical properties and intense absorption edge of Bi2O3/Bi2O2CO3/(BiO)4CO3(OH)2 reveal the proper visible light absorbing ability. The photocatalytic performance of the sample is investigated via the degradation of methylene orange (MeO) and rhodamine B (RB) under visible light irradiation. The photocatalytic activity of Bi2O3/Bi2O2CO3/(BiO)4CO3(OH)2 is compared with the synthesized sample in water, Bi2O3/Bi/Bi(OH)3, which exhibits much higher photocatalytic activity. Also, the stable photodegradation efficiency of Bi2O3/Bi2O2CO3/(BiO)4CO3(OH)2 after four cycles reveals the long-term stability and reusability of the synthesized photocatalyst. The PL intensity of Bi2O3/Bi2O2CO3/(BiO)4CO3(OH)2 shows an improved separation rate of electron-hole pairs and so enhanced photocatalytic performance. The improved photocatalytic activity can be ascribed to the formation of multi-heterojunctions, flake morphology and intrinsic internal electric field (IEF). Multi-heterojunction nanoflakes enhance the absorbance of visible light and facilitate the separation and transport of photogenerated electron holes through large IEF. Our work offers an effective method for the production of innovative bismuth-based photocatalyst with excellent prospects for the degradation of environmental pollutants and light harvesting for renewable energy generation under visible light.
RESUMO
Mesoporous palladium oxide (PdO)-functionalized tin dioxide (SnO2) composite nanotubes (SPCTs) were prepared via one-step synthesis by electrospinning technology using ethanol and N,N-dimethylformamide (DMF) as solvents. Compared with pure SnO2 nanotubes, there were abundant mesopores and multiheterojunctions in PdO-functionalized SnO2 nanotubes. The sample with the molar ratio of SnO2:PdO of 100:3 (3-SPCT) exhibited excellent response (â¼20.30) as a sensor with fast gas response speed (â¼1.33â¯s) to 100â¯ppm nitrogen dioxide (NO2) at room temperature (RT), and the detection limit reached to 10â¯ppb. The improved gas sensing performance of the 3-SPCT sensor was mainly attributed to the synergistic effect: the unique SnO2 tubular structure and well-dispersed mesopores provided the gas diffusion and adsorption channels, oxygen defects and chemisorbed oxygen were taken as the electron trap and charge transfer active sites, and a large number of heterojunctions acted as electron transport channels, thereby increasing the transfer rate.
RESUMO
In this work, flower-like Au/Bi2O2CO3/Bi2O3 multi-heterojunction photocatalysts were prepared by a in-situ growth method. The as-prepared samples were characterized by different techniques including Transmission Electron Microscopy (TEM), X-ray diffraction (XRD), UV-vis diffuse reflectance spectrometry (DRS), X-ray photoelectron spectroscopy (XPS), Photoluminescence (PL) and photo-induced current. The photocatalytic performance of the as prepared samples was evaluated by degradation of rhodamine B (RhB) under visible light (λ>400nm). Au/Bi2O2CO3/Bi2O3 exhibited much higher activity than pure Bi2O2CO3 or Bi2O2CO3/Bi2O3. The rate constant of best one Au/Bi2O2CO3/Bi2O3 sample is 100 and 14 times as that of pure Bi2O2CO3 and ß-Bi2O3/Bi2O2CO3, respectively. The enhanced photocatalytic activity of Au/Bi2O2CO3/Bi2O3 can be ascribed to the surface plasmon resonance (SPR) effects of Au nanoparticles and the formed multi-heterojunctions, which enhanced the absorbance of visible light and facilitated the transferring and separation of photogenerated electron-hole pairs, respectively.