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1.
Reprod Domest Anim ; 58(11): 1604-1611, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37727883

RESUMO

Pyometra is a potentially life-threatening condition that affects intact female dogs in their middle to advance age. Timely diagnosis and appropriate treatment are critical for the survival of patients, especially when pyometra advances to sepsis. This study aimed to investigate the prognostic potential of certain haematology, serum biochemical and inflammatory biomarker, secretory leucocyte protease inhibitor (SLPI) for pyometra in bitches (n = 41). Blood samples were collected after clinical diagnosis of pyometra for haematology and serum biochemistry. Based on the prognosis following medical/surgical treatment, animals were retrospectively categorized into survivor (n = 29) and dead (n = 12). Endometrial tissue sections were obtained from the bitches undergoing ovariohysterectomy (n = 21). Serum concentration of SLPI was quantified using sandwich ELISA and its expression in the endometrium was investigated using RT-qPCR. A marked increase in the total leucocyte count (TLC), neutrophils, blood urea nitrogen (BUN) and serum creatinine was observed in the female dogs that did not survive. Significant elevation in the serum SLPI concentration (3.49 ± 0.44 vs. 2.38 ± 0.13 ng/mL) was observed in the bitches those died after the treatment, in comparison to those survived (p < .01). Additionally, there was a notable upregulation of SLPI in the endometrium in the bitches those died due to pyometra. Based on the ROC analysis results, it was observed that a cut-off concentration of 2.93 ng/mL for SLPI, 27.77 mg/dL for BUN and 16.3 × 103 /µL for TLC could effectively distinguish the prognosis of pyometra-affected dogs. From this study, it can be concluded that upregulation of SLPI in the endometrium and its elevated concentration in peripheral circulation along with TLC and BUN concentration could serve as valuable indicators for predicting the prognosis of pyometra in bitches.


Assuntos
Doenças do Cão , Piometra , Humanos , Cães , Animais , Feminino , Piometra/veterinária , Estudos Retrospectivos , Prognóstico , Biomarcadores , Inibidores de Proteases , Inibidor Secretado de Peptidases Leucocitárias
2.
Environ Sci Pollut Res Int ; 30(32): 78692-78706, 2023 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-37273042

RESUMO

A novel ZnO-MoO3-ZnMoO3@graphene GZM composite catalyst prepared by microwave hydrothermal process for personal protective equipment textiles (PPE) is presented in this study. The results indicated that the GZM with defect vacancy sites of two types as observed by EPR showed significantly superior inactivation of the E. coli bacteria compared to GZM without the lower defect vacancy sites and concomitant lower electron densities. Photocatalytic activated oxidation by the GZM composites coatings was observed to proceed in acceptable times as well as the bacterial inactivation (log bact. C/Co > 107 within 3 h). Defect sites in the GZM seem to be important leading to the bacterial inactivation process. DFT calculations on the GZM with and without catalyst defect sites were carried out. The electron densities were estimated by the Fourier mapping. The results found in this study showed the potential of GZM-PPE for practical applications.


Assuntos
Escherichia coli , Luz , Oxirredução , Catálise
3.
Chem Rec ; 23(5): e202200171, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-37066717

RESUMO

Graphitic carbon nitride (g-C3 N4 ) has gained tremendous interest in the sector of power transformation and retention, because of its distinctive stacked composition, adjustable electronic structure, metal-free feature, superior thermodynamic durability, and simple availability. Furthermore, the restricted illumination and extensive recombination of photoexcitation electrons have inhibited the photocatalytic performance of pure g-C3 N4 . The dimensions of g-C3 N4 may impact the field of electronics confinement; as a consequence, g-C3 N4 with varying dimensions shows unique features, making it appropriate for a number of fascinating uses. Even if there are several evaluations emphasizing on the fabrication methods and deployments of g-C3 N4 , there is certainly an insufficiency of a full overview, that exhaustively depicts the synthesis and composition of diverse aspects of g-C3 N4 . Consequently, from the standpoint of numerical simulations and experimentation, several legitimate methodologies were employed to deliberately develop the photocatalyst and improve the optimal result, including elements loading, defects designing, morphological adjustment, and semiconductors interfacing. Herein, this evaluation initially discusses different dimensions, the physicochemical features, modifications and interfaces design development of g-C3 N4 . Emphasis is given to the practical design and development of g-C3 N4 for the various power transformation and inventory applications, such as photocatalytic H2 evolution, photoreduction of CO2 source, electrocatalytic H2 evolution, O2 evolution, O2 reduction, alkali-metal battery cells, lithium-ion batteries, lithium-sulfur batteries, and metal-air batteries. Ultimately, the current challenges and potential of g-C3 N4 for fuel transformation and retention activities are explored.

4.
Reprod Domest Anim ; 58(6): 802-812, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-37010813

RESUMO

As onset of sepsis adversely affects the prognosis of canine pyometra, finding biomarkers that would distinguish sepsis status would be useful in the clinical management. Accordingly, we hypothesized that differential expression of endometrial transcripts and circulating concentration of certain inflammatory mediators would discriminate pyometra-led sepsis (P-sepsis+) from those of pyometra without sepsis (P-sepsis-). Bitches with pyometra (n = 52) were classified into P-sepsis+ (n = 28) and P-sepsis- (n = 24) based on vital clinical score and total leukocyte count. A group of non-pyometra bitches (n = 12) served as control. The relative fold changes in the transcripts of IL6, IL8, TNFα, IL10, PTGS2, mPGES1 and PGFS, SLPI, S100A8, S100A12 and eNOS were determined by quantitative polymerase chain reaction. Furthermore, the serum concentrations of IL6, IL8, IL10, SLPI and prostaglandin F2α metabolite (PGFM) were assayed by ELISA. The relative fold changes in S100A12 and SLPI and mean concentrations of IL6 and SLPI were significantly (p < .05) higher in P-sepsis+ than that of P-sepsis- group. Receiver operating characteristic analysis revealed that serum IL6 had a diagnostic sensitivity of 78.6% and a positive likelihood ratio (LR+) of 2.09, at a cut-off value of 15.7 pg/mL to diagnose P-sepsis+ cases. Similarly, serum SLPI had a sensitivity of 84.6% and an LR+ of 2.23, at a cut-off value of 2.0 pg/mL. It was concluded that SLPI and IL6 would serve as putative biomarkers for pyometra-led sepsis in bitches. Monitoring SLPI and IL6 would be a useful adjunct to the established haemato-biochemical parameters in customizing the treatment strategies and arriving at the decision for management of pyometra bitches with critical illness.


Assuntos
Doenças do Cão , Piometra , Sepse , Feminino , Animais , Cães , Interleucina-6/metabolismo , Interleucina-8/metabolismo , Inibidor Secretado de Peptidases Leucocitárias/metabolismo , Interleucina-10/metabolismo , Proteína S100A12 , Piometra/veterinária , Biomarcadores , Sepse/diagnóstico , Sepse/veterinária
5.
Small ; 19(25): e2208179, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-36935369

RESUMO

The realization of solar-light-driven CO2  reduction reactions (CO2 RR) is essential for the commercial development of renewable energy modules and the reduction of global CO2 emissions. Combining experimental measurements and theoretical calculations, to introduce boron dopants and nitrogen defects in graphitic carbon nitride (g-C3 N4 ), sodium borohydride is simply calcined with the mixture of g-C3 N4 (CN), followed by the introduction of ultrathin Co phthalocyanine through phosphate groups. By strengthening H-bonding interactions, the resultant CoPc/P-BNDCN nanocomposite showed excellent photocatalytic CO2 reduction activity, releasing 197.76 and 130.32 µmol h-1  g-1 CO and CH4 , respectively, and conveying an unprecedented 10-26-time improvement under visible-light irradiation. The substantial tuning is performed towards the conduction and valance band locations by B-dopants and N-defects to modulate the band structure for significantly accelerated CO2 RR. Through the use of ultrathin metal phthalocyanine assemblies that have a lot of single-atom sites, this work demonstrates a sustainable approach for achieving effective photocatalytic CO2 activation. More importantly, the excellent photoactivity is attributed to the fast charge separation via Z-scheme transfer mechanism formed by the universally facile strategy of dimension-matched ultrathin (≈4 nm) metal phthalocyanine-assisted nanocomposites.

6.
Small ; 19(12): e2206472, 2023 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-36642818

RESUMO

The development of highly efficient and cost-effective hydrogen evolution reaction (HER) catalysts is highly desirable to efficiently promote the HER process, especially under alkaline condition. Herein, a polyoxometalates-organic-complex-induced carbonization method is developed to construct MoO2 /Mo3 P/Mo2 C triple-interface heterojunction encapsulated into nitrogen-doped carbon with urchin-like structure using ammonium phosphomolybdate and dopamine. Furthermore, the mass ratio of dopamine and ammonium phosphomolybdate is found critical for the successful formation of such triple-interface heterojunction. Theoretical calculation results demonstrate that such triple-interface heterojunctions possess thermodynamically favorable water dissociation Gibbs free energy (ΔGH2O ) of -1.28 eV and hydrogen adsorption Gibbs free energy (ΔGH* ) of -0.41 eV due to the synergistic effect of Mo2 C and Mo3 P as water dissociation site and H* adsorption/desorption sites during the HER process in comparison to the corresponding single components. Notably, the optimal heterostructures exhibit the highest HER activity with the low overpotential of 69 mV at the current density of 10 mA cm-2 and a small Tafel slope of 60.4 mV dec-1 as well as good long-term stability for 125 h. Such remarkable results have been theoretically and experimentally proven to be due to the synergistic effect between the unique heterostructures and the encapsulated nitrogen-doped carbon.

7.
Angew Chem Int Ed Engl ; 62(3): e202214988, 2023 Jan 16.
Artigo em Inglês | MEDLINE | ID: mdl-36401754

RESUMO

The regulation of electron distribution of single-atomic metal sites by atomic clusters is an effective strategy to boost their intrinsic activity of oxygen reduction reaction (ORR). Herein we report the construction of single-atomic Mn sites decorated with atomic clusters by an innovative combination of post-adsorption and secondary pyrolysis. The X-ray absorption spectroscopy confirms the formation of Mn sites via Mn-N4 coordination bonding to FeMn atomic clusters (FeMnac /Mn-N4 C), which has been demonstrated theoretically to be conducive to the adsorption of molecular O2 and the break of O-O bond during the ORR process. Benefiting from the structural features above, the FeMnac /Mn-N4 C catalyst exhibits excellent ORR activity with half-wave potential of 0.79 V in 0.5 M H2 SO4 and 0.90 V in 0.1 M KOH as well as preeminent Zn-air battery performance. Such synthetic strategy may open up a route to construct highly active catalysts with tunable atomic structures for diverse applications.

8.
Small Methods ; 6(12): e2201013, 2022 12.
Artigo em Inglês | MEDLINE | ID: mdl-36336653

RESUMO

Inspired by natural photosynthesis, harnessing the wide range of natural solar energy and utilizing appropriate semiconductor-based catalysts to convert carbon dioxide into beneficial energy species, for example, CO, CH4 , HCOOH, and CH3 COH have been shown to be a sustainable and more environmentally friendly approach. Graphitic carbon nitride (g-C3 N4 ) has been regarded as a highly effective photocatalyst for the CO2 reduction reaction, owing to its cost-effectiveness, high thermal and chemical stability, visible light absorption capability, and low toxicity. However, weaker electrical conductivity, fast recombination rate, smaller visible light absorption window, and reduced surface area make this catalytic material unsuitable for commercial photocatalytic applications. Therefore, certain procedures, including elemental doping, structural modulation, functional group adjustment of g-C3 N4 , the addition of metal complex motif, and others, may be used to improve its photocatalytic activity towards effective CO2 reduction. This review has investigated the scientific community's perspectives on synthetic pathways and material optimization approaches used to increase the selectivity and efficiency of the g-C3 N4 -based hybrid structures, as well as their benefits and drawbacks on photocatalytic CO2 reduction. Finally, the review concludes a comparative discussion and presents a promising picture of the future scope of the improvements.


Assuntos
Dióxido de Carbono , Grafite , Fotossíntese , Catálise
10.
J Colloid Interface Sci ; 627: 621-629, 2022 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-35872419

RESUMO

The development of copolymerized carbon nitride (CN)-based photocatalysts may support advances in photocatalytic overall water splitting. However, the recombination of charge carriers is the main bottleneck that reduces its overall photocatalytic activity. To overcome this problem, the construction of heterojunction technology has emerged as an effective approach to reduce the charge carrier recombination, thereby improving charge separation and transport efficiency. In this work, an innovative heterojunction was prepared between Quinolinic acid (QA) modified CN (CN-QAx) and novel nanorod-shaped bismuth vanadate (BiVO4) (BiVO4/CN-QAx) for overall water splitting through a simple in-situ solvent evaporation technique. The obtained results show that the synthesized samples have efficient and improved activities for releasing H2 (862.1 µmol/h) and O2 (31.58 µmol/h) under visible light irradiation. Furthermore, an exceptional apparent quantum yield (AQY) of 64.52 % has been recorded for BiVO4/CN-QA7.0 at 420 nm, which might be due to the substantial isolation of photoinducedcharge carriers. Therefore, this work opens up a new channel toward efficient CN-based photocatalysts in the sustainable energy production processes.

11.
ACS Sens ; 5(9): 2783-2791, 2020 09 25.
Artigo em Inglês | MEDLINE | ID: mdl-32551534

RESUMO

The preservation of cultural heritage materials requires extremely low concentration limits for indoor pollutants. This poses an unmet challenge for monitoring the artwork in museums and on exhibit, especially to do so in a cost-effective manner for a large number of locations. A novel type of colorimetric sensor array based on printed inks of 10 nm silver nanoparticles (AgNPs) with several different capping agents has been developed as an alternative to metal coupons or other passive sampling indicators traditionally used by conservators. The AgNP colorimetric sensor array, combined with digital imaging, offers ultrasensitive dosimetric identification of acidic and oxidizing gases and other air pollutants commonly found in a museum; the limits of detection are sub-ppb for 1 h exposures. For an array of AgNP inks with various capping agents, a unique and distinguishable color response pattern is observed for each specific analyte. Excellent discrimination among 11 gas pollutants over a wide range of concentrations was demonstrated using standard chemometric methods. The observed changes in color during pollutant exposure originate from the sintering of solid-state nanoparticles that leads to changes in the localized surface plasmon resonance. Such chemically induced sintering mechanism of nanoparticles paves the way for a new class of field-deployable solid-state optical sensor arrays. As an example, we have demonstrated the use of AgNP sensor arrays for the nondestructive analysis of acidic volatile emission from five types of printing paper, relevant for the conservation of cultural heritage objects, including ancient manuscripts and books.


Assuntos
Poluentes Ambientais , Nanopartículas Metálicas , Colorimetria , Museus , Prata
12.
J Colloid Interface Sci ; 560: 743-754, 2020 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-31706649

RESUMO

Research based on the full water splitting via heterogenous semiconducting photocatalyst is a significant characteristic nevertheless challenging for determining the energy and environmental crises. With respect to this, a photocatalytic water splitting by visible light through heterojunction semiconductors has been anticipated as a route to the sustainable energy. For the first time, we integrate a potential conjugated donor-acceptor (DA) co-monomer such as 2, 3-dichloroquinoxaline (DCQ) within the structure of polymeric carbon nitride (PCN) by a facile one-pot co-polymerization process. The DCQ which is acting as an organic motif that simulates a nucleophilic attack on the hosting PCN semiconductor which extends into a long chain of the polymer having enormous surface area and remarkable photocatalytic activity for H2 and O2 evolution as compared to the parental CNU. The supremacy of molecular geometry with DA ratio is effectively studied by absorbent, calculated band gap and migration of electrons on the photocatalytic performance of as-synthesized CNU-DCQx co-polymer. The density functional theory (DFT) calculation deliver supplementary evidence for the positive incorporation of DCQ in to the PCN matrix with reduced band gap upon copolymerization. Further, the hydrogen evolution rate (HER) for pure CNU with 14.2 µmol/h while for CNU-DCQ18.0 it is estimated at 124.9 µmol/h which remarkably fueled almost eight times more than blank sample. Similarly, the oxygen evolution rate (OER) analysis indicates the production 0.2 µmol/h (visible) and 1.5 µmol/h (non-visible) for CNU. However, the OER of copolymerized CNU-DCQ18.0 is found to be 1.9 µmol/h (visible) and 12.8 µmol/h (non-visible) which almost nine times higher than parental CNU. Hence, the output of this work reflects as an important step on the way to tailor-designed and elucidate the promising role of D-π-A system for the rational motifs of productive photocatalysts for forthcoming request.

13.
ACS Appl Mater Interfaces ; 11(50): 46756-46766, 2019 Dec 18.
Artigo em Inglês | MEDLINE | ID: mdl-31762261

RESUMO

Photocatalytic full water splitting remains the perfect way to generate oxygen (O2) and hydrogen (H2) gases driven by sunlight to address the future environmental issues as well as energy demands. Owing to its exceptional properties, polymeric carbon nitride (PCN) has been one of the most widely investigated semiconductor photocatalysts. Nevertheless, blank PCN characteristically displays restrained photocatalytic performance due to high-density defects in its framework that may perhaps perform the part of the recombination midpoint for photoproduced electron-hole pairs. Therefore, to overcome this problem, a simple approach to introduce 7,7,8,8-tetracyanoquinodimethane (TCNQ) with an electron-withdrawing characteristic modifier into the pristine PCN framework by the ionothermal method to enhance its optical, conductive, and photocatalytic properties has been undertaken. Results show that such integration of TCNQ results in the delocalization of the π-conjugated structure; significant changes in its chemical electronic configuration, band gap, and surface area; and enhanced production of electrons under visible light. As a result of this facile integration, our best sample (CNU-TCNQ9.0) produced a hydrogen evolution rate (HER) of 164.6 µmol h-1 for H2 and an oxygen evolution rate (OER) of 14.8 µmol h-1 for O2, which were found to be 2.4- and 2.6-fold greater than those produced with pure carbon nitride (CNU) sample, respectively. Hence, this work provides a reasonable alternative method to synthesize and design novel CNU-TCNQ backbone photocatalyst for organic photosynthesis, CO2 reduction, hydrogen evolution, etc.

14.
Opt Lett ; 44(19): 4901-4904, 2019 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-31568471

RESUMO

We present a method for realizing a solid-state volumetric display based on the chromatic dispersion properties of a 150 mm diffractive lens that images a series of planar patterns presented by a digital micro-mirror device projector. The projector is driven by a narrowband polychromatic source, where the position of each image plane is defined by a distinct wavelength of light. The volumetric display system achieves 20 image planes at a volume refresh rate of 20 Hz, creating a volume of 17.4 cm3 with 13 mm of depth and a field of view of 10° floating 145 mm above the lens in real space.

16.
Sci Rep ; 9(1): 13103, 2019 Sep 11.
Artigo em Inglês | MEDLINE | ID: mdl-31511596

RESUMO

Anatase TiO2 hollow nanoboxes were synthesized and combined with the graphene oxide to get nanocomposite of TiO2/rGO (TG). Graphene oxide was used to modify the Oxygen-Clusters and bulk to surface defects. Anatase and TG composite were characterized with the positron annihilation, XPS, EPR, EIS and photocurrent response analysis. The relative affects of defects on the photocatalytic reduction (CO2 to CH4) were studied. The TG composites showed highest photo-catalytic activity after GO coupling (49 µmol g-1 h-1), 28.6 times higher photocurrent yields much higher quantum efficiency (3.17%@400 nm) when compared to the TiO2 nanoboxes. The mechanism of enhanced photo-catalytic CO2 conversion to CH4 elucidated through electrochemical and photo-catalytic experiments with traceable isotope containing carbon dioxide (13CO2). For the first time we discovered that diminishing the comparative concentration ratio of anatase from the bulk to surface defects could significantly increase the conversion of CO2 to CH4.

17.
J Colloid Interface Sci ; 554: 627-639, 2019 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-31344529

RESUMO

The intertwined exploring of solar water driven into chemical energy configurated by a constituted semiconductor photocatalyst under sunlight approach toward a remediation eager method that solve the environmental issues. Currently we optimized polymeric carbon nitride PCN by a sophisticated molecular co-polymerization process which diffused with a mirror organic conjugated heterocyclic monomer to maximize its photocatalytic activity. Herein, for the 1st time we report an organic π-electron stacking conjugated thiazolothiazole (TT) as a small molecule within the framework of PCN to enhance the conductive optical and photocatalytic properties of PCN under solar energy irradiation. The fusion of this bicyclic thiazolothiazole (TT) co-monomer within PCN remarkably enhanced the charge carrier motilities and giving a rigid packing due to sulfur contents. Excitingly the as-synthesized samples were processed under different liberated characterization such as XRD, FTIR, BET, SEM, TEM, XPS, PL, DRS and EPR under both regions respectively. Results reflect that the integration of thiazolothiazole (TT) in the heptazine structure of PCN alter a prodigious delocalization in its π-conjugated system and similarly demonstrating an apparent fluctuation in its surface area, electronic structure, its calculated band gap, chemical composition analysis and maximize the process of generation of electrons under solar light from ground state (HOMO) to the excited state (LUMO) of polymeric carbon nitride (PCN). Beside, this unique integrity of TT co-monomer with in PCN matrix remarkably improve the photocatalytic activity toward prosperity and the amount optimized CNU-TT12.0 demonstrated an outstanding photocatalytic activity of water reduction for H2 evolution and as well of RhB pollutant photodegradation. The sample optimized display 10.6 enhancement comparatively pure pristine sample.

18.
Molecules ; 24(9)2019 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-31071946

RESUMO

This work incorporates a variety of conjugated donor-acceptor (DA) co-monomers such as 2,6-diaminopurine (DP) into the structure of a polymeric carbon nitride (PCN) backbone using a unique nanostructure co-polymerization strategy and examines its photocatalytic activity performance in the field of photocatalytic CO2 reduction to CO and H2 under visible light irradiation. The as-synthesized samples were successfully analyzed using different characterization methods to explain their electronic and optical properties, crystal phase, microstructure, and their morphology that influenced the performance due to the interactions between the PCN and the DPco-monomer. Based on the density functional theory (DFT) calculation result, pure PCN and CNU-DP15.0 trimers (interpreted as incorporation of the co-monomer at two different positions) were extensively evaluated and exhibited remarkable structural optimization without the inclusion of any symmetry constraints (the non-modified sample derived from urea, named as CNU), and their optical and electronic properties were also manipulated to control occupation of their respective highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO). Also, co-polymerization of the donor-acceptor 2,6-diamino-purine co-monomer with PCN influenced the chemical affinities, polarities, and acid-base functions of the PCN, remarkably enhancing the photocatalytic activity for the production of CO and H2 from CO2 by 15.02-fold compared than that of the parental CNU, while also improving the selectivity.


Assuntos
Dióxido de Carbono/química , Elétrons , Luz , Nitrilas/química , Polímeros/química , Adsorção , Espectroscopia de Ressonância Magnética Nuclear de Carbono-13 , Catálise/efeitos da radiação , Eletroquímica , Nitrogênio/química , Oxirredução , Espectroscopia Fotoeletrônica , Espectrofotometria Ultravioleta , Espectroscopia de Infravermelho com Transformada de Fourier , Difração de Raios X
19.
J Colloid Interface Sci ; 548: 197-205, 2019 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-31003166

RESUMO

The conjugated co-monomer, trimesic acid (TMA) was integrated into the triazine framework of polymeric carbon nitride (PCN), synthesized through chemical condensation of urea. The TMA-modified carbon nitride samples obtained were named as CNU-TMA and it was utilized for the photocatalytic reduction of carbon dioxide (CO2) under visible light illumination. The induction of such electron donor-acceptor co-monomer (TMA) dominates the intramolecular structure of PCN by acting as a nucleophilic substitution substrate to facilitate the electron density in the π-electron conjugated system of PCN and thus elevate its photocatalytic activity. Also, this process of copolymerization with TMA, not only cause a significant diversion in the specific area, band gap, chemical composition, and structure of PCN but also promote efficient charge transport from ground state (HOMO) to the excited state (LUMO) of the PCN. For comparison, CNU samples modified with other co-monomers were prepared by the same method and were named as CNU-FDA (2,5-Furandicarboxylic acid), CNU-PDA (2,6-pyridinedicarboxylic acid), CNU-PTA (Phthalic acid). Similarly, co-monomer TMA was incorporated in other PCN precursors such as dyandicyanamide (DCDA), thiourea (SCN) and ammonium thiocyanate (NH2SCN) and was named as CND-TMA13.0, CNT-TMA13.0, and CNA-TMA13.0, respectively. Besides, the average weight ratio between urea and TMA was well tuned and also CNU-TMA13.0 gain a fabulous 16 fold-enhanced photocatalytic performance than blank CNU.

20.
Nanoscale ; 9(28): 9913-9920, 2017 Jul 20.
Artigo em Inglês | MEDLINE | ID: mdl-28678289

RESUMO

A tri-layered photoelectrode for dye-sensitized solar cells (DSSCs) is assembled using single crystal hollow TiO2 nanoparticles (HTNPs), sub-micro hollow TiO2 mesospheres (SHTMSs) and hierarchical TiO2 microspheres (HTMSs). The bottom layer composed of single crystal hollow TiO2 nanoparticles serves to absorb dye molecules, harvest light due to its hollow structure and keep a better mechanical contact with FTO conducting glass; the middle layer consisting of sub-micro hollow mesospheres works as a multifunctional layer due to its high dye adsorption ability, strong light trapping and scattering ability and slow recombination rates; and the top layer consisting of hierarchical microspheres enhances light scattering. The DSSCs made of photoanodes with a tripartite-layer structure (Film 4) show a superior photoconversion efficiency (PCE) of 9.24%, which is 7.4% higher than a single layered photoanode composed of HTNPs (Film 1: 8.90%), 4.6% higher than a double layer-based electrode consisting of HTNPs and SHTMSs (Film 2: 9.03%) and 2.6% higher than a double layer-based electrode made of HTNPs and HTMSs (Film 3: 9.11%). The significant improvements in the PCE for tri-layered TiO2 photoanodes are mainly because of the combined effects of their higher light scattering ability, long electron lifetime, fast electron transport rate, efficient charge collection and a considerable surface area with high dye-loading capability. This study confirms that the facile tri-layered photoanode is an interesting structure for high-efficiency DSSCs.

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