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1.
Opt Express ; 32(9): 16414-16425, 2024 Apr 22.
Artigo em Inglês | MEDLINE | ID: mdl-38859268

RESUMO

Polarization detection and imaging technologies have attracted significant attention for their extensive applications in remote sensing, biological diagnosis, and beyond. However, previously reported polarimeters heavily relied on polarization-sensitive materials and pre- established mapping relationships between the Stokes parameters and detected light intensities. This dependence, along with fabrication and detection errors, severely constrain the working waveband and detection precision. In this work, we demonstrated a highly precise, stable, and broadband full-Stokes polarimeter based on large-area uniform chiral shells and a post-established mapping relationship. By precisely controlling the geometry through the deposition of Ag on a large-area microsphere monolayer with a uniform lattice, the optical chirality and anisotropy of chiral shells can reach about 0.15 (circular dichroism, CD) and 1.7, respectively. The post-established mapping relationship between the Stokes parameters and detected light intensities is established through training a deep learning algorithm (DLA) or fitting the derived mapping-relationship formula based on the Mueller matrix theory with a large dataset collected from our home-built polarization system. For the detection precision with DLA, the mean squared errors (MSEs) at 710 nm can reach 0.10% (S1), 0.41% (S2), and 0.24% (S3), while for the Mueller matrix theory, the corresponding values are 0.14% (S1), 0.46% (S2), and 0.48% (S3). The in-depth comparative studies indicate that the DLA outperforms the Mueller matrix theory in terms of detection precision and robustness, especially for weak illumination, small optical anisotropy and chirality. The averaged MSEs over a broad waveband ranging from 500 nm to 750 nm are 0.16% (S1), 0.46% (S2), and 0.61% (S3), which are significantly smaller than those derived from the Mueller matrix theory (0.45% (S1), 1% (S2), and 39.8% (S3)). The optical properties of chiral shells, the theory and DLA enabled mapping-relationships, the combination modes of chiral shells, and the MSE spectra have been systematically investigated.

2.
Heliyon ; 10(9): e29870, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38707395

RESUMO

Background: Abnormally expressed Runt-associated transcription factor (RUNX) family has been reported in multiple tumors. Nevertheless, the immunological role of RUNX family in kidney renal clear cell carcinoma (KIRC) remains unknown. Methods: We studied the RNA-seq data regarding tumor and healthy subjects from several public databases in detail for evaluating the prognostic and immunological functions owned by three RUNX genes in cancer patients. Quantitative real-time reverse transcription-polymerase chain reaction (qRT-PCR) and immunohistochemical (IHC) staining served for detecting their expressions in tumor and normal samples. Results: We observed that KIRC patients presented high expressions of RUNX1, RUNX2, and RUNX3. The expressions of three genes were validated by qRT-PCR, which was same as bioinformatical results. Prognostic analysis indicated that the overexpression of RUNX1 and RUNX2 negatively affects the outcomes in patients with KIRC. Related functional predictions indicated that the RUNXs and co-expression genes were significantly related to the immune response pathway. Moreover, three RUNX members were associated with immune infiltration cells and their related gene markers. The expression of RUNX family in several immune cells is positively or negatively correlated, and its dysregulation is obviously associated with the differential distribution of immune cells. RUNX family genes were abnormally expressed in KIRC patients, and were closely related to the crosstalk of immune cells. Conclusions: Our findings may help to understand the pathogenesis and immunologic roles of the RUNX family in KIRC patients from new perspectives.

3.
Proc Natl Acad Sci U S A ; 121(18): e2319751121, 2024 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-38662548

RESUMO

Defect engineering has been widely applied in semiconductors to improve photocatalytic properties by altering the surface structures. This study is about the transformation of inactive WO3 nanosheets to a highly effective CO2-to-CH4 conversion photocatalyst by introducing surface-ordered defects in abundance. The nonstoichiometric WO3-x samples were examined by using aberration-corrected electron microscopy. Results unveil abundant surface-ordered terminations derived from the periodic {013} stacking faults with a defect density of 20.2%. The {002} surface-ordered line defects are the active sites for fixation CO2, transforming the inactive WO3 nanosheets into a highly active catalyst (CH4: O2 = 8.2: 16.7 µmol h-1). We believe that the formation of the W-O-C-W-O species is a critical step in the catalytic pathways. This work provides an atomic-level comprehension of the structural defects of catalysts for activating small molecules.

4.
Small ; : e2402004, 2024 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-38686672

RESUMO

The selective conversion of ethane (C2H6) to ethylene (C2H4) under mild conditions is highly wanted, yet very challenging. Herein, it is demonstrated that a Pt/WO3-x catalyst, constructed by supporting ultrafine Pt nanoparticles on the surface of oxygen-deficient tungsten oxide (WO3-x) nanoplates, is efficient and reusable for photocatalytic C2H6 dehydrogenation to produce C2H4 with high selectivity. Specifically, under pure light irradiation, the optimized Pt/WO3-x photocatalyst exhibits C2H4 and H2 yield rates of 291.8 and 373.4 µmol g-1 h-1, respectively, coupled with a small formation of CO (85.2 µmol g-1 h-1) and CH4 (19.0 µmol g-1 h-1), corresponding to a high C2H4 selectivity of 84.9%. Experimental and theoretical studies reveal that the vacancy-rich WO3-x catalyst enables broad optical harvesting to generate charge carriers by light for working the redox reactions. Meanwhile, the Pt cocatalyst reinforces adsorption of C2H6, desorption of key reaction species, and separation and migration of light-induced charges to promote the dehydrogenation reaction with high productivity and selectivity. In situ diffuse reflectance infrared Fourier transform spectroscopy and density functional theory calculation expose the key intermediates formed on the Pt/WO3-x catalyst during the reaction, which permits the construction of the possible C2H6 dehydrogenation mechanism.

5.
Opt Lett ; 49(5): 1149-1152, 2024 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-38426960

RESUMO

General chiroptical effects describe all of the interaction differences between light carrying opposite spins and chiral matters, such as circular dichroism, optical activity, and chiral Raman optical activity, and have been proven to hold great promise for extensive applications in physics, chemistry, and biology. However, the underlying physical mechanism is usually explained intangibly by the twisted currents in chiral geometry, where the cross coupling between the electric and magnetic dipoles breaks the degeneracy of the helicity eigenmodes. In this Letter, we construct a clear sight on the origination of the chiroptical effect in the view of the eigenstates of a non-Hermitian system, i.e., quasi-normal modes (QNMs). The intrinsic chiroptical effect comes from the chiral QNMs, which have distinct excitation and emission differences in both phase and intensity for lights carrying opposite spins, while the extrinsic chiroptical effect coming from the achiral QNMs requires specific illumination and observation conditions, where the low symmetrical QNM can generate chiroptical effects in both absorption and scattering, but the highly symmetrical QNMs can only generate chiroptical effects in scattering through the coherent superposition of several QNMs. Our findings offer an in-depth understanding of the chiroptical effect and have the potential to bring broad inspiration to the design and applications of chiroptical effects.

6.
J Phys Chem A ; 128(11): 2130-2135, 2024 Mar 21.
Artigo em Inglês | MEDLINE | ID: mdl-38457480

RESUMO

The defect-based single-photon emitters (SPEs) in gallium nitride (GaN) have attracted considerable research interest due to their high emission rate, narrow line width, and room-temperature operation. However, the quenching effect greatly restricts the applications of these SPEs, and the origin of the quenching mechanism is still unclear. Here, based on systematic ab initio calculations, we reveal a possible quenching mechanism originating from the transformation between two different structures of the defect-pair NGaVN in wurtzite GaN. Our results indicate that the defect-pair NGaVN possesses two stable detect-structures A and B, where the structure B has a small zero phonon line (ZPL) and long lifetime. The transformation barrier from structures A to B is only 0.097 eV. Thus, structure A can easily transform to structure B under laser illumination due to thermal fluctuations, causing a quenching phenomenon. Our work also predicts that the barrier energy between defect structures A and B could be effectively adjusted through tuning the triaxial compressive strain of the crystal structure. This provides an effective method to suppress the quenching effect of defect-pair NGaVN in GaN, paving the way for practical applications of SPEs.

7.
Chemosphere ; 352: 141446, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38354866

RESUMO

Heterogeneous photocatalytic degradation of antibiotic involves the activation of antibiotic molecules and the photocatalytic oxidation process. However, the simultaneous improvement of these processes is still a challenge. Herein, S-scheme heterojunctions consisted of Cu2O nanocluster with defective WO3 nanosheets were constructed for efficient photocatalytic degradation of levofloxacin (LVX). The typical CNS-5 composite (5 wt% Cu2O/WO3) achieves an optimal LVX degradation efficiency of 97.9% within 80 min. The spatial charge separation and enhancement of redox capacity were realized by the formation of S-scheme heterojunction between Cu2O and WO3. Moreover, their interfacial interaction would lead to the loss of lattice oxygen and the generation of W5+ sites. It is witnessed that the C-N of piperazine ring and CO of carboxylic acid in LVX are coordinated with W5+ sites to build the electronic bridge to activate LVX, greatly promoting the further degradation. This work highlights the important role of selective coordination activation cooperated with S-type heterojunctions for the photocatalytic degradation and offers a new view to understand the degradation of antibiotics at molecular level.


Assuntos
Antibacterianos , Levofloxacino , Ácidos Carboxílicos , Eletrônica , Oxigênio
8.
J Environ Sci (China) ; 140: 103-112, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38331492

RESUMO

Highly crystalline carbon nitride polymers have shown great opportunities in overall water photosplitting; however, their mission in light-driven CO2 conversion remains to be explored. In this work, crystalline carbon nitride (CCN) nanosheets of poly triazine imide (PTI) embedded with melon domains are fabricated by KCl/LiCl-mediated polycondensation of dicyandiamide, the surface of which is subsequently deposited with ultrafine WO3 nanoparticles to construct the CCN/WO3 heterostructure with a S-scheme interface. Systematic characterizations have been conducted to reveal the compositions and structures of the S-scheme CCN/WO3 hybrid, featuring strengthened optical capture, enhanced CO2 adsorption and activation, attractive textural properties, as well as spatial separation and directed movement of light-triggered charge carriers. Under mild conditions, the CCN/WO3 catalyst with optimized composition displays a high photocatalytic activity for reducing CO2 to CO in a rate of 23.0 µmol/hr (i.e., 2300 µmol/(hr·g)), which is about 7-fold that of pristine CCN, along with a high CO selectivity of 90.6% against H2 formation. Moreover, it also manifests high stability and fine reusability for the CO2 conversion reaction. The CO2 adsorption and conversion processes on the catalyst are monitored by in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), identifying the crucial intermediates of CO2*-, COOH* and CO*, which integrated with the results of performance evaluation proposes the possible CO2 reduction mechanism.


Assuntos
Dióxido de Carbono , Nanopartículas , Nitrilas , Adsorção , Imidas
9.
J Am Chem Soc ; 145(50): 27415-27423, 2023 Dec 20.
Artigo em Inglês | MEDLINE | ID: mdl-38078702

RESUMO

Synchronized conversion of CO2 and H2O into hydrocarbons and oxygen via infrared-ignited photocatalysis remains a challenge. Herein, the hydroxyl-coordinated single-site Ru is anchored precisely on the metallic TiN surface by a NaBH4/NaOH reforming method to construct an infrared-responsive HO-Ru/TiN photocatalyst. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (ac-HAADF-STEM) and X-ray absorption spectroscopy (XAS) confirm the atomic distribution of the Ru species. XAS and density functional theory (DFT) calculations unveil the formation of surface HO-RuN5-Ti Lewis pair sites, which achieves efficient CO2 polarization/activation via dual coordination with the C and O atoms of CO2 on HO-Ru/TiN. Also, implanting the Ru species on the TiN surface powerfully boosts the separation and transfer of photoinduced charges. Under infrared irradiation, the HO-Ru/TiN catalyst shows a superior CO2-to-CO transformation activity coupled with H2O oxidation to release O2, and the CO2 reduction rate can further be promoted by about 3-fold under simulated sunlight. With the key reaction intermediates determined by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and predicted by DFT simulations, a possible photoredox mechanism of the CO2 reduction system is proposed.

10.
Angew Chem Int Ed Engl ; 62(37): e202307930, 2023 Sep 11.
Artigo em Inglês | MEDLINE | ID: mdl-37463869

RESUMO

Poly (triazine imide) (PTI/Li+ Cl- ), one of the crystalline versions of polymeric carbon nitrides, holds great promise for photocatalytic overall water splitting. In principle, the photocatalytic activity of PTI/Li+ Cl- is closely related to the morphology, which could be reasonably tailored by the modulation of the polycondensation process. Herein, we demonstrate that the hexagonal prisms of PTI/Li+ Cl- could be converted to hexagonal nanosheets by adjusting the binary eutectic salts from LiCl/KCl or NaCl/LiCl to ternary LiCl/KCl/NaCl. Results reveal that the extension of in-plane conjugation is preferred, when the polymerisation was performed in the presence of ternary eutectic salts. The hexagonal nanosheets bears longer lifetimes of charge carriers than that of hexagonal prisms due to lower intensity of structure defects and shorter hopping distance of charge carriers along the stacking direction of triazine nanosheets. The optimized hexagonal nanosheets exhibits a record apparent quantum yield value of 25 % (λ=365 nm) for solar hydrogen production by one-step excitation overall water splitting.

11.
Angew Chem Int Ed Engl ; 62(37): e202304694, 2023 Sep 11.
Artigo em Inglês | MEDLINE | ID: mdl-37162371

RESUMO

In situ photo-deposition of both Pt and CoOx cocatalysts on the facets of poly (triazine imide) (PTI) crystals has been developed for photocatalytic overall water splitting. However, the undesired backward reaction (i.e., water formation) on the noble Pt surface is a spontaneously down-hill process, which restricts their efficiency to run the overall water splitting reaction. Herein, we demonstrate that the efficiency for photocatalytic overall water splitting could be largely promoted by the decoration of Rh/Cr2 O3 and CoOx as H2 and O2 evolution cocatalysts, respectively. Results reveal that the dual cocatalysts greatly extract charges from bulk to surface, while the Rh/Cr2 O3 cocatalyst dramatically restrains the backward reaction, achieving an apparent quantum efficiency (AQE) of 20.2 % for the photocatalytic overall water splitting reaction.

12.
Opt Express ; 31(5): 7237-7248, 2023 Feb 27.
Artigo em Inglês | MEDLINE | ID: mdl-36859859

RESUMO

Laser-driven flyers (LDFs), which can drive metal particles to ultra-high speeds by feeding high-power laser, have been widely used in many fields, such as ignition, space debris simulation, and dynamic high-pressure physics. However, the low energy-utilization efficiency of the ablating layer hinders the development of LDF devices towards low power consumption and miniaturization. Herein, we design and experimentally demonstrate a high-performance LDF based on the refractory metamaterial perfect absorber (RMPA). The RMPA consists by a layer of TiN nano-triangular array, a dielectric layer and a layer of TiN thin film, and is realized by combing the vacuum electron beam deposition and colloid-sphere self-assembled techniques. RMPA can greatly improve the absorptivity of the ablating layer to about 95%, which is comparable to the metal absorbers, but obviously larger than that of the normal Al foil (∼10%). This high-performance RMPA brings a maximum electron temperature of ∼7500 K at ∼0.5 µs and a maximum electron density of ∼1.04 × 1016 cm-3 at ∼1 µs, which are higher than that the LDFs based on normal Al foil and metal absorbers due to the robust structure of RMPA under high-temperature. The final speed of the RMPA-improved LDFs reaches to about 1920 m/s measured by the photonic Doppler velocimetry system, which is about 1.32 times larger than the Ag and Au absorber-improved LDFs, and about 1.74times larger than the normal Al foil LDFs under the same condition. This highest speed unambiguously brings a deepest hole on the Teflon slab surface during the impact experiments. The electromagnetic properties of RMPA, transient speed and accelerated speed, transient electron temperature and density have been systematically investigated in this work.

13.
Opt Lett ; 48(6): 1359-1362, 2023 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-36946927

RESUMO

Portable fiber optical spectrometers (PFOSs) have been widely used in the contemporary industrial and agricultural production and life due its low cost and small volume. PFOSs mainly combine one fiber to guide light and one optical spectrometer to detect spectra. In this work, we demonstrate that PFOSs can work as a broadband full-Stokes polarimeter through slightly bending the fiber several times and establishing the mapping relationship between the Stokes parameters S^ and the bending-dependent light intensities I^, i.e., S^=f(I^). The different bending geometries bring different birefringence effects and reflection effects that change the polarization state of the out-going light. In the meanwhile, the grating owns a polarization-depended diffraction efficiency especially for the asymmetric illumination geometry that introduces an extrinsic chiroptical effect, which is sensitive to both the linear and spin components of light. The minimum mean squared error (MSE) can reach to smaller than 1% for S1, S2, and S3 at 810 nm, and the averaged MSE in the wave band from 440 nm to 840 nm is smaller than 2.5%, where the working wavelength can be easily extended to arbitrary wave band by applying PFOSs with proper parameters. Our findings provide a convenient and practical method for detecting full-Stokes parameters.

14.
Adv Sci (Weinh) ; 10(11): e2207178, 2023 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-36737852

RESUMO

Bottom-up assembly of nanoparticle-on-mirror (NPoM) nanocavities enables precise inter-metal gap control down to ≈ 0.4 nm for confining light to sub-nanometer scales, thereby opening opportunities for developing innovative nanophotonic devices. However limited understanding, prediction, and optimization of light coupling and the difficulty of controlling nanoparticle facet shapes restricts the use of such building blocks. Here, an ultraprecise symmetry-breaking plasmonic nanocavity based on gold nanodecahedra is presented, to form the nanodecahedron-on-mirror (NDoM) which shows highly consistent cavity modes and fields. By characterizing > 20 000 individual NDoMs, the variability of light in/output coupling is thoroughly explored and a set of robust higher-order plasmonic whispering gallery modes uniquely localized at the edges of the triangular facet in contact with the metallic substrate is found. Assisted by quasinormal mode simulations, systematic elaboration of NDoMs is proposed to give nanocavities with near hundred-fold enhanced radiative efficiencies. Such systematically designed and precisely-assembled metallic nanocavities will find broad application in nanophotonic devices, optomechanics, and surface science.

15.
Angew Chem Int Ed Engl ; 62(14): e202216434, 2023 Mar 27.
Artigo em Inglês | MEDLINE | ID: mdl-36748541

RESUMO

Poly (triazine imide) photocatalysts prepared via molten salt methods emerge as promising polymer semiconductors with one-step excitation capacity of overall water splitting. Unveiling the molecular conjugation, nucleation, and crystallization processes of PTI crystals is crucial for their controllable structure design. Herein, microscopy characterization was conducted at the PTI crystallization front from meso to nano scales. The heptazine-based precursor was found to depolymerize to triazine monomers within molten salts and KCl cubes precipitate as the leading cores that guide the directional stacking of PTI molecular units to form aggregated crystals. Upon this discovery, PTI crystals with improved dispersibility and enhanced photocatalytic performance were obtained by tailoring the crystallization fronts. This study advances insights into the directional assembling of PTI monomers on salt templates, placing a theoretical foundation for the ordered condensation of polymer crystals.

16.
Chemosphere ; 311(Pt 1): 137053, 2023 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-36332732

RESUMO

ZnIn2S4 ultrathin 2D nanosheets with a positive surface charge are synthesized by a hydrothermal method and different contents of surface S vacancies are induced via heat treatment of as-prepared ZnIn2S4 (ZIS). As the S vacancies contents increased, the photocatalytic degradation efficiency of ceftriaxone (CTRX) sodium is promoted. Especially, ZIS-300 shows the best degradation efficiency (88.8%) for an initial CTRX concentration of 10 mg L-1 in 2 h. It is found that S vacancies cause the electron density of surface metal atoms (Zn, In) to be decreased, which makes the effective adsorption and activation of ceftriaxone anions through electrostatic adsorption interactions. Meanwhile, S vacancies also serve as active centers to promote the absorption of O2 and gather electrons to form •O2- species. The photogenerated holes quickly transfer to the surface of the catalyst to directly degrade the adsorbed CTRX. Thus, the photocatalytic CTRX degradation efficiency is significantly improved. Finally, a possible mechanism for over defective ZIS is proposed. This work provides a feasible strategy for the efficient degradation of antibiotics from the perspective of electrostatic adsorption and molecule activation.


Assuntos
Antibacterianos , Ceftriaxona , Eletricidade Estática , Catálise , Adsorção
17.
ACS Appl Mater Interfaces ; 14(47): 53183-53192, 2022 Nov 30.
Artigo em Inglês | MEDLINE | ID: mdl-36379040

RESUMO

Low-cost and large-area chiral metamaterials (CMs) are highly desirable for practical applications in chiral biosensors, nanophotonic chiral emitters, and beyond. A promising fabrication method takes advantage of self-assembled colloidal particles, onto which metal patches with defined orientation are created using glancing angle deposition (GLAD). However, using this method to make uniform and well-defined CMs over macroscopic areas is challenging. Here, we fabricate a uniform large-area colloidal particle array by interface-mediated self-assembly and precisely control the structural handedness of chiral plasmonic shells (CPSs) using GLAD. Strong chiroptical signals arise from twisted currents at the main, corner, and edge of CPSs, allowing a balance between strong chiroptical and high transmittance properties. Our shell-like chiral geometry shows excellent sensor performance in detecting chiral molecules due to the formation of uniform superchiral fields. Systematic investigations optimize the interplay between peak and null point resonances in different CPSs and result in a record consistency chiral sensor parameter U, i.e., 3.77 for null points and 0.0867 for peaks, which are about 54 and 1.257 times larger than the highest value (0.068) of previously reported CMs. The geometrical chirality, surface plasmonic resonance, chiral surface lattice resonance, and chiral sensor performance evidence the chiroptical effect and the excellent chiral sensor performance.

18.
Nanoscale ; 14(48): 18115-18122, 2022 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-36449012

RESUMO

Point defects in wide bandgap III-nitride semiconductors have been recently reported to be one kind of the most promising near-infrared (NIR) quantum emitters operating at room temperature (RT). But the identification of the point defect species and the energy level structures as well as the transition dynamics remain unclear. Here, the photophysical properties of single-photon emission from point defects in AlGaN films are investigated in detail. According to the first-principles calculations, a three-level model was established to explain the transition dynamics of the quantum emitters. An anti-site nitrogen vacancy complex (VNNGa) was demonstrated to be the most likely origin of the measured emitter since the calculated zero-phonon line (ZPL) and the lifetime of VNNGa in the AlGaN film coincide well with the experimental results. Our results provide new insights into the optical properties and energy level structures of quantum emission from point defects in AlGaN films at RT and establish the foundation for future AlGaN-based on-chip quantum technologies.

19.
Opt Express ; 30(17): 31486-31497, 2022 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-36242228

RESUMO

Ultraviolet chiral metamaterials (UCM) are highly desired for their strong interaction with the intrinsic resonance of molecules and ability in manipulating the polarization state of high energy photons, but rarely reported to date due to their small feature size and complex geometry. Herein, we design and fabricate a kind of novel ultraviolet chiral plasmonic shell (UCPS) by combing the stepwise Al deposition and colloid-sphere assembled techniques. The cancellation effect originated from the disorder lattices of micro-domains in the colloid monolayer has been successfully overcome by optimizing the deposition parameters, and a strong CD signal of larger than 1 deg in the UV region is demonstrated both in simulation and experiment. This strong ultraviolet chiroptical resonances mainly come from the surface chiral lattice resonance mode, the whispering gallery mode and also the interaction between neighbor shells, and can be effectively tuned by changing structural parameters, for example, the sphere diameter, or even slightly increasing the deposition temperature in experiment. To improve the stability, the fabricated UCPSs are protected by N2 in the deposition chamber and then passivated by UV-ozone immediately after each deposition step. The formed UCPS show an excellent stability when exposing in the atmospheric environment. The computer-aided geometrical model, electromagnetic modes, and the tunable chiroptical resonance modes have been systematically investigated.

20.
Chem Sci ; 13(25): 7541-7551, 2022 Jun 29.
Artigo em Inglês | MEDLINE | ID: mdl-35872826

RESUMO

Photoelectrochemical (PEC) water splitting is an appealing approach by which to convert solar energy into hydrogen fuel. Polymeric semiconductors have recently attracted intense interest of many scientists for PEC water splitting. The crystallinity of polymer films is regarded as the main factor that determines the conversion efficiency. Herein, potassium poly(heptazine) imide (K-PHI) films with improved crystallinity were in situ prepared on a conductive substrate as a photoanode for solar-driven water splitting. A remarkable photocurrent density of ca. 0.80 mA cm-2 was achieved under air mass 1.5 global illumination without the use of any sacrificial agent, a performance that is ca. 20 times higher than that of the photoanode in an amorphous state, and higher than those of other related polymeric photoanodes. The boosted performance can be attributed to improved charge transfer, which has been investigated using steady state and operando approaches. This work elucidates the pivotal importance of the crystallinity of conjugated polymer semiconductors for PEC water splitting and other advanced photocatalytic applications.

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