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Insights into the thermo-photo catalytic production of hydrogen from water on a low-cost NiOx-loaded TiO2 catalyst
摘要： Thermo-photo catalytic water splitting, where the introduction of thermal energy increases the oxidation driving force for narrow-band-gap photocatalysts (with a low valence band potential), exhibited significantly advanced performance for hydrogen production compared with general water splitting at room temperature. Herein, a low-cost NiOx-loaded TiO2 catalyst was reported for thermo-photo catalytic water splitting with methanol as the sacrificial agent. The catalyst with an optimal Ni ratio of 5 wt.% achieved a hydrogen evolution rate of 53.7 mmol/h/g under simulated AM 1.5G sunlight at 260℃, which was 2.5 times more than that without illumination, with apparent quantum efficiencies of 66.24%, 33.55%, 32.52% and 15.35% at 380, 420, 450 and 500 nm, respectively. More impressively, under the irradiation of visible light (λ>420 nm) at this temperature, and photohydrogen yield could still reach 26.9 mmol/h/g, which was 5 orders of magnitude greater than that (0.0011 mmol/h/g) conducted at room temperature. Isotope tracer experiments demonstrated that the introduction of photo energy promoted the hydrogen production mainly by enhancing hydrogen evolution from water splitting rather than methanol decomposition or reformation. Furthermore, the step-wise reaction mechanism was revealed with insights into the synergistic roles of thermo-energy and photo-energy for production of hydrogen from water. Those findings highlight the great promise of thermo-photo catalysis and should inspire more efforts for water splitting.
关键词： visible light,Hydrogen production,nickel-based catalysts,thermo-photo catalysis,titanium dioxide
更新于2025-11-14 17:03:37
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Visible light-induced oxidation of aqueous arsenite using facile Ag2O/TiO2 composites: Performance and mechanism
摘要： Conversion of aqueous arsenite [As(III)] to less toxic arsenate [As(V)] is a critical step for the arsenic pollution remediation. In this study, Ag2O/TiO2 composites synthesized via the pH-induced precipitation method were employed into the photocatalytic oxidation of As(III) under visible light irradiation. X-ray diffraction, transmission electron microscope and X-ray photoelectron spectroscopy analysis verified the formation of Ag2O/TiO2 heterostructures. Compared to pure Ag2O and TiO2, the 30% Ag2O/TiO2 composite exhibited much higher photochemical reactivities for the oxidation of As(III) under visible light irradiation. Under the optimal conditions [pH=4.0, the photocatalyst dosage being 0.3 g L-1 and initial As(III) concentration being 10 mg L-1], the oxidation and removal percent of As(III) was 60.7% and 83.0% after reaction for 120 min, respectively. Moreover, the formation of Ag(0) over the surface of Ag2O by photo-induced electrons contributed to the high stability of Ag2O/TiO2 composite. It was also found that photo-generated holes and superoxide radicals played the predominant roles in the As(III) oxidation. The improved photocatalytic activities were attributed to the formation of the hetero-junctions between Ag2O and TiO2, the strong visible light absorption, and the high separation efficiency of photo-generated electron-hole pairs resulted from the Schottky barriers at the Ag-Ag2O interface.
关键词： visible light,arsenite oxidation,Ag2O/TiO2 composite,photocatalytic
更新于2025-11-14 17:03:37
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Synthesis of visible light responsive iodine-doped mesoporous TiO2 by using biological renewable lignin as template for degradation of toxic organic pollutants
摘要： The visible light responsive I-doped mesoporous TiO2 (I/TiO2-T) catalysts were synthesized by facile hydrolysis method with lignin as a template. The resulting I/TiO2-T catalysts synthesized from different amounts of I as a dopant and lignin as a template were characterized by X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), transmission electron microscopy (TEM), UV-Vis diffuse spectroscopy (DRS), Fourier transform infrared spectroscopy (FTIR), photoluminescence (PL), and electrochemical impedance spectroscopy (EIS). The photocatalytic activities of the resulting catalysts were investigated by the degradation of p-chlorophenol under artificial visible light irradiation. The results showed that the lignin-templated TiO2 with a suitable amount of I-doping (I/TiO2-T) had higher catalytic activity than the catalyst prepared form I-doped TiO2 without lignin template (I/TiO2). Complete degradation of p-chlorophenol was achieved by I/TiO2-T with suitable amount of I-doping at 60 min. However, 95.7, 10.7, and 5.5% of the p-chlorophenol was degraded with I/TiO2, TiO2-T, and P25 catalysts, respectively, under 140 min visible light irradiation. The enhanced catalytic activities of the samples with template and I-doping may be due to the small grain size and high specific surface area of the catalysts. The band gap and the electrical properties of TiO2 also could be adjusted with I-doping. The I-doped TiO2 with the extrinsic I5+-to-Ti4+ and the iodine-to-oxygen donor defects could be excited by visible irradiation for efficient pollutants degradation. A possible photocatalytic mechanism for the degradation of the pollutants with I/TiO2-T under visible light irradiation was also proposed.
关键词： Mesoporous TiO2,Visible light,I-doped,Lignin template
更新于2025-11-14 17:03:37
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Novel hole blocking materials based on 2,6-disubstituted dibenzo[ <i>b</i> , <i>d</i> ]furan and dibenzo[ <i>b</i> , <i>d</i> ]thiophene segments for high-performance blue phosphorescent organic light-emitting diodes
摘要： Novel hole blocking materials (HBMs) based on 2,6-disubstituted dibenzo[b,d]furan and dibenzo[b,d]thiophene segments, 3,30,300,30 0 0-(dibenzo[b,d]furan-2,6-diylbis(benzene-5,3,1-triyl))tetrapyridine (26DBFPTPy) and 3,30,300,30 0 0-(dibenzo[b,d]thiophene-2,6-diylbis(benzene-5,3,1-triyl))tetrapyridine (26DBTPTPy), are successfully designed and synthesized for high-performance blue phosphorescent organic light-emitting diodes (PhOLEDs) for the first time. Computational simulation is used to investigate the optimal structure, orbital distribution, and physicochemical properties of both molecules. Thermal, optical, and electrochemical analysis shows that 26DBFPTPy and 26DBTPTPy possess high thermal stability, deep HOMO energy levels ((cid:2)7.08 and (cid:2)6.91 eV), and a high triplet energy (ET) (2.75 and 2.70 eV). Blue PhOLEDs with 26DBFPTPy or 26DBTPTPy as a hole blocking layer (HBL) exhibit a low turn-on voltage (3.0 V) and operating voltage (4.5 V) at 1000 cd m(cid:2)2. In addition, the blue PhOLEDs with 26DBFPTPy or 26DBTPTPy show superior external quantum e?ciencies (24.1 and 23.6%) and power e?ciencies (43.9 and 42.7 lm W(cid:2)1). They also show a very small e?ciency roll-o? of about 8.5% from 100 to 1000 cd m(cid:2)2. Furthermore, they exhibit improved lifetimes compared to the similarly designed HBL with a pyridine electron transport unit and a phenyl core structure.
关键词： dibenzo[b,d]furan,hole blocking materials,dibenzo[b,d]thiophene,blue phosphorescent organic light-emitting diodes,high-performance
更新于2025-11-14 15:32:45
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Ultrathin, Core–Shell Structured SiO <sub/>2</sub> Coated Mn <sup>2+</sup> ‐Doped Perovskite Quantum Dots for Bright White Light‐Emitting Diodes
摘要： All-inorganic semiconductor perovskite quantum dots (QDs) with outstanding optoelectronic properties have already been extensively investigated and implemented in various applications. However, great challenges exist for the fabrication of nanodevices including toxicity, fast anion-exchange reactions, and unsatisfactory stability. Here, the ultrathin, core–shell structured SiO2 coated Mn2+ doped CsPbX3 (X = Br, Cl) QDs are prepared via one facile reverse microemulsion method at room temperature. By incorporation of a multibranched capping ligand of trioctylphosphine oxide, it is found that the breakage of the CsPbMnX3 core QDs contributed from the hydrolysis of silane could be effectively blocked. The thickness of silica shell can be well-controlled within 2 nm, which gives the CsPbMnX3@SiO2 QDs a high quantum yield of 50.5% and improves thermostability and water resistance. Moreover, the mixture of CsPbBr3 QDs with green emission and CsPbMnX3@SiO2 QDs with yellow emission presents no ion exchange effect and provides white light emission. As a result, a white light-emitting diode (LED) is successfully prepared by the combination of a blue on-chip LED device and the above perovskite mixture. The as-prepared white LED displays a high luminous efficiency of 68.4 lm W?1 and a high color-rendering index of Ra = 91, demonstrating their broad future applications in solid-state lighting fields.
关键词： quantum dots,white light-emitting diodes,core–shells,Mn2+-doping,SiO2-coating
更新于2025-11-14 15:32:45
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Far-Red Spectrum of Second Emerson Effect: A Study Using Dual-Wavelength Pulse Amplitude Modulation Fluorometry
摘要： Non-additive enhancement of the photosynthesis excited by simultaneous illumination with far-red light and light of shorter wavelengths is called as “second Emerson effect”. Its action spectra are well-known as a photosynthetic yield’s dependence on light wavelength in red (630-690 nm) spectral region at a constant-wavelength far-red illumination near 700-715 nm. However, the opposite dependence of the photosynthetic yield’s of shorter constant-wavelength light (red or blue) on light wavelength in far-red (690-760 nm) spectral region was never studied. In this study the action spectrum of second Emerson effect was studied using a fast-Fourier dual-wavelength Pulse Amplitude Modulation (PAM) fluorometry. Chlorophyll fluorescence in ailanthus (Ailanthus altissima Mill.) leaves was excited with blue modulated light. Far-red induced decrease of fluorescence (fluorescence shift-FRIFS) was studied in response to illumination of leaves with a background light from 690 to 760 nm (10 nm step), calculating FRIFS = (F0-Fs)/F0, where F0-fluorescence measured without and Fs-with far-red light. Maximum FRIFS was observed at 720 nm (11.8%), but it still remained considerable at 740, 750 nm and a low FRIFS values were revealed at 690 and even at 760 nm. Measurements carried out with blue saturating flashes during and after far-red illumination showed the increase of quantum yield of Photosystem II (PSII), calculated as Fv/Fm at 720 nm background light. FRIFS had lower values under excitation with red modulating light. It is concluded that FRIFS is a result of a photochemical quenching caused by an additional selective far-red excitation of PSI in conditions when PSII is preferably excited by blue light thus leading the PSI to limit non-cyclic electron flow. The contradiction between the known absorption spectra of PSI-light harvesting complex I and the observed action spectrum of second Emerson effect (FRIFS spectrum) is discussed.
关键词： Photosystem II,Ailanthus Altissima,Photosystem I,Second Emerson Effect,Fast-Fourier PAM-Fluorometry,Far-Red Light,Thylakoid Electron Transport
更新于2025-11-14 15:30:11
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Optical Characterization of Doped Thermoplastic and Thermosetting Polymer-Optical-Fibers
摘要： The emission properties of a graded-index thermoplastic polymer optical fiber and a step-index thermosetting one, both doped with rhodamine 6G, have been studied. The work includes a detailed analysis of the amplified spontaneous emission together with a study of the optical gains and losses of the fibers. The photostability of the emission of both types of fibers has also been investigated. Comparisons between the results of both doped polymer optical fibers are presented and discussed.
关键词： polymer optical fibers,thermoplastic fibers,rhodamine 6G,light-emitting polymers,optical gain,amplified spontaneous emission,thermosetting fibers
更新于2025-11-14 15:30:11
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Tricolor- and White Light–Emitting Ce <sup>3+</sup> /Tb <sup>3+</sup> /Mn <sup>2+</sup> -Coactivated Li <sub/>2</sub> Ca <sub/>4</sub> Si <sub/>4</sub> O <sub/>13</sub> Phosphor via Energy Transfer
摘要： Single-component tunable Li2Ca4Si4O13:Ce3+,Tb3+,Mn2+ phosphors were successfully synthesized at 950 °C. Li2Ca4Si4O13:Ce3+,Tb3+ exhibits two luminescence peaking at 430 and 550 nm, which originated from the allowed 5d → 4f transition of the Ce3+ ion and the 5D4 → 7FJ (J = 6, 5, 4, 3) transition of the Tb3+ ion, respectively. Moreover, by codoping Ce3+ ions in the Li2Ca4Si4O13:Mn2+ system, yellow-red emission from the forbidden transition of Mn2+ could be enhanced. Under UV excitation, dual energy transfers (ETs), namely, Ce3+ → Mn2+ and Ce3+ → Tb3+, are present in the Li2Ca4Si4O13:Ce3+,Tb3+,Mn2+ system. The ET process was confirmed by the overlap of the excitation spectra, variations in the emission spectra, ET efficiency, and decay times of phosphors. In addition, quantum yields and CIE chromatic coordinates are presented. The emission color of these phosphors can be tuned precisely from blue to green via ET of Ce3+ → Tb3+ and from blue to yellow via ET of Ce3+ → Mn2+. White light can also be achieved upon excitation of UV light by properly tuning the relative composition of Tb3+/Mn2+. This result indicates that the developed phosphor may be regarded as a good tunable emitting phosphor for UV light-emitting diodes.
关键词： phosphor,energy transfer,Mn2+,Tb3+,Li2Ca4Si4O13,Ce3+,white light-emitting diodes
更新于2025-11-14 15:29:11
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Directed Nanoscale Self-assembly of Natural Photosystems on Nitrogen-doped Carbon Nanotubes for Solar Energy Harvesting
摘要： Natural photosystems (PSs) have received much attention as a biological solar energy harvester because of their high quantum efficiency for energy transfer. However, the PSs hybridized with solid electrodes exhibit low light-harvesting efficiencies because of poor interface properties and random orientations of PSs, all of which interfere with efficient charge extraction and transfer. Herein, we report the linker-free, oriented self-assembly of natural PSs with nitrogen-doped carbon nanotubes (NCNTs) via electrostatic interaction. Protonated nitrogen-doped sites on the NCNTs facilitate spontaneous immobilization of the negatively charged stroma side of PSs, which provides a favorable orientation for electron transfer without electrically insulating polymer linkers. The resulting PS/NCNT hybrids exhibit a photocurrent density of 1.25 ± 0.08 μA cm-2, which is much higher than that of PS/CNT hybrids stabilized with polyethylenimine (0.60 ± 0.01 μA cm-2) and sodium dodecyl sulfate (0.14 ± 0.01 μA cm-2), respectively. This work emphasizes the importance of the linker-free assembly of PSs into well-oriented hybrid structures to construct an efficient light-harvesting electrode.
关键词： Light-harvesting,Electrostatic interaction,Photosystems,Nitrogen-doped carbon nanotubes,Self-assembly
更新于2025-11-14 15:29:11
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Increasing photoluminescence quantum yield by nanophotonic design of quantum-confined halide perovskite nanowire arrays
摘要： High photoluminescence quantum yield (PLQY) is required to reach optimal performance in solar cells, lasers and light-emitting diodes (LEDs). Typically, PLQY can be increased by improving the material quality to reduce the non-radiative recombination rate. It is in principle equally effective to improve the optical design by nanostructuring a material to increase light out-coupling efficiency and introduce quantum confinement, both of which can increase the radiative recombination rate. However, increased surface recombination typically minimizes nanostructure gains in PLQY. Here a template guided vapor phase growth of CH3NH3PbI3 (MAPbI3) nanowire (NW) arrays with unprecedented control of NW diameter from the bulk (250 nm) to the quantum confined regime (5.7 nm) is demonstrated, while simultaneously providing a low surface recombination velocity of 18 cm s-1. This enables a 56-fold increase in the internal PLQY, from 0.81 % to 45.1 %, and a 2.3-fold increase in light out-coupling efficiency to increase the external PLQY by a factor of 130, from 0.33 % up to 42.6 %, exclusively using nanophotonic design.
关键词： light out-coupling,photoluminescence quantum yield,quantum confinement,perovskite,photodetector
更新于2025-11-14 15:28:36