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Triplet-State Photochemistry of Dissolved Organic Matter: Triplet-State Energy Distribution and Surface Electric Charge Conditions
摘要： Excited triplet states of chromophoric dissolved organic matter (3CDOM*) are highly reactive species in sunlit surface waters and play a critical role in reactive oxygen species (ROS) formation and pollutant attenuation. In the present study, a series of chemical probes, including sorbic acid, sorbic alcohol, sorbic amine, trimethylphenol, and furfuryl alcohol, were employed to quantitatively determine 3CDOM* and 1O2 in various organic matters. Using a high concentration of sorbic alcohol as high-energy triplet states quencher, 3CDOM* can be first distinguished as high-energy triplet states (>250 kJ mol?1) and low-energy triplet states (<250 kJ mol?1). The terrestrial-origin natural organic matter (NOM) was found to mainly consist of low-energy triplet states, while high-energy triplet states were predominant in autochthonous-origin NOM and effluent/wastewater organic matter (EfOM/WWOM). The 1O2 quantum yields and electron transfer quantum yield coefficients (f TMP) generated from low-energy triplet states remained constant in all tested organic matters. External phenolic compound showed quenching effects on triplet-state formation and tended to have a higher quenching efficiency for aromatic ketone triplet states, which are the main high-energy triplet states. In comparison with terrestrial-origin NOM, autochthonous-origin NOM and EfOM/WWOM presented lower reaction rate constants for sorbic amines and higher reaction rate constants for sorbic acid, and these differences are likely due to dissimilar surface electric charge conditions. Understanding the triplet-state photochemistry of CDOM is essential for providing useful insights into their photochemical effects in aquatic systems.
关键词： surface charge,triplet-state photochemistry,energy distribution,dissolved organic matter,reactive oxygen species,chemical probes
更新于2025-11-19 16:56:35
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Assembly structure and free energy change of a chromonic liquid crystal formed by a perylene dye
摘要： The nematic (chromonic N) and isotropic phases formed by aqueous solutions of a perylene dye are investigated by x-ray diffraction and visible light absorption spectroscopy. X-ray diffraction shows that the molecules assemble into columns one molecule wide. The change in the visible absorption spectrum with concentration indicates that the molecules stack in a more or less isodesmic manner and that the free energy change associated with the addition or removal of a single molecule from a stack is 16–20 kBT. This range is appreciably higher than those of any previously-measured simple chromonic systems, i.e. those with single molecule-wide columns. It is suggested that the large free energy change promotes the formation of extremely long columns of molecules, and in turn leads to the low concentration at which mesophase formation takes place.
关键词： chromonic,isodesmic,scission energy,perylene dye,assembly structure,lyotropic chromonic,Liquid crystals
更新于2025-11-19 16:56:35
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Tuning Molecular Solar Thermal properties by modification of a promising norbornadiene photoswitch
摘要： Carefully targeted modifications to the norbornadiene-quadricyclane couple should give molecules with great potential for solar energy storage. Here we report the synthesis of derivatives of a well-studied compound, 2-cyano-3-anisyl norbornadiene (NBD5). The conjugation was extended by conversion of the nitrile into acrylonitrile and acrylate derivatives over two steps. Despite red-shifting the absorbance properties, the metastable quadricyclanes exhibited extremely short lifetimes. Meanwhile, treatment of NBD5 with acetyl halides in the presence of aluminum trihalides led to the formation of 7-acetyl norbornenes through a Meerwein-Wagner rearrangement. Subsequent transformations made it possible to synthesise norbornadienes with varying degrees of steric bulk at the 7-position of the molecular scaffold. It was found that the bulkier this group was, the more stable the quadricyclane form. This reaction sequence allows for the synthesis of norbornadiene derivatives which are more suited to molecular solar thermal applications in domestic heating despite providing a slightly lower energy density.
关键词： Meerwein-Wagner rearrangement,conjugation,strained molecules,photochromism,energy density
更新于2025-11-19 16:56:35
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Vanadium salt assisted solvothermal reduction of graphene oxide and the thermoelectric characterisation of the reduced graphene oxide in bulk and as composite
摘要： The solvothermal reduction of graphene oxide (GO), modified by the addition of vanadium chloride, resulted in an increased reduction degree of the reduced graphene oxide (rGO), which is reflected by a remarkably increased electrically conductivity of up to 8.5 S/cm, a value 30 times higher than that of rGO prepared without vanadium salt addition. Parallel with this increase, the thermoelectrical properties of rGO are improved, with a reached maximum Seebeck coefficient of 13.7 μV/K. The rGOs were used as fillers in flexible styrene-butadiene-styrene triblock copolymer composites prepared by solution mixing. Compared to the traditionally prepared reduced graphene oxide, the new product provides up to 60 times higher conductivity to the composite, while the Seebeck coefficient is nearly the same. The highest power factor of 4.6 x 10-4 μW/(m·K2) was achieved at 100 °C with 30 wt% loading, which is 30 times higher than that of the traditional reduced graphene oxide containing composite.
关键词： nanomaterials,functional materials,energy materials,composites,polymers
更新于2025-11-19 16:56:35
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Correlation between the morphology and the opto-electronic and electrical properties of organometallic halide perovskite (CH<sub>3</sub>NH<sub>3</sub>MH<sub>3</sub>) thin films
摘要： Organometallic halide perovskites are emerging as a promising class of materials for optoelectronic applications. Crystal morphology is important for improving the organic-inorganic lead halide perovskite semiconductor property in optoelectronic, electrical and photovoltaic devices. It is thus important to investigate how the changes in crystal morphology affect the semiconductor behavior. This work presents a study that was carried out to assess the relationship between different deposition methodologies and the opto-electronic and electrical properties of the resultant organometallic halide perovskite thin films. Herein, single step solution deposition method and two step solution deposition methods have been used to deposit perovskite thin films. The structure and morphology of perovskite was controlled by changing concentration, annealing temperatures and dip coating times. From the study, prepared films showed different morphologies as the concentration, annealing temperatures and dip coating times were varied. Optical band gap energies of 2.23 eV, 2.13 eV and 2.09 eV were obtained for samples prepared by single step solution deposition method and 1.57 eV, 1.55 eV and 1.52 eV for two step solution deposition method. The sheet resistance values decreased with an increase in concentration, annealing temperatures and dip coating times. The decrease in optical band gap energy and sheet resistances are excellent properties for high performance photovoltaic devices.
关键词： Perovskite,sheet resistivity,activation energy,band gap,sheet resistance,spectroscopy
更新于2025-11-19 16:56:35
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Cu3MS4 (M=V, Nb, and Ta) and their solid solutions with sulvanite structure for photocatalytic and photoelectrochemical H2 evolution under visible light irradiation
摘要： Solid solutions with a sulvanite structure between Cu3VS4 and either Cu3NbS4 or Cu3TaS4 (Cu3Nb1-xVxS4, Cu3Ta1-xVxS4) were successfully prepared by a solid-state reaction. Their band gaps were 1.6–1.7 eV corresponding to the absorption of a wide range of visible light. Ru-cocatalyst loaded Cu3MS4 (M=V, Nb, Ta), Cu3Nb1-xVxS4, and Cu3Ta1-xVxS4 showed photocatalytic activities for sacrificial H2 evolution under visible light irradiation. Most solid solutions showed better activities than the single Cu3MS4 (M=V, Nb, Ta). Cu3MS4 (M=V, Nb), Cu3Nb1-xVxS4, and Cu3Ta1-xVxS4 also functioned as a photoelectrode and gave cathodic photocurrents under visible light irradiation, indicating a p-type semiconductor character. Cu3Nb0.9V0.1S4 showed the best photocatalytic and photoelectrochemical performances. When Ru-loaded Cu3Nb0.9V0.1S4 was used as a photocathode with a CoOx-loaded BiVO4 photoanode, photoelectrochemical water splitting proceeded under simulated sunlight irradiation without an external bias.
关键词： Energy conversion,Water splitting,Heterogeneous catalysis,Photocatalysis
更新于2025-11-19 16:51:07
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Broad-Spectrum Tunable Photoluminescent Material Based on Cascade Fluorescence Resonance Energy Transfer between Three Fluorophores Encapsulated within the Self-Assembled Surfactant Systems
摘要： A broad spectrum tunable photoluminescent material with dual encryption based on a two-step Fluorescence Resonance Energy Transfer (FRET) between Pyrene (Py), Coumarin480 (Cou480) and Rhodamine6G (R6G) in micelles of SDS and bmimDS is presented. The phenomenon is achievable due to the encapsulation of the fluorophores within these micelles. The transfer of energy as FRET between the pair Py and Cou480 showed ON at 336 nm and OFF at 402 nm in contrast to the FRET observed between the pair Cou480 and R6G that showed ON at 402nm and OFF at 336 nm. However, the transfer of energy as FRET occurs from Py to R6G in the presence of Cou480 when excited at 336 nm, thereby making it a chain of three fluorophores with Cou480 acting as a relay fluorophore receiving energy from Py and transferring it to R6G. The different FRET scenarios between the three fluorophores in micelles provide a window for the generation of a matrix of colors, which occupies a significant 2D area in the chromaticity diagram, having potential applications in security printing. The different fluorophoric ratios generate different colors based on their individual photonic emissions and the FRET processes taking place between them. Writing tests were carried out using varied ratios of the fluorophores in the micellar systems producing different colored outputs under the UV light with insignificant visibility under the white light. We envision that this as-discovered three fluorophoric FRET system could form the basis for the future development of multi-FRET light-harvesting devices and anti-counterfeiting security inks based on much simpler non-covalent interaction aided encapsulation of the fluorophores within the self-assembled soft systems.
关键词： micelles,security printing,Rhodamine6G (R6G),SDS,Pyrene (Py),Coumarin480 (Cou480),bmimDS,Fluorescence Resonance Energy Transfer (FRET),photoluminescent material
更新于2025-11-19 16:46:39
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High lying energy of charge-transfer states and small energetic offsets enabled by fluorinated quinoxaline-based alternating polymer and alkyl-thienyl side-chain modified non-fullerene acceptor
摘要： Significant driving forces are the prerequisite to achieve fast and efficient charge separation in fullerene derivatives-based polymer solar cells to achieve high power conversion efficiency (PCE). However, the large driving forces both in photo-induced hole transfer (PHT) and in photo-induced electron transfer (PET) processes lead to significant energy losses, resulting in low open-circuit voltage in the devices. Recent studies indicate the driving forces in non-fullerene acceptors-based devices can be reduced to very low values but still with high PCE and low energy losses. Herein, we report a new donor:acceptor system with high lying energy of charge-transfer excitons (ECT) of 1.50 eV and very small driving forces (PHT of 0.28 eV and PET of 0.11 eV), in which a fluorinated quinoxaline-based alternating polymer (FTQ) and an alkyl-thienyl side-chain modified small molecule (ITIC-Th) are taken as the donor material and non-fullerene acceptor material, respectively. A high power conversion efficiency (PCE) of 8.19% with maximal external quantum efficiency of 71% are achieved successfully in FTQ:ITIC-Th-based device after appropriate thermal annealing treatment, indicating FTQ can be further applied as donor materials with other highly efficient NF-acceptors to achieve enhanced performances and low energy losses.
关键词： Power conversion efficiency,Driving forces,Energy of charge-transfer states,Polymer solar cells
更新于2025-11-14 17:28:48
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Tailored nanocomposite energy harvesters with high piezoelectric voltage coefficient through controlled nanowire dispersion
摘要： Composites composed of piezoelectric nanomaterials dispersed in a flexible polymer have emerged as promising materials for highly durable and flexible energy harvesters and sensors. Although piezoelectric materials in their bulk form have a high electromechanical coupling coefficient and can efficiently convert mechanical energy to electrical energy, the ceramic form has low fracture toughness and thus they are limited in certain applications due to difficulty in machining and conforming to curved surfaces. Recently, additive manufacturing processes such as direct write, have been developed to incorporate piezoelectric nanowires into a polymer matrix with controlled alignment to realize printed piezoelectrics. Given the multiphase structure of a nanocomposite, it is possible to control the material structure such that the piezoelectric coupling and dielectric properties can be varied independently. In this paper, experimentally validated finite element (FE) and micromechanics models are developed for calculation and optimization of the piezoelectric voltage coefficient, g31, of a nanocomposite. It is shown that by using high aspect ratio nanowires with controlled alignment, the piezoelectric coupling can be disproportionately increased with respect to the dielectric constant which yields a g31 coefficient that can be enhanced more than seven times compared to the bulk piezoelectric material. Moreover, it is demonstrated that the use of high aspect ratio nanowires in the energy harvester resulted in significant improvement on the output electrical power of an energy harvester.
关键词： Energy harvesting,Nanowires,Finite element modeling (FEM),Voltage coefficient,Piezoelectric,The Mori-Tanaka method,Direct write,Nanocomposite
更新于2025-11-14 17:28:48
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Electrical and optical properties of organic light-emitting diodes with rhenium(I) complexes using DC and AC methods
摘要： Four rhenium(I) tricarbonyl complexes with 1,10-phenanthroline and derivative bearing electron-donating CH3 and OCH3 substituents were doped into host material poly (9-vinylcarbazole) (PVK) with a mass ratio of 8% as the emissive layer in organic light-emitting diodes (OLEDs). All complexes showed photoluminescence in the solution and embedded into a PVK matrix (λmax～520–550 nm). The comparison with the bare PVK emission and the compound/PVK ?lm shows that the emission of the polymer was quenched through an energy transfer process from PVK to the dopant. The electrical properties of the devices with FTO/PEDOT:PSS/Complex:PVK/Al architecture were investigated using the DC method by curves of current density-voltage and the AC method as admittance spectroscopy, which showed that the behavior of the devices is controlled by charge carrier injection rather than bulk transport.
关键词： Energy transfer,Re(I) complexes,Charge injection,Admittance spectroscopy,Emission,OLEDs
更新于2025-11-14 17:28:48