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Diffusion Behavior of Differently Charged Molecules in Self-Assembled Organic Nanotubes Studied Using Imaging Fluorescence Correlation Spectroscopy
摘要： The diffusion behavior of fluorescent molecules within bolaamphiphile-based organic nanotubes (ONTs) was systematically investigated using imaging fluorescence correlation spectroscopy (imaging FCS). Anionic sulforhodamine B (SRB), zwitterionic/cationic rhodamine B (RB) or cationic rhodamine 123 (R123) was loaded into ONTs having cylindrical hollow structures (ca. 10 nm in inner diameter) with amine and glucose groups on the inner and outer surfaces, respectively. Wide-field fluorescence video microscopy was used to acquire imaging FCS data for dye-doped ONTs in aqueous solutions of different ionic strengths (1 – 500 mM) at different pH (3.4 – 8.4). The diffusion behavior of these dyes was discussed on the basis of their apparent diffusion coefficients (D) that were determined by autocorrelating the time transient of fluorescence intensity at each pixel on an ONT. Molecular diffusion in the ONTs was significantly slowed by molecule-nanotube interactions, as shown by the very small D (10-1 – 10-2 μm2/s). The pH-dependence of D revealed that dye diffusion was basically controlled by electrostatic interactions associated with the protonation of the amine groups on the ONT inner surface. The pH-dependent change in D was observed over a wide pH range, possibly due to electrostatically induced variations in the pKa of the densely packed ammonium ions on the ONT inner surface. On the other hand, the influence of ionic strength on D was relatively unclear, suggesting the involvement of non-coulombic interactions with the ONTs in molecular diffusion. Importantly, individual ONTs of different lengths (1 – 5 μm) afforded similar diffusion coefficients for each type of dye at each solution condition, implying that the properties of ONTs were uniform in terms of solute loading and release. These results highlight the characteristics of molecular diffusion behavior within the ONTs, and will help in the design of organic nanotubes better suited for use as drug vehicles and contaminant adsorbents.
关键词： Electrostatic Interactions,Diffusion Behavior,Ionic Strength,pH-dependence,Imaging Fluorescence Correlation Spectroscopy,Organic Nanotubes
更新于2025-11-19 16:56:42
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Strategies towards rational design of gold(iii) complexes for high-performance organic light-emitting devices
摘要： Gold(iii) complexes are attractive candidates as phosphorescent dopants in organic light-emitting devices for high-luminance full-colour displays. However, no data on the stability of such devices have been reported to date. Through rational molecular design and synthesis, we have successfully generated a new class of cyclometalated gold(iii) C^C^N complexes with tunable emission colours spanning from sky-blue to red. These complexes exhibit high photoluminescence quantum yields of up to 80% in solid-state thin films, excellent solubility and high thermal stability. Solution-processable and vacuum-deposited organic light-emitting devices based on these complexes operate with external quantum efficiencies of up to 11.9% and 21.6%, respectively, and operational half-lifetimes of up to 83,000 h at 100 cd m?2.
关键词： operational stability,phosphorescent dopants,organic light-emitting devices,cyclometalated,gold(iii) complexes,C^C^N complexes
更新于2025-11-19 16:56:35
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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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Synthesis, Photophysical and Electroluminescent Properties of Iridium(III) Complexes with 2-Aryl-thiazole and Oxadiazol-substituted Amide Derivative Ligands
摘要： By using aryl-thiazole as cyclometalated ligand and oxadiazol-substituted amide as ancillary ligand, three novel iridium(III) complexes have been synthesized and characterized, and the photophysical and electrochemical properties have been investigated. Complexes 1–3 exhibit efficient phosphorescence emissions at 542, 555 and 585 nm with photoluminescence quantum yields (PLQYs) of 0.04, 0.03 and 0.02 in CH3CN solutions, respectively. In the 10 wt% doped 2,4-diphenyl-6-bis(12-phenylindolo)[2,3-a]carbazole-11-yl)-1,3,5-triazine (Dictrz) film, the PLQYs (0.88 for complex 1, 0.47 for complex 2 and 0.37 for complex 3) increase significantly owing to the great restriction of rotations and vibrations in rigid host. The organic light-emitting diodes based on these complexes show good performance with the maximum current efficiencies of 20.06, 22.20 and 13.45 cd A-1 and maximum power efficiencies of 13.54, 17.31 and 9.48 lm W?1 with the CIE coordinates of (0.46, 0.53), (0.49, 0.50) and (0.59, 0.40) for complexes 1?3, respectively.
关键词： Iridium complex,Aryl-thiazole,Organic light-emitting diodes,Oxadiazol-substituted amide
更新于2025-11-19 16:56:35
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An AND logic gate-based fluorescence probe for the detection of homovanillic acid, an indicator of the tumor
摘要： Homovanillic acid (HVA) is one of the major metabolites of catecholamine in human. An elevated level of HVA in urine and blood has been associated with many diseases, including catecholamine-secreting tumors. Consequently, detection of the biomarker HVA in urine is an effective strategy to detect cancer precursors and early stage cancers. In this study, a fluorescence probe is designed and fabricated by integrating lanthanide ions with metal-organic frameworks (MOFs). The fluorescence probe shows distinguished response toward HVA and exhibits ratiometric detection of HVA, rendering it an excellent candidate for sensing devices. Thus, we have designed logic gate operation integrating the probe with logical operations for the intelligent sensing of HVA. Furthermore, this type of luminesce based sensors integrated with logic gate augur for the further application in real-time early diagnosis of tumors in the future.
关键词： Rare earth,Homovanillic acid,Fluorescent probe,Logic gate,Ratiometric sensing,Metal-organic frameworks
更新于2025-11-19 16:56:35
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An anti-symmetric dual (ASD) Z-scheme photocatalytic system: (ZnIn2S4/Er3+:Y3Al5O12@ZnTiO3/CaIn2S4) for organic pollutants degradation with simultaneous hydrogen evolution
摘要： An anti-symmetric dual (ASD) Z-scheme ZnIn2S4/Er3+:Y3Al5O12@ZnTiO3/CaIn2S4 photocatalyst was prepared by isoelectric point and calcination methods. The photocatalytic activity is estimated via degradation of Acid Orange II as a target organic contaminant with simultaneous hydrogen evolution under simulated solar-light irradiation. The prepared ASD Z-scheme ZnIn2S4/Er3+:Y3Al5O12@ZnTiO3/CaIn2S4 photocatalyst has a high photocatalytic activity, which can be assigned to the enlarged photoresponse range, increased reduction surface and enhanced separation efficiency of photo-induced carriers. Furthermore, the cyclic experiment proves that the prepared ASD Z-scheme ZnIn2S4/Er3+:Y3Al5O12@ZnTiO3/CaIn2S4 photocatalyst still maintains a high photocatalytic activity within five repetitive cycles. Moreover, the mechanism on photocatalytic degradation of organic pollutants with simultaneous hydrogen evolution caused by ASD Z-scheme ZnIn2S4/Er3+:Y3Al5O12@ZnTiO3/CaIn2S4 photocatalyst is proposed. It is wished that this study could provide a promising pathway for effective degradation and rapid hydrogen production.
关键词： Simultaneous hydrogen evolution,Organic contaminants,Anti-symmetric dual (ASD) Z-scheme photocatalytic system,ZnIn2S4/Er3+:Y3Al5O12@ZnTiO3/CaIn2S4 composite,Up-conversion luminescence agent,Photocatalytic degradation
更新于2025-11-19 16:51:07
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A Luminescent Metal-Organic Framework with Pre-Designed Functionalized Ligands as an Efficient Fluorescence Sensing for Fe3+ Ions
摘要： Metal-organic frameworks are a class of attractive materials for fluorescent sensing. Here, we report the exploration of fluorescent Zn-based amine/azine-functionalized MOF, TMU-17-NH2, ([Zn(NH2-BDC)(4-bpdb)].2DMF; NH2-BDC = amino-1,4-benzenedicarboxylic acid, 4-bpdb = 1,4-bis(4-pyridyl)-2,3-diaza-2,3-butadiene) for highly selective and sensitive detection of Fe3+ in DMF solution. TMU-17-NH2 shows fast recognition of Fe3+ ion with a response time of <1 min and detection limit of 0.7 μM (40 ppb), and the luminescence is completely quenched in 10-3 M DMF solution of Fe3+. Furthermore, the static quenching constant is calculated to be upper than 41000 M-1 by the fluorescence titration experiment in low concentration of Fe3+. No interferences from 250 μM As3+, Cd2+, Zn2+, Co3+, Ni2+, Cu2+, Pb2+, Mn2+ and Al3+ were found for the detection of Fe3+. The efficient fluorescent quenching effect is attributed to the photoinduced electron transfer between Fe3+ ions and the amino-functionalized ligand in this MOF. Moreover, the introduced azine N donors in the 4-bpdb ligand of TMU-17-NH2 additionally donate their lone-pair electrons to the Fe3+ ions, leading to significantly enhanced detection ability. Furthermore, the regenerated TMU-17-NH2 still has high selectivity for Fe3+ ions, which suggests that the functionalized TMU-17-NH2 is a promising luminescent probe for selectively sensing of Fe3+ ions.
关键词： Metal-Organic Frameworks,Sensing,Fluorescence,Functionalization,Fe3+
更新于2025-11-19 16:46:39
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Highly Sensitive and Selective Fluorescent Sensor based on a Multi-Responsive Ultrastable Amino-Functionalized Zn(II)-MOF for Hazardous Chemicals
摘要： A microscale amino-functionalized Zn(II)-MOF, namely [Zn(NH2-bdc)(4,4’-bpy)] (1) (NH2-H2bdc = 2-amino-1,4-benzenedicarboxylic acid and 4,4’-bpy = 4,4’-bipyridine), has been successfully synthesized, structurally characterized and further utilized as multi-responsive fluorescent sensor for highly sensitive and selective detection of Cr(VI) and 2,4,6-trinitrophenol (TNP). Compound 1 features non-porous 5-fold interpenetrated 3D framework with the Lewis basic sites including the uncoordinated amino and carboxylate groups on the framework for anchoring and recognizing the guest. 1 exhibits not only excellent water and thermal stability but also tolerance to acidic and basic media over an extensive pH range of 2-12. This ultrastable material can sensitively and selectively detect Cr2O7 2- and CrO4 2- in water based on the luminescent quenching with relatively low limits of detection (2.21 μM for CrO4 2- and 1.30 μM for Cr2O7 2-). Moreover, the unprecedented solvent-dependent luminescent response of 1 as a fluorescent probe for high-efficiency TNP detection was observed. Significantly, 1 not only displays high sensitive fluorescent enhancement upon TNP binding in ethanol but also exhibits fluorescent quenching toward TNP in water with very low limits of detection of 4.47 nM and 0.32 μM in ethanol and water, respectively. This work reports the first example of the utilization of MOF as a sensor for the detection of TNP based on dual responsive luminescence. Importantly, 1 can be simply and rapidly regenerated, displaying excellent recyclability after the sensing experiments.
关键词： Multi-responsive fluorescent sensors,Fluorescent quenching,Metal-organic framework,2,4,6-trinitrophenol,Fluorescent enhancement,Cr(VI)
更新于2025-11-19 16:46:39
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Preparation of high-purity α-Si3N4 nano-powder by precursor-carbothermal reduction and nitridation
摘要： This work investigated the role of natural organic matter (NOM) in the environmental processes of silver nanoparticles (AgNP) and the uptake and accumulation of AgNP in wheat. Different NOMs (Suwannee River humic acids [SRHA], fulvic acid [FA]) and Ag elements (Ag(0) and Ag+) were incubated in a hydroponic media for 15 days. The results showed that the NOM (10 mg C L-1) altered the dissolution, stabilization, uptake and accumulation of AgNP. The dissolution of AgNP declined in the presence of NOM. Compared with FA, the dissolved Ag+ decreased much more from 0.30 mg L-1 to 0.10 mg L-1 in the presence of SRHA. The fluorescence quenching results indicated that SRHA exhibited stronger binding to Ag+ than that of FA, and the quenching constants Ksv were 0.1309 (SRHA) and 0.0074 (FA), respectively. CeO, CeH, CeOeC, and MeeOH were involved in the interaction between NOM and AgNP. The NOM decreased the accumulated content of Ag in wheat. Hence, NOM alleviated the inhibition of AgNP to wheat growth. SRHA reduced the Ag content of wheat roots approximately 3-fold. These results clearly indicated the importance of NOM on altering the behavior, fate and toxicity of AgNP in an environment.
关键词： Wheat,Nanoparticle fate,Accumulation,Natural organic matter,Silver nanoparticle
更新于2025-11-19 16:46:39
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Building Intermixed Donor-Acceptor Architectures for Water-Processable Organic Photovoltaics
摘要： A modified synthesis method for aqueous nanoparticle printing inks, based upon vacuum-assisted solvent removal, is reported. Poly(3-hexylthiophene) : phenyl C61 butyric acid methyl ester nanoparticle inks were prepared via this modified miniemulsion method; leading to both an improvement in photoactive layer morphology and a substantial reduction in the ink fabrication time. A combination of UV-visible spectroscopy, photoluminescence spectroscopy and scanning transmission X-ray microscopy measurements revealed a nanoparticle morphology comprised of highly intermixed donor-acceptor domains. Consistent with these measurements, dynamic mechanical thermal analysis of the nanoparticles showed a glass transition temperature (Tg) of 104 °C, rather than a pure polymer phase or pure fullerene phase Tg. Together the spectroscopy, microscopy and thermomechanical data indicate that rapid solvent removal generates a more blended nanoparticle morphology. As such, this study highlights a new experimental lever for optimising nanostructure in the photoactive layer of nanoparticulate organic photovoltaic devices by enabling highly intermixed donor-acceptor architectures to be built from customised nanoparticulate inks.
关键词： organic photovoltaic,scanning transmission X-ray microscopy,morphology,colloidal inks,exciton dissociation,Nanostructure,eco-friendly processing
更新于2025-11-19 16:46:39