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71.
Conventional thermally activated delayed fluorescence (TADF) molecules achieve small energy differences between the lowest singlet and triplet excited states (ΔEST) by enhancing the intramolecular charge transfer, which inevitably leads to a wide emission spectrum and low fluorescence rate. Here, we prepared a deep blue TADF molecule via a small ΔEST pyridine-phenol fluoroboron complex as the acceptor. The small ΔEST is maintained when carbazole donors are attached to the 4-position of the phenyl rings in the fluoroboron complex. Benefiting from the strong electron coupling between the donor (D) and acceptor (A) moieties, the compound Cz-4-BF exhibits a high fluorescence rate of 4.8 × 108 s−1 and a small D-A dihedral angle change in the excited state. Consequently, a photoluminescence (PL) quantum yield of nearly 100% and a PL spectrum with full-width at half-maximum (FWHM) < 60 nm were obtained in solution and low-concentration doped films. A TADF-sensitized fluorescence (TSF) device containing Cz-4-BF achieves an external quantum efficiency of 21%, which is higher than the devices employing classical fluorescent emitters and multiple resonance-type TADF emitters. The Cz-4-BF-based TSF device shows significantly improved color coordinates of (0.14, 0.10) versus a control device without Cz-4-BF. 相似文献
72.
Robert Groth Luke T. Cravigan Sadegh Niazi Zoran Ristovski Graham R. Johnson 《Journal of the Royal Society Interface》2021,18(178)
The airborne dynamics of respiratory droplets, and the transmission routes of pathogens embedded within them, are governed primarily by the diameter of the particles. These particles are composed of the fluid which lines the respiratory tract, and is primarily mucins and salts, which will interact with the atmosphere and evaporate to reach an equilibrium diameter. Measuring organic volume fraction (OVF) of cough aerosol has proved challenging due to large variability and low material volume produced after coughing. Here, the diametric hygroscopic growth factors (GF) of the cough aerosol produced by healthy participants were measured in situ using a rotating aerosol suspension chamber and a humidification tandem differential mobility analyser. Using hygroscopicity models, it was estimated that the average OVF in the evaporated cough aerosol was 0.88 ± 0.07 and the average GF at 90% relative humidity (RH) was 1.31 ± 0.03. To reach equilibrium in dry air the droplets will reduce in diameter by a factor of approximately 2.8 with an evaporation factor of 0.36 ± 0.05. Hysteresis was observed in cough aerosol at RH = ∼35% and RH = ∼65% for efflorescence and deliquescence, respectively, and may depend on the OVF. The same behaviour and GF were observed in nebulized bovine bronchoalveolar lavage fluid. 相似文献
73.
Jinfeng Han Huidong Fan Qingyang Zhang Qin Hu Thomas P. Russell Howard E. Katz 《Advanced functional materials》2021,31(5):2005901
Two donor–acceptor (D–A) polymers are obtained by coupling difluoro- and dichloro-substituted forms of the electron-deficient unit BDOPV and the relatively weak donor moiety dichlorodithienylethene (ClTVT). The conductivity and power factors of doped devices are different for the chlorinated and fluorinated BDOPV polymers. A high electron conductivity of 38.3 and 16.1 S cm−1 are obtained from the chlorinated and fluorinated polymers with N-DMBI, respectively, and 12.4 and 2.4 S cm−1 are obtained from the chlorinated and fluorinated polymers with CoCp2, respectively, from drop-cast devices. The corresponding power factors are 22.7, 7.6, 39.5, and 8.0 µ W m−1 K−2, respectively. Doping of PClClTVT with N-DMBI results in excellent air stability; the electron conductivity of devices with 50 mol% N-DMBI as dopant remained up to 4.9 S m−1 after 222 days in the air, the longest for an n-doped polymer stored in air, with a thermoelectric power factor of 9.3 µ W m−1 K−2. However, the conductivity of PFClTVT-based devices can hardly be measured after 103 days. These observations are consistent with morphologies determined by grazing incidence wide angle X-ray scattering and atomic force microscopy. 相似文献
74.
James E. Tyrrell Martyn G. Boutelle Alasdair J. Campbell 《Advanced functional materials》2021,31(1):2007086
Biological environments use ions in charge transport for information transmission. The properties of mixed electronic and ionic conductivity in organic materials make them ideal candidates to transduce physiological information into electronically processable signals. A device proven to be highly successful in measuring such information is the organic electrochemical transistor (OECT). Previous electrophysiological measurements performed using OECTs show superior signal-to-noise ratios than electrodes at low frequencies. Subsequent development has significantly improved critical performance parameters such as transconductance and response time. Here, interdigitated-electrode OECTs are fabricated on flexible substrates, with one such state-of-the-art device achieving a peak transconductance of 139 mS with a 138 µs response time. The devices are implemented into an array with interconnects suitable for micro-electrocorticographic application and eight architecture variations are compared. The two best-performing arrays are subject to the full electrophysiological spectrum using prerecorded signals. With frequency filtering, kHz-scale frequencies with 10 µV-scale voltages are resolved. This is supported by a novel quantification of the noise, which compares the gate voltage input and drain current output. These results demonstrate that high-performance OECTs can resolve the full electrophysiological spectrum and suggest that superior signal-to-noise ratios could be achieved in high frequency measurements of multiunit activity. 相似文献
75.
Timothy Zurrer Kenneth Wong Jonathan Horlyck Emma C. Lovell Joshua Wright Nicholas M. Bedford Zhaojun Han Kang Liang Jason Scott Rose Amal 《Advanced functional materials》2021,31(9):2007624
The vast chemical and structural tunability of metal–organic frameworks (MOFs) are beginning to be harnessed as functional supports for catalytic nanoparticles spanning a range of applications. However, a lack of straightforward methods for producing nanoparticle-encapsulated MOFs as efficient heterogeneous catalysts limits their usage. Herein, a mixed-metal MOF, NiMg-MOF-74, is utilized as a template to disperse small Ni nanoclusters throughout the parent MOF. By exploiting the difference in Ni O and Mg O coordination bond strength, Ni2+ is selectively reduced to form highly dispersed Ni nanoclusters constrained by the parent MOF pore diameter, while Mg2+ remains coordinated in the framework. By varying the ratio of Ni to Mg in the parent MOF, accessible surface area and crystallinity can be tuned upon thermal treatment, influencing CO2 adsorption capacity and hydrogenation selectivity. The resulting Ni nanoclusters prove to be an active catalyst for CO2 methanation and are examined using extended X-ray absorption fine structure and X-ray photoelectron spectroscopy. By preserving a segment of the Mg2+-containing MOF framework, the composite system retains a portion of its CO2 adsorption capacity while continuing to deliver catalytic activity. The approach is thus critical for designing materials that can bridge the gap between carbon capture and CO2 utilization. 相似文献
76.
77.
采用水溶液聚合法制备了低分子量聚丙烯酸钾(PAAK),并作为新型消焰剂加入单基发射药中。通过火焰原子吸收光谱法测试了PAAK中钾的含量;用乌氏黏度计测定了特性黏度;采用DSC法研究不同pH值的PAAK与硝化棉(NC)的相容性;利用充氮氧弹法对添加PAAK、硝酸钾KNO3、硫酸钾K2SO4的单基发射药的燃烧残渣进行了对比研究。结果表明,合成的PAAK中,钾的质量分数为15.21%,相对分子量在3 000左右,有利于和NC均匀混合,且在中性或微碱性(pH=7.0~7.5)的情况与NC相容性良好。与传统的KNO3、K2SO4消焰剂相比,PAAK能够和NC均匀混合,制备均质透明的单基发射药;PAAK发射药的燃烧残渣最少,占发射药质量的0.18%。 相似文献
78.
Solid acids as a substitution for hazardous liquid acids (e.g., HF and H2SO4) can promote many important reactions in the industry, such as carbon cracking, to proceed in a more sustainable way. Starting from a zirconium‐based metal‐organic framework (UiO‐66 nanocrystals), herein a transformative method is reported to prepare micro/mesoporous yttria‐stabilized zirconia (YSZ) encapsulated inside a mesoporous silica shell. It is then further demonstrated that the resultant reactor‐like catalysts can be used for a wide range of catalytic reactions. The acidity of the YSZ phase is found with rich accessible Lewis acid and Brønsted acid sites and they display superior performances for esterification (acetic acid and ethanol) and Friedel‐Crafts alkylation (benzylation of toluene). After being loaded with different noble metals, furthermore, hydrogenation of CO2 and a one‐pot cascade reaction (nitrobenzene and benzaldehyde to N‐benzylaniline) are used as model reactions to prove the versatility and stability of catalysts. Based on the findings of this work, it is believed that this class of reactor‐like catalysts can meet future challenges in the development of new catalyst technology for greener heterogeneous catalysis. 相似文献
79.
80.
Choaro D. Dithugoe Dr. Jacqueline van Marwijk Prof. Martha S. Smit Dr. Diederik J. Opperman 《Chembiochem : a European journal of chemical biology》2019,20(1):96-102
Biocatalytic production of lactones, and in particular ϵ-caprolactone (CL), have gained increasing interest as a greener route to polymer building blocks, especially through the use of Baeyer–Villiger monooxygenases (BVMOs). Despite several advances in the field, BVMOs, however, still suffer several practical limitations. Alcohol dehydrogenase (ADH)-mediated lactonization of diols in turn has received far less attention and very few enzymes have been identified for the conversion of diols to lactones, with horse-liver ADH (HLADH) remaining the catalyst of choice. Screening of a diverse panel of ADHs, AaSDR-1, a member of the short-chain dehydrogenase/reductase family, was found to produce ϵ-caprolactone from hexane-1,6-diol. Moreover, cofactor regeneration by an NADH oxidase eliminated the requirement of co-substrates, yielding water as the sole by-product. Despite lower turnover frequencies as compared to HLADH, higher selectivity was found for the production of CL, with HLADH forming significant amounts of 6-hydroxyhexanoic acid and adipic acid through aldehyde dehydrogenation/oxidation of the gem-diol intermediates. Also, CL yield were shown to be dependent on buffer choice, as structural elucidation of a Tris adduct confirmed the buffer amine to react with aliphatic aldehydes forming a Schiff-base intermediate which through further ADH oxidation, forms a tricyclic acetal product. 相似文献