Poly(3‐hexyl thiophene) (P3HT) can be easily synthesized, demonstrating the large potential to decrease the cost in large‐scale synthesis. Thus, the development of novel non‐fullerene acceptor to ...match well with P3HT is urgent and necessary. The first benzotriazole‐containing non‐fullerene acceptor is designed and synthesized, and high open‐circuit voltage (V
oc) of 1.02 V, fill factor (FF) of 0.70, and power conversion efficiency (PCE) of 5.24% are realized, which are remarkably higher than that of P3HT: 6,6‐phenyl‐C61‐butyric acid methyl ester (PC61BM) system (V
oc = 0.59 V, FF = 0.57, and PCE = 3.34%).
Reported herein is an asymmetric Pd/PC‐Phos‐catalyzed denitrogenative cyclization of benzotriazoles with allenes and N‐allenamides, representing the first example of enantioselective denitrogenative ...cyclizations of benzotriazoles. A series of optically active 3‐methyleneindolines were obtained in good yields with high ee values. The use of inexpensive and readily available starting materials, high regio‐ and enantioselectivity, a broad substrate scope, mild reaction conditions, no need for base, as well as versatile functionalization of the 3‐methyleneindolines make this approach attractive.
The first example of an enantioselective denitrogenative cyclization of benzotriazoles with allenes and N‐allenamides is enabled using Pd/PC‐Phos catalysis, and provides rapid access to optically active 3‐methyleneindolines in good yields with high ee values. The method features a general substrate scope, high regioselectivity, and mild reaction conditions. Tf=trifluoromethanesulfonyl.
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•CeO2/Fe3O4 (CeFe) was synthesized and used for PMS activation.•CeFe was magnetic recoverable catalyst for four cycles of reuse.•CeFe/PMS was effective for remediating organic ...pollutants and real wastewater.•UV and US irradiation improved the performance of CeFe/PMS.•Sulfate radical was dominant agent in CeFe/PMS process.
In this work, CeO2-Fe3O4 nano-composite (CeFe) was synthesized and applied to activate peroxymonosulfate (PMS) for degradation of synthetic dye Direct red 16 (DR16). X-ray powder diffraction (XRD), field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), vibrating sample magnetometery (VSM), Brunauer–Emmett–Teller (BET) specific surface area and energy dispersive spectroscopy (EDS) were used to characterize CeFe. Operational parameters of pH, PMS and CeFe dosages were studied. Complete decolorization was obtained at pH = 7.0, 1.5 mM PMS and 0.3 g/L catalyst dosage and 25 min reaction time. Reusability and leaching experiments showed that CeFe nano-composite was a stable and recoverable catalyst for four cycles. Ultraviolet (UV) and ultrasound (US) irradiation improved the rate constant considerably. Fulvic acid, bicarbonate ions and sodium dodecyl sulfate exhibited the inhibitory effect on decolorization in CeFe/PMS. CeFe was effective to activate other chemical oxidants such as persulfate, hydrogen peroxide and percarbonate. Sulfate radical was found as dominant radical in CeFe/PMS while hydroxyl radicals also contributed in DR16 degradation in CeFe/PMS/UVA-LED and CeFe/PMS/US. The performance of CeFe/PMS was also studied on several organic pollutants (direct orange 26, bisphenol A, 2,4,6-trichlorophenol and benzotriazole) and real wastewater.
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We studied the inhibition performances of IMB (imidazoline quaternary salt (IM) and benzotriazole (BTAH)) and IMO (IM and octyl phenol ethoxylates (OP)) mixtures as inhibitors of L245 ...steel placed in 10 vol% HCl solution at 298 K using experimental methods and theoretical calculations. We found that the mixtures adsorb on the steel by an endothermic spontaneous process, and the adsorption model follows Langmuir isotherm. The mixtures exhibit good synergistic inhibition effect, and the inhibition efficiency enhanced in turn (IMB < IMO). The relationship between synergistic effect of organic inhibitors and their energetic position of molecular frontier orbitals was discussed.
•Chlorogenic acid (CGA) and high deacetylation degree of chitosan was conjugated.•The substitution degree of CGA reached up to 144.8mg CGA equivalent/g complex.•The solubility of conjugate was ...greatly enhanced due to conjugation.•The conjugate exhibited higher inhibitory effect on lipid peroxidation than CGA.•The conjugate had higher inhibition on β-carotene-linoleic acid bleaching than CGA.
Chlorogenic acid-chitosan conjugate was synthesized by introducing of chlorogenic acid onto chitosan with the aid of 1-ethyl-3-(3-dimethylaminopropyl) carbodiimide and hydroxybenzotriazole. The data of UV–vis, FT-IR and NMR for chlorogenic acid-chitosan conjugates demonstrated the successful conjugation of chlorogenic acid with chitosan. Compared to chitosan, chlorogenic acid-chitosan conjugates exhibited increased solubility in distilled water, 1% acetic acid solution (v/v) or 50% ethanol solution (v/v) containing 0.5% acetic acid. Moreover, chlorogenic acid-chitosan conjugates showed dramatic enhancements in metal ion chelating activity, total antioxidant capacity, scavenging activities on 2,2′-azino-bis-(3-ethylbenzothiazoline-6-sulphonic acid) and superoxide radicals, inhibitory effects on lipid peroxidation and β-carotene-linoleic acid bleaching, and protective effect on H2O2-induced oxidative injury of PC12 cells. Particularly, chlorogenic acid-chitosan conjugate exhibited higher inhibitory effects on lipid peroxidation and β-carotene-linoleic acid bleaching than chlorogenic acid. The results suggested that chlorogenic acid-chitosan conjugates could serve as food supplements to enhance the function of foods in future.
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•ZIF–MG shows a high adsorption capacity for benzotriazole (BTA) beyond 300mgg−1.•Adsorption kinetics, isotherm and thermodynamics are obtained and modeled.•Factors affecting the BTA ...adsorption are examined including pH, salts and surfactants.•ZIF–MG exhibits a higher selectivity toward BTA over benzimidazole in adsorption.•ZIF–MG is re-used and the regeneration efficiency remains above 98% over 4 cycles.
Benzotriazole (BTA) is extensively-used in industry and households, leading to the increasing detection of BTA in surface water and wastewater. The toxicity of BTA renders it harmful to aquatic organisms and even human; thus BTA has been recognized as an emerging pollutant. Although adsorption is preferable to remove BTA from water, adsorbents proposed for BTA adsorption are quite limited. Considering the positive surface charge and high BTA adsorption capacity of zeolitic imidazole frameworks (ZIFs), a self-assembly of ZIF-67 and negatively-charged magnetic reduced graphene oxide (MG) is prepared via the electrostatic attraction. The resultant ZIF–MG preserves chemical characteristics of ZIF-67 and magnetic property of MG. Thus, ZIF–MG not only shows a high adsorption capacity for BTA but also exhibits magnetic controllability, allowing ZIF–MG to be recovered easily by magnets. The adsorption kinetics, isotherms, and thermodynamics are also determined. With a maximal adsorption capacity of ∼300mgg−1, ZIF–MG is one of the most effective adsorbents when compared with reported adsorbents. ZIF–MG also exhibited relatively stable adsorption capacities at pH=4–9 and a higher selectivity over benzimidazole. Effects of salts and ionic surfactants are insignificant on the BTA adsorption to ZIF–MG. ZIF–MG can be also re-used for the BTA adsorption for multiple cycles and the regeneration efficiency remained 98%. The high adsorption capacity and the magnetically recoverable feature make ZIF–MG a promising and potent adsorbent for BTA in water.
Compared with inorganic or perovskite solar cells, the relatively large non‐radiative recombination voltage losses (ΔVnon‐rad) in organic solar cells (OSCs) limit the improvement of the open‐circuit ...voltage (Voc). Herein, OSCs are fabricated by adopting two pairs of D–π–A polymers (PBT1‐C/PBT1‐C‐2Cl and PBDB‐T/PBDB‐T‐2Cl) as electron donors and a wide‐bandgap molecule BTA3 as the electron acceptor. In these blends, a charge‐transfer state energy (ECT) as high as 1.70–1.76 eV is achieved, leading to small energetic differences between the singlet excited states and charge‐transfer states (ΔECT ≈ 0.1 eV). In addition, after introducing chlorine atoms into the π‐bridge or the side chain of benzodithiophene (BDT) unit, electroluminescence external quantum efficiencies as high as 1.9 × 10−3 and 1.0 × 10−3 are realized in OSCs based on PBTI‐C‐2Cl and PBDB‐T‐2Cl, respectively. Their corresponding ΔVnon‐rad are 0.16 and 0.17 V, which are lower than those of OSCs based on the analog polymers without a chlorine atom (0.21 and 0.24 V for PBT1‐C and PBDB‐T, respectively), resulting in high Voc of 1.3 V. The ΔVnon‐rad of 0.16 V and Voc of 1.3 V achieved in PBT1‐C‐2Cl:BTA3 OSCs are thought to represent the best values for solution‐processed OSCs reported in the literature so far.
The relatively large non‐radiative recombination voltage loss (ΔVnon‐rad) is the main challenge for the development of organic solar cells (OSCs). ΔVnon‐rad of OSCs can be effectively reduced to 0.16 V by adopting material combinations that deliver high ECT (the energy of charge‐transfer state) and low ΔECT (energetic difference between singlet excited state and CT state), together with chlorination in donors.
•An intelligent coating is developed by doping BTA-encapsulated nanocontainers in an epoxy.•The nanocontainers are distributed uniformly in the coating matrix.•The encapsulated inhibitors ...self-release in response to the changes of solution pH.•The intelligent coating effectively inhibits steel corrosion for a long-term immersion.
In this work, an intelligent coating was developed based on encapsulation of benzotriazole (BTA) inhibitors in prepared SiO2 nanoparticle based polyelectrolyte nanocontainers, and self-releasing of the inhibitors for corrosion inhibition to a pipeline steel in a chloride solution. Various morphological, compositional and structural characterizations demonstrate that the inhibitors BTA are effectively encapsulated in the nanocontainers, and the weight percentage of the loaded inhibitors is about 6.7wt% in the nanocontainers. The nanocontainers can be dispersed uniformly in an industry-used epoxy coating under the testing condition, and do not change the coating properties, as shown by the identical glass-transitional temperature of the coatings containing various contents of nanocontainers. The encapsulated BTA can self-release for corrosion inhibition in response to changes of solution pH, as characterized by UV–vis spectroscopy. For the steel coated with the intelligent coating, the corrosion inhibition is time dependent upon self-releasing of the encapsulated inhibitors from the nanocontainers. With the increasing content of the nanocontainers in the coating, both the coating resistance and the corrosion resistance of the steel increase. The released inhibitors inhibit the steel corrosion by forming a layer of inhibitor-adsorptive film, which is detected on the steel surface after 30days of immersion in the solution by elemental and structural characterizations.
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•Catalytic membrane was prepared by citrate sol-gel assisted wet impregnation method.•CeOx-impregnated membrane only required 2.1 mg O3(aq) mg−1 TOC removed.•MnOx-impregnated membrane ...unable to decompose O3(aq) into reactive oxygen species.•Al2O3 substrate could slightly improve HO• and O2•− generation but not TOC removal.•Micropores as microreactor for effective micropollutants mineralization.
This study investigated the degradation of three micropollutants (MPs), namely bisphenol A (BPA), benzotriazole (BTZ) and clofibric acid (CA) by a novel hybrid catalytic ozonation-membrane filtration process. The catalytic ceramic membranes (CCMs) were fabricated via citrate sol-gel assisted wet impregnation method. The surface morphologies and elemental distributions across the CCMs were characterized by FESEM-EDX and AFM. The characterization results suggested that the metal oxides were successfully impregnated throughout the porous structure of the CCMs. The performance of the CCMs was evaluated by a custom-made Hybrid Oxidation Separation Technology (HOST) system. Results indicated that CeOx-impregnated CCM (Ce-CCM) exhibited higher MPs mineralization ability with a 2.1 mg O3(aq) mg−1 TOC removal, as compared to that of MnOx-impregnated CCM (Mn-CCM). The CeOx loading in Ce-CCM could be increased by multiple impregnation cycles, at the expense of decrease in its water permeability. The effect of hydraulic retention time (HRT) towards the hybrid process was further investigated, whereby a higher HRT of 13.7 s was able to achieve up to 38% TOC removal. The quantification of reactive oxygen species (ROS) revealed that the O3(aq) decomposition and ROS generation were enhanced by Ce-CCM, with 0.14 μmol HO• L−1 and 8.78 μmol O2•− L−1 detected. The intermediate by-products of the hybrid process were detected by LC-MS/MS and the MPs degradation pathways via catalytic ozonation were identified. The mechanism of heterogenous catalytic ozonation by Ce-CCM was proposed, based on the presence of surface hydroxyl groups as catalytic sites and involvement of Ce(III/IV) redox pair for electron transfer facilitation in ROS generation. The CCM pores could act as microreactors for effective MPs mineralization in the hybrid process.
A broad‐spectrum, catalytic method has been developed for the synthesis of sulfonamides and sulfamates. With the activation by the combination of a catalytic amount of 1‐hydroxybenzotriazole (HOBt) ...and silicon additives, amidations of sulfonyl fluorides and fluorosulfates proceeded smoothly and excellent yields were generally obtained (87–99 %). Noticeably, this protocol is particularly efficient for sterically hindered substrates. Catalyst loading is generally low and only 0.02 mol % of catalyst is required for the multidecagram‐scale synthesis of an amantadine derivative. In addition, the potential of this method in medicinal chemistry has been demonstrated by the synthesis of the marketed drug Fedratinib via a key intermediate sulfonyl fluoride 13. Since a large number of amines are commercially available, this route provides a facile entry to access Fedratinib analogues for biological screening.
1‐Hydroxybenzotriazole (HOBt) was identified as an efficient nucleophilic catalyst to activate sulfonyl fluorides and fluorosulfates for a broad‐spectrum, catalytic amidation to prepare various sulfonamides and sulfamates, including sterically hindered ones. The potential of this methodology in medicinal and process chemistry has been demonstrated by multidecagram‐scale synthesis of an amantadine derivative and synthesis of the drug Fedratinib.
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