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Nature Communications Sep 2023With the increasing pressure to decarbonize our society, green hydrogen has been identified as a key element in a future fossil fuel-free energy infrastructure. Solar...
With the increasing pressure to decarbonize our society, green hydrogen has been identified as a key element in a future fossil fuel-free energy infrastructure. Solar water splitting through photoelectrochemical approaches is an elegant way to produce green hydrogen, but for low-value products like hydrogen, photoelectrochemical production pathways are difficult to be made economically competitive. A possible solution is to co-produce value-added chemicals. Here, we propose and demonstrate the in situ use of (photo)electrochemically generated H for the homogeneous hydrogenation of itaconic acid-a biomass-derived feedstock-to methyl succinic acid. Coupling these two processes offers major advantages in terms of stability and reaction flexibility compared to direct electrochemical hydrogenation, while minimizing the overpotential. An overall conversion of up to ~60% of the produced hydrogen is demonstrated for our coupled process, and a techno-economic assessment of our proposed device further reveals the benefit of coupling solar hydrogen production to a chemical transformation.
PubMed: 37758705
DOI: 10.1038/s41467-023-41742-4 -
Molecules (Basel, Switzerland) Oct 2023Crop fungal diseases pose a serious threat to global crop production and quality. Developing new and efficient fungicides is an important measure to control crop...
Crop fungal diseases pose a serious threat to global crop production and quality. Developing new and efficient fungicides is an important measure to control crop diseases. Phenylthiazole was found to be an excellent antifungal skeleton based on our previous study on the structural optimization and biological activity of the natural product thiasporine A. To find new fungicides, 45 phenylthiazole derivatives containing an acylhydrazone moiety were designed and synthesized by the principle of active substructure splicing. Forty-two of the forty-five compounds are novel, except for compounds , , and . Their structures were structurally characterized by H NMR, C NMR, and HRMS. The antifungal activities of the target compounds against , , and were evaluated at 25 μg/mL. The bioassay results revealed that most of these compounds exhibited excellent antifungal activities against and at 25 μg/mL. In particular, compounds , , , , , , and showed the inhibition rate of more than 80% against , with EC values of 1.66, 2.01, 2.26, 1.45, 1.50, 1.29, and 2.65 μg/mL, respectively, which were superior to that of the commercial fungicides Isoprothiolane (EC = 3.22 μg/mL) and Phenazine-1-carboxylic acid (EC = 27.87 μg/mL). The preliminary structure-activity relationship (SAR) results suggested that introducing methyl, halogen, or methoxy at the ortho-position of R and the para-position of R can endow the final structure with excellent antifungal activity against . The current results provide useful data for developing phenylthiazole derivatives as new fungicides for controlling rice blast caused by .
Topics: Antifungal Agents; Fungicides, Industrial; Magnaporthe; Structure-Activity Relationship; Magnetic Resonance Spectroscopy
PubMed: 37894562
DOI: 10.3390/molecules28207084 -
RSC Advances Apr 2024In this research and in the line of our researches on the use of nano-substrates modified with ionic liquid in organic reactions, an efficient and green method for the...
In this research and in the line of our researches on the use of nano-substrates modified with ionic liquid in organic reactions, an efficient and green method for the one-pot three-component synthesis of pyrimido[1,2-]benzimidazole and 1-(benzothiazolylamino)methyl-2-naphthol derivatives is reported using a new nanoporous catalyst formulated as ZnO@SOH@Tropine. Further analysis of the catalyst for its characterization has been performed using thermal gravimetric analysis (TGA), field emission scanning electron microscopy (FESEM), X-ray diffraction (XRD), energy dispersive spectrometer (EDS) and Fourier-transform infrared spectroscopy (FT-IR). The present approach creates a variety of biologically active heterocyclic compounds with excellent yields and short reaction times. Among the other advantages of the current method are: ease of operation, clean reaction profiles and ease of separation. Also, this catalyst can be reused five times without loss of its catalytic activity.
PubMed: 38665495
DOI: 10.1039/d3ra08960f -
Molecules (Basel, Switzerland) May 2024Efficient and thorough treatment of dye wastewater is essential to achieve ecological harmony. In this study, a new type of calcium-based modified coal gangue (Ca-CG)...
Efficient and thorough treatment of dye wastewater is essential to achieve ecological harmony. In this study, a new type of calcium-based modified coal gangue (Ca-CG) was prepared by using solid waste coal gangue as raw material and a CaCl modifier, which was used for the removal of malachite green, methylene blue, crystal violet, methyl violet and other dyes in water. When the dosage of Ca-CG was 1-5 g/L, the dosage of Ca-CG was the main factor affecting the dye adsorption effect. The adsorption effects of Ca-CG on four dyes were as follows: malachite green > crystal violet > methylene blue > methyl violet. Kinetics, isotherms and thermodynamic analysis showed that the adsorption of malachite green, methyl blue, crystal violet and methyl violet by Ca-CG fitted the second-order kinetic model, and adsorption with chemical reaction is the main process. The adsorption of four dyes by Ca-CG conformed to the Freundlich model, which is dominated by multi-molecular layer adsorption, and the adsorption was easy to carry out. The adsorption process of Ca-CG on the four dyes was spontaneous. The results of FTIR, XRD and SEM showed that the calcium-based materials such as lipscombite and dolomite were the key to the adsorption of malachite green by Ca-CG, and the main mechanisms for the adsorption of malachite green by Ca-CG are surface precipitation, electrostatic action, and chelation reaction. Ca-CG adsorption has great potential for the removal of dye wastewater.
PubMed: 38792045
DOI: 10.3390/molecules29102183 -
Membranes Nov 2023Membrane technology has been embraced as a feasible and suitable substitute for conventional time- and energy-intensive biodiesel synthesis processes. It is ecofriendly,...
Cleaner Biofuel Production via Process Parametric Optimization of Nonedible Feedstock in a Membrane Reactor Using a Titania-Based Heterogeneous Nanocatalyst: An Aid to Sustainable Energy Development.
Membrane technology has been embraced as a feasible and suitable substitute for conventional time- and energy-intensive biodiesel synthesis processes. It is ecofriendly, easier to run and regulate, and requires less energy than conventional approaches, with excellent stability. Therefore, the present study involved the synthesis and application of a highly reactive and recyclable Titania-based heterogeneous nanocatalyst (TiO) for biodiesel production from nonedible seed oil via a membrane reactor, since is easily and widely accessible and has a rich oil content (39% /). The high free fatty acids content (6.52 mg/g KOH) of the nonedible oil was decreased to less than 1% via two-step esterification. Following the esterification, transesterification was performed using a heterogeneous TiO nanocatalyst under optimum conditions, such as a 9:1 methanol-oil molar ratio, 90 °C reaction temperature, 2 wt.% catalyst loading, and an agitation rate of 600 rpm, and the biodiesel yield was optimized through response surface methodology (RSM). seed oil contains 68.98% unsaturated (61.01% oleic acid, 8.97% linoleic acid) and 31.02% saturated fatty acids (15.91% palmitic acid, 15.11% stearic acid). These fatty acids transformed into respective methyl esters, with a total yield up to 95% achieved. The biodiesel was analyzed via advanced characterization techniques like gas chromatography-mass spectrometry (GC-MS), Fourier transform infrared spectroscopy (FT-IR), and nuclear magnetic resonance (NMR), whereas the catalyst was characterized via X-ray diffraction (XRD), scanning electron microscopy (SEM), energy-dispersive X-ray (EDX), and Fourier transform infrared spectroscopy (FT-IR). Due to its physicochemical properties, seed oil is a highly recommended feedstock for biodiesel production. Moreover, it is concluded that the Titania-based heterogeneous nanocatalyst (TiO) is effective for high-quality liquid fuel synthesis from nonedible seed oil in a membrane reactor, which could be an optional green route to cleaner production of bioenergy, eventually leading to sustenance, robustness, and resilience that will aid in developing a holistic framework for integrated waste management.
PubMed: 38132893
DOI: 10.3390/membranes13120889 -
Current Research in Food Science 2023Changes in flavor volatiles of three colored wheat grains (black, green, and yellow) after cooking were detected via gas chromatography-ion migration spectrometry...
Changes in flavor volatiles of three colored wheat grains (black, green, and yellow) after cooking were detected via gas chromatography-ion migration spectrometry (GC-IMS) to explore corresponding volatile flavor traits. A total of 52 volatile chemicals were spotted among these cooked wheat grains, including 30 aldehydes (accounting for 73.86-83.78%), 11 ketones (9.53-16.98%), 3 alcohols (0.88-1.21%), 4 furans (4.82-7.44%), 2 esters (0.28-0.42%), and 2 pyrazines (0.18-0.32%). Aldehydes, ketones, and furans were the main volatile compounds in three different cooked wheat. For black-colored wheat, the relative contents of benzene acetaldehyde, benzaldehyde, 2-methyl butanal, and 3-methyl butanal were much higher (p < 0.05). For green-colored wheat, the relative contents of nonanal, 2-pentyl furan, ()-hept-2-enal, 2-butanone, and acetone were significantly higher ( < 0.05). For yellow-colored wheat, the relative amounts of heptanal, hexanal, and pentanal were much higher ( < 0.05). The overall volatile substances of the three cooked wheat grains might be classified by GC-IMS data coupled with principal component analysis and heatmap clustering analysis. A reliable forecast set was established through orthogonal partial least squares-discriminant analysis (OPLS-DA), and 22 differential volatile compounds were screened out based on variable importance in projection (VIP) being higher than 1.0, as flavor markers for distinguishing the three cooked wheat grains. These results suggest that GC-IMS could be used for characterizing the flavor volatiles of different colored wheat, and the findings could contribute certain information for understand the aroma traits in different colored cooked wheat and related products in the future.
PubMed: 37691695
DOI: 10.1016/j.crfs.2023.100583 -
Nature Communications May 2024Photocatalytic coupling of methane to ethane and ethylene (C compounds) offers a promising approach to utilizing the abundant methane resource. However, the...
Photocatalytic coupling of methane to ethane and ethylene (C compounds) offers a promising approach to utilizing the abundant methane resource. However, the state-of-the-art photocatalysts usually suffer from very limited C formation rates. Here, we report our discovery that the anatase TiO nanocrystals mainly exposing {101} facets, which are generally considered less active in photocatalysis, demonstrate surprisingly better performances than those exposing the high-energy {001} facet. The palladium co-catalyst plays a pivotal role and the Pd site on co-catalyst accounts for the selective C formation. We unveil that the anatase {101} facet favors the formation of hydroxyl radicals in aqueous phase near the surface, where they activate methane molecules into methyl radicals, and the Pd site participates in facilitating the adsorption and coupling of methyl radicals. This work provides a strategy to design efficient nanocatalysts for selective photocatalytic methane coupling by reaction-space separation to optimize heterogeneous-homogeneous reactions at solid-liquid interfaces.
PubMed: 38789454
DOI: 10.1038/s41467-024-48866-1 -
The Science of the Total Environment Jun 2024Pesticide contamination poses a significant threat to non-target wildlife, including amphibians, many of which are already highly threatened. This study assessed the...
Pesticide contamination poses a significant threat to non-target wildlife, including amphibians, many of which are already highly threatened. This study assessed the extent of pesticide exposure in dead frogs collected during a mass mortality event across eastern New South Wales, Australia between July 2021 and March 2022. Liver tissue from 77 individual frogs of six species were analysed for >600 legacy and contemporary pesticides, including rodenticides. More than a third (36 %) of the liver samples contained at least one of the following pesticides: brodifacoum, dieldrin, DDE, heptachlor/heptachlor epoxide, fipronil sulfone, and 2-methyl-4-chlorophenoxyacetic acid (MCPA). Brodifacoum, a second-generation anticoagulant rodenticide, was found in four of the six frog species analysed: the eastern banjo frog (Limnodynastes dumerilii), cane toad (Rhinella marina), green tree frog (Litoria caerulea) and Peron's tree frog (Litoria peronii). This is the first report of anticoagulant rodenticide detected in wild amphibians, raising concerns about potential impacts on frogs and extending the list of taxa shown to accumulate rodenticides. Dieldrin, a banned legacy pesticide, was also detected in two species: striped marsh frog (Limnodynastes peronii) and green tree frog (Litoria caerulea). The toxicological effects of these pesticides on frogs are difficult to infer due to limited comparable studies; however, due to the low frequency of detection the presence of these pesticides was not considered a major contributing factor to the mass mortality event. Additional research is needed to investigate the effects of pesticide exposure on amphibians, particularly regarding the impacts of second-generation anticoagulant rodenticides. There is also need for continued monitoring and improved conservation management strategies for the mitigation of the potential threat of pesticide exposure and accumulation in amphibian populations.
Topics: Animals; Rodenticides; Anura; Anticoagulants; Pesticides; Environmental Monitoring; New South Wales; Australia
PubMed: 38636866
DOI: 10.1016/j.scitotenv.2024.172526 -
Gels (Basel, Switzerland) Dec 2023Novel chemically cross-linked hydrogels derived from carboxymethyl cellulose (CMC) and alginate (Alg) were prepared through the utilization of the norbornene (Nb)-methyl...
Novel chemically cross-linked hydrogels derived from carboxymethyl cellulose (CMC) and alginate (Alg) were prepared through the utilization of the norbornene (Nb)-methyl tetrazine (mTz) click reaction. The hydrogels were designed to generate reactive oxygen species (ROS) from an NIR dye, indocyanine green (ICG), for combined photothermal and photodynamic therapy (PTT/PDT). The cross-linking reaction between Nb and mTz moieties occurred via an inverse electron-demand Diels-Alder chemistry under physiological conditions avoiding the need for a catalyst. The resulting hydrogels exhibited viscoelastic properties (G' ~ 492-270 Pa) and high porosity. The hydrogels were found to be injectable with tunable mechanical characteristics. The ROS production from the ICG-encapsulated hydrogels was confirmed by DPBF assays, indicating a photodynamic effect (with NIR irradiation at 1-2 W for 5-15 min). The temperature of the ICG-loaded hydrogels also increased upon the NIR irradiation to eradicate tumor cells photothermally. In vitro cytocompatibility assessments revealed the non-toxic nature of CMC-Nb and Alg-mTz towards HEK-293 cells. Furthermore, the ICG-loaded hydrogels effectively inhibited the metabolic activity of Hela cells after NIR exposure.
PubMed: 38131947
DOI: 10.3390/gels9120961 -
Ecotoxicology and Environmental Safety Jul 2024The purpose of this study is to evaluate the decolorization ability and detoxification effect of LAC-4 laccase on various types of single and mixed dyes, and lay a good...
The purpose of this study is to evaluate the decolorization ability and detoxification effect of LAC-4 laccase on various types of single and mixed dyes, and lay a good foundation for better application of laccase in the efficient treatment of dye pollutants. The reaction system of the LAC-4 decolorizing single dyes (azo, anthraquinone, triphenylmethane, and indigo dyes, 17 dyes in total) were established. To explore the decolorization effect of the dye mixture by LAC-4, two dyes of the same type or different types were mixed at the same concentration (100 mg/L) in the reaction system containing 0.5 U laccase, and time-course decolorization were performed on the dye mixture. The combined dye mixtures consisted of azo + azo, azo + anthraquinone, azo + indigo, azo + triphenylmethane, indigo + triphenylmethane, and triphenylmethane + triphenylmethane. The results obtained in this study were as follows. Under optimal conditions of 30 °C and pH 5.0, LAC-4 (0.5 U) can efficiently decolorize four different types of dyes. The 24-hour decolorization efficiencies of LAC-4 for 800 mg/L Orange G and Acid Orange 7 (azo), Remazol Brilliant Blue R (anthraquinone), Bromophenol Blue and Methyl Green (triphenylmethane), and Indigo Carmine (indigo) were 75.94%, 93.30%, 96.56%, 99.94%, 96.37%, and 37.23%, respectively. LAC-4 could also efficiently decolorize mixed dyes with different structures. LAC-4 can achieve a decolorization efficiency of over 80% for various dye mixtures such as Orange G + Indigo Carmine (100 mg/L+100 mg/L), Reactive Orange 16 + Methyl Green (100 mg/L+100 mg/L), and Remazol Brilliant Blue R + Methyl Green (100 mg/L+100 mg/L). During the decolorization process of the mixed dyes by laccase, four different interaction relationships were observed between the dyes. Decolorization efficiencies and rates of the dyes that were difficult to be degraded by laccase could be greatly improved when mixed with other dyes. Degradable dyes could greatly enhance the ability of LAC-4 to decolorize extremely difficult-to-degrade dyes. It was also found that the decolorization efficiencies of the two dyes significantly increased after mixing. The possible mechanisms underlying the different interaction relationships were further discussed. Free, but not immobilized, LAC-4 showed a strong continuous batch decolorization ability for single dyes, two-dye mixtures, and four-dye mixtures with different structures. LAC-4 exhibited high stability, sustainable degradability, and good reusability in the continuous batch decolorization. The LAC-4-catalyzed decolorization markedly reduced or fully abolished the toxic effects of single dyes (azo, anthraquinone, and indigo dye) and mix dyes (nine dye mixtures containing four structural types of dyes) on plants. Our findings indicated that LAC-4 laccase had significant potential for use in bioremediation due to its efficient degradation and detoxification of single and mixed dyes with different structural types.
Topics: Coloring Agents; Laccase; Azo Compounds; Reishi; Trityl Compounds; Water Pollutants, Chemical; Biodegradation, Environmental; Anthraquinones; Indigo Carmine; Hydrogen-Ion Concentration; Water Decolorization; White
PubMed: 38768540
DOI: 10.1016/j.ecoenv.2024.116450