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Pettersson MacGregor posted an update 6 months, 3 weeks ago
Besides photoelectrode materials, realizing the synergy of the photochemical environment and photoelectrodes for high charge carrier utilization is crucial for enhancing the performance of photoelectrochemical (PEC) water splitting systems. However, few researchers have focused on this important aspect. Herein, the effect of the photochemical environment on photoanodes in PEC water splitting, including the redox potential of electrolytes and light direction, is rationally discussed. A combined study of the potential distribution and electrochemical impedance spectroscopy reveals that the low redox potential of electrolytes facilitates the interior charge transfer and surface charge utilization by enlarging the depletion layer. In addition, it is found that the optimum thickness of semiconductors in photoelectrodes is the length of the depletion layer plus diffusion layer.Gd3+ and Tm3+ doped Prussian blue (Gd/Tm-PB) with high uniformity and dispersibility was synthesized by a facile solvothermal method. The conditions for the synthesis of Gd/Tm-PB were explored. Through the regulation of the ratio of Gd3+/Tm3+, the Gd/Tm-PB particles with the optimal size (about 150-200 nm) and the best fluorescence and photothermal effect were obtained. On the basis of the optimal Gd/Tm-PB, further coated by polydopamine (PDA) functionalized metal-organic frameworks (MOFs), a multifunctional platform Gd/Tm-PB@ZIF-8/PDA for cancer diagnosis and treatment was established. Doxorubicin (DOX) was selected as a drug model and the drug loading of Gd/Tm-PB@ZIF-8/PDA was found to be 81 mg g-1. Cytotoxicity analysis indicated that Gd/Tm-PB@ZIF-8/PDA was highly biocompatible. The DOX release at different pH values and GSH concentrations revealed an excellent pH/GSH-triggered drug release. Through the combination of the near infrared photothermal performance of Gd/Tm-PB, chemo-photothermal therapy can be achieved to further improve the anti-cancer efficiency. In addition, the Gd/Tm-PB@ZIF-8/PDA nanoparticles can be tracked by fluorescence imaging (FOI) and magnetic resonance imaging (MRI). Cell FOI and in vivo MRI experiments showed the potential application of Gd/Tm-PB@ZIF-8/PDA in dual mode imaging guided therapy. In vivo antitumor experiments demonstrated the higher anticancer efficacy of Gd/Tm-PB@ZIF-8/PDA with a combined effect of chemo-photothermal therapy. This work provides a new strategy for nano-drug carriers in the direction of integrated diagnosis and treatment.3D printing of chitosan hydrogels has attracted wide interest because of their excellent biocompatibility, antibacterial activities, biodegradability, zero toxicity and low cost. However, chitosan inks are often involved in toxic and organic solvents. Moreover, the recently reported 3D-printed chitosan scaffolds lack enough strength, thus limiting their use in tissue engineering. 5-Chloro-2′-deoxyuridine mouse Here, we reported a chitosan ink obtained by dissolving chitosan into an alkali aqueous solution. This chitosan ink is a stable solution at low temperature (5 °C), but once heated, the chitosan chains self-assemble to lead to gelation. Based on this principle, a corresponding direct ink writing (DIW) method was developed to print high-strength chitosan hydrogels. Specifically, the chitosan ink was extruded into heated deionized water to complete the in situ gelation. The temperature of the nozzle and hot water was well controlled to keep the printing process stable. The rheological behavior of the chitosan ink was investigated and the printing parameters were systematically studied to print chitosan hydrogel scaffolds with high quality and high strength. Based on these, high-strength (2.31 MPa for compressive strength) and complex chitosan hydrogel structures can be directly printed. The cell culture and the wound healing results further show that the printed chitosan scaffolds with this method have great potential in tissue engineering.Bio-derived isobutanol has been approved as a gasoline additive in the US, but our understanding of its combustion chemistry still has significant uncertainties. Detailed quantum calculations could improve model accuracy leading to better estimation of isobutanol’s combustion properties and its environmental impacts. This work examines 47 molecules and 38 reactions involved in the first oxygen addition to isobutanol’s three alkyl radicals located α, β, and γ to the hydroxide. Quantum calculations are mostly done at CCSD(T)-F12/cc-pVTZ-F12//B3LYP/CBSB7, with 1-D hindered rotor corrections obtained at B3LYP/6-31G(d). The resulting potential energy surfaces are the most comprehensive isobutanol peroxy networks published to date. Canonical transition state theory and a 1-D microcanonical master equation are used to derive high-pressure-limit and pressure-dependent rate coefficients, respectively. At all conditions studied, the recombination of γ-isobutanol radical with O2 forms HO2 + isobutanal. The recombination of β-isobutanol radical with O2 forms a stabilized hydroperoxy alkyl radical below 400 K, water + an alkoxy radical at higher temperatures, and HO2 + an alkene above 1200 K. The recombination of β-isobutanol radical with O2 results in a mixture of products between 700-1100 K, forming acetone + formaldehyde + OH at lower temperatures and forming HO2 + alkenes at higher temperatures. The barrier heights, high-pressure-limit rates, and pressure-dependent kinetics generally agree with the results from previous quantum chemistry calculations. Six reaction rates in this work deviate by over three orders of magnitude from kinetics in detailed models of isobutanol combustion, suggesting the rates calculated here can help improve modeling of isobutanol combustion and its environmental fate.In order to develop highly active non-precious metal catalysts for the selective oxidation of the platform compound 5-hydroxymethylfurfural (HMF) to the value-added bio-chemical 2,5-diformylfuran (DFF), we prepared high purity bivalent Mn5O8 nanoplates by a microwave-assisted ionic liquid route. The precursor of bivalent Mn5O8 nanoplates was formed through π-π stacking between imidazolium rings of the ionic liquid 1-butyl-3-methyl-imidazolium chloride and extending hydrogen bonds between Cl anions and hydrohausmannite. An oriented aggregation growth occurred on the basis of the Ostwald ripening under microwave heating. The high purity bivalent Mn5O8 nanoplates obtained through calcination at 550 °C for 2 h exhibited high HMF conversion (51%) and DFF selectivity (94%) at 5 bar of oxygen pressure in 2 h. The high concentration of Mn4+ on the exterior surfaces of Mn5O8 nanoplates as active sites coupled with good crystallinity played key roles for desirable mass and heat transfer, and for fast desorption avoiding over-oxidation.
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