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41.
Activity-directed synthesis (ADS) is a structure-blind, functional-driven molecular discovery approach. In this Concept, four case studies highlight the general applicability of ADS and showcase its flexibility to support different medicinal chemistry strategies. ADS deliberately harnesses reactions with multiple possible outcomes, and allows many chemotypes to be evaluated in parallel. Resources are focused on bioactive molecules, which emerge in tandem with associated synthetic routes. Some of the future challenges for ADS are highlighted, including the realisation of an autonomous molecular discovery platform. The prospects for ADS to become a mainstream lead generation approach are discussed. 相似文献
42.
《Ceramics International》2020,46(15):23695-23705
Solid electrolytes are the key component in designing all-solid-state batteries. The Li1.3Al0.3Ti1.7(PO4)3 (LATP) structure and its derivatives obtained by doping various elements at Ti and Al site acts as good solid electrolytes. However, there is still scope for enhancing the ionic conductivity using simple precursors and preparation methods. In this study, the Li superionic conductors Li1.3Al0.3Ti1.7-xZrx(PO4)3 (LATZP) with 0 ≤ x ≤ 0.2 have been successfully prepared by the solid-state reaction route. The structural, morphological, and ionic transport properties were analyzed using several experimental techniques including powder X-ray diffraction (XRD), scanning electron microscopy (SEM), and impedance spectroscopy (IS). The presence of two relaxation processes corresponding to grain and grain boundary was studied using various formalisms. We have observed that grain effects dominate at lower temperatures (<100 °C) while the grain boundary at higher temperatures (> 200 °C) on ionic conductivity. The relaxation mechanisms of grain and grain boundaries were investigated by the Summerfield scaling of AC conductivity. The highest total ionic conductivity of 2.48 × 10-4 S/cm at 150 °C and 5.50 × 10-3 S/cm at 250 °C was obtained for x = 0.1 in Li1.3Al0.3Ti1.6Zr0.1(PO4)3 sintered at 950 °C/6 h in the air. The ionic conductivity value was found to be higher than the ionic conductivity reported for LATP prepared via solid-state reaction mechanism using the same precursors and conditions. 相似文献
43.
Simona Renda Antonio Ricca Vincenzo Palma 《International Journal of Hydrogen Energy》2021,46(22):12117-12127
This paper reports the preparation and the evaluation of the performance of Ni-based powder catalysts with low nickel loading on the CO2 methanation reaction, that is an integral part of the power-to-gas (PtG) technology. CeO2, CeZrO4 and CeO2/SiO2 were selected as possible supports, and the results of this first screening pointed out that 10%Ni/CeO2 catalyst could offer the best reaction performances because of ceria's peculiar characteristics. Moreover, the promotion of this promising formulation with the addition of a small amount of noble metals (Pt, Ru, Rh) was investigated, showing that platinum in particular can enhance the catalyst performances. A further study related to the noble metal loading pointed out that platinum and ruthenium have a different optimum loading condition: this result, together with the activity tests performed on monometallic formulations with only the noble metal, suggested that the two metals are able to catalyse two different reactions, thus promoting two different reaction mechanisms. 相似文献
44.
Real‐time monitoring by proton relaxometry of radical polymerization reactions of acrylamide in aqueous solution 下载免费PDF全文
Elton Jorge da Rocha Rodrigues Roberto Pinto Cucinelli Neto Pedro José Oliveira Sebastião Maria Inês Bruno Tavares 《Polymer International》2018,67(6):675-683
The potential of time‐domain nuclear magnetic resonance (TD‐NMR) for the real‐time monitoring of solution radical polymerizations is demonstrated. A model system composed of a redox‐pair initiator system, acrylamide as monomer and water as solvent was investigated. A second‐generation continuous wave free precession technique was employed to measure the longitudinal relaxation time constant (T1) of the samples throughout the polymerization reactions. This parameter was shown to be sensitive to the reactant feed free‐radical enhancement of the water molecule relaxation time, making it a good probe to monitor monomer conversion in real time in an automated, non‐destructive fashion. It was found that the T1 value was better than the transverse relaxation time constant (T2) for describing the evolution of the polymerization reactions, due to its greater sensitivity to paramagnetic effects. The TD‐NMR signal variation observed was linked to the formation, propagation and termination steps of the radical polymerization kinetics scheme. These first results may contribute to the application of real‐time monitoring of radical polymerization reactions employing low‐cost and robust TD‐NMR spectrometers. © 2018 Society of Chemical Industry 相似文献
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47.
《International Journal of Hydrogen Energy》2020,45(16):9546-9554
Hierarchical composites represent a class of efficient electrocatalysts for renewable energy storage and conversion technologies owing to the porous structure and additional exposure of metal sites. Herein, a Ni-based metal organic frameworks (MOFs) (marked as Ni-BDC, BDC stands for 1,4-benzenedicarboxylic acid) nanosheet is successfully fabricated on hydroxyl iron oxide (FeOOH) array with carbon fiber cloth (CFC) as substrate. Benefit from the coordination tuning synergistic effect of the distinct chemical composition and the hierarchical structure for fast mass transportation, the as-obtained FeOOH@Ni-BDC illustrates excellent catalytic ability for electrochemical water oxidation with low overpotential of 270 mV to reach 10 mA/cm2 current and good durability in alkaline electrolyte. The novelty of this work lies in the modulation of electronic structure of the FeOOH with Ni-BDC through coordination effect to enhance the activity of the hierarchical composite electrocatalyst. This work is expected to guide the preparation of efficient electrocatalyst for new type alternative energy sources exploitation in near future. 相似文献
48.
《International Journal of Hydrogen Energy》2020,45(1):849-860
The glassy carbon electrode is modified by poly(brilliant cresyl blue) (PBCB) to be applied as a new green and efficient platform for Pt and Pt–Ru alloy nanoparticles deposition. Surface composition, morphology and catalytic activity of these modified electrodes towards methanol oxidation are assessed by applying X-ray diffraction, field emission scanning electron microscopy, cyclic voltammetry and electrochemical impedance spectroscopy techniques. The X-ray diffraction patterns reveal that the highly crystalline Pt and Pt–Ru alloy and RuO2 nanoparticles with low crystallinity are deposited on the PBCB modified glassy carbon electrodes. The microscopic images indicate smaller size and better distribution of deposited nanoparticles on the surface of PBCB modified electrodes. Cyclic voltammetry and electrochemical impedance spectroscopy results reveal that PBCB supported Pt and Pt–Ru nanoparticles have better electrocatalytic performance and durability towards methanol oxidation rather than the unsupported nanoparticles. From the obtained results it can be concluded that the presence of PBCB not only improves the stability of nanoparticles on the surface, but also leads to the formation of smaller size and more uniform distribution of nanoparticles on the surface, which, in turn, cause the nanoparticles to provide a higher accessible surface area and more active centers for the oxidation of methanol. The results will be valuable in extending the applications of this polymer in surface modification steps and in developing promising catalyst supports to be applied in direct methanol fuel cells. 相似文献
49.
《International Journal of Hydrogen Energy》2021,46(56):28397-28405
Water electrolysis powered by renewable electricity will likely be critical to a future hydrogen economy. However, the typical use of strongly acidic or alkaline electrolytes necessitates the use of expensive materials, while bubbles add to capital and operational costs, due to blocking of the electrode surface and the necessary use of pumps and gas-liquid separators. Here ‘bubble-free’ oxygen evolution at mild pH is carried out using an electrocatalyst that mimics photosystem II (PSII). The bubble-free electrode includes a gas-extracting Gore-Tex® membrane. Edge-functionalised graphene (EFG) is included to mimic the metal-binding local protein environment, and the tyrosine residue, in the oxygen evolving complex (OEC) of PSII, while MnOx and Ca2+ are incorporated to mimic the Mn4CaO5 cluster. Interaction between EFG, MnOx, and Ca2+ results in a significant, 130 mV fall in the overpotential required to drive electrocatalytic oxygen evolution at 10 mA cm−2, compared to the electrode without these biomimetic components. 相似文献
50.
Previous studies indicate that the properties of graphene oxide (GO) can be significantly improved by enhancing its graphitic domain size through thermal diffusion and clustering of functional groups. Remarkably, this transition takes place below the decomposition temperature of the functional groups and thus allows fine tuning of graphitic domains without compromising with the functionality of GO. By studying the transformation of GO under mild thermal treatment, we directly observe this size enhancement of graphitic domains from originally ≤40 nm2 to >200 nm2 through an extensive transmission electron microscopy (TEM) study. Additionally, we confirm the integrity of the functional groups during this process by a comprehensive chemical analysis. A closer look into the process confirms the theoretical predicted relevance for the room temperature stability of GO and the development of the composition of functional groups is explained with reaction pathways from theoretical calculations. We further investigate the influence of enlarged graphitic domains on the hydration behaviour of GO and the catalytic performance of single atom catalysts supported by GO. Additionally, we show that the sheet resistance of GO is reduced by several orders of magnitude during the mild thermal annealing process. 相似文献