A general strategy for the synthesis of porous, fluorescent, triazine-framework-based membranes with intrinsic porosity through an aromatic nitrile trimerization reaction is presented. The essence of this strategy lies in the use of a superacid to catalyze the cross-linking reaction efficiently at a low temperature, allowing porous polymer membrane architectures to be facilely derived. With functionalized triazine units, the membrane exhibits an increased selectivity for membrane separation of CO(2) over N(2). The good ideal CO(2)/N(2) selectivity of 29 ± 2 was achieved with a CO(2) permeability of 518 ± 25 barrer. Through this general synthesis protocol, a new class of porous polymer membranes with tunable functionalities and porosities can be derived, significantly expanding the currently limited library of polymers with intrinsic microporosity for synthesizing functional membranes in separation, catalysis, and energy storage/conversion.
Crystalline high-entropy ceramics (CHC), a new class of solids that contain five or more elemental species, have attracted increasing interest because of their unique structure and potential applications. Up to now, only a couple of CHCs (e.g., high-entropy metal oxides and diborides) have been successfully synthesized. Here, a new strategy for preparing high-entropy metal nitride (HEMN-1) is proposed via a soft urea method assisted by mechanochemical synthesis. The as-prepared HEMN-1 possesses five highly dispersed metal components, including V, Cr, Nb, Mo, Zr, and simultaneously exhibits an interesting cubic crystal structure of metal nitrides. By taking advantage of these unique features, HEMN-1 can function as a promising candidate for supercapacitor applications. A specific capacitance of 78 F g is achieved at a scan rate of 100 mV s in 1 m KOH. In addition, such a facile synthetic strategy can be further extended to the fabrication of other types of HEMNs, paving the way for the synthesis of HEMNs with attractive properties for task-specific applications.
Platinum nanoparticles (Pt NPs) are one of the most efficient cocatalysts in photocatalysis, and their size determines the activity and the selectivity of the catalytic reaction. Nevertheless, an in-depth understanding of the platinum’s size effect in the carbon dioxide photocatalytic reduction is still lacking. Through analyses of the geometric features and electronic properties with variable-sized Pt NPs, here we show a prominent size effect of Pt NPs in both the activity and selectivity of carbon dioxide photocatalytic reduction. Decreasing the size of Pt NPs promotes the charge transfer efficiency, and thus enhances both the carbon dioxide photocatalytic reduction and hydrogen evolution reaction (HER) activity, but leads to higher selectivity towards hydrogen over methane. Combining experimental results and theoretical calculations, in Pt NPs, the terrace sites are revealed as the active sites for methane generation; meanwhile, the low-coordinated sites are more favorable in the competing HER.
A flexible and robust electrode is demonstrated by assembling the 3D ordered macroporous MoS @C nanostructure on carbon cloth with ultrasmall few-layered MoS nanosheets homogenously embedded into the interconnected carbon wall. Such unique nanostructures are favorable for enhancing lithium storage capacity, directly applied as a flexible electrode, demonstrating a very high electrochemical performance and superior cycling stability for lithium-ion batteries.
Halogen bonding should intentionally be used as a powerful tool, comparable with hydrogen bonding, to enhance the binding affinity and also influence the binding selectivity. Rational design of new and potent inhibitors against therapeutic targets through halogen bonding continues to be an exciting area, which will be further elucidated with the combination of various experimental techniques and theoretical calculations in the forthcoming years.
A porous triazine and carbazole bifunctionalized task-specific polymer has been synthesized via a facile Friedel-Crafts reaction. The resultant porous framework exhibits excellent CO2 uptake (18.0 wt%, 273 K and 1 bar) and good adsorption selectivity for CO2 over N2.
The development of novel electrolytes and electrodes for supercapacitors is hindered by a gap of several orders of magnitude between experimentally measured and theoretically predicted charging time scales. Here, we propose an electrode model, containing many parallel stacked electrodes, that explains the slow charging dynamics of supercapacitors. At low applied potentials, the charging behavior of this model is described well by an equivalent circuit model. Conversely, at high potentials, charging dynamics slow down and evolve on two relaxation time scales: a generalized RC time and a diffusion time, which, interestingly, become similar for porous electrodes. The charging behavior of the stack-electrode model presented here helps to understand the charging dynamics of porous electrodes and agrees qualitatively with experimental time scales measured with porous electrodes.
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