The components of petroleum asphaltenes exhibit complex bridged structures comprising sulfur, nitrogen, aromatic, and naphthenic groups linked by alkyl chains. These components aggregate in crude oil and toluene over a wide range of concentrations and temperatures, exhibit strong adhesion to a wide range of surfaces, occlude components that are otherwise soluble, are porous to solvents, and are elastic under tension. None of these properties is consistent with an architecture dominated only by aromatic stacking by electrostatic and/or van der Waals forces, often called π–π stacking. We propose an alternate paradigm based on supramolecular assembly of molecules, combining cooperative binding by Brønsted acid–base interactions, hydrogen bonding, metal coordination complexes, and interactions between cylcoalkyl and alkyl groups to form hydrophobic pockets, in addition to aromatic π–π stacking. A range of architectures are suggested, which almost certainly occur simultaneously, including porous networks and host–guest complexes. The latter may include organic clathrates, in which occluded guest molecules stabilize the assembly of a cage, as methane does in gas hydrates. This model has a number of implications for analysis of asphaltene mixtures and predicting asphaltene phase behavior and transport properties.
Designing highly durable and active electrocatalysts applied in polymer electrolyte membrane (PEM) electrolyzer for the oxygen evolution reaction remains a grand challenge due to the high dissolution of catalysts in acidic electrolyte. Hindering formation of oxygen vacancies by tuning the electronic structure of catalysts to improve the durability and activity in acidic electrolyte was theoretically effective but rarely reported. Herein we demonstrated rationally tuning electronic structure of RuO2 with introducing W and Er, which significantly increased oxygen vacancy formation energy. The representative W0.2Er0.1Ru0.7O2-δ required a super-low overpotential of 168 mV (10 mA cm−2) accompanied with a record stability of 500 h in acidic electrolyte. More remarkably, it could operate steadily for 120 h (100 mA cm−2) in PEM device. Density functional theory calculations revealed co-doping of W and Er tuned electronic structure of RuO2 by charge redistribution, which significantly prohibited formation of soluble Rux>4 and lowered adsorption energies for oxygen intermediates.
Few-layered graphene oxide (FGO) was synthesized from graphite by using the modified Hummers method, and was characterized by scanning electron microscopy, atomic force microscopy, powder X-ray diffraction, X-ray photoelectron spectroscopy and Raman spectroscopy. The prepared FGO was used to adsorb Pb(II) ions from aqueous solutions. The abundant oxygen-containing groups on the surfaces of FGO played an important role in Pb(II) ion adsorption on FGO. The adsorption of Pb(II) ions on FGO was dependent on pH values and independent of ionic strength. The adsorption of Pb(II) ions on FGO was mainly dominated by strong surface complexation. From the adsorption isotherms, the maximum adsorption capacities (C(smax)) of Pb(II) ions on FGO calculated from the Langmuir model were about 842, 1150, and 1850 mg g(-1) at 293, 313, and 333 K, respectively, higher than any currently reported. The FGO had the highest adsorption capacities of today's nanomaterials. The thermodynamic parameters calculated from the temperature dependent adsorption isotherms indicated that the adsorption of Pb(II) ions on FGO was a spontaneous and endothermic process.
In this Article, we report a remarkably simple and efficient method for the preparation of layered double hydroxides and graphene oxide (LDHs/GO) nanocomposites with varying GO amounts via a hydrothermal process. The graphene nature in the resulting LDHs/GO nanocomposites was confirmed by X-ray diffraction (XRD), Fourier transformed infrared (FTIR) spectroscopy, field-emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), N2 adsorption-desorption, and X-ray photoelectron spectroscopy (XPS). The LDHs/GO nanocomposites exhibited swelling behavior in water and forming a gel. The adsorption performance of the LDHs/GO nanocomposites was evaluated for the removal of arsenate (As(V)) from aqueous solutions, and the results showed that the ratio of GO to LDHs in the nanocomposites significantly affected the adsorption capacity. Higher and lower amounts of GO in LDHs/GO nanocomposites showed lower adsorption capacity of As(V). A maximum adsorption capacity of 183.11 mg/g (2.44 mmol/g) was achieved on the LDHs/GO containing 6.0% GO due to the higher Brunauer-Emmett-Teller (BET) surface area than other samples. Owing to their high uptake capability of As(V), water-swellable LDHs/GO nanocomposites are expected to have potential applications as adsorbents for As(V) polluted water cleanup.
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