Heteroatom-incorporated 2D ordered mesoporous carbons (OMCs) were fabricated via a one-pot organic−organic aqueous self-assembly approach, using resorcinol (R) and formaldehyde (F) as the carbon precursor and triblock copolymer Pluronic F127 as the mesoporous structure template. In this approach, RF resin, boric acid and/or phosphoric acid, and F127 underwent a self-assembly process under a strong acidic condition to form a polymer with ordered mesostructure, which was then carbonized at 800 °C in a nitrogen atmosphere to form B-incorporated, P-incorporated, or B, P-coincorporated OMCs. Nitrogen sorption, X-ray diffraction (XRD), and transmission electron microscopy (TEM) revealed that the heteroatom-incorporated OMCs possessed highly ordered mesoporous structures, uniform pore size distributions, and large surface areas ranging from 500 to 700 m2/g. The incorporation of heteroatoms effectively limited the framework shrinkage during the carbonization process, and simultaneously increased the surface oxygen groups in the carbons. The resulting heteroatom-incorporated OMCs exhibited superior electrochemical performances to nonincorporated counterpart when used as electrodes of supercapacitors.
Single/pseudo-single atom Pt catalyst was prepared on mesoporous WOx . The large surface area and abundant oxygen vacancies of WOx improve the Pt dispersion and stabilize the Pt isolation. This newly prepared catalyst exhibited outstanding hydrogenolysis activity under 1 MPa H2 pressure with a very high space-time yield towards 1,3-propanediol (3.78 g gPt (-1) h(-1) ) in Pt-W catalysts. The highly isolated Pt structure is thought to contribute to the excellent H2 dissociation capacity over Pt/WOx . The high selectivity towards 1,3-propanediol is attributed to the heterolytic dissociation of H2 at the interface of Pt and WOx (providing specific Brønsted acid sites and the concerted dehydration-hydrogenation reaction) and the bond formation between glycerol and WOx , which favors/stabilizes the formation of a secondary carbocation intermediate as well as triggers the redox cycle of the W species (W(6+) ⇄W(5+) ).
Graphene with mediated surface properties and three-dimensional hierarchical architectures show unexpected performance in energy conversion and storage. To achieve advanced graphene electrode supercapacitors, manipulating the graphene building-blocks into hierarchical nanostructured carbon materials with large electrical double layer capacitance and pseudo-capacitance is a key issue. Here, it is shown that the hierarchically aminated graphitic honeycombs (AGHs) with large surface area for electrical double layer capacitance, tunable surface chemistry for pseudo-capacitance, mediated 3D macropores for ion buffering, and low-resistant pathways for ion diffusion are fabricated for electrochemical capacitive energy storage application through a facile high vacuum promoted thermal expansion and subsequent amination process. In the initial stage of amination (200 °C), NH3 reacts with carboxylic acid species to form mainly intermediate amides and amines through nucleophilic substitution. As the temperature increases, the intramolecular dehydration and decarbonylation will take place to generate thermally more stable heterocyclic aromatic moieties such as pyridine, pyrrole, and quaternary type N sites. The AGH exhibits a promising prospect in supercapacitor electrodes with high capacitance (e.g. maximum gravimetric capacitance 207 F g−1 and specific capacitance 0.84 F m−2 at a scan rate of 3 mV s−1) and extraordinary stability (e.g. 97.8% of capacitance retention after 3000 cycles, and 47.8% of capacitance maintaining at a high scan rate of 500 mV s−1 comparing with that at 3 mV s−1). This provides a novel structure platform for catalysis, separation, and drug delivery, which require fast mass transfer through mesopores, reactant reservoirs, and tunable surface chemistry
A three-dimensional bubble graphene film, with controllable and uniform macropores and tailorable microstructure, was fabricated by a facile hard templating strategy and exhibit extraordinary electrochemical capacitance with high rate capability (1.0 V s(-1)).
Graphene oxide (GO-ene), the two-dimensional carbon lattice decorated by abundant oxygen functionalities, is demonstrated as an efficient green catalyst towards selective hydrolysis of cellulose to glucose. The synergy of its carboxylic/phenolic groups and its layered, soft structure rendered GO-ene superior hydrolytic activity.
Functionalized mesoporous carbon catalysts can be used in the acid catalyzed dehydration of fructose to 5-hydroxymethyl furfural (HMF). However, strong deactivation can be observed after preconditioning of the material in the reaction solvent 2-butanol. Surface changes caused by the pretreatment have been studied by XPS. The comparison of the pristine sample and the pretreated carbon sample showed similar distribution of oxygen functional groups by ex-situ XPS, as well as similar behavior during heating in vacuum. However, the addition of water (0.1 mbar vapor pressure) and subsequent heating to 130°C exhibited prominent differences in the evolution of the O1s, as well as for the C1s spectra of the two samples. Changes in the surface termination and hydrophobicity of the materials are discussed under the aspect of possible reactions of surface functional groups with the alcoholic solvent and water.
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