Removal of confined space carbon dioxide (CO) that is in low concentration and with coexisting water is necessary but challenging by physical adsorption method. To make the removal process effective, rendering the nanopore surface hydrophobic to resist water is the popular way. Instead of preventing water from occupying the nanopores, in this work, we propose to utilize the guest water for the spatially selective formation of local surface bound water and further induce the preferential CO capture.
View Article and Find Full Text PDFAmorphous carbon holds great promise as anode material for sodium-ion batteries due to its cost-effectiveness and good performance. However, its sodium storage mechanism, particularly the insertion process and origin of plateau capacity, remains controversial. Here, an extended adsorption/insertion-filling sodium storage mechanism is proposed using petroleum coke-derived amorphous carbon as a multi-microcrystalline model.
View Article and Find Full Text PDFACS Appl Mater Interfaces
September 2024
Alumina-supported PtSn is an industrialized catalyst for propane dehydrogenation. During the catalyst impregnation, the acidic impregnation solution with chloroplatinic acid as a precursor inevitably leads to the partial dissolution of the surface of amphoteric alumina support and finally varies catalytic performance. Herein, the structure evolution of the active phase, induced by an impregnated acidic solution, was studied with special care.
View Article and Find Full Text PDFRingy nanostructures are amazing materials, displaying unique optical, magnetic, and electronic properties highly related to their dimensions. A strategy capable of continuously tailoring the diameter of nanorings is the key to elucidating their structure-function relationship. Herein, a method of bi-component micellar-configuration-transformation induced by hydrophobicity for the synthesis of nanorings with diameters ranging from submicron (≈143 nm) to micron (≈4.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2024
Propane dehydrogenation (PDH) is crucial for propylene production, but commercially employed Pt-based catalysts face susceptibility to deactivation due to the Pt sintering during reaction and regeneration steps. Here, we report a SiO supported nanometric (MnCoCuZnPt) high-entropy PDH catalyst with high activity and stability. The catalyst exhibited a super high propane conversion of 56.
View Article and Find Full Text PDFRational design of γ-alumina-based catalysts relies on an extensive understanding of the distribution of hydroxyl groups on the surface of γ-alumina and their physicochemical properties, which remain unclear and challenging to determine experimentally due to the structural complexity. In this work, by means of DFT and thermodynamic calculations, various hydroxylation modes of γ-alumina (110) and (100) surfaces at different OH coverages were evaluated, based on which a thermodynamic model to reflect the relationship between temperature and the surface structure was established and the stable hydroxylation modes under experimental conditions were predicted. This enables us to identify the experimentally measured IR spectra.
View Article and Find Full Text PDFSelective separation of ethylene and ethane (CH/CH) is a formidable challenge due to their close molecular size and boiling point. Compared to industry-used cryogenic distillation, adsorption separation would offer a more energy-efficient solution when an efficient adsorbent is available. Herein, a class of CH/CH separation adsorbents, doped carbon molecular sieves (d-CMSs) is reported which are prepared from the polymerization and subsequent carbonization of resorcinol, m-phenylenediamine, and formaldehyde in ethanol solution.
View Article and Find Full Text PDFJ Phys Chem A
March 2024
Oxidative dehydrogenation (ODH) of light alkanes is a key process in the oxidative conversion of alkanes to alkenes, oxygenated hydrocarbons, and CO ( = 1,2). Understanding the underlying mechanisms extensively is crucial to keep the ODH under control for target products, e.g.
View Article and Find Full Text PDFMagnetic nanocatalysts with properties of easy recovery, induced heating, or magnetic levitation play a crucial role in advancing intelligent techniques. Herein, we report a method for the synthesis of versatile core-shell-type magnetic nanocatalysts through "noncontact" hydrogen spillover-driven reduction and migration of iron oxide with the assistance of Pd. analysis techniques were applied to visualize the dynamic evolution of the magnetic nanocatalysts.
View Article and Find Full Text PDFPorous alumina has been widely used as catalytic support for industrial processes. Under carbon emission constraints, developing a low-carbon porous aluminum oxide synthesis method is a long-standing challenge for low-carbon technology. Herein, we report a method involving the only use of elements of the aluminum-containing reactants (e.
View Article and Find Full Text PDFSelective separation of industrial important C , C and C hydrocarbon pairs by physisorbents can greatly reduce the energy intensity related to the currently used cryogenic distillation techniques. The achievement of size-sieving based on carbonaceous materials is desirable, but commonly hindered by the random structure of carbons often with a broad pore size distribution. Herein, a pH-regulated pre-condensation strategy was introduced to control the carbon pore architecture by the sp /sp hybridization of precursor.
View Article and Find Full Text PDFEthylene glycol is a useful organic compound and chemical intermediate for manufacturing various commodity chemicals of industrial importance. Nevertheless, the production of ethylene glycol in a green and safe manner is still a long-standing challenge. Here, we established an integrated, efficient pathway for oxidizing ethylene into ethylene glycol.
View Article and Find Full Text PDFOxidative dehydrogenation (ODH) of alkane over boron nitride (BN) catalyst exhibits high olefin selectivity as well as a small ecological carbon footprint. Here we report an unusual phenomenon that the in-situ formed olefins under reactions are in turn actively accelerating parent alkane conversion over BN by interacting with hydroperoxyl and alkoxyl radicals and generating reactive species which promote oxidation of alkane and olefin formation, through feeding a mixture of alkane and olefin and DFT calculations. The isotope tracer studies reveal the cleavage of C-C bond in propylene when co-existing with propane, directly evidencing the deep-oxidation of olefins occur in the ODH reaction over BN.
View Article and Find Full Text PDFBoron-based materials catalyzing oxidative dehydrogenation is emerging as a promising protocol for efficient conversion of light alkanes to olefins, while the origin of its remarkable selectivity remains unclear. By means of density functional theory calculations, this work addresses the crucial role of boron peroxo as the mild oxidant in propane ODH: (1) Surface boron peroxo species can be generated in the presence of peroxo species, preferably at the >B-O-B< sites of the zigzag edge, and show high activity to dehydrogenate propane (Δ = 13.5 kcal/mol, Δ = 8.
View Article and Find Full Text PDFSize regulation of uniform polymer nanospheres (PNSs) and carbon nanospheres (CNSs) below 100 nm has been difficult and is limited by multiple factors, such as ongoing nucleation, Ostwald ripening, minimization of surface energy, and high viscosity during the nucleation and growth process. In this study, a kinetics-controlled regulation is reported for the synthesis of monodispersed PNSs and corresponding CNSs with adjustable size below 100 nm. During the synthesis of PNSs, three distinct stages including surface energy control, surface tension control and viscosity control have been observed, where the concentration of block copolymer F127 () plays a vital role in affecting the nucleation rate of PNSs and tunes the diffusion rate of monomers and migration of particles during the nucleation and growth process.
View Article and Find Full Text PDFRapid and highly efficient CH/CH separation over porous carbons is seriously hindered by the trade-off effect between adsorption capacity and selectivity. Here, we report a new type of porous carbon nanoplate (CNP) featuring an ultrathin thickness of around 8 nm and easily accessible ultramicropores (approximately 5.0 Å).
View Article and Find Full Text PDFLight hydrocarbons (LHs) separation is an important process in petrochemical industry. The current separation technology predominantly relies on cryogenic distillation, which results in considerable energy consumption. Adsorptive separation using porous solids has received widespread attention due to its lower energy footprint and higher efficiency.
View Article and Find Full Text PDFCancer treatment is imminent, and controlled drug carriers are an important development direction for future clinical chemotherapy. Visual guidance is a feasible means to achieve precise treatment, reduce toxicity and increase drug efficacy. However, the existing visual control methods are limited by imaging time-consuming, sensitivity and side effects.
View Article and Find Full Text PDFHere we report on the facile formation of asymmetric heterojunctions between laterally size different 2D flakes, which leads to a prominent gradient in charge distribution at the nanocontact interface and triggers ionic diode-like transport behaviour with a rectification ratio of 110.
View Article and Find Full Text PDFControlled-release drug carriers in cancer therapy are the most ideal way to reduce toxicity and improve drug efficacy. Since light stimulation is precise and operable, most multi-stimulation response carriers utilize phototherapy to enhance release efficiency. However, phototoxicity severely limits the application of phototherapy.
View Article and Find Full Text PDFThe emergence of nano-targeted controlled release liposomal drug carriers has provided a breakthrough in cancer therapy. However, their clinical efficacy is unsatisfactory, which is related to individualized differences in targeted drugs and poor release efficiency. In this paper, we prepared a class of personalized targeted and precisely controlled-release therapeutic drug carriers (GF liposomes) by co-assembling targeting and traceable nitrobenzyl ester lipids to propose a magnetic resonance imaging (MRI)-guided personalized targeted drug screening strategy and a multi-stimulus superimposed controlled-release strategy.
View Article and Find Full Text PDFThe selective synthesis of energetically less favorable ring-shaped nanostructures by liquid phase synthetic chemistry is a huge challenge. Herein, we report a precise synthesis of carbon nanorings with a well-defined morphology and tunable thickness based on asymmetric intramicellar phase-transition-induced tip-to-tip assembly via mixing hydrophobic long-chain octadecanol and block copolymer F127. This orientational self-assembly depends on the hydrophobicity difference of the intermediate's surface, which triggers directional interactions that surpass the entropy cost of undesired connections and help assemble intermediates into defined ringlike structures.
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