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1.
Rev Sci Instrum ; 94(6)2023 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-37862533

RESUMO

As the novel suspension bearing, Magnetic-Liquid Double Suspension Bearing (MLDSB) is mainly supported by magnetic suspension and supplemented by a liquid hydrostatic bearing. Due to its great bearing capacity and stiffness, rapid response, great active control, and so on, MLDSB is suitable for medium speed heavy loads and has a large carrying capacity and high operating stability. In addition, the radial inertia coupling and gyroscopic coupling between radial 4-DOF control channels can reduce control precision, operation stability, and reliability of MLDSB. Therefore, a mathematical model of radial 4-DOF rotor-dynamics of MLDSB is established in this paper, and the inherent coupling mechanism is explored. Taking inertial coupling, gyroscopic coupling, and external disturbance loads as lumped disturbances, a decoupled controller based on Generalized Extended State Observer (GESO) is established. The influence of the GESO controller on the decoupling and control performance of radial 4-DOF control channels is simulated. The results indicate that the decoupling effect of the GESO controller is great. Under the action of step signal, the steady displacement, maximum displacement, adjustment time, and peak time of the rotor after decoupling are all reduced, among which the steady displacement and maximum displacement are the most obvious. Under the sinusoidal signal, the steady displacement and maximum displacement are reduced by 90%, which can effectively avoid the "gap-impact" fault. Under the pulse signal, the steady displacement, maximum displacement, adjustment time, and peak time are all reduced, among which the maximum displacement is the most obvious. The research in this paper can provide a theoretical reference for the stable support and decoupling control of MLDSB.

2.
Angew Chem Int Ed Engl ; 61(16): e202200190, 2022 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-35132761

RESUMO

Carbon monoxide (CO) is notorious for its strong adsorption to poison platinum group metal catalysts in the chemical industry. Here, we conceptually distinguish and quantify the effects of the occupancy and energy of d electrons, emerging as the two vital factors in d-band theory, for CO poisoning of Pt nanocatalysts. The stepwise defunctionalization of carbon support is adopted to fine-tune the 5d electronic structure of supported Pt nanoparticles. Excluding other promotional mechanisms, the increase of Pt 5d band energy strengthens the competitive adsorption of hydrogen against CO for the preferential oxidation of CO, affording the scaling relationship between Pt 5d band energy and CO/H2 adsorption energy difference. The decrease of Pt 5d band occupancy lowers CO site coverage to promote its association with oxygen for the total oxidation of CO, giving the scaling relationship between Pt 5d occupancy and activation energy. The above insights outline a molecular-level understanding of CO poisoning.

3.
Nat Commun ; 12(1): 6888, 2021 Nov 25.
Artigo em Inglês | MEDLINE | ID: mdl-34824271

RESUMO

A molecular-level understanding of how the electronic structure of metal center tunes the catalytic behaviors remains a grand challenge in heterogeneous catalysis. Herein, we report an unconventional kinetics strategy for bridging the microscopic metal electronic structure and the macroscopic steady-state rate for CO oxidation over Pt catalysts. X-ray absorption and photoelectron spectroscopy as well as electron paramagnetic resonance investigations unambiguously reveal the tunable Pt electronic structures with well-designed carbon support surface chemistry. Diminishing the electron density of Pt consolidates the CO-assisted O2 dissociation pathway via the O*-O-C*-O intermediate directly observed by isotopic labeling studies and rationalized by density-functional theory calculations. A combined steady-state isotopic transient kinetic and in situ electronic analyses identifies Pt charge as the kinetics indicators by being closely related to the frequency factor, site coverage, and activation energy. Further incorporation of catalyst structural parameters yields a novel model for quantifying the electronic effects and predicting the catalytic performance. These could serve as a benchmark of catalyst design by a comprehensive kinetics study at the molecular level.

4.
Chem Asian J ; 15(23): 4014-4022, 2020 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-33094915

RESUMO

Herein, we report the crucial importance of C-defective sites on the CO adsorption over ϵ-Fe2 C and η-Fe2 C Fischer-Tropsch catalysts via systematic DFT calculations. The simulated XRD and Wulff construction show the significant differences in their equilibrium shapes and most exposed surfaces. It is observed that the ϵ-Fe2 C exposes a high proportion (89 %) of facets (1 2 ‾ 1) with similar structure to that of η-Fe2 C (011) which has been proved to be the active surface of CO activation.

5.
ACS Nano ; 14(5): 6164-6172, 2020 May 26.
Artigo em Inglês | MEDLINE | ID: mdl-32379422

RESUMO

Developing a convenient and effective method to prepare single-atom catalysts at mild synthetic conditions remains a challenging task. Herein, a voltage-gauged electrofiltration method was demonstrated to synthesize single-atom site catalysts at room temperature. Under regulation of the graphene oxide membrane, a bulk Fe plate was directly converted into Fe single atoms, and the diffusion rate of Fe ions was greatly reduced, resulting in an ultralow concentration of Fe2+ around the working electrode, which successfully prevented the growing of nuclei and aggregating of metal atoms. Monatomic Fe atoms are homogeneously anchored on the as-prepared nitrogen-doped carbon. Owing to the fast photoelectron injection from photosensitizers to atomically dispersed Fe sites through the highly conductive supported N-C, the Fe-SAs/N-C exhibits an outstanding photocatalytic activity toward CO2 aqueous reduction into syngas with a tunable CO/H2 ratio under visible light irradiation. The gas evolution rates for CO and H2 are 4500 and 4950 µmol g-1 h-1, respectively, and the tunable CO/H2 ratio is from 0.3 to 8.8. This article presents an efficient strategy to develop the single-atom site catalysts and bridges the gap between heterogeneous and homogeneous catalysts toward photocatalytic CO2 aqueous reduction into syngas.

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