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Controlling Surface Defects and Photophysics in TiO2 Nanoparticles
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Controlled surface segregation leads to efficient coke-resistant nickel/platinum bimetallic catalysts for the dry reforming of methane
Surface composition and structure are of vital importance for heterogeneous catalysts, especially for bimetallic catalysts, which often vary as a function of reaction conditions (known as surface segregation). The preparation of bimetallic catalysts with controlled metal surface composition and structure is very challenging. In this study, we synthesize a series of Ni/Pt bimetallic catalysts with controlled metal surface composition and structure using a method derived from surface organometallic chemistry. The evolution of the surface composition and structure of the obtained bimetallic catalysts under simulated reaction conditions is investigated by various techniques, which include CO-probe IR spectroscopy, high-angle annular dark-field scanning transmission electron microscopy, energy-dispersive X-ray spectroscopy, extended X-ray absorption fine structure analysis, X-ray absorption near-edge structure analysis, XRD, and X-ray photoelectron spectroscopy. It is demonstrated that the structure of the bimetallic catalyst is evolved from Pt monolayer island-modified Ni nanoparticles to core–shell bimetallic nanoparticles composed of a Ni-rich core and a Ni/Pt alloy shell upon thermal treatment. As a result, these catalysts are active for the dry reforming of methane, and their catalytic activities, stabilities, and carbon formation vary with their surface composition and structure.
Spectral modeling of an oscillating surge wave energy converter with control surfaces
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Surface-Controlled TiO 2 Nanocrystals with Catalytically Active Single-Site Co Incorporation for the Oxygen Evolution Reaction
The design of advanced electrocatalysts is often hindered by uncertainties in identifying and controlling the active surfaces and catalytic centers within heterogeneous materials. Here we present the synthesis of single-site Co catalysts, substitutionally doped into surface-controlled TiO 2 anatase nanocrystals, aimed at enhancing the oxygen evolution reaction (OER). Grand canonical quantum mechanics calculations reveal that the kinetics of the OER, following an adsorbate evolution mechanism, is markedly influenced by the coordination environment of Co. The simulations suggest significantly higher turnover frequencies when Co is doped into the (001) surface of TiO 2 compared to the (101) surface. Consistent with the computational findings, experimental results show that Co-doped TiO 2 (Co-TiO 2 ) nanoplates with selectively exposed {001} surfaces exhibit enhanced current densities and turnover frequencies compared to Co-TiO 2 nanobipyramids with {101} surfaces. This study highlights the synergy between theoretical calculations and precision synthesis in the development of more effective catalysts.
Enhancing Electron Mobility at the LaAlO 3 /SrTiO 3 Interface by Surface Control
Mobility of electrons confined at the LaAlO 3 /SrTiO 3 interface is significantly enhanced by surface control using surface charges and adsorbates, reaching a low temperature value more than 20 000 cm 2 V -1 s -1 . A uniform trend that mobility increases with decreasing sheet carrier density is observed.
Chaos control of the brushless direct current motor using adaptive dynamic surface control based on neural network with the minimum weights
This paper investigates chaos control for the brushless DC motor (BLDCM) system by adaptive dynamic surface approach based on neural network with the minimum weights. The BLDCM system contains parameter perturbation, chaotic behavior, and uncertainty. With the help of radial basis function (RBF) neural network to approximate the unknown nonlinear functions, the adaptive law is established to overcome uncertainty of the control gain. By introducing the RBF neural network and adaptive technology into the dynamic surface control design, a robust chaos control scheme is developed. It is proved that the proposed control approach can guarantee that all signals in the closed-loop system are globally uniformly bounded, and the tracking error converges to a small neighborhood of the origin. Simulation results are provided to show that the proposed approach works well in suppressing chaos and parameter perturbation.
Approaching the Limits of Optoelectronic Performance in Mixed Cation Mixed Halide Perovskites by Controlling Surface Recombination
topic: Approaching the Limits of Optoelectronic Performance in Mixed Cation Mixed Halide Perovskites by Controlling Surface Recombination
Approaching the Limits of Optoelectronic Performance in Mixed Cation Mixed Halide Perovskites by Controlling Surface Recombination
topic: Approaching the Limits of Optoelectronic Performance in Mixed Cation Mixed Halide Perovskites by Controlling Surface Recombination
Bulk Stoichiometry-Controlled Surface Reconstruction of Nanosized Ni−In Intermetallic Catalysts Steers Methanol Selectivity in CO2 Hydrogenation
Intermetallic compounds (IMCs) are attractive platforms for elucidating structure−catalysis relationships due to their ordered atomic structure and well-defined bulk composition. Yet, how their surfaces reconstruct under reaction conditions and how such reconstruction is governed by bulk stoichiometry remain poorly understood. Here, we show that SiO2-supported Ni−In IMCs undergo reaction-driven surface reconstruction during CO2 hydrogenation and that bulk stoichiometry can be used to steer this evolution toward methanol formation. Among the compositions examined (Ni2In1, Ni1In1, Ni2In3, and Ni1In2), Ni2In3/SiO2 exhibits the highest methanol selectivity (∼70%) and a methanol space-time yield of 652 mg·gmetal−1·h−1 at 250 °C and 30 bar. Combined structural, surface characterization, and kinetic analyses suggest that the intermetallic bulk remains largely preserved, whereas the surface departs from the stoichiometric bulk and evolves toward InOx-enriched surface domains coupled to an electron-rich Ni−In intermetallic phase. The extent of this evolution depends strongly on the bulk Ni:In stoichiometry and is most pronounced for Ni2In3/SiO2. These findings identify bulk stoichiometry as a handle for tuning the working-state surface of intermetallic catalysts and provide a basis for designing methanol synthesis catalysts through controlled surface reconstruction.
Adaptive fuzzy dynamic surface control for the chaotic permanent magnet synchronous motor using Nussbaum gain
This paper is concerned with the problem of adaptive fuzzy dynamic surface control (DSC) for the permanent magnet synchronous motor (PMSM) system with chaotic behavior, disturbance and unknown control gain and parameters. Nussbaum gain is adopted to cope with the situation that the control gain is unknown. And the unknown items can be estimated by fuzzy logic system. The proposed controller guarantees that all the signals in the closed-loop system are bounded and the system output eventually converges to a small neighborhood of the desired reference signal. Finally, the numerical simulations indicate that the proposed scheme can suppress the chaos of PMSM and show the effectiveness and robustness of the proposed method.
Neutral Silicon Vacancy Centers in Undoped Diamond via Surface Control
Neutral silicon vacancy centers (SiV 0 ) in diamond are promising candidates for quantum applications; however, stabilizing SiV 0 requires high-purity, boron-doped diamond, which is not a readily available material. Here, we demonstrate an alternative approach via chemical control of the diamond surface. We use low-damage chemical processing and annealing in a hydrogen environment to realize reversible and highly stable charge state tuning in undoped diamond. The resulting SiV 0 centers display optically detected magnetic resonance and bulklike optical properties. Controlling the charge state tuning via surface termination offers a route for scalable technologies based on SiV 0 centers, as well as charge state engineering of other defects.
Effects of temperature on surface-controlled dislocation multiplication in body-centered-cubic metal nanowires
Recent computational studies revealed that screw dislocations in body-centered-cubic (bcc) metal nanowires can self-multiply through cross-slip near the free surface. This unique process was termed surface-controlled dislocation multiplication (SCDM). In bcc metals, screw dislocation motion and its cross-slip behavior are often related to thermally activated processes; due to this relation, SCDM is expected to be highly temperature-sensitive. In this study, therefore, we investigated how temperature influences the SCDM in bcc molybdenum and niobium nanowires using atomistic simulations. Regardless of the difference in lattice resistance at a given temperature, both systems show similar trends of critical shear stress of SCDM with respect to temperature. Further, the temperature dependence was found to be divided into three different regimes; (1) lattice-resistance-dominant; (2) segmentation-dominant; (3) steady-state segmentation. The presence of these three regimes will be discussed in terms of the temperature-dependence of the lattice resistance and the dynamics of dislocation segmentation in the nano-scale volume. Our results provide a fundamental understanding of screw dislocation behavior in bcc metals at the nanometer scale and varying temperatures.
Influence of controlled surface oxidation on the magnetic anisotropy of Co ultrathin films
We studied the influence of controlled surface-limited oxidation of electrodeposited epitaxial Co(0001)/Au(111) films on their magnetic anisotropy energy using real time in situ magneto optical Kerr effect and density functional theory (DFT) calculations. We investigated the Co first electrochemical oxidation step which we demonstrate to be completely reversible and determined the structure of this oxide layer. We show that the interface magnetic anisotropy of the Co film increases by 0.36 erg/cm{sup 2} upon Co surface oxidation. We performed DFT calculations to determine the different surface structures in a wide potential range as well as the charge transfer at the Co surface. Our results suggest that the magnetic anisotropy change is correlated with a positive charge increase of 0.54 e{sup −} for the Co surface atom upon oxidation.
Electrostatically controlled surface boundary conditions in nematic liquid crystals and colloids
Differing from isotropic fluids, liquid crystals exhibit highly anisotropic interactions with surfaces, which define boundary conditions for the alignment of constituent rod-like molecules at interfaces with colloidal inclusions and confining substrates. We show that surface alignment of the nematic molecules can be controlled by harnessing the competing aligning effects of surface functionalization and electric field arising from surface charging and bulk counterions. The control of ionic content in the bulk and at surfaces allows for tuning orientations of shape-anisotropic particles like platelets within an aligned nematic host and for changing the orientation of director relative to confining substrates. The ensuing anisotropic elastic and electrostatic interactions enable colloidal crystals with reconfigurable symmetries and orientations of inclusions.
Studying femtosecond-laser hyperdoping by controlling surface morphology
We study the fundamental properties of femtosecond-laser (fs-laser) hyperdoping by developing techniques to control the surface morphology following laser irradiation. By decoupling the formation of surface roughness from the doping process, we study the structural and electronic properties of fs-laser doped silicon. These experiments are a necessary step toward developing predictive models of the doping process. We use a single fs-laser pulse to dope silicon with sulfur, enabling quantitative secondary ion mass spectrometry, transmission electron microscopy, and Hall effect measurements. These measurements indicate that at laser fluences at or above 4 kJ m{sup -2}, a single laser pulse yields a sulfur dose >(3 {+-} 1) x 10{sup 13} cm{sup -2} and results in a 45-nm thick amorphous surface layer. Based on these results, we demonstrate a method for hyperdoping large areas of silicon without producing the surface roughness.
Gas-phase microactuation using kinetically controlled surface states of ultrathin catalytic sheets
Biological systems convert chemical energy into mechanical work by using protein catalysts that assume kinetically controlled conformational states. Synthetic chemomechanical systems using chemical catalysis have been reported, but they are slow, require high temperatures to operate, or indirectly perform work by harnessing reaction products in liquids (e.g., heat or protons). Here, we introduce a bioinspired chemical strategy for gas-phase chemomechanical transduction that sequences the elementary steps of catalytic reactions on ultrathin (<10 nm) platinum sheets to generate surface stresses that directly drive microactuation (bending radii of 700 nm) at ambient conditions (T = 20 °C; P total = 1 atm). When fueled by hydrogen gas and either oxygen or ozone gas, we show how kinetically controlled surface states of the catalyst can be exploited to achieve fast actuation (600 ms/cycle) at 20 °C. Finally, we also show that the approach can integrate photochemically controlled reactions and can be used to drive the reconfiguration of microhinges and complex origami- and kirigami-based microstructures.
How Topological Polymer Loops on the Nanoparticle Surface Control the Mechanical Properties of Nanocomposites
Carbon black (CB) and silica (SiO 2 ) filled elastomers are known to be the most successful polymer nanocomposites (PNCs) in industry, where “bound rubber (BR)” (i.e., polymer chains that are physically or chemically adsorbed on the nanofiller surface) plays a critical role in their reinforcement. Here, we report a molecular-scale mechanism underlying the “BR-induced reinforcement” by integrating neutron scattering experiments and molecular dynamics simulations. Simplified non-cross-linked SiO 2 -filled polybutadiene (PB) and CB-filled PB reveal the critical role of topological polymer loops in the BR for the enhanced mechanical performance. The average loop size on the SiO 2 surface modified with a silane coupling agent is much smaller than that on the CB surface and the loops on the SiO 2 surface are densely formed, preventing interdigitation with the matrix chains. On the other hand, the larger, uncrowded loops formed on the CB surface facilitate the interdigitation with the matrix polymer chains even near the filler surface. In this way, a strong connectivity is established between a matrix and a nanofiller, resulting in an adhesive filler–polymer interface. Furthermore, our findings shed light on rich and complex physics and materials design problems in PNCs, where the topological polymer structure on the nanofiller surface directly controls the macroscopic mechanical properties.