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327 result(s) for "Hensen, M. T. T."
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External Human–Machine Interfaces: The Effect of Display Location on Crossing Intentions and Eye Movements
In the future, automated cars may feature external human–machine interfaces (eHMIs) to communicate relevant information to other road users. However, it is currently unknown where on the car the eHMI should be placed. In this study, 61 participants each viewed 36 animations of cars with eHMIs on either the roof, windscreen, grill, above the wheels, or a projection on the road. The eHMI showed ‘Waiting’ combined with a walking symbol 1.2 s before the car started to slow down, or ‘Driving’ while the car continued driving. Participants had to press and hold the spacebar when they felt it safe to cross. Results showed that, averaged over the period when the car approached and slowed down, the roof, windscreen, and grill eHMIs yielded the best performance (i.e., the highest spacebar press time). The projection and wheels eHMIs scored relatively poorly, yet still better than no eHMI. The wheels eHMI received a relatively high percentage of spacebar presses when the car appeared from a corner, a situation in which the roof, windscreen, and grill eHMIs were out of view. Eye-tracking analyses showed that the projection yielded dispersed eye movements, as participants scanned back and forth between the projection and the car. It is concluded that eHMIs should be presented on multiple sides of the car. A projection on the road is visually effortful for pedestrians, as it causes them to divide their attention between the projection and the car itself.
Engineering bunched Pt-Ni alloy nanocages for efficient oxygen reduction in practical fuel cells
Development of efficient and robust electrocatalysts is critical for practical fuel cells. We report one-dimensional bunched platinum-nickel (Pt-Ni) alloy nanocages with a Pt-skin structure for the oxygen reduction reaction that display high mass activity (3.52 amperes per milligram platinum) and specific activity (5.16 milliamperes per square centimeter platinum), or nearly 17 and 14 times higher as compared with a commercial platinum on carbon (Pt/C) catalyst. The catalyst exhibits high stability with negligible activity decay after 50,000 cycles. Both the experimental results and theoretical calculations reveal the existence of fewer strongly bonded platinum-oxygen (Pt-O) sites induced by the strain and ligand effects. Moreover, the fuel cell assembled by this catalyst delivers a current density of 1.5 amperes per square centimeter at 0.6 volts and can operate steadily for at least 180 hours.
Tuning Pt-CeO2 interactions by high-temperature vapor-phase synthesis for improved reducibility of lattice oxygen
In this work, we compare the CO oxidation performance of Pt single atom catalysts (SACs) prepared via two methods: (1) conventional wet chemical synthesis (strong electrostatic adsorption–SEA) with calcination at 350 °C in air; and (2) high temperature vapor phase synthesis (atom trapping–AT) with calcination in air at 800 °C leading to ionic Pt being trapped on the CeO 2 in a thermally stable form. As-synthesized, both SACs are inactive for low temperature (<150 °C) CO oxidation. After treatment in CO at 275 °C, both catalysts show enhanced reactivity. Despite similar Pt metal particle size, the AT catalyst is significantly more active, with onset of CO oxidation near room temperature. A combination of near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) and CO temperature-programmed reduction (CO-TPR) shows that the high reactivity at low temperatures can be related to the improved reducibility of lattice oxygen on the CeO 2 support. While single-atom catalysts (SACs) have attracted a lot of interest, the nature of the active sites in SACs remains elusive. Here the authors elucidate that depositing single atoms via high temperature synthesis leads to improved reducibility of lattice oxygen on CeO2 yielding low temperature reactivity of Pt catalysts in CO oxidation.
Unconditional quantum teleportation between distant solid-state quantum bits
Realizing robust quantum information transfer between long-lived qubit registers is a key challenge for quantum information science and technology. Here we demonstrate unconditional teleportation of arbitrary quantum states between diamond spin qubits separated by 3 meters. We prepare the teleporter through photon-mediated heralded entanglement between two distant electron spins and subsequently encode the source qubit in a single nuclear spin. By realizing a fully deterministic Bell-state measurement combined with real-time feed-forward, quantum teleportation is achieved upon each attempt with an average state fidelity exceeding the classical limit. These results establish diamond spin qubits as a prime candidate for the realization of quantum networks for quantum communication and network-based quantum computing.
Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol
Copper-exchanged zeolites with mordenite structure mimic the nuclearity and reactivity of active sites in particulate methane monooxygenase, which are enzymes able to selectively oxidize methane to methanol. Here we show that the mordenite micropores provide a perfect confined environment for the highly selective stabilization of trinuclear copper-oxo clusters that exhibit a high reactivity towards activation of carbon–hydrogen bonds in methane and its subsequent transformation to methanol. The similarity with the enzymatic systems is also implied from the similarity of the reversible rearrangements of the trinuclear clusters occurring during the selective transformations of methane along the reaction path towards methanol, in both the enzyme system and copper-exchanged mordenite. Copper-exchanged zeolites with mordenite structure can mimic the active sites in particulate methane monooxygenase. Here, the authors show that mordenite micropores can stabilize trinuclear copper-oxo clusters that exhibit a high reactivity towards activation of carbon–hydrogen bonds in methane.
Imaging the facet surface strain state of supported multi-faceted Pt nanoparticles during reaction
Nanostructures with specific crystallographic planes display distinctive physico-chemical properties because of their unique atomic arrangements, resulting in widespread applications in catalysis, energy conversion or sensing. Understanding strain dynamics and their relationship with crystallographic facets have been largely unexplored. Here, we reveal in situ, in three-dimensions and at the nanoscale, the volume, surface and interface strain evolution of single supported platinum nanocrystals during reaction using coherent x-ray diffractive imaging. Interestingly, identical { hkl } facets show equivalent catalytic response during non-stoichiometric cycles. Periodic strain variations are rationalised in terms of O 2 adsorption or desorption during O 2 exposure or CO oxidation under reducing conditions, respectively. During stoichiometric CO oxidation, the strain evolution is, however, no longer facet dependent. Large strain variations are observed in localised areas, in particular in the vicinity of the substrate/particle interface, suggesting a significant influence of the substrate on the reactivity. These findings will improve the understanding of dynamic properties in catalysis and related fields. Understanding strain dynamics and their relationship with crystallographic facets have been largely unexplored. Here the authors demonstrate how the 3D lattice displacement and strain evolution depend on the crystallographic facets of Pt nanoparticles during CO oxidation reaction, providing new insights in the relationship between facet-related surface strain and chemistry.
Understanding carbon dioxide activation and carbon–carbon coupling over nickel
Carbon dioxide is a desired feedstock for platform molecules, such as carbon monoxide or higher hydrocarbons, from which we will be able to make many different useful, value-added chemicals. Its catalytic hydrogenation over abundant metals requires the amalgamation of theoretical knowledge with materials design. Here we leverage a theoretical understanding of structure sensitivity, along with a library of different supports, to tune the selectivity of methanation in the Power-to-Gas concept over nickel. For example, we show that carbon dioxide hydrogenation over nickel can and does form propane, and that activity and selectivity can be tuned by supporting different nickel particle sizes on various oxides. This theoretical and experimental toolbox is not only useful for the highly selective production of methane, but also provides new insights for carbon dioxide activation and subsequent carbon–carbon coupling towards value-added products thereby reducing the deleterious effects of this environmentally harmful molecule. Carbon dioxide is a desired feedstock for platform molecules, such as carbon monoxide and higher hydrocarbons, but needs improved catalysts. Here, the authors use a combined theoretical and experimental approach to tune the activity and selectivity of CO 2 conversion over nickel towards desired products.
N-formyl-stabilizing quasi-catalytic species afford rapid and selective solvent-free amination of biomass-derived feedstocks
Nitrogen-containing compounds, especially primary amines, are vital building blocks in nature and industry. Herein, a protocol is developed that shows in situ formed N-formyl quasi-catalytic species afford highly selective synthesis of formamides or amines with controllable levels from a variety of aldehyde- and ketone-derived platform chemical substrates under solvent-free conditions. Up to 99% yields of mono-substituted formamides are obtained in 3 min. The C-N bond formation and N-formyl species are prevalent in the cascade reaction sequence. Kinetic and isotope labeling experiments explicitly demonstrate that the C-N bond is activated for subsequent hydrogenation, in which formic acid acts as acid catalyst, hydrogen donor and as N-formyl species source that stabilize amine intermediates elucidated with density functional theory. The protocol provides access to imides from aldehydes, ketones, carboxylic acids, and mixed-substrates, requires no special catalysts, solvents or techniques and provides new avenues for amination chemistry. Processes for efficient production of primary, secondary or ternary aminated compounds are constant challenges for chemical and pharmaceutical industries. Here, the authors develop selective and sustainable amination chemistry widely applicable to chemical substrates via formic acid.
Interface dynamics of Pd–CeO2 single-atom catalysts during CO oxidation
In recent years, noble metals atomically dispersed on solid oxide supports have become a frontier of heterogeneous catalysis. In pursuit of an ultimate atom efficiency, the stability of single-atom catalysts is pivotal. Here we compare two Pd/CeO 2 single-atom catalysts that are active in low-temperature CO oxidation and display drastically different structural dynamics under the reaction conditions. These catalysts were obtained by conventional impregnation on hydrothermally synthesized CeO 2 and one-step flame spray pyrolysis. The oxidized Pd atoms in the impregnated catalyst were prone to reduction and sintering during CO oxidation, whereas they remained intact on the surface of the Pd-doped CeO 2 derived by flame spray pyrolysis. A detailed in situ characterization linked the stability of the Pd single atoms to the reducibility of the Pd–CeO 2 interface and the extent of reverse oxygen spillover. To understand the chemical phenomena that underlie the metal–support interactions is crucial to the rational design of stable single-atom catalysts. Single-atom catalysts have become a frontier of heterogeneous catalysis, but to achieve a high stability under turnover is often a challenge. Now, a Pd/CeO 2 single-atom catalyst prepared using flame spray pyrolysis is able to stabilize the isolated Pd species during CO oxidation due to a high mobility of surface lattice oxygen.
Structure–performance descriptors and the role of Lewis acidity in the methanol-to-propylene process
The combination of well-defined acid sites, shape-selective properties and outstanding stability places zeolites among the most practically relevant heterogeneous catalysts. The development of structure–performance descriptors for processes that they catalyse has been a matter of intense debate, both in industry and academia, and the direct conversion of methanol to olefins is a prototypical system in which various catalytic functions contribute to the overall performance. Propylene selectivity and resistance to coking are the two most important parameters in developing new methanol-to-olefin catalysts. Here, we present a systematic investigation on the effect of acidity on the performance of the zeolite ‘ZSM-5’ for the production of propylene. Our results demonstrate that the isolation of Brønsted acid sites is key to the selective formation of propylene. Also, the introduction of Lewis acid sites prevents the formation of coke, hence drastically increasing catalyst lifetime.