Surface frustrated Lewis pairs (SFLPs) have been implicated in the gas‐phase heterogeneous (photo)catalytic hydrogenation of CO 2 to CO and CH 3 OH by In 2 O 3− x (OH) y . A key step in the reaction pathway is envisi...
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Surface frustrated Lewis pairs (SFLPs) have been implicated in the gas‐phase heterogeneous (photo)catalytic hydrogenation of CO 2 to CO and CH 3 OH by In 2 O 3− x (OH) y . A key step in the reaction pathway is envisioned to be the heterolysis of H 2 on a proximal Lewis acid–Lewis base pair, the SFLP, the chemistry of which is described as In⋅⋅⋅In‐OH + H 2 → In‐OH 2 + ⋅⋅⋅In‐H − . The product of the heterolysis, thought to be a protonated hydroxide Lewis base In‐OH 2 + and a hydride coordinated Lewis acid In‐H − , can react with CO 2 to form either CO or CH 3 OH. While the experimental and theoretical evidence is compelling for heterolysis of H 2 on the SFLP, all conclusions derive from indirect proof, and direct observation remains lacking. Unexpectedly, we have discovered rhombohedral In 2 O 3− x (OH) y can enable dissociation of H 2 at room temperature, which allows its direct observation by several analytical techniques. The collected analytical results lean towards the heterolysis rather than the homolysis reaction pathway.
Energy harvesting through periodic snap-through of a buckled sheet has recently gained considerable attention because of its potential applications in energy harvesting in low incoming *** the snapping dynamics of uni...
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Energy harvesting through periodic snap-through of a buckled sheet has recently gained considerable attention because of its potential applications in energy harvesting in low incoming *** the snapping dynamics of uniform buckled sheets has been extensively studied,the present work focuses on the energy harvesting and dynamics of a nonuniform snapping sheet with both of its ends clamped in a channel *** analysis reveals that the sheet undergoes periodic snap-through oscillations,with its rear half consistently serving as the main contributor to effective energy harvesting,and the potential energy contributing significantly more than the kinetic *** the stiffness differenceΔEI^(*)shows that increasing the stiffness of the rear part and decreasing that of the fore part shifts the deformation wave toward upstream and enhances the snapping amplitude of the fore part,optimizing energy *** a length compression ratioΔL^(*)=0.3,the maximum potential energy is observed forΔEI^(*)=1,and the total energy peaks atΔEI^(*)=*** study also identifies an optimalΔL^(*)=0.4that maximizes both total and potential energies,and triples the potential energy in comparison withΔL^(*)=***,the enhancement of nonuniformity disappears atΔL^(*)>0.3 for the total energy andΔL^(*)>0.2 for the potential *** findings provide insights to aid optimization of the design and performance of snapping sheet energy harvesters.
Whether the goal is to meet global challenges or to enable a paradigm shift, it is always essential for science to move beyond conventional thinking. Moreover, the mutually beneficial interactions between global chall...
Whether the goal is to meet global challenges or to enable a paradigm shift, it is always essential for science to move beyond conventional thinking. Moreover, the mutually beneficial interactions between global challenges and paradigm shifts require a great deal of effort. To this end, it is imperative for the scientific
Metal nanoclusters have recently attracted considerable attention, not only because of their special size range but also because of their well‐defined compositions and structures. However, subtly tailoring the compos...
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Metal nanoclusters have recently attracted considerable attention, not only because of their special size range but also because of their well‐defined compositions and structures. However, subtly tailoring the compositions and structures of metal nanoclusters for potential applications remains challenging. Now, a two‐phase anti‐galvanic reduction (AGR) method is presented for precisely tailoring Au 44 (TBBT) 28 to produce Au 47 Cd 2 (TBBT) 31 nanoclusters with a hard‐sphere random close‐packed structure, exhibiting Faradaic efficiencies of up to 96 % at −0.57 V for the electrocatalytic reduction of CO 2 to CO.
Achieving active and stable heterogeneous catalysts by encapsulating noble metal species within zeolites is highly promising for high utilization and cost efficiency in thermal and environmental catalytic reactions. R...
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Achieving active and stable heterogeneous catalysts by encapsulating noble metal species within zeolites is highly promising for high utilization and cost efficiency in thermal and environmental catalytic reactions. Ru, considered an economical noble metal alternative with comparable performance, faces great challenges within MFI-type microporous zeolites due to its high cohesive energy and mobility. Herein, an innovative strategy was explored that couples hydrothermal in situ ligand protection with stepwise calcination in a flowing atmosphere to embed ultrasmall Ru clusters anchored at K + -healed silanol sites (≡Si−Ru δ+ −O−K complexes) within 10-membered ring sinusoidal channels of MFI. Comprehensive experiments and theoretical calculations unveiled that the interplay between confined Ru clusters and MFI induces local strain in MFI, creating a unique catalytic microenvironment around the Ru clusters. This synergy interaction enhances alkane deep oxidation as the confined Ru clusters and the MFI microenvironment collectively pre-activate C 3 H 8 and O 2 , facilitate the cleavage of C−H and C−C bonds at low temperatures. Notably, the stable geometric and electronic properties of the confined Ru show exceptional thermal stability up to 1000 °C, rivaling fresh catalysts. These findings shed vital methodological and mechanistic insights for developing efficacious heterogeneous catalysts for thermal catalysis.
In the last decades, shale oil, mainly distributed in the nanopores of shale, has been considered as the representative of unconventional energy to alleviate the energy crisis. But the ideal pore models greatly overes...
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In the last decades, shale oil, mainly distributed in the nanopores of shale, has been considered as the representative of unconventional energy to alleviate the energy crisis. But the ideal pore models greatly overestimate the flowing capability of shale oil. To get more accurate and reasonable flow behavior, the multicomponent shale oil in the realistic kerogen channel is studied by using molecular dynamic simulation. Both density and velocity distributions that along and perpendicular to the flow direction are studied in kerogen channel, where the influence of branch chain of kerogen is also took into consideration. The heavy component tends to form the adsorbed layers on the kerogen wall, as a result of the extremely strong affinity between kerogen and hydrocarbons, and some asphaltene molecules in bulk phase form the cluster in middle of slit. On the flow direction, the velocity profile preforms the peristaltic behavior due to the effect of branch chain of kerogen, and the toluene and asphaltene components contribute it mostly. According to the heterogeneous characteristics of shale oil flow, we define the fictitious slip boundary, which corresponds to the boundary between bulk phase and adsorbed phase, to describe shale oil flow precisely. We also examine the effects of driving pressure gradient, temperature and pore size on the flow behaviors. The enhancements of driving force and temperature both facilitate shale oil flow, and the maximum velocity reaches the stable value within larger kerogen pores. The potential energy distribution and the interaction force contour verified the peristaltic flow behavior and the validity of fictitious slip boundary.
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