Tuning metal–support interaction has been considered as an effective approach to modulate the electronic structure and catalytic activity of supported metal catalysts. At the atomic level, the understanding of the structure–activity relationship still remains obscure in heterogeneous catalysis, such as the conversion of water (alkaline) or hydronium ions (acid) to hydrogen (hydrogen evolution reaction, HER). Here, we reveal that the fine control over the oxidation states of single-atom Pt catalysts through electronic metal–support interaction significantly modulates the catalytic activities in either acidic or alkaline HER. Combined with detailed spectroscopic and electrochemical characterizations, the structure–activity relationship is established by correlating the acidic/alkaline HER activity with the average oxidation state of single-atom Pt and the Pt–H/Pt–OH interaction. This study sheds light on the atomic-level mechanistic understanding of acidic and alkaline HER, and further provides guidelines for the rational design of high-performance single-atom catalysts.
Sparse localized decomposition is a useful technique to extract meaningful deformation components out of a training set of mesh data. However, existing methods cannot capture large rotational motion in the given mesh dataset. In this paper we present a new decomposition technique based on deformation gradients. Given a mesh dataset, the deformation gradient field is extracted, and decomposed into two groups: rotation field and stretching field, through polar decomposition. These two groups of deformation information are further processed through the sparse localized decomposition into the desired components. These sparse localized components can be linearly combined to form a meaningful deformation gradient field, and can be used to reconstruct the mesh through a least squares optimization step. Our experiments show that the proposed method addresses the rotation problem associated with traditional deformation decomposition techniques, making it suitable to handle not only stretched deformations, but also articulated motions that involve large rotations.
Ceramic dielectrics are reported with superior energy storage performance for applications, such as power electronics in electrical vehicles. A recoverable energy density ( W rec ) of ∼4.55 J cm –3 with η ∼ 90% is achieved in lead-free relaxor BaTiO 3 -0.06Bi 2/3 (Mg 1/3 Nb 2/3 )O 3 ceramics at ∼520 kV cm –1 . These ceramics may be co-fired with Ag/Pd, which constitutes a major step forward toward their potential use in the fabrication of commercial multilayer ceramic capacitors. Compared to stoichiometric Bi(Mg 2/3 Nb 1/3 )O 3 -doped BaTiO 3 (BT), A-site deficient Bi 2/3 (Mg 1/3 Nb 2/3 )O 3 reduces the electrical heterogeneity of BT. Bulk conductivity differs from the grain boundary only by 1 order of magnitude which, coupled with a smaller volume fraction of conducting cores due to enhanced diffusion of the dopant via A-site vacancies in the A-site sublattice, results in higher breakdown strength under an electric field. This strategy can be employed to develop new dielectrics with improved energy storage performance.
This paper reports on studies of the effect of temperature step-change (between a cool and a neutral environment) on human thermal sensation and skin temperature. Experiments with three temperature conditions were carried out in a climate chamber during the period in winter. Twelve subjects participated in the experiments simulating moving inside and outside of rooms or cabins with air conditioning. Skin temperatures and thermal sensation were recorded. Results showed overshoot and asymmetry of TSV due to the step-change. Skin temperature changed immediately when subjects entered a new environment. When moving into a neutral environment from cool, dynamic thermal sensation was in the thermal comfort zone and overshoot was not obvious. Air-conditioning in a transitional area should be considered to limit temperature difference to not more than 5°C to decrease the unacceptability of temperature step-change. The linear relationship between thermal sensation and skin temperature or gradient of skin temperature does not apply in a step-change environment. There is a significant linear correlation between TSV and Qloss in the transient environment. Heat loss from the human skin surface can be used to predict dynamic thermal sensation instead of the heat transfer of the whole human body.
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