A Fullerene-Platinum Complex for Direct Functional Patterning of Single Metal Atom-Embedded Carbon Nanostructures.

The development of patterning materials ("resists") at the nanoscale involves two distinct trends: one is toward high sensitivity and resolution for miniaturization, the other aims at functionalization of the resists to realize bottom-up construction of distinct nanoarchitectures. Patterning of carbon nanostructures, a seemingly ideal application for organic functional resists, has been highly reliant on complicated pattern transfer processes because of a lack of patternable precursors. Herein, we present a fullerene-metal coordination complex as a fabrication material for direct functional patterning of sub-10 nm metal-containing carbon structures. The attachment of one platinum atom per fullerene molecule not only leads to significant improvement of sensitivity and resolution but also enables stable atomic dispersion of the platinum ions within the carbon matrix, which may gain fundamentally new interest in functional patterning of hierarchical carbon nanostructures.

Blurring the boundary between homogenous and heterogeneous catalysis using palladium nanoclusters with dynamic surfaces.

Using a magnetron sputtering approach that allows size-controlled formation of nanoclusters, we have created palladium nanoclusters that combine the features of both heterogeneous and homogeneous catalysts. Here we report the atomic structures and electronic environments of a series of metal nanoclusters in ionic liquids at different stages of formation, leading to the discovery of Pd nanoclusters with a core of ca. 2 nm surrounded by a diffuse dynamic shell of atoms in [C4C1Im][NTf2]. Comparison of the catalytic activity of Pd nanoclusters in alkene cyclopropanation reveals that the atomically dynamic surface is critically important, increasing the activity by a factor of ca. 2 when compared to compact nanoclusters of similar size. Catalyst poisoning tests using mercury and dibenzo[a,e]cyclooctene show that dynamic Pd nanoclusters maintain their catalytic activity, which demonstrate their combined features of homogeneous and heterogeneous catalysts within the same material. Additionally, kinetic studies of cyclopropanation of alkenes mediated by the dynamic Pd nanoclusters reveal an observed catalyst order of 1, underpinning the pseudo-homogeneous character of the dynamic Pd nanoclusters.

Electrode Shifts Estimation and Adaptive Correction for Improving Robustness of sEMG-Based Recognition.

In sEMG-based recognition systems, accuracy is severely worsened by disturbances, such as electrode shifts by doffing/donning. Traditional recognition models are fixed or static, with limited abilities to work in the presence of the disturbances. In this paper, a transfer learning method is proposed to reduce the impact of electrode shifts. In the proposed method, a novel activation angle is introduced to locate electrodes within a polar coordinate system. An adaptive transformation is utilized to correct electrode-shifted sEMG samples. The transformation is based on estimated shifts relative to the initial position. The experiments acquisition data from ten subjects consist of sEMG signals under eight gestures in seven or nine arbitrary positions, and recorded shifts from a 3D-printed annular ruler. In our extensive experiments, the errors between recorded shifts (as the reference) and estimated shifts is about -0.017±0.13 radians. Eight gestures recognition results have shown an average accuracy around 79.32%, which represents a significant improvement over the 35.72% ( ) average accuracy of results obtained using nonadaptive models, and 60.99% ( ) results of the other method iGLCM (an improved gray-level co-occurrence matrix). More importantly, by only using one-label samples, the proposed method updates the pre-trained model in an initial position. As a result, the pre-trained model can be adaptively corrected to recognize eight-label gestures in arbitrarily rotary positions. It is proven a highly efficient way to relieve subjects' re-training burden of sEMG-based rehabilitation systems.

Ultrathin dendritic Pt3Cu triangular pyramid caps with enhanced electrocatalytic activity.

Here we report on the synthesis of novel dendritic Pt3Cu triangular pyramid caps via a solvothermal coreduction method. These caps had three-dimensional caved structures with ultrathin branches, as evidenced by high-resolution transmission electron microscopy (HRTEM) and HAADF-STEM characterization. Tuning the reduction kinetics of two metal precursors by an iodide ion was believed to be the key for the formation of an alloyed nanostructure. Electro-oxidation of methanol and formic acid showed dramatically improved electrocatalytic activities and poison-tolerance for these nanoalloys as compared to commercial Pt/C catalysts, which was attributed to their unique open porous structure with interconnected network, ultrahigh surface areas, as well as synergetic effect of the two metallic components.