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1.
Proc Natl Acad Sci U S A ; 116(6): 1974-1983, 2019 02 05.
Article in English | MEDLINE | ID: mdl-30670659

ABSTRACT

Ordered intermetallic nanoparticles are promising electrocatalysts with enhanced activity and durability for the oxygen-reduction reaction (ORR) in proton-exchange membrane fuel cells (PEMFCs). The ordered phase is generally identified based on the existence of superlattice ordering peaks in powder X-ray diffraction (PXRD). However, after employing a widely used postsynthesis annealing treatment, we have found that claims of "ordered" catalysts were possibly/likely mixed phases of ordered intermetallics and disordered solid solutions. Here, we employed in situ heating, synchrotron-based, X-ray diffraction to quantitatively investigate the impact of a variety of annealing conditions on the degree of ordering of large ensembles of Pt3Co nanoparticles. Monte Carlo simulations suggest that Pt3Co nanoparticles have a lower order-disorder phase transition (ODPT) temperature relative to the bulk counterpart. Furthermore, we employed microscopic-level in situ heating electron microscopy to directly visualize the morphological changes and the formation of both fully and partially ordered nanoparticles at the atomic scale. In general, a higher degree of ordering leads to more active and durable electrocatalysts. The annealed Pt3Co/C with an optimal degree of ordering exhibited significantly enhanced durability, relative to the disordered counterpart, in practical membrane electrode assembly (MEA) measurements. The results highlight the importance of understanding the annealing process to maximize the degree of ordering in intermetallics to optimize electrocatalytic activity.

2.
Lab Chip ; 14(1): 189-99, 2014 Jan 07.
Article in English | MEDLINE | ID: mdl-24196070

ABSTRACT

One strategy for actuating soft machines (e.g., tentacles, grippers, and simple walkers) uses pneumatic inflation of networks of small channels in an elastomeric material. Although the management of a few pneumatic inputs and valves to control pressurized gas is straightforward, the fabrication and operation of manifolds containing many (>50) independent valves is an unsolved problem. Complex pneumatic manifolds-often built for a single purpose-are not easily reconfigured to accommodate the specific inputs (i.e., multiplexing of many fluids, ranges of pressures, and changes in flow rates) required by pneumatic systems. This paper describes a pneumatic manifold comprising a computer-controlled Braille display and a micropneumatic device. The Braille display provides a compact array of 64 piezoelectric actuators that actively close and open elastomeric valves of a micropneumatic device to route pressurized gas within the manifold. The positioning and geometries of the valves and channels in the micropneumatic device dictate the functionality of the pneumatic manifold, and the use of multi-layer soft lithography permits the fabrication of networks in a wide range of configurations with many possible functions. Simply exchanging micropneumatic devices of different designs enables rapid reconfiguration of the pneumatic manifold. As a proof of principle, a pneumatic manifold controlled a soft machine containing 32 independent actuators to move a ball above a flat surface.


Subject(s)
Microfluidic Analytical Techniques/instrumentation , Elasticity , Equipment Design , Pressure
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