Dataset Information

Conformational Effects of Pt-Shells on Nanostructures and Corresponding Oxygen Reduction Reaction Activity of Au-Cluster-Decorated NiO_x@Pt Nanocatalysts.

ABSTRACT: Herein, ternary metallic nanocatalysts (NCs) consisting of Au clusters decorated with a Pt shell and a Ni oxide core underneath (called NPA) on carbon nanotube (CNT) support were synthesized by combining adsorption, precipitation, and chemical reduction methods. By a retrospective investigation of the physical structure and electrochemical results, we elucidated the effects of Pt/Ni ratios (0.4 and 1.0) and Au contents (2 and 9 wt.%) on the nanostructure and corresponding oxygen reduction reaction (ORR) activity of the NPA NCs. We found that the ORR activity of NPA NCs was mainly dominated by the Pt-shell thickness which regulated the depth and size of the surface decorated with Au clusters. In the optimal case, NPA-1004006 (with a Pt/Ni of 0.4 and Au of ~2 wt.%) showed a kinetic current (J_K) of 75.02 mA cm^-2 which was nearly 17-times better than that (4.37 mA cm^-2) of the commercial Johnson Matthey-Pt/C (20 wt.% Pt) catalyst at 0.85 V vs. the reference hydrogen electrode. Such a high J_K value resulted in substantial improvements in both the specific activity (by ~53-fold) and mass activity (by nearly 10-fold) in the same benchmark target. Those scenarios rationalize that ORR activity can be substantially improved by a syngeneic effect at heterogeneous interfaces among nanometer-sized NiO_x, Pt, and Au clusters on the NC surface.

SUBMITTER: Bhalothia D

PROVIDER: S-EPMC6669587 | biostudies-literature | 2019 Jul

REPOSITORIES: biostudies-literature

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Conformational Effects of Pt-Shells on Nanostructures and Corresponding Oxygen Reduction Reaction Activity of Au-Cluster-Decorated NiO<i><sub>x</sub></i>@Pt Nanocatalysts.

Bhalothia Dinesh D Fan Yu-Jui YJ Lai Yen-Chun YC Yang Ya-Tang YT Yang Yaw-Wen YW Lee Chih-Hao CH Chen Tsan-Yao TY

Nanomaterials (Basel, Switzerland) 20190711 7

Herein, ternary metallic nanocatalysts (NCs) consisting of Au clusters decorated with a Pt shell and a Ni oxide core underneath (called NPA) on carbon nanotube (CNT) support were synthesized by combining adsorption, precipitation, and chemical reduction methods. By a retrospective investigation of the physical structure and electrochemical results, we elucidated the effects of Pt/Ni ratios (0.4 and 1.0) and Au contents (2 and 9 wt.%) on the nanostructure and corresponding oxygen reduction reacti ...[more]

PMID: 31336802

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Project description:Integration of plasmonic nanoantennas with catalytically active reactors in deliberately designed hybrid supra-nanostructures creates a dual-functional materials platform, based upon which precise modulation of catalytic reaction kinetics becomes accomplishable through optical excitations of plasmon resonances. Here, we have developed a multistep synthetic approach that enables us to assemble colloidal Au@C/Pt core@shell/satellite supra-nanostructures, in which the Au core functions as a light-harvesting plasmonic nanoantenna, the Pt satellites act as catalytically active reactors, and the C shell serves as a nanoscale dielectric spacer separating the reactors from the antenna, respectively. By adjusting several synthetic parameters, the size of the Au core, the thickness of the C shell, and the surface coverage of Pt satellites can all be tuned independently. Choosing Pt-catalyzed cascade oxidation of 3,3',5,5'-tetramethylbenzidine in an aerobic aqueous environment as a model reaction, we have systematically studied the detailed kinetic features of the catalytic reactions both in the dark and under visible light illumination over a broad range of reaction conditions, which sheds light on the interplay between plasmonic and catalytic effects in these antenna-reactor nanohybrids. The plasmonic antenna effect can be effectively harnessed to kinetically modulate multiple crucial steps during the cascade reactions, benefiting from plasmon-enhanced interband electronic transitions in the Pt satellites and plasmon-enhanced intramolecular electronic excitations in chromogenic intermediate species. In addition to the plasmonic antenna effect, photothermal transduction derived from plasmonic excitations can also provide significant contributions to the kinetic enhancements under visible light illumination. The knowledge gained from this work serves as important guiding principles for rational design and structural optimization of plasmonic antenna-reactor hybrid nanomaterials, endowing us with enhanced capabilities to kinetically modulate targeted catalytic/photocatalytic molecule-transforming processes through light illumination.

Dataset Information

Conformational Effects of Pt-Shells on Nanostructures and Corresponding Oxygen Reduction Reaction Activity of Au-Cluster-Decorated NiO_x@Pt Nanocatalysts.

Publications

Conformational Effects of Pt-Shells on Nanostructures and Corresponding Oxygen Reduction Reaction Activity of Au-Cluster-Decorated NiO<i><sub>x</sub></i>@Pt Nanocatalysts.

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Conformational Effects of Pt-Shells on Nanostructures and Corresponding Oxygen Reduction Reaction Activity of Au-Cluster-Decorated NiOx@Pt Nanocatalysts.

Publications

Conformational Effects of Pt-Shells on Nanostructures and Corresponding Oxygen Reduction Reaction Activity of Au-Cluster-Decorated NiO<i><sub>x</sub></i>@Pt Nanocatalysts.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets

Conformational Effects of Pt-Shells on Nanostructures and Corresponding Oxygen Reduction Reaction Activity of Au-Cluster-Decorated NiO_x@Pt Nanocatalysts.