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Journal ArticleDOI

The effect of particle proximity on the oxygen reduction rate of size-selected platinum clusters

TLDR
It is observed that the Pt cluster coverage, and hence the interparticle distance, decisively influence the observed catalytic activity and that closely packed assemblies of Pt clusters approach the surface activity of bulk Pt.
Abstract
The diminished surface-area-normalized catalytic activity of highly dispersed Pt nanoparticles compared with bulk Pt is particularly intricate, and not yet understood. Here we report on the oxygen reduction reaction (ORR) activity of well-defined, size-selected Pt nanoclusters; a unique approach that allows precise control of both the cluster size and coverage, independently. Our investigations reveal that size-selected Pt nanoclusters can reach extraordinarily high ORR activities, especially in terms of mass-normalized activity, if deposited at high coverage on a glassy carbon substrate. It is observed that the Pt cluster coverage, and hence the interparticle distance, decisively influence the observed catalytic activity and that closely packed assemblies of Pt clusters approach the surface activity of bulk Pt. Our results open up new strategies for the design of catalyst materials that circumvent the detrimental dispersion effect, and may eventually allow the full electrocatalytic potential of Pt nanoclusters to be realized.

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Citations
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Journal ArticleDOI

Recent Advances in Electrocatalysts for Oxygen Reduction Reaction

TL;DR: This comprehensive Review focuses on the low- and non-platinum electrocatalysts including advanced platinum alloys, core-shell structures, palladium-based catalysts, metal oxides and chalcogenides, carbon-based non-noble metal catalysts and metal-free catalysts.
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Metal Catalysts for Heterogeneous Catalysis: From Single Atoms to Nanoclusters and Nanoparticles.

TL;DR: This Review will compare the results obtained from different systems and try to give a picture on how different types of metal species work in different reactions and give perspectives on the future directions toward better understanding of the catalytic behavior of different metal entities in a unifying manner.
Journal ArticleDOI

Oxygen electrochemistry as a cornerstone for sustainable energy conversion

TL;DR: A promising strategy to develop such an understanding is the investigation of the impact of material properties on reaction activity/selectivity and on catalyst stability under the conditions of operation, as well as the application of complementary in situ techniques for the Investigation of catalyst structure and composition.
Journal ArticleDOI

Atomically Precise Noble Metal Nanoclusters as Efficient Catalysts: A Bridge between Structure and Properties.

TL;DR: The model catalyst role of NCs in catalysis is illustrated from theoretical and experimental perspectives, particularly in electrocatalysis, photocatalysis, photoelectric conversion, and catalysis of organic reactions.
Journal ArticleDOI

Bottom-up precise synthesis of stable platinum dimers on graphene.

TL;DR: Pt2 dimers can be fabricated with a bottom–up approach on graphene using atomic layer deposition, through proper nucleation sites creation, Pt1 single-atom deposition and attaching a secondary Pt atom selectively on the preliminary one.
References
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Journal ArticleDOI

Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode

TL;DR: In this paper, the stability of reaction intermediates of electrochemical processes on the basis of electronic structure calculations was analyzed and a detailed description of the free energy landscape of the electrochemical oxygen reduction reaction over Pt(111) as a function of applied bias was presented.
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Activity benchmarks and requirements for Pt, Pt-alloy, and non-Pt oxygen reduction catalysts for PEMFCs

TL;DR: In this article, the authors quantified the activities and voltage loss modes for state-of-the-art MEAs (membrane electrode assemblies), specifies performance goals needed for automotive application, and provides benchmark oxygen reduction activities for state of the art platinum electrocatalysts.
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Alloys of platinum and early transition metals as oxygen reduction electrocatalysts

TL;DR: A new set of ORR electrocatalysts consisting of Pd or Pt alloyed with early transition metals such as Sc or Y, identified using density functional theory calculations as being the most stable Pt- and Pd-based binary alloys with ORR activity likely to be better than Pt.
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Lattice-strain control of the activity in dealloyed core–shell fuel cell catalysts

TL;DR: It is shown how lattice strain can be used experimentally to tune the catalytic activity of dealloyed bimetallic nanoparticles for the oxygen-reduction reaction, a key barrier to the application of fuel cells and metal-air batteries.
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Surface science studies of model fuel cell electrocatalysts

TL;DR: In this paper, the authors discuss progress in the understanding of electrocatalytic reactions through the study of model systems with surface spectroscopies and discuss the limitations of using pure metal single crystals and well-characterized bulk alloys as models for real catalysts.
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