Pt-Based electrocatalysts with high atom utilization efficiency: from nanostructures to single atoms

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Abstract

This review presents recent developments in the design and synthesis of Pt-based catalysts with high atom utilization efficiency and their enhanced catalytic performance in electrochemical catalytic reactions.

Abstract

In recent years, development to increase the performance of Pt-based catalysts and reduce the cost has received significant attention. Among them, the preparation of Pt-based catalysts with high atom utilization efficiency can induce more active sites between the Pt atoms and participating molecules, resulting in improved mass activity. In addition, the combination of high atom utilization efficiency with well-controlled surface structure and composition could boost the mass activity for Pt-based catalysts. This review describes recent progress in the design and synthesis of Pt-based catalysts with high atom utilization efficiency and their enhanced catalytic performance in electrochemical catalytic reactions. The significance for the fabrication of nanostructures and single atom catalysts with high atom utilization will be presented in the introduction section. We discuss the synthetic strategies according to two routes: (1) the rational design of Pt nanostructures, including porous, nanowire, core–shell and hollow structures; and (2) preparation of Pt single atom catalysts and the stabilization of single atoms. Additionally, we discuss the superior electro-catalytic applications of Pt-based catalysts with high atom utilization efficiency. These recent advancements in rational design of Pt-based catalysts offer numerous cases for potential industrialized catalysts with high mass activity and reduced cost in the future.

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Platinum-based heterogeneous catalysts are critical to many important commercial chemical processes, but their efficiency is extremely low on a per metal atom basis, because only the surface active-site atoms are used. Catalysts with single-atom dispersions are thus highly desirable to maximize atom efficiency, but making them is challenging. Here we report the synthesis of a single-atom catalyst that consists of only isolated single Pt atoms anchored to the surfaces of iron oxide nanocrystallites. This single-atom catalyst has extremely high atom efficiency and shows excellent stability and high activity for both CO oxidation and preferential oxidation of CO in H2. Density functional theory calculations show that the high catalytic activity correlates with the partially vacant 5d orbitals of the positively charged, high-valent Pt atoms, which help to reduce both the CO adsorption energy and the activation barriers for CO oxidation.

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Supported metal nanostructures are the most widely used type of heterogeneous catalyst in industrial processes. The size of metal particles is a key factor in determining the performance of such catalysts. In particular, because low-coordinated metal atoms often function as the catalytically active sites, the specific activity per metal atom usually increases with decreasing size of the metal particles. However, the surface free energy of metals increases significantly with decreasing particle size, promoting aggregation of small clusters. Using an appropriate support material that strongly interacts with the metal species prevents this aggregation, creating stable, finely dispersed metal clusters with a high catalytic activity, an approach industry has used for a long time. Nevertheless, practical supported metal catalysts are inhomogeneous and usually consist of a mixture of sizes from nanoparticles to subnanometer clusters. Such heterogeneity not only reduces the metal atom efficiency but also frequently leads to undesired side reactions. It also makes it extremely difficult, if not impossible, to uniquely identify and control the active sites of interest. The ultimate small-size limit for metal particles is the single-atom catalyst (SAC), which contains isolated metal atoms singly dispersed on supports. SACs maximize the efficiency of metal atom use, which is particularly important for supported noble metal catalysts. Moreover, with well-defined and uniform single-atom dispersion, SACs offer great potential for achieving high activity and selectivity. In this Account, we highlight recent advances in preparation, characterization, and catalytic performance of SACs, with a focus on single atoms anchored to metal oxides, metal surfaces, and graphene. We discuss experimental and theoretical studies for a variety of reactions, including oxidation, water gas shift, and hydrogenation. We describe advances in understanding the spatial arrangements and electronic properties of single atoms, as well as their interactions with the support. Single metal atoms on support surfaces provide a unique opportunity to tune active sites and optimize the activity, selectivity, and stability of heterogeneous catalysts, offering the potential for applications in a variety of industrial chemical reactions.

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Author and article information

Contributors

Xueliang Sun: (View ORCID Profile)

Journal

Journal ID (publisher-id): EESNBY

Title: Energy & Environmental Science

Abbreviated Title: Energy Environ. Sci.

Publisher: Royal Society of Chemistry (RSC)

ISSN (Print): 1754-5692

ISSN (Electronic): 1754-5706

Publication date Created: February 13 2019

Publication date (Electronic): 2019

Volume: 12

Issue: 2

Pages: 492-517

Affiliations

[1 ]Department of Mechanical and Materials Engineering

[2 ]The University of Western Ontario

[3 ]London

[4 ]Canada

Article

DOI: 10.1039/C8EE02939C

SO-VID: 53987775-ef2f-45ab-bfe3-14d60769d4b2

License:

http://rsc.li/journals-terms-of-use

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