Revealing the atomic ordering of binary intermetallics using in situ heating techniques at multilength scales

Xiong, Yin; Yang, Yao; Joress, Howie; Padgett, Elliot; Gupta, Unmukt; Yarlagadda, Venkata; Agyeman-Budu, David N.; Huang, Xin; Moylan, Thomas E.; Zeng, Rui; Kongkanand, Anusorn; Escobedo, Fernando A.; Brock, J. D.; DiSalvo, Francis J.; Muller, David A.; Abruña, Héctor D.

doi:10.1073/pnas.1815643116

Cited by 117 publications

(150 citation statements)

References 49 publications

(68 reference statements)

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“…This is particularly true for nanoparticles, as annealing them at elevated temperatures can result in particle aggregation (32). We note that ordered PtNi nanoparticles (33) and L12-ordered Pt3Co nanoparticles (34)(35)(36) have been successfully synthesized, although the ordering in Pt3Co likely occurs more readily than in Pt3Ni (28). There are regions in the Pt-Ni phase diagram in which there is a discontinuous change in the surface structure and composition with an incremental change in bulk composition (Fig.…”

Section: Ptmentioning

confidence: 95%

Computationally Generated Maps of Surface Structures and Catalytic Activities for Alloy Phase Diagrams

Cao¹,

Niu²,

Mueller³

2019

Preprint

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To facilitate the rational design of alloy catalysts, we introduce a method for rapidly calculating the structure and catalytic properties of a substitutional alloy surface that is in equilibrium with the underlying bulk phase. We implement our method by developing a way to generate surface cluster expansions that explicitly account for the lattice parameter of the bulk structure. This approach makes it possible to computationally map the structure and catalytic activity of an alloy surface at every point in the alloy phase diagram, enabling the identification of synthesis conditions likely to result in highly active catalysts. We demonstrate our approach by analyzing Pt-rich Pt–Ni catalysts for the oxygen reduction reaction, finding two regions in the phase diagram that are predicted to result in highly active catalysts. Our analysis indicates that the Pt3Ni(111) surface, which has the highest known specific activity for the oxygen reduction reaction, is likely able to achieve its high activity through the formation of an intermetallic phase with L12 order. We use the generated surface structure and catalytic activity maps to demonstrate how the intermetallic nature of this phase leads to high catalytic activity and discuss how the underlying principles can be used in catalysis design. We further discuss the importance of surface phases and demonstrate how they can dramatically affect catalytic activity.

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Section: Ptmentioning

confidence: 95%

Computationally Generated Maps of Surface Structures and Catalytic Activities for Alloy Phase Diagrams

Cao¹,

Niu²,

Mueller³

2019

Preprint

View full text Add to dashboard Cite

show abstract

“…Analytical TEM has been a useful technique to investigate the structural characters and chemical properties of catalysts at the atomic scale. However, the necessity of understanding the fundamental mechanisms puts forward new requirements for in situ probing the size, morphology, composition, and structure evolutions during the catalytic reactions under working conditions . Environmental TEM (ETEM) and specialized gas holders have been developed to directly probe catalytic reactions in gaseous environment at high spatial resolution.…”

Section: In Situ Tem On Catalytic Gas Reactionmentioning

confidence: 99%

In Situ Transmission Electron Microscopy on Energy‐Related Catalysis

Hwang

Chen

Zhou

et al. 2019

Advanced Energy Materials

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Energy‐related catalytic reactions have been extensively investigated in past years in order to efficiently utilize clean and environmentally benign energy sources. In these systems, the catalysts and the catalyst/active medium interfaces play a crucial role in determining their performance. Thus, understanding the physical and chemical properties of catalysts during reactions is of importance to provide fundamental insights for designing the devices. Transmission electron microscopy can provide tremendous information regarding materials' morphology, microstructure, and chemical properties at nanoscales. With in situ electron microscopy, dynamic processes of catalytic reactions in both gas and liquid environments have been investigated in real time. In this paper, the recent research progress of in situ and operando electron microscopy techniques are introduced with the representative works in energy‐related reactions, including electrochemical catalysis in liquid media and heterogeneous catalysis in gas media. The uniqueness of the specific electron microscopy methods and scientific merits of each work are highlighted. Finally, outlooks on emerging research opportunities are discussed.

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“…nanoparticles (38)(39)(40) have been successfully synthesized, although the ordering in Pt3Co likely occurs more readily than in Pt3Ni (32).…”

Section: Ptmentioning

confidence: 99%

Computationally Generated Maps of Surface Structures and Catalytic Activities for Alloy Phase Diagrams

Cao¹,

Niu²,

Mueller³

2019

Preprint

View full text Add to dashboard Cite

To facilitate the rational design of alloy catalysts, we introduce a method for rapidly calculating the structure and catalytic properties of a substitutional alloy surface that is in equilibrium with the underlying bulk phase. We implement our method by developing a way to generate surface cluster expansions that explicitly account for the lattice parameter of the bulk structure. This approach makes it possible to computationally map the structure of an alloy surface and statistically sample adsorbate binding energies at every point in the alloy phase diagram. When combined with a method for predicting catalytic activities from adsorbate binding energies, maps of catalytic activities at every point in the phase diagram can be created, enabling the identification of synthesis conditions likely to result in highly active catalysts. We demonstrate our approach by analyzing Pt-rich Pt–Ni catalysts for the oxygen reduction reaction, finding two regions in the phase diagram that are predicted to result in highly active catalysts. Our analysis indicates that the Pt3Ni(111) surface, which has the highest known specific activity for the oxygen reduction reaction, is likely able to achieve its high activity through the formation of an intermetallic phase with L12 order. We use the generated surface structure and catalytic activity maps to demonstrate how the intermetallic nature of this phase leads to high catalytic activity and discuss how the underlying principles can be used in catalysis design. We further discuss the importance of surface phases and demonstrate how they can dramatically affect catalytic activity.

show abstract

Revealing the atomic ordering of binary intermetallics using in situ heating techniques at multilength scales

Cited by 117 publications

References 49 publications

Computationally Generated Maps of Surface Structures and Catalytic Activities for Alloy Phase Diagrams

Computationally Generated Maps of Surface Structures and Catalytic Activities for Alloy Phase Diagrams

In Situ Transmission Electron Microscopy on Energy‐Related Catalysis

Computationally Generated Maps of Surface Structures and Catalytic Activities for Alloy Phase Diagrams

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