Investigation of Catalytic Finite-Size-Effects of Platinum Metal Clusters

Li, Lin; Larsen, Ask Hjorth; Romero, Nichols A.; Morozov, Vitali; Glinsvad, Christian; Abild‐Pedersen, Frank; Greeley, Jeff; Jacobsen, Karsten Wedel; Nørskov, Jens K.

doi:10.1021/jz3018286

Cited by 271 publications

(304 citation statements)

References 27 publications

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“…Commercial Pt catalyst was also simulated to have a ΔE O of 0.1 eV based on the QM−MM method and the 3 nm NP model, which was consistent with the previous reported value through DFT calculations. 30 We can easily expect that a NP catalyst more active than commercial Pt NP should possess a ΔE O in the range of 0.1−0.3 eV (0.2 eV is the optimal value). Our fccFePt/Pt and fct-FePt/Pt fall into this regime.…”

Section: Resultsmentioning

confidence: 99%

Tuning Nanoparticle Structure and Surface Strain for Catalysis Optimization

et al. 2014

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Controlling nanoparticle (NP) surface strain, i.e. compression (or stretch) of surface atoms, is an important approach to tune NP surface chemistry and to optimize NP catalysis for chemical reactions. Here we show that surface Pt strain in the core/shell FePt/Pt NPs with Pt in three atomic layers can be rationally tuned via core structural transition from cubic solid solution [denoted as face centered cubic (fcc)] structure to tetragonal intermetallic [denoted as face centered tetragonal (fct)] structure. The high activity observed from the fct-FePt/Pt NPs for oxygen reduction reaction (ORR) is due to the release of the overcompressed Pt strain by the fct-FePt as suggested by quantum mechanics−molecular mechanics (QM−MM) simulations. The Pt strain effect on ORR can be further optimized when Fe in FePt is partially replaced by Cu. As a result, the fct-FeCuPt/Pt NPs become the most efficient catalyst for ORR and are nearly 10 times more active in specific activity than the commercial Pt catalyst. This structure-induced surface strain control opens up a new path to tune and optimize NP catalysis for ORR and many other chemical reactions.

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Section: Resultsmentioning

confidence: 99%

Tuning Nanoparticle Structure and Surface Strain for Catalysis Optimization

et al. 2014

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“…For example, Alfè et al have performed calculations on molten iron with over 1000 atoms which has provided new unique insights about processes taking place in the Earth's core, 35 which can not be obtained by experimental means. Other examples can be found in the work of Nørskov et al who have studied small molecule adsorption on platinum nanoparticles of up to 1500 atoms 90 and in the work of Skylaris and Ruiz-Serrano who have reported calculations on gold nanoparticles with up to 2000 atoms. 44 These three examples have used approaches which minimize the number of O(N 3 ) operations, either the approach of Kresse et al as in VASP and GPAW, in the first two examples, respectively, or the approach of Skylaris et al in the latter example.…”

Section: Discussionmentioning

confidence: 99%

Perspective: Methods for large-scale density functional calculations on metallic systems

Aarons

Sarwar

Thompsett

et al. 2016

The Journal of Chemical Physics

122

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Perspective: Explicitly correlated electronic structure theory for complex systems The Journal of Chemical Physics 146, 080901 (2017) Current research challenges in areas such as energy and bioscience have created a strong need for Density Functional Theory (DFT) calculations on metallic nanostructures of hundreds to thousands of atoms to provide understanding at the atomic level in technologically important processes such as catalysis and magnetic materials. Linear-scaling DFT methods for calculations with thousands of atoms on insulators are now reaching a level of maturity. However such methods are not applicable to metals, where the continuum of states through the chemical potential and their partial occupancies provide significant hurdles which have yet to be fully overcome. Within this perspective we outline the theory of DFT calculations on metallic systems with a focus on methods for large-scale calculations, as required for the study of metallic nanoparticles. We present early approaches for electronic energy minimization in metallic systems as well as approaches which can impose partial state occupancies from a thermal distribution without access to the electronic Hamiltonian eigenvalues, such as the classes of Fermi operator expansions and integral expansions. We then focus on the significant progress which has been made in the last decade with developments which promise to better tackle the lengthscale problem in metals. We discuss the challenges presented by each method, the likely future directions that could be followed and whether an accurate linear-scaling DFT method for metals is in sight. Published by AIP Publishing. [http://dx

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“…In this size regime, particle size effects are often referred to as 'catalytic finite size effects', and small variations in size induce drastic changes in the NP's electronic structure, while quantum effects may become non-negligible (62,63). Following the arguments on stepped surfaces, step and kink atoms of Cu NPs with such low CNs are expected to exhibit stronger chemisorption of CO 2 , CO, atomic H and CO y H x as compared to larger particles or bulk Cu surfaces.…”

Section: R E T R a C T E Dmentioning

confidence: 99%

RETRACTED ARTICLE: An overview of CO₂ electroreduction into hydrocarbons and liquid fuels on nanostructured copper catalysts

Abbas

Ullah

Ali

et al. 2016

Green Chemistry Letters and Reviews

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The increasing atmospheric levels of carbon dioxide (CO 2 ) must be controlled or better reverted to avoid undesirable climate changes. The electrochemical reduction of CO 2 into hydrocarbons is the best approach to solve this problem because it will recycle the 'spent' CO 2 , known as carbon neutral cycle, and will probably be able to remit the energy crises. Nanostructured copper is a novel material known for the efficient and selective reduction of CO 2 into hydrocarbons. This review attempts to summarize the recent development of enlarged surface area nanostructured copper for the efficient reduction of CO 2 into hydrocarbons using renewable energy resources at low overpotentials. The effects of different reaction conditions (e.g. applied potential, CO 2 concentration and electrode surface) on the products and some relationships between these conditions and products are discussed here. Latest achievements in the CO 2 electroreduction technology, remaining challenges and perspective research directions for practical applications are also presented. ARTICLE HISTORY

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Investigation of Catalytic Finite-Size-Effects of Platinum Metal Clusters

Cited by 271 publications

References 27 publications

Tuning Nanoparticle Structure and Surface Strain for Catalysis Optimization

Tuning Nanoparticle Structure and Surface Strain for Catalysis Optimization

Perspective: Methods for large-scale density functional calculations on metallic systems

RETRACTED ARTICLE: An overview of CO₂ electroreduction into hydrocarbons and liquid fuels on nanostructured copper catalysts

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Investigation of Catalytic Finite-Size-Effects of Platinum Metal Clusters

Cited by 271 publications

References 27 publications

Tuning Nanoparticle Structure and Surface Strain for Catalysis Optimization

Tuning Nanoparticle Structure and Surface Strain for Catalysis Optimization

Perspective: Methods for large-scale density functional calculations on metallic systems

RETRACTED ARTICLE: An overview of CO2 electroreduction into hydrocarbons and liquid fuels on nanostructured copper catalysts

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Product

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RETRACTED ARTICLE: An overview of CO₂ electroreduction into hydrocarbons and liquid fuels on nanostructured copper catalysts