Colloidal Platinum–Copper Nanocrystal Alloy Catalysts Surpass Platinum in Low-Temperature Propene Combustion

Tahsini, Nadia; Yang, An‐Chih; Streibel, Verena; Werghi, Baraa; Goodman, Emmett D.; Aitbekova, Aisulu; Bare, Simon R.; Li, Yuejin; Abild‐Pedersen, Frank; Cargnello, Matteo

doi:10.1021/jacs.1c10248

Cited by 41 publications

(34 citation statements)

References 56 publications

(80 reference statements)

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“…The alloyed Cu-Rh phase obtained after annealing at 800 °C had higher activity for CO oxidation compared to its initial core-shell structure. The effect of alloying Cu and a noble metal on catalytic properties has been reported in previous work. , Complex synergetic effects can potentially explain the increased activity of alloyed Cu-Rh.…”

Section: Results and Discussionmentioning

confidence: 99%

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Synthesis and Characterization of Core-Shell Cu-Ru, Cu-Rh, and Cu-Ir Nanoparticles

et al. 2022

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Optimizing the use of expensive precious metals is critical to developing sustainable and low-cost processes for heterogeneous catalysis or electrochemistry. Here, we report a synthesis method that yields core-shell Cu-Ru, Cu-Rh, and Cu-Ir nanoparticles with the platinum-group metals segregated on the surface. The synthesis of Cu-Ru, Cu-Rh, and Cu-Ir particles allows maximization of the surface area of these metals and improves catalytic performance. Furthermore, the Cu core can be selectively etched to obtain nanoshells of the platinum-group metal components, leading to a further increase in the active surface area. Characterization of the samples was performed with X-ray absorption spectroscopy, X-ray powder diffraction, and ex situ and in situ transmission electron microscopy. CO oxidation was used as a reference reaction: the three core-shell particles and derivatives exhibited promising catalyst performance and stability after redox cycling. These results suggest that this synthesis approach may optimize the use of platinum-group metals in catalytic applications.

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Section: Results and Discussionmentioning

confidence: 99%

“…The effect of alloying Cu and a noble metal on catalytic properties has been reported in previous work. 54,55 Complex synergetic effects can potentially explain the increased activity of alloyed Cu-Rh. The results for the three core-shell particles confirm the presence of exposed precious metals, with no Cu layer covering the catalysts.…”

Section: Resultsmentioning

confidence: 99%

Synthesis and Characterization of Core-Shell Cu-Ru, Cu-Rh, and Cu-Ir Nanoparticles

et al. 2022

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“…Some of the present authors have recently demonstrated the promise of this second approach for propene combustion by alloying Pt with the cheaper base metal Cu. 74 In this study, we show that, while monometallic Cu adsorbs O* more strongly than monometallic Pt (adsorption on Cu is stronger by 0.4 eV), adding moderate amounts of Cu (<50 at. %) into Pt actually slightly weakens the oxygen binding strength on the surface by 0.1 eV.…”

Section: ■ Results and Discussionmentioning

confidence: 57%

Microkinetic Modeling of Propene Combustion on a Stepped, Metallic Palladium Surface and the Importance of Oxygen Coverage

et al. 2022

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Better emission control of internal combustion engines can be achieved by more efficient catalytic hydrocarbon combustion at low temperatures. For a knowledge-based design of suitable catalyst candidates, a promising approach integrates theoretical models with experimental benchmarks. Studying catalytic hydrocarbon combustion theoretically is challenging, however, since hydrocarbon reaction networks are complex: even simple C2 combustion reactions include hundreds of possible elementary steps. Herein, we present a paradigm to address this challenge by (1) supplementing experimental insights with extensive density functional theory studies to derive a proxy combustion reaction network; (2) using machine learning-enhanced transition state search to rigorously scan reaction coordinates; and (3) combining ab initio thermodynamics, microkinetic modeling, and a degree of rate control analysis to unveil adsorbate coverage effects and rate-limiting reaction steps. Our systematic approach permits modeling a reaction as complex as propene combustion on palladium while maintaining the computationally efficient mean-field approximation. Using a partially oxygen-covered palladium surface model, which includes adsorbate–adsorbate interactions, we predict experimentally measured rates within 2 orders of magnitude without parameter fitting. The corresponding degree of rate control analysis yields that the second and penultimate dehydrogenation step in the reaction network limit the rate of propene combustion on palladium.

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“…32 This is also consistent with previous publications as Cu is not considered an efficient catalyst for CO oxidation. 41,42,43 .…”

Section: Resultsmentioning

confidence: 99%

Synthesis and Characterization of Stable Cu-Pt Nanoparticles under Reductive and Oxidative Conditions

Foucher

Yang

Rosen

et al. 2023

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We report a synthesis method for highly monodisperse Cu-Pt alloy nanospheres. Small and large Cu-Pt particles with a Cu:Pt ratio of 1:1 can be obtained through colloidal synthesis at 300 °C. The fresh particles have a Pt-rich surface and a Cu-rich core and can be converted into an intermetallic phase after annealing at 800 °C under H2. First, we demonstrated the stability of fresh particles under redox conditions at 400 °C, as the Pt-rich surface prevents substantial oxidation of Cu. Then, a combination of in situ scanning transmission electron microscopy, in situ X-ray absorption spectroscopy, and CO oxidation measurements of the intermetallic CuPt phase before and after redox treatments at 800 °C showed promising activity and stability for CO oxidation. Full oxidation of Cu was prevented after exposure to O2 at 800 °C. The activity and structure of the particles was only slightly changed after exposure to O2 at 800 °C and were recovered after re-reduction at 800 °C. Additionally, the intermetallic CuPt phase showed enhanced catalytic properties compared to the fresh particles with a Pt-rich surface or pure Pt particles of the same size. Thus, the incorporation of Pt with Cu does not lead to a rapid deactivation and degradation of the material, as seen with other bimetallic systems. This work provides a synthesis route to control the design of Cu-Pt nanostructures and underlines the promising properties of these alloys (intermetallic and non-intermetallic) for heterogeneous catalysis.

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Colloidal Platinum–Copper Nanocrystal Alloy Catalysts Surpass Platinum in Low-Temperature Propene Combustion

Cited by 41 publications

References 56 publications

Synthesis and Characterization of Core-Shell Cu-Ru, Cu-Rh, and Cu-Ir Nanoparticles

Synthesis and Characterization of Core-Shell Cu-Ru, Cu-Rh, and Cu-Ir Nanoparticles

Microkinetic Modeling of Propene Combustion on a Stepped, Metallic Palladium Surface and the Importance of Oxygen Coverage

Synthesis and Characterization of Stable Cu-Pt Nanoparticles under Reductive and Oxidative Conditions

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