Synthesis of thin film AuPd alloys and their investigation for electrocatalytic CO<sub>2</sub>reduction

Hahn, Christopher; Abram, David N.; Hansen, Heine Anton; Hatsukade, Toru; Jackson, Ariel; Johnson, Nathalie Weier; Hellstern, Thomas R.; Kuhl, Kendra P.; Cave, Etosha R.; Feaster, Jeremy T.; Jaramillo, Thomas F.

doi:10.1039/c5ta04863j

Cited by 121 publications

(122 citation statements)

References 28 publications

(35 reference statements)

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“…Hahn et al. employed electron‐beam deposition techniques to prepare Au‐Pd alloy thin films with varying atomic compositions and demonstrated that the alloys showed improved selectivities for HCOO − compared to either Au or Pd . Another level of control over the selectivity of CO 2 reduction could be achieved by growing thin Pd layers at Au surfaces.…”

Section: Introductionsupporting

confidence: 76%

Electrochemical Reduction of Carbon Dioxide at Gold‐Palladium Core–Shell Nanoparticles: Product Distribution versus Shell Thickness

et al. 2016

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The electrocatalytic reduction of CO2 at carbon-supported Au-Pd core-shell nanoparticles is systematically investigated as a function of Pd shell thickness. Liquid and gas phase products were determined by off-line 1 H NMR and on-line electrochemical mass spectrometry (OLEMS). Our results uncover the relationship between the nature of products generated and the Pd shell thickness. CO and H2 are the only products generated at 1 nm thick shells, while shells of 5 and 10 nm produced HCOO -, CH4 and C2H6. The concentration of HCOO -detected in the electrolyte was dependent on the applied potential, reaching a maximum Faradaic efficiency of 27% at -0.5 V vs. RHE for 10 nm thick shells. We conclude that collisions between absorbed hydrogen at relaxed Pd lattices and strongly bound "COlike" intermediates promote the complete hydrogenation to C1 and C2 alkanes, without the generation of other products such as alcohols and aldehydes.

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Section: Introductionsupporting

confidence: 76%

Electrochemical Reduction of Carbon Dioxide at Gold‐Palladium Core–Shell Nanoparticles: Product Distribution versus Shell Thickness

et al. 2016

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“…10 However, their implementation at an industrial scale is unsustainable and has limitations owing to the scarcity of noble metals. [7][8][9][10] Previous studies by Hori and coworkers have demonstrated that Cu is unique compared with other metals in its ability to produce hydrocarbons at potentials more negative than −1 V vs RHE. 11 Nevertheless, the large overpotential renders the process inefficient.…”

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confidence: 99%

Cu–Sn Bimetallic Catalyst for Selective Aqueous Electroreduction of CO₂ to CO

et al. 2016

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ABSTRACT. We report a selective and stable electrocatalyst utilizing non-noble metals consisting of Cu and Sn for the efficient and selective reduction of CO 2 to CO over a wide potential range. The bimetallic electrode was prepared through the electrodeposition of Sn species on the surface of oxide-derived copper (OD-Cu). The Cu surface, when decorated with an optimal amount of Sn, resulted in a Faradaic efficiency (FE) for CO greater than 90% and a current density of −1.0 mA cm −2 at −0.6 V vs. RHE, compared to the CO FE of 63% and −2.1 mA cm −2 for OD-Cu. Excess Sn on the surface caused H 2 evolution with a decreased current density. X-ray diffraction (XRD) suggests the formation of Cu-Sn alloy. Auger electron spectroscopy of the sample surface exhibits zero-valent Cu and Sn after the electrodeposition step. Density functional theory (DFT) calculations show that replacing a single Cu atom with a Sn atom leaves the d-band orbitals mostly unperturbed, signifying no dramatic shifts in the bulk electronic structure. However, the Sn atom discomposes the multi-fold sites on pure Cu, Page 1 of 37 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 2 disfavoring the adsorption of H and leaving the adsorption of CO relatively unperturbed. Our catalytic results along with DFT calculations indicate that the presence of Sn on reduced OD-Cu diminishes the hydrogenation capability-i.e., the selectivity towards H 2 and HCOOH-while hardly affecting the CO productivity. While the pristine monometallic surfaces (both Cu and Sn) fail to selectively reduce CO 2 , the Cu-Sn bimetallic electrocatalyst generates a surface that inhibits adsorbed H*, resulting in improved CO FE. This study presents a strategy to provide a low-cost non-noble metals that can be utilized as a highly selective electrocatalyst for the efficient aqueous reduction of CO 2 . ACS Paragon Plus Environment ACS Catalysis

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“…Indeed, the effects of alloying are shown to take advantage of the electronic and geometric effects of the individual metals to create synergistic effects. For instance, Au and Pd are known to be selective for the generation of only CO during CO 2 RR but Au–Pd alloy is capable of generating formate with 10% FE . Similarly, a Pt–Pd alloy was reported to demonstrate a very high FE HCOO − of 88% at −0.4 V …”

Section: Active Sites In Metal‐based Catalystsmentioning

confidence: 99%

A Disquisition on the Active Sites of Heterogeneous Catalysts for Electrochemical Reduction of CO₂ to Value‐Added Chemicals and Fuel

Daiyan

Saputera

Masood

et al. 2020

Advanced Energy Materials

128

104

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Renewable‐electricity‐powered electrocatalytic CO2 reduction reactions (CO2RR) have been identified as an emerging technology to address the issue of rising CO2 emissions in the atmosphere. While the CO2RR has been demonstrated to be technically feasible, further improvements in catalyst performance through active sites engineering are a prerequisite to accelerate its commercial feasibility for utilization in large CO2‐emitting industrial sources. Over the years, the improved understanding of the interaction of CO2 with the active sites has allowed superior catalyst design and subsequent attainment of prominent CO2RR activity in literature. This review tracks the evolution of the understanding of CO2RR active sites on different electrocatalysts such as metals, metal‐oxides, single atoms, metal‐carbon, and subsequently metal‐free carbon‐based catalysts. Despite the tremendous research efforts in the field, many scientific questions on the role of various active sites in governing CO2RR activity, selectivity, stability, and pathways are still unanswered. These gaps in knowledge are highlighted and a discussion is set forth on the merits of utilizing advanced in‐situ and operando characterization techniques and machine learning (ML). Using this technique, the underlying mechanisms can be discerned, and as a result new strategies for designing active sites may be uncovered. Finally, this review advocates an interdisciplinary approach to discover and design CO2RR active sites (rather than focusing merely on catalyst activity) in a bid to stimulate practical research for industrial application.

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Synthesis of thin film AuPd alloys and their investigation for electrocatalytic CO₂reduction

Abstract: Alloying of Au and Pd leads to new synergistic catalytic effects, providing insights into electrocatalytic CO2 reduction on alloy surfaces.

Cited by 121 publications

References 28 publications

Electrochemical Reduction of Carbon Dioxide at Gold‐Palladium Core–Shell Nanoparticles: Product Distribution versus Shell Thickness

Electrochemical Reduction of Carbon Dioxide at Gold‐Palladium Core–Shell Nanoparticles: Product Distribution versus Shell Thickness

Cu–Sn Bimetallic Catalyst for Selective Aqueous Electroreduction of CO₂ to CO

A Disquisition on the Active Sites of Heterogeneous Catalysts for Electrochemical Reduction of CO₂ to Value‐Added Chemicals and Fuel

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Synthesis of thin film AuPd alloys and their investigation for electrocatalytic CO2reduction

Abstract: Alloying of Au and Pd leads to new synergistic catalytic effects, providing insights into electrocatalytic CO2 reduction on alloy surfaces.

Cited by 121 publications

References 28 publications

Electrochemical Reduction of Carbon Dioxide at Gold‐Palladium Core–Shell Nanoparticles: Product Distribution versus Shell Thickness

Electrochemical Reduction of Carbon Dioxide at Gold‐Palladium Core–Shell Nanoparticles: Product Distribution versus Shell Thickness

Cu–Sn Bimetallic Catalyst for Selective Aqueous Electroreduction of CO2 to CO

A Disquisition on the Active Sites of Heterogeneous Catalysts for Electrochemical Reduction of CO2 to Value‐Added Chemicals and Fuel

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Product

Resources

About

Synthesis of thin film AuPd alloys and their investigation for electrocatalytic CO₂reduction

Cu–Sn Bimetallic Catalyst for Selective Aqueous Electroreduction of CO₂ to CO

A Disquisition on the Active Sites of Heterogeneous Catalysts for Electrochemical Reduction of CO₂ to Value‐Added Chemicals and Fuel