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Heterogeneous Catalysis01:22

Heterogeneous Catalysis

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Heterogeneous catalysis involves a catalyst in a different phase from the reactants. It is a process where the catalyst and the reactants are in distinct phases, typically solid and gas or liquid.Most heterogeneous catalysts are metals, metal oxides, or acids. The list includes transition metals like iron (Fe), cobalt (Co), nickel (Ni), palladium (Pd), platinum (Pt), chromium (Cr), manganese (Mn), tungsten (W), silver (Ag), and copper (Cu). These metals possess partially vacant d orbitals that...
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Related Experiment Video

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Multiscale Sampling of a Heterogeneous Water/Metal Catalyst Interface using Density Functional Theory and Force-Field Molecular Dynamics
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Tracking a Common Surface-Bound Intermediate during CO2-to-Fuels Catalysis.

Anna Wuttig1, Can Liu2, Qiling Peng2

  • 1Department of Chemistry, Massachusetts Institute of Technology , Cambridge, Massachusetts 02139, United States.

ACS Central Science
|September 10, 2016
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Understanding carbon monoxide (CO) binding on copper (Cu) surfaces is key for designing efficient CO2-to-fuels electrocatalysts. This study reveals the potential, concentration, and pH dependencies of CO surface populations on Cu under reaction conditions.

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Area of Science:

  • Electrochemistry
  • Surface Science
  • Catalysis

Background:

  • Metallic copper (Cu) is a versatile catalyst for converting carbon dioxide (CO2) into fuels like methane, ethylene, and ethanol.
  • The formation of these products is believed to proceed through a common surface-bound carbon monoxide (CO) intermediate.
  • Understanding the adsorption behavior of this CO intermediate on Cu is crucial for optimizing catalyst selectivity and efficiency.

Purpose of the Study:

  • To directly observe and quantify the surface-bound CO intermediate during CO2 electroreduction on Cu under catalytic conditions.
  • To establish the influence of electrode potential, CO concentration, and electrolyte pH on CO adsorption dynamics.
  • To elucidate the role of CO surface binding equilibria in CO2-to-fuels conversion.

Main Methods:

  • Synthesis of nanostructured Cu films on IR-transparent silicon prisms to enhance infrared absorption.
  • In situ infrared (IR) spectroelectrochemistry to monitor CO adsorption on Cu electrodes during CO2 reduction.
  • Systematic variation of electrode potential, CO concentration, and pH to study adsorption dependencies.

Main Results:

  • Cu surfaces bind electrogenerated CO from CO2 starting at -0.60 V vs RHE, with surface coverage increasing at more negative potentials.
  • Adsorbed CO exists in dynamic equilibrium with dissolved CO and exchanges rapidly under reaction conditions.
  • CO adsorption is pH-independent, but adsorbed CO species undergo a reversible transformation in alkaline electrolytes.

Conclusions:

  • The study establishes the potential, concentration, and pH dependencies of the CO surface population on Cu.
  • These findings provide direct insights into the crucial CO intermediate pool that fuels further reduction to higher-order products.
  • This work facilitates the rational design of more selective and efficient CO2-to-fuels electrocatalysts.