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Scalable Syntheses of Graphene Oxide and Reduced Graphene Oxide using Cascade Design Oxidation and Highly Basic Reduction Reactions

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First Principles Study on the CO Oxidation on Mn-Embedded Divacancy Graphene.

Quanguo Jiang¹, Jianfeng Zhang¹, Zhimin Ao²

¹College of Mechanics and Materials, Hohai University, Nanjing, China.

Frontiers in Chemistry

|June 19, 2018

Summary

Manganese-embedded divacancy graphene (Mn-DG) demonstrates excellent catalytic activity for carbon monoxide (CO) oxidation. This noble-metal-free catalyst efficiently oxidizes CO at low temperatures via the Langmuir-Hinshelwood mechanism.

Keywords:

CO oxidation Mn-embedded divacancy first principles calculations graphene

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Area of Science:

Materials Science
Catalysis
Computational Chemistry

Background:

Carbon monoxide (CO) oxidation is crucial in many chemical processes.
Developing efficient, low-cost catalysts is essential for industrial applications.
Graphene-based materials offer unique properties for catalysis.

Purpose of the Study:

To investigate the CO oxidation mechanism on transition metal-embedded divacancy graphene (DG).
To identify the most effective transition metal for enhancing catalytic activity.
To elucidate the role of electronic structure in catalytic performance.

Main Methods:

First-principles calculations were employed to study CO oxidation.
The Langmuir-Hinshelwood (LH) and Eley-Rideal (ER) mechanisms were considered.
Hirshfeld charge analysis was used to understand charge transfer dynamics.

Main Results:

Oxygen (O2) adsorption was favored on Sc, Ti, V, Cr, Mn, and Fe-DG, preventing CO poisoning.
Manganese-embedded divacancy graphene (Mn-DG) exhibited superior catalytic properties.
The CO oxidation on Mn-DG proceeds via the LH mechanism with a low energy barrier of 0.41 eV.

Conclusions:

Mn-DG is a highly efficient, noble-metal-free catalyst for CO oxidation.
Charge transfer from the embedded Mn atom to adsorbed molecules is key to catalytic activity.
This catalyst shows promise for low-temperature CO oxidation applications.