A theoretical study of single-atom catalysis of CO oxidation using au embedded 2D h-BN monolayer: A CO-promoted O2 activation

Keke Mao; Lei Li; Wenhua Zhang; Yong Pei; Xiao Cheng Zeng; Xiaojun Wu; Jinlong Yang

doi:10.1038/srep05441

A theoretical study of single-atom catalysis of CO oxidation using au embedded 2D h-BN monolayer: A CO-promoted O₂ activation

Keke Mao, Lei Li, Wenhua Zhang, Yong Pei, Xiao Cheng Zeng, Xiaojun Wu, Jinlong Yang

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

220 Citations (Scopus)

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Abstract

The CO oxidation behaviors on single Au atom embedded in two-dimensional h-BN monolayer are investigated on the basis of first-principles calculations, quantum Born-Oppenheim molecular dynamic simulations (BOMD) and micro-kinetic analysis. We show that CO oxidation on h-BN monolayer support single gold atom prefers an unreported tri-molecular Eley-Rideal (E-R) reaction, where O 2 molecule is activated by two pre-adsorbed CO molecules. The formed OCOAuOCO intermediate dissociates into two CO₂ molecules synchronously, which is the rate-limiting step with an energy barrier of 0.47 eV. By using the micro-kinetic analysis, the CO oxidation following the tri-molecular E-R reaction pathway entails much higher reaction rate (1.43 × 10 5 s1) than that of bimolecular Langmuir-Hinshelwood (L-H) pathway (4.29 s 1). Further, the quantum BOMD simulation at the temperature of 300 K demonstrates the complete reaction process in real time.

Original language	English
Article number	5441
Journal	Scientific Reports
Volume	4
DOIs	https://doi.org/10.1038/srep05441
Publication status	Published - 25 Jun 2014
Externally published	Yes

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title = "A theoretical study of single-atom catalysis of CO oxidation using au embedded 2D h-BN monolayer: A CO-promoted O2 activation",

abstract = "The CO oxidation behaviors on single Au atom embedded in two-dimensional h-BN monolayer are investigated on the basis of first-principles calculations, quantum Born-Oppenheim molecular dynamic simulations (BOMD) and micro-kinetic analysis. We show that CO oxidation on h-BN monolayer support single gold atom prefers an unreported tri-molecular Eley-Rideal (E-R) reaction, where O 2 molecule is activated by two pre-adsorbed CO molecules. The formed OCOAuOCO intermediate dissociates into two CO2 molecules synchronously, which is the rate-limiting step with an energy barrier of 0.47 eV. By using the micro-kinetic analysis, the CO oxidation following the tri-molecular E-R reaction pathway entails much higher reaction rate (1.43 × 10 5 s1) than that of bimolecular Langmuir-Hinshelwood (L-H) pathway (4.29 s 1). Further, the quantum BOMD simulation at the temperature of 300 K demonstrates the complete reaction process in real time.",

author = "Keke Mao and Lei Li and Wenhua Zhang and Yong Pei and Zeng, {Xiao Cheng} and Xiaojun Wu and Jinlong Yang",

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T1 - A theoretical study of single-atom catalysis of CO oxidation using au embedded 2D h-BN monolayer

T2 - A CO-promoted O2 activation

AU - Mao, Keke

AU - Li, Lei

AU - Zhang, Wenhua

AU - Pei, Yong

AU - Zeng, Xiao Cheng

AU - Wu, Xiaojun

AU - Yang, Jinlong

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PY - 2014/6/25

Y1 - 2014/6/25

N2 - The CO oxidation behaviors on single Au atom embedded in two-dimensional h-BN monolayer are investigated on the basis of first-principles calculations, quantum Born-Oppenheim molecular dynamic simulations (BOMD) and micro-kinetic analysis. We show that CO oxidation on h-BN monolayer support single gold atom prefers an unreported tri-molecular Eley-Rideal (E-R) reaction, where O 2 molecule is activated by two pre-adsorbed CO molecules. The formed OCOAuOCO intermediate dissociates into two CO2 molecules synchronously, which is the rate-limiting step with an energy barrier of 0.47 eV. By using the micro-kinetic analysis, the CO oxidation following the tri-molecular E-R reaction pathway entails much higher reaction rate (1.43 × 10 5 s1) than that of bimolecular Langmuir-Hinshelwood (L-H) pathway (4.29 s 1). Further, the quantum BOMD simulation at the temperature of 300 K demonstrates the complete reaction process in real time.

AB - The CO oxidation behaviors on single Au atom embedded in two-dimensional h-BN monolayer are investigated on the basis of first-principles calculations, quantum Born-Oppenheim molecular dynamic simulations (BOMD) and micro-kinetic analysis. We show that CO oxidation on h-BN monolayer support single gold atom prefers an unreported tri-molecular Eley-Rideal (E-R) reaction, where O 2 molecule is activated by two pre-adsorbed CO molecules. The formed OCOAuOCO intermediate dissociates into two CO2 molecules synchronously, which is the rate-limiting step with an energy barrier of 0.47 eV. By using the micro-kinetic analysis, the CO oxidation following the tri-molecular E-R reaction pathway entails much higher reaction rate (1.43 × 10 5 s1) than that of bimolecular Langmuir-Hinshelwood (L-H) pathway (4.29 s 1). Further, the quantum BOMD simulation at the temperature of 300 K demonstrates the complete reaction process in real time.

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