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 O2 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) s(-1)) 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.
authors: 1] Key Lab of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, Anhui 230026, China [2] Hefei National Lab for Physical Sciences at Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China.
authors: Keke
authors: K
authors: Mao
authors: Department of Chemistry and Department Mechanics and Materials Engineering, University of Nebraska-Lincoln, Lincoln, NE 68588, USA.
authors: Lei
authors: L
authors: Li
authors: 1] Key Lab of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, Anhui 230026, China [2] Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China.
authors: Wenhua
authors: W
authors: Zhang
authors: Department of Chemistry, Xiangtan University, Hunan 411105, China.
authors: Yong
authors: Y
authors: Pei
authors: Department of Chemistry and Department Mechanics and Materials Engineering, University of Nebraska-Lincoln, Lincoln, NE 68588, USA.
authors: Xiao Cheng
authors: XC
authors: Zeng
authors: 1] Key Lab of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, Anhui 230026, China [2] Hefei National Lab for Physical Sciences at Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China [3] Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China.
authors: Xiaojun
authors: X
authors: Wu
authors: 1] Hefei National Lab for Physical Sciences at Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China [2] Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China.
authors: Jinlong
authors: J
authors: Yang