Stability and Catalytic Performance of Single-Atom Supported on Ti2CO2 for Low-Temperature CO Oxidation: A First-Principles Study

Ali，Sajjad1; Xie，Zijuan1,2; Xu，Hu1,3,4

2021

10.1002/cphc.202100436

CHEMPHYSCHEM   影响因子和分区

1439-4235

1439-7641

Based on first-principles calculations, the potential of TiCO monolayer (MXene) as a single-atom catalyst (SAC) support for 3d transition metal (TM) atoms (Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, and Zn) is studied for CO oxidation. We first screen the support effect according to the stability of a single metal atom and find that Sc and Ti supported on TiCO have stronger adsorption energy than the cohesive energy of their bulk counterparts and therefore, we selected Sc and Ti supported on TiCO for further catalytic reactions. The stability and the potential catalytic reactivity are verified by electronic structure and charge transfer analysis. Both Eley−Rideal (ER) and Langmuir−Hinshelwood (LH) mechanisms are considered in this study, and lower energy barriers of 0.002 and 0.37 eV were found in the ER mechanism compared to the LH mechanism, which are 0.25 and 0.34 eV for Sc and Ti catalysts, respectively. Moreover, kinetic ER and LH mechanisms are favorable for both Sc- and Ti/TiCO because of the comparable energy barrier to other metals and SAC supported on 2D materials. However, Ti/TiCO catalyst is thermodynamically unfavorable. Based on these calculations, we propose that Sc supported on TiCO is the best catalyst for CO-oxidation. The current study not only broadens the scope of the single-atom Sc catalyst but also extends the consideration of MXene support for catalyst optimization.

CO-oxidation density functional calculations MXene single-atom catalyst stability

SCI ; EI

英语

第一 ; 通讯

WOS:000700115200001

20213910954850

Atoms ; Calculations ; Catalysis ; Catalyst supports ; Catalytic oxidation ; Charge transfer ; Electronic structure ; Energy barriers ; Monolayers ; Temperature ; Titanium ; Titanium compounds

Air Pollution Control:451.2 ; Titanium and Alloys:542.3 ; Thermodynamics:641.1 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Mathematics:921 ; Atomic and Molecular Physics:931.3

CHEMISTRY

2-s2.0-85115699180

Scopus

1.Department of Physics,Southern University of Science and Technology,Shenzhen,518055,China
2.Institute for Quantum Science and Engineering,Southern University of Science and Technology,Shenzhen,518055,China
3.Guangdong Provincial Key Laboratory of Computational Science and Material Design,Southern University of Science and Technology,Shenzhen,518055,China
4.Shenzhen Key Laboratory of for Advanced Quantum Functional Materials and Devices,Southern University of Science and Technology,Shenzhen,518055,China

Ali，Sajjad,Xie，Zijuan,Xu，Hu. Stability and Catalytic Performance of Single-Atom Supported on Ti2CO2 for Low-Temperature CO Oxidation: A First-Principles Study[J]. CHEMPHYSCHEM,2021,22:2352-2361.

Ali，Sajjad,Xie，Zijuan,&Xu，Hu.(2021).Stability and Catalytic Performance of Single-Atom Supported on Ti2CO2 for Low-Temperature CO Oxidation: A First-Principles Study.CHEMPHYSCHEM,22,2352-2361.

Ali，Sajjad,et al."Stability and Catalytic Performance of Single-Atom Supported on Ti2CO2 for Low-Temperature CO Oxidation: A First-Principles Study".CHEMPHYSCHEM 22(2021):2352-2361.