CO oxidation on MXene (Mo2CS2) supported single-atom catalyst: A termolecular Eley-Rideal mechanism

Talib，Shamraiz Hussain1,2; Lu，Zhansheng1; Bashir，Beenish3; Hussain，Sajjad4; Ahmad，Khalil5; Khan，Salahuddin6; Haider，Sajjad7; Yang，Zongxian1; Hermansson，Kersti8; Li，Jun2,9

2023-02-01

10.1016/j.cclet.2022.04.010

Chinese Chemical Letters   影响因子和分区

1001-8417

1878-5964

Finding transition metal catalysts for effective catalytic conversion of CO to CO has attracted much attention. MXene as a new 2D layered material of early transition metal carbides, nitrides, and carbo-nitrides is a robust support for achoring metal atoms. In this study, the electronic structure, geometries, thermodynamic stability, and catalytic activity of MXene (MoCS) supported single noble metal atoms (NM = Ru, Rh, Pd, Ir, Pt and Au) have been systematically examined using first-principles calculations and ab initio molecular dynamic (AIMD) simulations. First, AIMD simulations and phonon spectra demonstrate the dynamic and thermal stabilities of MoCS monolayer. Three likely reaction pathways, Langmuir-Hinshelwood (LH), Eley-Rideal (ER), and Termolecular Eley–Rideal (TER) for CO oxidation on the Ru- and Ir@MoCS SACs, have been studied in detail. It is found that CO oxidation mainly proceeds via the TER mechanism under mild reaction conditions. The corresponding rate-determining steps are the dissociation of the intermediate (OCO-Ru-OCO) and formation of OCO-Ir-OCO intermediate. The downshift d-band center of Ru- and Ir@MoCS help to enhance activity and improve catalytst stability. Moreover, a microkinetic study predicts a maximum CO oxidation rate of 4.01 × 10 s and 4.15 × 10 s (298.15 K) following the TER pathway for the Ru- and Ir@MoCS catalysts, respectively. This work provides guideline for fabricating and designing highly efficient SACs with superb catalyts using MXene materials.

2D MXene monolayer CO oxidation M1@Mo2CS2 Quantum chemical study Single-atom catalysis Termolecular Eley–Rideal

SCI

英语

通讯

National Natural Science Foundation of China["11874141","22033005"] ; Henan Over-seas Expertise Introduction Center for Discipline Innovation[CXJD2019005] ; Guangdong Provincial Key Laboratory of Catalysis[2020B121201002] ; King Saud University, Riyadh, Saudi Arabia[RSP-2021/399]

Chemistry

Chemistry, Multidisciplinary

WOS:000916110700001

ELSEVIER SCIENCE INC

CHEMISTRY

2-s2.0-85133955318

Scopus

1.School of Physics,Henan Normal University,Xinxiang,453007,China
2.Department of Chemistry and Key Laboratory of Organic Optoelectronics & Molecular Engineering of Ministry of Education,Tsinghua University,Beijing,100084,China
3.Department of Materials Science and Engineering,Southern University of Science and Technology,Shenzhen,518055,China
4.School of Chemistry,Minhaj University,Lahore,54000,Pakistan
5.Department of Chemistry,Mirpur University of Science and Technology (MUST),Mirpur,AJK,10250,Pakistan
6.College of Engineering,King Saud University,Riyadh,PO Box 800,11421,Saudi Arabia
7.Chemical Engineering Department,College of Engineering,King Saud University,Riyadh,PO Box 800,11421,Saudi Arabia
8.Department of Chemistry-Ångström,Uppsala University,Uppsala,Box 538,75121,Sweden
9.Department of Chemistry,Southern University of Science and Technology,Shenzhen,518055,China

Talib，Shamraiz Hussain,Lu，Zhansheng,Bashir，Beenish,et al. CO oxidation on MXene (Mo2CS2) supported single-atom catalyst: A termolecular Eley-Rideal mechanism[J]. Chinese Chemical Letters,2023,34(2).

Talib，Shamraiz Hussain.,Lu，Zhansheng.,Bashir，Beenish.,Hussain，Sajjad.,Ahmad，Khalil.,...&Li，Jun.(2023).CO oxidation on MXene (Mo2CS2) supported single-atom catalyst: A termolecular Eley-Rideal mechanism.Chinese Chemical Letters,34(2).

Talib，Shamraiz Hussain,et al."CO oxidation on MXene (Mo2CS2) supported single-atom catalyst: A termolecular Eley-Rideal mechanism".Chinese Chemical Letters 34.2(2023).