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Theoretical studies of MXene-supported single-atom catalysts: Os1/Ti2CS2 for low-temperature CO oxidation

MXene负载的锇单原子催化剂Os1/Ti2CS2催化低温 CO氧化反应的理论研究

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Abstract

We report herein a new sulfur-functionalized MXene Ti2C (Ti2CS2)-supported osmium-metal single-atom catalyst (SAC) Os1/Ti2CS2 with high low-temperature catalytic activity for CO oxidation. Using periodic density functional theory calculations, the most stable SAC, Os1/Ti2CS2, has been screened from a series of group 8–11 transition metal SACs M1/Ti2CS2 (M = Fe, Co, Ni, Cu; Ru, Rh, Pd, Ag; Os, Ir, Pt, Au). The calculations show that it is favorable for O2 and CO to be coadsorbed on the Os1 single atom (SA) of Os1/Ti2CS2 and the adsorption energy of the first O2 molecule is slightly higher than that of CO. Moreover, the termolecular co-adsorption of O2 + 2CO on Os1 SA is also possible, which is favorable for CO oxidation on Os1 SA through a novel three-molecule reaction mechanism. Accordingly, four different catalytic mechanisms, the Langmuir-Hinshelwood (L-H), Eley-Rideal (E-R), termolecular Langmuir-Hinshelwood-A (TLH-A) and termolecular Langmuir-Hinshelwood-B (TLH-B), are systematically studied for CO oxidation by O2 on Os1/Ti2CS2. The theoretical studies indicate that the TLH-B mechanism is the most feasible for CO oxidation with the reaction barrier energy of only 0.74 eV, which is far lower than for L-H, E-R and TLH-A with barrier energies of 1.06, 1.09 and 1.47 eV, respectively. The results provide fundamental understanding to the surface chemistry of MXene and designing new sulfur-functionalized two-dimensional MXene catalytic nanomaterials.

摘要

本文报道了一种对CO氧化反应具有低温催化活性的新型硫功能 化MXene-Ti2C (Ti2CS2)负载的锇金属单原子催化剂Os1/Ti2CS2. 通过密 度泛函理论计算, 从一系列过渡金属(M = Fe, Co, Ni, Cu; Ru, Rh, Pd, Ag; Os, Ir, Pt, Au)中筛选出最稳定的锇金属单原子催化剂. 计算结果表 明, Os1/Ti2CS2有利于O2和CO的共吸附, 且O2分子的吸附能略高于CO 分子. 此外, 由于O2+2CO能稳定地共吸附在Os1单原子上, CO氧化反应 可能通过三分子反应机理进行. 因此, 我们研究了CO在Os1/Ti2CS2单原 子催化剂上发生氧化反应的四种不同的催化机理: Langmuir-Hinshelwood (L–H)、Eley Rideal (E–R)、termolecular Langmuir-Hinshelwood-A (TLH-A)和termolecular Langmuir-Hinshelwood-B (TLH-B)机 理. 结果表明TLH-B机理最可能发生, 其反应势垒仅为0.74 eV, 远低于 L–H、E–R和TLH-A的反应势垒(分别为1.06, 1.09和1.47 eV). 上述研究 结果有助于理解MXene的表面化学并设计稳定的新型二维硫端基 MXene催化材料.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (21963005, 21763006, 22033005 and 22038002), the Natural Science Foundation of Guizhou University ([2021]40 and [2020] 32) and Guangdong Provincial Key Laboratory of Catalysis (2020B121201002). The calculations were performed by using supercomputers at SUSTech and Shanghai Supercomputing Center. The authors are grateful to Dr. Yafei Jiang for discussion.

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Authors and Affiliations

  1. School of Chemistry and Chemical Engineering, Guizhou University, Guiyang, 550025, China

    Yang Meng  (孟洋), Jin-Xia Liang  (梁锦霞) & Chun Zhu  (朱纯)

  2. Department of Chemistry, Southern University of Science and Technology, Shenzhen, 518055, China

    Chun Zhu  (朱纯), Cong-Qiao Xu  (许聪俏) & Jun Li  (李隽)

  3. Department of Chemistry and Key Laboratory of Organic Optoelectronics & Molecular Engineering of Ministry of Education, Tsinghua University, Beijing, 100084, China

    Jun Li  (李隽)

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Contributions

Li J directed the research. Zhu C, Liang JX and Meng Y conducted the DFT calculations. Zhu C, Liang JX, Xu CQ and Meng Y analyzed the data. All the authors discussed the results and co-wrote the manuscript.

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Correspondence to Chun Zhu  (朱纯) or Jun Li  (李隽).

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The authors declare that they have no conflict of interest.

Supplementary information

See supplementary material for the way of oxygen-terminated Ti2C, the different adsorption sites of metal single atoms on Os1/Ti2CS2, as well as the optimized geometry of Ir1/Ti2CS2. In addition, the optimized stable structures and the calculated relative energies of different molecule adsorption on Os1/Ti2CS2 SAC are also available in the online version of the paper.

Yang Meng is a PhD candidate at the School of Chemistry and Chemical Engineering, Guizhou University, under the supervision of Prof. Chun Zhu. Her research focuses on the theoretical investigations on single-atom catalysts.

Chun Zhu received his PhD degree from the College of Chemistry and Chemical Engineering, Xiamen University in 2013, under the supervision of Prof. Zexing Cao. He worked as a visiting scholar at the Department of Chemistry and the Department of Biochemistry and Molecular Biology, Michigan State University from 2017 to 2018. He was also a visiting scholar at the Department of Chemistry, Southern University of Science and Technology. He is now a professor at the School of Chemistry and Chemical Engineering, Guizhou University. His research interests focus on the theoretical chemistry, organometallic chemistry, and computational catalysis science.

Jun Li received his PhD degree from Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences in 1992. He did postdoctoral research at the University of Siegen (Germany) and The Ohio State University (USA) from 1994 to 1997. He worked as a Research Scientist at The Ohio State University and a Senior Research Scientist and Chief Scientist at the Pacific Northwest National Laboratory (USA) from 1997 to 2009. He is now a full professor at Tsinghua University. His research involves theoretical chemistry, relativistic heavy-element chemistry, and computational catalysis science.

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Meng, Y., Liang, JX., Zhu, C. et al. Theoretical studies of MXene-supported single-atom catalysts: Os1/Ti2CS2 for low-temperature CO oxidation. Sci. China Mater. 65, 1303–1312 (2022). https://doi.org/10.1007/s40843-021-1950-0

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