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Triazine COF-supported single-atom catalyst (Pd1/trzn-COF) for CO oxidation

三嗪-共价有机框架材料负载的单原子催化剂Pd1/trzn-COF催化CO氧化的理论研究

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Abstract

Single-atom catalysts (SACs) with well-defined and specific single-atom dispersion on supports offer great potential for achieving both high catalytic activity and selectivity. Covalent organic frameworks (COFs) with tailor-made crystalline structures and designable atomic composition is a class of promising supports for SACs. Herein, we have studied the binding sites and stability of Pd single atoms (SAs) dispersed on triazine COF (Pd1/trzn-COF) and the reaction mechanism of CO oxidation using the density functional theory (DFT). By evaluating different adsorption sites, including the nucleophilic sp2 C atoms, heteroatoms and the conjugated π-electrons of aromatic ring and triazine, it is found that Pd SAs can stably combine with trzn-COF with a binding energy around −5.0 eV, and there are two co-existing dynamic Pd1/trzn-COFs due to the adjacent binding sites on trzn-COF. The reaction activities of CO oxidation on Pd1/trzn-COF can be regulated by the anion-π interaction between a + δ phenyl center and the related −δ moieties as well as the electron-withdrawing feature of imine in the specific complexes. The Pd1/trzn-COF catalyst is found to have a high catalytic activity for CO oxidation via a plausible tri-molecular Eley-Rideal (TER) reaction mechanism. This work provides insights into the d-π interaction between Pd SAs and trzn-COF, and helps to better understand and design new SACs supported on COF nanomaterials.

摘要

共价有机框架材料(COF)是一类新兴的可裁剪、 原子组成可控的催化剂载体. 单原子催化剂(SACs)具有明确的活性中心结构和原子组成, 为同时满足催化剂的高活性和高选择性提供可能, 并为催化剂的实验和理论的高契合度研究提供桥梁. 因此, 本论文采用密度泛函理论(DFT), 系统研究了以典型三嗪-共价有机框架材料为载体的钯单原子催化剂(Pd1/trzn-COF)的金属负载位点、 稳定性和反应活性. 基于sp2 C原子、 N/O杂原子和芳香环与三嗪环的共轭π电子的亲核性, 一系列不同的吸附位点被用于负载Pd原子, 研究结果表明Pd原子以约−5.0 eV的结合能稳定地结合在该COF材料上; 基于两个最稳定构型间的位置毗邻性、 能量相近性及其温和的迁移能垒, 可以预测该体系中存在动态共存的单原子催化位点. 此外, CO氧化机理研究表明, Pd1/trzn-COF的催化活性可通过特定−δ基团与+δ苯环中心的阴离子−π相互作用以及亚胺基团的吸电子特性进行调控. 我们设计了一种新型的单原子催化剂Pd1/trzn-COF, 并预测了其可能的CO氧化反应机理为三分子Eley-Rideal机理. 该工作揭示了Pd原子与trzn-COF之间的d−π相互作用 模式对于单原子催化剂Pd1/trzn-COF的稳定性和反应活性的影响, 其研究结果有助于理解和设计基于COF的新型单原子催化剂.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (22033005, 21590792 and 21763006), and Guangdong Provincial Key Laboratory of Catalysis (2020B121201002). The calculations were performed using supercomputers at SUSTech and Tsinghua National Laboratory for Information Science and Technology. We thank Professor Xufeng Lin (hatrick2009@upc.edu.cn) for helpful discussion during the preparation of the manuscript.

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Authors and Affiliations

  1. State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum (East China), Qingdao, 266580, China

    Yin-Juan Chen  (陈银娟), Yuan Pan  (潘原) & Chen-Guang Liu  (刘晨光)

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

    Yin-Juan Chen  (陈银娟), Hong-Ying Zhuo  (卓红英) & Jun Li  (李隽)

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

    Jin-Xia Liang  (梁锦霞) & Jun Li  (李隽)

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  1. Yin-Juan Chen  (陈银娟)
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Contributions

Author contributions Li J directed the research. Liang JX, Liu CG and Chen YJ conducted the DFT calculations. Chen YJ, Zhuo HY, and Pan Y analyzed the data. All the authors discussed the results and co-wrote the manuscript.

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Correspondence to Jin-Xia Liang  (梁锦霞), Chen-Guang Liu  (刘晨光) or Jun Li  (李隽).

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Conflict of interest The authors declare no competing financial interest.

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Yin-Juan Chen is currently a PhD candidate in Prof. Chen-Guang Liu’s group at China University of Petroleum (East China), and also a visiting student in Prof. Jun Li’s group, Department of Chemistry, Tsinghua University (Beijing, China). Her current research interests focus on theoretical investigations on heterogeneous single-atom catalysts (SACs).

Jin-Xia Liang received her BSc degree from the Department of Chemistry at Shaanxi University of Technology in 2004, MS degree from the School of Chemistry and Chemical Engineering at Shaanxi Normal University in 2009, and PhD degree from the College of Chemistry and Chemical Engineering at Xiamen University in 2012. She did her postdoctoral research at the Department of Chemistry, Tsinghua University. She joined the faculty of Guizhou Provincial Key Laboratory of Computational Nano Material Science, Guizhou Education University in 2014. She is currently a research associate professor at the Department of Chemistry, Southern University of Science and Technology. Her research interests focus on the theoretical design of functional nanomaterials and investigation of catalytic mechanisms of SACs.

Chen-Guang Liu received his PhD degree in 1991 in applied chemistry at China University of Petroleum. He is now a professor in the State Key Laboratory of Heavy Oil Processing and College of Chemical Engineering at China University of Petroleum. His current research interests include petrochemistry, petroleum refining and chemical engineering, green fine chemical technology and renewable energy and oxygen-containing fuel applications.

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 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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Chen, YJ., Zhuo, HY., Pan, Y. et al. Triazine COF-supported single-atom catalyst (Pd1/trzn-COF) for CO oxidation. Sci. China Mater. 64, 1939–1951 (2021). https://doi.org/10.1007/s40843-021-1662-8

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