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Nano Research 2023, 16(1): 343-351 https://doi.org/10.1007/s12274-022-4823-3
Research Article | Issue | Published: 10 August 2022

Rational design of graphyne-based dual-atom site catalysts for CO oxidation

Show Author's Information Zhenwei Zhang1,2,  Liang Zhang3,  Xiaoyang Wang4,  Yuan Feng5,  Xiangwen Liu4( ),  Wenming Sun1( )
Department of Chemistry, Beijing Key Laboratory for Optical Materials and Photonic Devices, Capital Normal University, Beijing 100048, China
Linyi Vocational University of Science and Technology (Linyi Institute of Industrial Technology), Linyi 276000, China
Dassault Systemes (Shanghai) Information Technology Co., Ltd., Shanghai 200120, China
Institute of Analysis and Testing, Beijing Academy of Science and Technology (Beijing Center for Physical and Chemical Analysis), Beijing 100094, China
TianHe Supercomputing Center of Huaihai, Linyi 276000, China
Keywords:
single-atom catalyst, density functional theory calculations, CO oxidation, graphyne, dual-atom site catalyst
Topics:
TheoryGrapheneOxidation
Cite this article:
Zhang Z, Zhang L, Wang X, et al. Rational design of graphyne-based dual-atom site catalysts for CO oxidation. Nano Research, 2023, 16(1): 343-351. https://doi.org/10.1007/s12274-022-4823-3
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Abstract Full text Electronic supplementary material About this article

There are increasing concerns about the environmental impact of rising atmospheric carbon monoxide concentrations, thus it is necessary to develop new catalysts for efficient CO oxidation. Based on first-principles calculations, the potential of γ-graphyne (GY) as substrate for metals in the 4th and 5th periods under single-atom and dual-atoms concentration modes has been systematically investigated. It was found that single-atom Co, Ir, Rh, and Ru could effectively oxidate CO molecules, especially for single Rh. Furthermore, proper atoms concentration could boost the CO oxidation activity by supplying more reaction centers, such as Rh2/GY. It was determined that two Rh atoms in Rh2/GY act different roles in the catalytic reaction: one structural and another functional. Screening tests suggest that substituting the structural Rh atom in the center of acetylenic ring by Co or Cu atom is a possible way to maintain the reaction performance while reducing the noble metal cost. This systemic investigation will help in understanding the fundamental reaction mechanisms on GY-based substrates. We emphasize that properly exposed frontier orbital of functional metal atom is crucial in adsorption configuration as well as entire catalytic performance. This study constructs a workflow and provides valuable information for rational design of CO oxidation catalysts.


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Electronic supplementary material
About this article

Rational design of graphyne-based dual-atom site catalysts for CO oxidation

Show Author's information Zhenwei Zhang1,2, Liang Zhang3, Xiaoyang Wang4, Yuan Feng5, Xiangwen Liu4( ), Wenming Sun1( )
Department of Chemistry, Beijing Key Laboratory for Optical Materials and Photonic Devices, Capital Normal University, Beijing 100048, China
Linyi Vocational University of Science and Technology (Linyi Institute of Industrial Technology), Linyi 276000, China
Dassault Systemes (Shanghai) Information Technology Co., Ltd., Shanghai 200120, China
Institute of Analysis and Testing, Beijing Academy of Science and Technology (Beijing Center for Physical and Chemical Analysis), Beijing 100094, China
TianHe Supercomputing Center of Huaihai, Linyi 276000, China

Abstract

There are increasing concerns about the environmental impact of rising atmospheric carbon monoxide concentrations, thus it is necessary to develop new catalysts for efficient CO oxidation. Based on first-principles calculations, the potential of γ-graphyne (GY) as substrate for metals in the 4th and 5th periods under single-atom and dual-atoms concentration modes has been systematically investigated. It was found that single-atom Co, Ir, Rh, and Ru could effectively oxidate CO molecules, especially for single Rh. Furthermore, proper atoms concentration could boost the CO oxidation activity by supplying more reaction centers, such as Rh2/GY. It was determined that two Rh atoms in Rh2/GY act different roles in the catalytic reaction: one structural and another functional. Screening tests suggest that substituting the structural Rh atom in the center of acetylenic ring by Co or Cu atom is a possible way to maintain the reaction performance while reducing the noble metal cost. This systemic investigation will help in understanding the fundamental reaction mechanisms on GY-based substrates. We emphasize that properly exposed frontier orbital of functional metal atom is crucial in adsorption configuration as well as entire catalytic performance. This study constructs a workflow and provides valuable information for rational design of CO oxidation catalysts.

Keywords: single-atom catalyst, density functional theory calculations, CO oxidation, graphyne, dual-atom site catalyst

References(66)

[1]

Liu, Z. P.; Hu, P. CO oxidation and NO reduction on metal surfaces: Density functional theory investigations. Top. Catal. 2004, 28, 71–78.
DOI Google Scholar
[2]

Molina, L. M.; Hammer, B. Active role of oxide support during CO oxidation at Au/MgO. Phys. Rev. Lett. 2003, 90, 206102.
DOI Google Scholar
[3]

Min, B. K.; Friend, C. M. Heterogeneous gold-based catalysis for green chemistry: Low-temperature CO oxidation and propene oxidation. Chem. Rev. 2007, 107, 2709–2724.
DOI Google Scholar
[4]

van Spronsen, M. A.; Frenken, J. W. M.; Groot, I. M. N. Surface science under reaction conditions: CO oxidation on Pt and Pd model catalysts. Chem. Soc. Rev. 2017, 46, 4347–4374.
DOI Google Scholar
[5]

Zhu, P.; Xiong, X.; Wang, D. S. Regulations of active moiety in single atom catalysts for electrochemical hydrogen evolution reaction. Nano Res. 2022, 15, 5792–5815.
DOI Google Scholar
[6]
Zheng, X. B.; Li, B. B.; Wang, Q. S.; Wang, D. S.; Li, Y. D. Emerging low-nuclearity supported metal catalysts with atomic level precision for efficient heterogeneous catalysis. Nano Res., in press, https://doi.org/10.1007/s12274-022-4429-9.
[7]

Jing, H. Y.; Zhu, P.; Zheng, X. B.; Zhang, Z. D.; Wang, D. S.; Li, Y. D. Theory-oriented screening and discovery of advanced energy transformation materials in electrocatalysis. Adv. Powder Mater. 2022, 1, 100013.
DOI Google Scholar
[8]

Li, R. Z.; Wang, D. S. Understanding the structure-performance relationship of active sites at atomic scale. Nano Res., 2022, 15, 6888–6923.
DOI Google Scholar
[9]

Zhang, Z. D.; Zhou, M.; Chen, Y. J.; Liu, S. J.; Wang, H. F.; Zhang, J.; Ji, S. F.; Wang, D. S.; Li, Y. D. Pd single-atom monolithic catalyst: Functional 3D structure and unique chemical selectivity in hydrogenation reaction. Sci. China Mater. 2021, 64, 1919–1929.
DOI Google Scholar
[10]

Huang, C. S.; Li, Y. J.; Wang, N.; Xue, Y. R.; Zuo, Z. C.; Liu, H. B.; Li, Y. L. Progress in research into 2D graphdiyne-based materials. Chem. Rev. 2018, 118, 7744–7803.
DOI Google Scholar
[11]

Zeng, M. Q.; Xiao, Y.; Liu, J. X.; Yang, K. N.; Fu, L. Exploring two-dimensional materials toward the next-generation circuits: From monomer design to assembly control. Chem. Rev. 2018, 118, 6236–6296.
DOI Google Scholar
[12]

Jin, H. Y.; Guo, C. X.; Liu, X.; Liu, J. L.; Vasileff, A.; Jiao, Y.; Zheng, Y.; Qiao, S. Z. Emerging two-dimensional nanomaterials for electrocatalysis. Chem. Rev. 2018, 118, 6337–6408.
DOI Google Scholar
[13]

Gerber, I. C.; Serp, P. A theory/experience description of support effects in carbon-supported catalysts. Chem. Rev. 2020, 120, 1250–1349.
DOI Google Scholar
[14]

Yang, Y. L.; Xu, X. M. Mechanical properties of graphyne and its family-a molecular dynamics investigation. Comput. Mater. Sci. 2012, 61, 83–88.
DOI Google Scholar
[15]

Gu, Y. B.; Chen, X. L.; Cao, Y. Y.; Zhuang, G. L.; Zhong, X.; Wang, J. G. Atomically dispersed Pd catalysts in graphyne nanopore: Formation and reactivity. Nanotechnology 2017, 28, 295403.
DOI Google Scholar
[16]

Shi, H.; Xia, M.; Jia, L. T.; Hou, B.; Wang, Q.; Li, D. B. First principles study on the adsorption and diffusion properties of non-noble (Fe, Co, Ni and Cu) and noble (Ru, Rh, Pt and Pd) metal single atom on graphyne. Chem. Phys. 2020, 536, 110783.
DOI Google Scholar
[17]

He, C. Z.; Wang, R.; Xiang, D.; Li, X. Y.; Fu, L.; Jian, Z. Y.; Huo, J. R.; Li, S. Charge-regulated CO2 capture capacity of metal atom embedded graphyne: A first-principles study. Appl. Surf. Sci. 2020, 509, 145392.
DOI Google Scholar
[18]

Darvishnejad, M. H.; Reisi-Vanani, A. Synergetic effects of metals in graphyne 2D carbon structure for high promotion of CO2 capturing. Chem. Eng. J. 2021, 406, 126749.
DOI Google Scholar
[19]

Srinivasu, K.; Ghosh, S. K. Transition metal decorated graphyne: An efficient catalyst for oxygen reduction reaction. J. Phys. Chem. C 2013, 117, 26021–26028.
DOI Google Scholar
[20]

Ni, Y. X.; Miao, L. C.; Wang, J. Q.; Liu, J. X.; Yuan, M. J.; Chen, J. Pore size effect of graphyne supports on CO2 electrocatalytic activity of Cu single atoms. Phys. Chem. Chem. Phys. 2020, 22, 1181–1186.
DOI Google Scholar
[21]

Wu, P.; Du, P.; Zhang, H.; Cai, C. X. Graphyne-supported single Fe atom catalysts for CO oxidation. Phys. Chem. Chem. Phys. 2015, 17, 1441–1449.
DOI Google Scholar
[22]

Ma, J. P.; Wu, S.; Yuan, Y.; Mao, H.; Lee, J. Y.; Kang, B. T. Graphyne-anchored single Fe atoms as efficient CO oxidation catalysts as predicted by DFT calculations. Phys. Chem. Chem. Phys. 2020, 22, 6004–6009.
DOI Google Scholar
[23]

Ma, D. W.; Li, T. X.; Wang, Q. G.; Yang, G.; He, C. Z.; Ma, B. Y.; Lu, Z. S. Graphyne as a promising substrate for the noble-metal single-atom catalysts. Carbon 2015, 95, 756–765.
DOI Google Scholar
[24]

Talib, S. H.; Hussain, S.; Baskaran, S.; Lu, Z. S.; Li, J. Chromium single-atom catalyst with graphyne support: A theoretical study of NO oxidation and reduction. ACS Catal. 2020, 10, 11951–11961.
DOI Google Scholar
[25]

He, J. J.; Ma, S. Y.; Zhou, P.; Zhang, C. X.; He, C. Y.; Sun, L. Z. Magnetic properties of single transition-metal atom absorbed graphdiyne and graphyne sheet from DFT plus U calculations. J. Phys. Chem. C 2012, 116, 26313–26321.
DOI Google Scholar
[26]

Kim, S.; Ruiz Puigdollers, A.; Gamallo, P.; Viñes, F.; Lee, J. Y. Functionalization of gamma-graphyne by transition metal adatoms. Carbon 2017, 120, 63–70.
DOI Google Scholar
[27]

Kim, S.; Gamallo, P.; Viñes, F.; Lee, J. Y. The nano gold rush: Graphynes as atomic sieves for coinage and Pt-group transition metals. Appl. Surf. Sci. 2020, 499, 143927.
DOI Google Scholar
[28]

Gao, X. P.; Mei, L.; Zhou, Y. N.; Shen, Z. M. Impact of electron transfer of atomic metals on adjacent graphyne layers on electrochemical water splitting. Nanoscale 2020, 12, 7814–7821.
DOI Google Scholar
[29]

Arachchige, L. J.; Xu, Y. J.; Dai, Z. X.; Zhang, X. L.; Wang, F.; Sun, C. H. Theoretical investigation of single and double transition metals anchored on graphyne monolayer for nitrogen reduction reaction. J. Phys. Chem. C 2020, 124, 15295–15301.
DOI Google Scholar
[30]

Cao, Y. Y.; Gao, Y. J.; Zhou, H.; Chen, X. L.; Hu, H.; Deng, S. W.; Zhong, X.; Zhuang, G. L.; Wang, J. G. Highly efficient ammonia synthesis electrocatalyst: Single Ru atom on naturally nanoporous carbon materials. Adv. Theory Simul. 2018, 1, 1800018.
DOI Google Scholar
[31]

Gao, X. P.; Zhou, Y. N.; Tan, Y. J.; Liu, S. Q.; Cheng, Z. W.; Shen, Z. M. Strain effects on Co, N Co-decorated graphyne catalysts for overall water splitting electrocatalysis. Phys. Chem. Chem. Phys. 2020, 22, 2457–2465.
DOI Google Scholar
[32]

Gao, X. P.; Zhou, Y. N.; Liu, S. Q.; Cheng, Z. W.; Tan, Y. J.; Shen, Z. M. Single cobalt atom anchored on N-doped graphyne for boosting the overall water splitting. Appl. Surf. Sci. 2020, 502, 144155.
DOI Google Scholar
[33]

He, T. W.; Matta, S. K.; Du, A. J. Single tungsten atom supported on N-doped graphyne as a high-performance electrocatalyst for nitrogen fixation under ambient conditions. Phys. Chem. Chem. Phys. 2019, 21, 1546–1551.
DOI Google Scholar
[34]

Perdew, J. P.; Wang, Y. Accurate and simple analytic representation of the electron-gas correlation energy. Phys. Rev. B 1992, 45, 13244–13249.
DOI Google Scholar
[35]

Delley, B. Hardness conserving semilocal pseudopotentials. Phys. Rev. B 2002, 66, 155125.
DOI Google Scholar
[36]

Kim, B. G.; Choi, H. J. Graphyne: Hexagonal network of carbon with versatile Dirac cones. Phys. Rev. B 2012, 86, 115435.
DOI Google Scholar
[37]

Govind, N.; Petersen, M.; Fitzgerald, G.; King-Smith, D.; Andzelm, J. A generalized synchronous transit method for transition state location. Comput. Mater. Sci. 2003, 28, 250–258.
DOI Google Scholar
[38]

Wang, X. Y.; Ye, J. M.; Zhang, L.; Bu, Y. X.; Sun, W. M. Strain engineering to tune the performance of CO oxidation on Cu2O(1 1 1) surface: A theoretical study. Appl. Surf. Sci. 2021, 540, 148331.
DOI Google Scholar
[39]

Delley, B. An all-electron numerical method for solving the local density functional for polyatomic molecules. J. Chem. Phys. 1990, 92, 508–517.
DOI Google Scholar
[40]

Delley, B. From molecules to solids with the DMol3 approach. J. Chem. Phys. 2000, 113, 7756–7764.
DOI Google Scholar
[41]

Giannozzi, P.; Baroni, S.; Bonini, N.; Calandra, M.; Car, R.; Cavazzoni, C.; Ceresoli, D.; Chiarotti, G. L.; Cococcioni, M.; Dabo, I. et al. QUANTUM ESPRESSO: A modular and open-source software project for quantum simulations of materials. J. Phys. Condens. Matter 2009, 21, 395502.
DOI Google Scholar
[42]

Giannozzi, P.; Andreussi, O.; Brumme, T.; Bunau, O.; Buongiorno Nardelli, M.; Calandra, M.; Car, R.; Cavazzoni, C.; Ceresoli, D.; Cococcioni, M. et al. Advanced capabilities for materials modelling with quantum ESPRESSO. J. Phys. Condens. Matter 2017, 29, 465901.
DOI Google Scholar
[43]

Perdew, J. P.; Burke, K.; Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 1996, 77, 3865–3868.
DOI Google Scholar
[44]

Garrity, K. F.; Bennett, J. W.; Rabe, K. M.; Vanderbilt, D. Pseudopotentials for high-throughput DFT calculations. Comput. Mater. Sci. 2014, 81, 446–452.
DOI Google Scholar
[45]

Wang, L.; Maxisch, T.; Ceder, G. Oxidation energies of transition metal oxides within the GGA + U framework. Phys. Rev. B 2006, 73, 195107.
DOI Google Scholar
[46]

Marzari, N.; Vanderbilt, D.; De Vita, A.; Payne, M. C. Thermal contraction and disordering of the Al(110) surface. Phys. Rev. Lett. 1999, 82, 3296–3299.
DOI Google Scholar
[47]

Qiao, B. T.; Lin, J.; Wang, A. Q.; Chen, Y.; Zhang, T.; Liu, J. Y. Highly active Au1/Co3O4 single-atom catalyst for CO oxidation at room temperature. Chin. J. Catal. 2015, 36, 1505–1511.
DOI Google Scholar
[48]

Schilling, C.; Ziemba, M.; Hess, C.; Ganduglia-Pirovano, M. V. Identification of single-atom active sites in CO oxidation over oxide-supported Au catalysts. J. Catal. 2020, 383, 264–272.
DOI Google Scholar
[49]

Khan, A. A.; Ullah, R.; Esrafili, M. D.; Ahmad, R.; Ahmad, I. Co anchored B36 cluster as a novel single atom catalyst for removing toxic CO molecules: A mechanistic first-principles study. ChemistrySelect 2022, 7, e202103798.
DOI Google Scholar
[50]

Qin, L.; Cui, Y. Q.; Deng, T. L.; Wei, F. H.; Zhang, X. F. Highly stable and active Cu1/CeO2 single-atom catalyst for CO oxidation: A DFT study. ChemPhysChem 2018, 19, 3346–3349.
DOI Google Scholar
[51]

Lu, Y. B.; Wang, J. M.; Yu, L.; Kovarik, L.; Zhang, X. W.; Hoffman, A. S.; Gallo, A.; Bare, S. R.; Sokaras, D.; Kroll, T. et al. Identification of the active complex for CO oxidation over single-atom Ir-on-MgAl2O4 catalysts. Nat. Catal. 2019, 2, 149–156.
DOI Google Scholar
[52]

Muravev, V.; Spezzati, G.; Su, Y. Q.; Parastaev, A.; Chiang, F. K.; Longo, A.; Escudero, C.; Kosinov, N.; Hensen, E. J. M. Interface dynamics of Pd-CeO2 single-atom catalysts during CO oxidation. Nat. Catal. 2021, 4, 469–478.
DOI Google Scholar
[53]

Qiao, B. T.; Wang, A. Q.; Yang, X. F.; Allard, L. F.; Jiang, Z.; Cui, Y. T.; Liu, J. Y.; Li, J.; Zhang, T. Single-atom catalysis of CO oxidation using Pt1/FeOx. Nat. Chem. 2011, 3, 634–641.
DOI Google Scholar
[54]

Kropp, T.; Lu, Z. L.; Li, Z.; Chin, Y. H. C.; Mavrikakis, M. Anionic single-atom catalysts for CO oxidation: Support-independent activity at low temperatures. ACS Catal. 2019, 9, 1595–1604.
DOI Google Scholar
[55]

DeRita, L.; Dai, S.; Lopez-Zepeda, K.; Pham, N.; Graham, G. W.; Pan, X. Q.; Christopher, P. Catalyst architecture for stable single atom dispersion enables site-specific spectroscopic and reactivity measurements of CO adsorbed to Pt atoms, oxidized Pt clusters, and metallic Pt clusters on TiO2. J. Am. Chem. Soc. 2017, 139, 14150–14165.
DOI Google Scholar
[56]

Han, B.; Li, T. B.; Zhang, J. Y.; Zeng, C. B.; Matsumoto, H.; Su, Y.; Qiao, B. T.; Zhang, T. A highly active Rh1/CeO2 single-atom catalyst for low-temperature CO Oxidation. Chem. Commun. 2020, 56, 4870–4873.
DOI Google Scholar
[57]

Mao, K. K.; Li, L.; Zhang, W. H.; Pei, Y.; Zeng, X. C.; Wu, X. J.; Yang, J. L. A theoretical study of single-atom catalysis of CO oxidation using Au embedded 2D h-BN monolayer: A CO-promoted O2 activation. Sci. Rep. 2014, 4, 5441.
DOI Google Scholar
[58]

Cui, T. T.; Wang, Y. P.; Ye, T.; Wu, J.; Chen, Z. Q.; Li, J.; Lei, Y. P.; Wang, D. S.; Li, Y. D. Engineering dual single-atom sites on 2D ultrathin N-doped carbon nanosheets attaining ultra-low-temperature zinc-air battery. Angew. Chem., Int. Ed. 2022, 61, e202115219.
DOI Google Scholar
[59]

Wang, J.; Huang, Z. Q.; Liu, W.; Chang, C. R.; Tang, H. L.; Li, Z. J.; Chen, W. X.; Jia, C. J.; Yao, T.; Wei, S. et al. Design of N-coordinated dual-metal sites: A stable and active Pt-free catalyst for acidic oxygen reduction reaction. J. Am. Chem. Soc. 2017, 139, 17281–17284.
DOI Google Scholar
[60]

Zhu, X. R.; Yan, J. X.; Gu, M.; Liu, T. Y.; Dai, Y. F.; Gu, Y. H.; Li, Y. F. Activity origin and design principles for oxygen reduction on dual-metal-site catalysts: A combined density functional theory and machine learning study. J. Phys. Chem. Lett. 2019, 10, 7760–7766.
DOI Google Scholar
[61]

Zang, W. J.; Kou, Z. K.; Pennycook, S. J.; Wang, J. Heterogeneous single atom electrocatalysis, where “Singles” are “Married”. Adv. Energy Mater. 2020, 10, 1903181.
DOI Google Scholar
[62]

Han, A. L.; Wang, X. J.; Tang, K.; Zhang, Z. D.; Ye, C. L.; Kong, K. J.; Hu, H. B.; Zheng, L. R.; Jiang, P.; Zhao, C. X. et al. An adjacent atomic platinum site enables single-atom iron with high oxygen reduction reaction performance. Angew. Chem., Int. Ed. 2021, 60, 19262–19271.
DOI Google Scholar
[63]

Zhang, N. Q.; Zhang, X. X.; Kang, Y. K.; Ye, C. L.; Jin, R.; Yan, H.; Lin, R.; Yang, J. R.; Xu, Q.; Wang, Y. et al. A supported Pd2 dual-atom site catalyst for efficient electrochemical CO2 reduction. Angew. Chem., Int. Ed. 2021, 60, 13388–13393.
DOI Google Scholar
[64]
Zheng, X. B.; Yang, J. R.; Xu, Z. F.; Wang, Q. S.; Wu, J. B.; Zhang, E. H.; Dou, S. X.; Sun, W. P.; Wang, D. S.; Li, Y. D. Ru−Co pair sites catalyst boosts the energetics for the oxygen evolution reaction. Angew. Chem., in press, https://doi.org/10.1002/ange.202205946.
[65]

Chatt, J.; Duncanson, L. A. 586. Olefin co-ordination compounds. Part III. Infra-red spectra and structure:Attempted preparation of acetylene complexes. J. Chem. Soc. 1953, 2939–2947.
DOI Google Scholar
[66]

Chatt, J.; Duncanson, L. A.; Venanzi, L. M. Directing effects in inorganic substitution reactions. Part I. A hypothesis to explain the trans-effect. J. Chem. Soc. 1955, 4456–4460.
DOI Google Scholar
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Publication history
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Acknowledgements

Publication history

Received: 16 June 2022
Revised: 21 July 2022
Accepted: 22 July 2022
Published: 10 August 2022
Issue date: January 2023

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© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 22101029 and 21703219), Beijing Municipal Natural Science Foundation (No. 2222006), Beijing Municipal Financial Project BJAST Scholar Programs B (No. BS202001), and Beijing Municipal Financial Project BJAST Young Scholar Programs B (No. YS202202). The authors acknowledge computational resources of TianHe-1A supercomputer at the National Supercomputing Center in Tianjin and technical support from Tianhe Supercomputing Center of Huaihai.

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