Volume 35 Issue 4
Aug.  2022
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Ting-Ting Liu, Xin-Ping Wu, Xue-Qing Gong. Substituent Effects on the Photocatalytic Properties of a Symmetric Covalent Organic Framework[J]. Chinese Journal of Chemical Physics , 2022, 35(4): 647-654. doi: 10.1063/1674-0068/cjcp2205088
Citation: Ting-Ting Liu, Xin-Ping Wu, Xue-Qing Gong. Substituent Effects on the Photocatalytic Properties of a Symmetric Covalent Organic Framework[J]. Chinese Journal of Chemical Physics , 2022, 35(4): 647-654. doi: 10.1063/1674-0068/cjcp2205088

Substituent Effects on the Photocatalytic Properties of a Symmetric Covalent Organic Framework

doi: 10.1063/1674-0068/cjcp2205088
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  • Corresponding author: Xin-Ping Wu, E-mail: xpwu@ecust.edu.cn; Xue-Qing Gong, E-mail: xgong@ecust.edu.cn
  • Received Date: 2022-05-13
  • Accepted Date: 2022-06-14
  • Publish Date: 2022-08-27
  • Symmetric covalent organic framework (COF) photocatalysts generally suffer from inefficient charge separation and short-lived photoexcited states. By performing density functional theory (DFT) and time-dependent density functional theory (TDDFT) calculations, we find that partial substitution with one or two substituents (N or NH$_2$) in the linkage of the representative symmetric COF (N$_0$-COF) gives rise to the separation of charge carriers in the resulting COFs (\emph{i.e}., N$_1$-COF, N$_2$-COF, (NH$_2$)$_1$-N$_0$-COF, and (NH$_2$)$_2$-N$_0$-COF). Moreover, we also find that the energy levels of the highest occupied crystal orbital (HOCO) and the lowest unoccupied crystal orbital (LUCO) of the N$_0$-COF can shift away from or toward the vacuum level, depending on the electron-withdrawing or electron-donating characters of the substituent. Therefore, we propose that partial substitution with carefully chosen electron-withdrawing or electron-donating substituents in the linkages of symmetric COFs can lead to efficient charge separation as well as appropriate HOCO and LUCO positions of the generated COFs for specific photocatalytic reactions. The proposed rule can be utilized to further boost the photocatalytic performance of many symmetric COFs.

     

  • Part of Special Topic "the 1st Young Scientist Symposium on Computational Catalysis".
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  • [1]
    A. P. Côté, A. I. Benin, N. W. Ockwig, M. O'Keeffe, A. J. Matzger, and O. M. Yaghi, Science. 310, 1166 (2005). doi: 10.1126/science.1120411
    [2]
    C. S. Diercks and O. M. Yaghi, Science 355, 1585 (2017). doi: 10.1126/science.aal1585
    [3]
    S. Y. Ding and W. Wang, Chem. Soc. Rev. 42, 548 (2013). doi: 10.1039/C2CS35072F
    [4]
    R. Chen, J. L. Shi, Y. Ma, G. Lin, X. Lang, and C. Wang, Angew. Chem. Int. Ed. 58, 6430 (2019). doi: 10.1002/anie.201902543
    [5]
    Q. Fang, S. Gu, J. Zheng, Z. Zhuang, S. Qiu, and Y. Yan, Angew. Chem. Int. Ed. 53, 2878 (2014). doi: 10.1002/anie.201310500
    [6]
    J. L. Shi, R. Chen, H. Hao, C. Wang, and X. Lang, Angew. Chem. Int. Ed. 59, 9088 (2020). doi: 10.1002/anie.202000723
    [7]
    H. Wang, H. Wang, Z. Wang, L. Tang, G. Zeng, P. Xu, M. Chen, T. Xiong, C. Zhou, X. Li, D. Huang, Y. Zhu, Z. Wang, and J. Tang, Chem. Soc. Rev. 49, 4135 (2020). doi: 10.1039/D0CS00278J
    [8]
    H. Fan, A. Mundstock, A. Feldhoff, A. Knebel, J. Gu, H. Meng, and J. Caro, J. Am. Chem. Soc. 140, 10094 (2018). doi: 10.1021/jacs.8b05136
    [9]
    X. Y. Liu, J. He, J. X. Yu, Z. X. Li, and Z. Q. Fan, Chin. Phys. B 23, 067303 (2014). doi: 10.1088/1674-1056/23/6/067303
    [10]
    E. Vitaku, C. N. Gannett, K. L. Carpenter, L. Shen, H. D. Abruna, and W. R. Dichtel, J. Am. Chem. Soc. 142, 16 (2020). doi: 10.1021/jacs.9b08147
    [11]
    J. Li, X. Jing, Q. Li, S. Li, X. Gao, X. Feng, and B. Wang, Chem. Soc. Rev. 49, 3565 (2020). doi: 10.1039/D0CS00017E
    [12]
    P. Pachfule, S. Kandambeth, D. D. Diaz, and R. Banerjee, Chem. Commun. 50, 3169 (2014). doi: 10.1039/C3CC49176E
    [13]
    Z. Fu, X. Wang, A. M. Gardner, X. Wang, S. Y. Chong, G. Neri, A. J. Cowan, L. Liu, X. Li, A. Vogel, R. Clowes, M. Bilton, L. Chen, R. S. Sprick, and A. I. Cooper, Chem. Sci. 11, 543 (2020). doi: 10.1039/C9SC03800K
    [14]
    W. Liu, X. Li, C. Wang, H. Pan, W. Liu, K. Wang, Q. Zeng, R. Wang, and J. Jiang, J. Am. Chem. Soc. 141, 17431 (2019). doi: 10.1021/jacs.9b09502
    [15]
    T. Banerjee, F. Haase, G. Savasci, K. Gottschling, C. Ochsenfeld, and B. V. Lotsch, J. Am. Chem. Soc. 139, 16228 (2017). doi: 10.1021/jacs.7b07489
    [16]
    W. Chen, L. Wang, D. Mo, F. He, Z. Wen, X. Wu, H. Xu, and L. Chen, Angew. Chem. Int. Ed. 59, 16902 (2020). doi: 10.1002/anie.202006925
    [17]
    X. Wang, L. Chen, S. Y. Chong, M. A. Little, Y. Wu, W. H. Zhu, R. Clowes, Y. Yan, M. A. Zwijnenburg, R. S. Sprick, and A. I. Cooper, Nat. Chem. 10, 1180 (2018). doi: 10.1038/s41557-018-0141-5
    [18]
    X. Song, Y. Wu, X. Zhang, X. Li, Z. Zhu, C. Ma, Y. Yan, P. Huo, and G. Yang, Chem. Eng. J. 408, 127292 (2021). doi: 10.1016/j.cej.2020.127292
    [19]
    L. Li, D. Yin, and X. Guo, New J. Chem. 45, 15789 (2021). doi: 10.1039/D1NJ03133C
    [20]
    G. Li, Z. Xie, Q. Wang, X. Chen, Y. Zhang, and X. Wang, Chem. Eur. J. 27, 939 (2021). doi: 10.1002/chem.202003856
    [21]
    V. S. Vyas, F. Haase, L. Stegbauer, G. Savasci, F. Podjaski, C. Ochsenfeld, and B. V. Lotsch, Nat. Commun. 6, 8508 (2015). doi: 10.1038/ncomms9508
    [22]
    L. Li, Z. B. Fang, D. Weng, J. D. Yi, R. Wang, and T. F. Liu, CCS Chem. 3, 2839 (2021).
    [23]
    A. A. Zhang, X. Cheng, X. Heng, W. Liu, S. Deng, R. Cao, and T. F. Liu, Research 2021, 9874273 (2021).
    [24]
    D. Kresse and J. Furthmüller, Comput. Mater. Sci. 6, 15 (1996). doi: 10.1016/0927-0256(96)00008-0
    [25]
    P. E. Blochl, Phys. Rev. B 50, 17953 (1994). doi: 10.1103/PhysRevB.50.17953
    [26]
    J. P. Perdew, A. Ruzsinszky, G. I. Csonka, O. A. Vydrov, G. E. Scuseria, L. A. Constantin, X. Zhou, and K. Burke, Phys. Rev. Lett. 100, 136406 (2008). doi: 10.1103/PhysRevLett.100.136406
    [27]
    S. Grimme, J. Comput. Chem. 27, 1787 (2006). doi: 10.1002/jcc.20495
    [28]
    A. V. Krukau, O. A. Vydrov, A. F. Izmaylov, and G. E. Scuseria, J. Chem. Phys. 125, 224106 (2006). doi: 10.1063/1.2404663
    [29]
    X. P. Wu, L. Gagliardi, and D. G. Truhlar, J. Am. Chem. Soc. 140, 7904 (2018). doi: 10.1021/jacs.8b03613
    [30]
    X. P. Wu, L. Gagliardi, and D. G. Truhlar, J. Chem. Phys. 150, 041701 (2019). doi: 10.1063/1.5043538
    [31]
    X. P. Wu and D. G. Truhlar, ACS Symp. Ser. 1331, 309 (2019).
    [32]
    M. J. Frisch, G. W. Trucks, H. B. Schlegel, G. E. Scuseria, M. A. Robb, J. R. Cheeseman, G. Scalmani, V. Barone, G. A. Petersson, H. Nakatsuji, X. Li, M. Caricato, V. A. Marenich, J. Bloino, B. G. Janesko, R. Gomperts, B. Mennucci, H. P. Hratchian, J. V. Ortiz, A. F. Izmaylov, J. L. Sonnenberg, F. Ding, F. Lipparini, F. Egidi, J. Goings, B. Peng, A. Petrone, T. Henderson, D Ranasinghe, V. G. Zakrzewski, J. Gao, N. Rega, G. Zheng, W. Liang, M. Hada, M. Ehara, K. Toyota, R. Fukuda, J. Hasegawa, M. Ishida, T. Nakajima, Y. Honda, O. Kitao, H. Nakai, T. Vreven, K. Throssell, J. A. Montgomery, J. E. Peralta, F. Ogliaro, M. J. Bearpark, J. J. Heyd, E. N. Brothers, K. N. Kudin, V. N. Staroverov, T. A. Keith, R. Kobayashi, J. Normand, K. Raghavachari, A. P. Rendell, J. C. Burant, S. S. Iyengar, J. Tomasi, M. Cossi, J. M. Millam, M. Klene, C. Adamo, R. Cammi, J. W. Ochterski, R. L. Martin, K. Morokuma, O. Farkas, J. B. Foresman, and D. J. Fox, Gaussian 16, Wallingford, CT: Gaussian Inc., (2016).
    [33]
    S. Grimme, J. Antony, S. Ehrlich, and H. Krieg, J. Chem. Phys. 132, 154104 (2010). doi: 10.1063/1.3382344
    [34]
    F. J. Weigend, Phys. Chem. Chem. Phys. 8, 1057 (2006). doi: 10.1039/b515623h
    [35]
    Z. Liu, T. Lu, and Q. Chen, Carbon 165, 461 (2020). doi: 10.1016/j.carbon.2020.05.023
    [36]
    Z. Liu and F. Chen, J. Comput. Chem. 33, 580 (2012). doi: 10.1002/jcc.22885
    [37]
    C. Zhang, X. Wang, and H. J. Huang, J. Am. Chem. Soc. 130, 8359 (2008). doi: 10.1021/ja800712e
    [38]
    W. Chen, P. Chen, D. Chen, Y. Liu, G. Zhang, L. Wang, and L. Chen, Adv. Sci. 9, 2105517 (2022). doi: 10.1002/advs.202105517
    [39]
    X. P. Wu, I. Choudhuri, and D. G. Truhlar, Energy Environ. Mater. 2, 251 (2019). doi: 10.1002/eem2.12051
    [40]
    T. T. Liu, X. P. Wu, and X. Q. Gong, J. Phys. Energy 3, 034016 (2021). doi: 10.1088/2515-7655/abf41b
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