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Lijun Xiong, Dandan Zhu, Chenglong Qiu, Weihong Zeng, Mingshi Xu, Shanshan Wang, Yong Yang. Metal-free C(CN)3 cooperated with Co-Ti dual sites in bimetallic CoTi-MOF as a tandem photocatalyst for highly efficient C2H4 production. Green Energy&Environment. doi: 10.1016/j.gee.2025.12.019
Citation: Lijun Xiong, Dandan Zhu, Chenglong Qiu, Weihong Zeng, Mingshi Xu, Shanshan Wang, Yong Yang. Metal-free C(CN)3 cooperated with Co-Ti dual sites in bimetallic CoTi-MOF as a tandem photocatalyst for highly efficient C2H4 production. Green Energy&Environment. doi: 10.1016/j.gee.2025.12.019
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Metal-free C(CN)3 cooperated with Co-Ti dual sites in bimetallic CoTi-MOF as a tandem photocatalyst for highly efficient C2H4 production

doi: 10.1016/j.gee.2025.12.019

  • a. School of Biomedical and Pharmaceutical Engineering, Hefei Institute of Technology, Hefei 238076, China;

  • b. School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, China

Funds:

This work was supported by the National Natural Science Foundation of China (51303083), the National Natural Science Foundation of China for Excellent Young Scholars (51922050), the Natural Science Foundation of Jiangsu Province (BK20191293), and the Fundamental Research Funds for the Central Universities (30920021123).

  • Received date 17 September 2025, Accepted date 30 December 2025, RevRecd date 22 November 2025, Available online 06 January 2026
    Abstract
  • The photocatalytic reduction of carbon dioxide (CO2) into high-value C2+ hydrocarbons represents a sustainable pathway to alleviate energy shortages and reduce atmospheric CO2 levels. In this study, a unique tandem photocatalyst (CoTi-CN), is constructed by integrating bimetallic CoTi-MOF with metal-free half-metallic C(CN)3. This composite demonstrates markedly enhanced activity and selectivity in the photocatalytic CO2 reduction to ethylene (C2H4), achieving a C2H4 selectivity of 36.8% and a generation yield of 31.3 μmol g−1 over 5 h. Density functional theory (DFT) calculations combined with in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) analysis reveal that C(CN)3 acts as an efficient CO2 to CO converter, while CoTi-MOF favors the adsorption and C-C coupling of *CO intermediates. The spatially decoupled CO generation and C-C coupling processes lead to optimized intermediate coverage and reduced energy barriers, resulting in superior selectivity toward multi-carbon products. This work opens new horizons for the design of tandem photocatalysts that combine half-metallic catalysts with bimetallic MOFs, achieving a significant enhancement in the activity and selectivity of photocatalytic C2H4 production.

     

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    • References(59)
  • [1]
    L. Guo, J. Sun, Q. Ge, N. Tsubaki, J. Mater. Chem. A. 6 (2018) 23244−23262.
    [2]
    J. Wang, C. Yang, L. Mao, X. Cai, Z. Geng, H. Zhang, J. Zhang, X. Tan, J. Ye, T. Yu, Adv. Funct. Mater. 33 (2023) 2213901.
    [3]
    Z. Zhao, H. Zhu, J. Huang, P. Liao, X. Chen, ACS Catal. 12 (2022) 7986−7993.
    [4]
    Y. Hori, H. Wakebe, T. Tsukamoto, O. Koga, Electrochim. Acta. 39 (1994) 1833−1839.
    [5]
    A. Bagger, W. Ju, A. S. Varela, P. Strasser, J. Rossmeisl, ChemPhysChem. 18 (2017) 3266−3273.
    [6]
    G. Jia, Y. Zhang, JC. Yu, Z. Guo, Adv. Mater. 36 (2024) 2403153.
    [7]
    J. Huang, M. Mensi, E. Oveisi, V. Mantella, R. Buonsanti, J. Am. Chem. Soc. 141(2019) 2490-2499.
    [8]
    H. Liang, T. Beweries, R. Francke, M. Beller, Angew. Chem., Int. Ed. 134 (2022) e202200723.
    [9]
    C. Chen, Y. Li, S. Yu, S. Louisia, J. Jin, M. Li, M. B. Ross, P. Yang, Joule. 4 (2020) 1688−1699.
    [10]
    J. Liu, T. Liu, P. Du, L. Zhang, J. Lei, Angew. Chem. Int. Ed. 58 (2019) 7808−7812.
    [11]
    J. Zhang, W. He, T. Quast, J. R. C. Junqueira, S. Saddeler, S. Schulz, W. Schuhmann, Angew. Chem. Int. Ed. 62 (2023) e202214830.
    [12]
    J. Ge, P. Yin, Y. Chen, H. Cheng, J. Liu, B. Chen, C. Tan, P. Yin, H. Zheng, Q. Li, S. Chen, W. Xu, X. Wang, G. Wu, R. Sun, X. Shan, X. Hong, H. Zhang, Adv Mater. 33 (2021) 2006711.
    [13]
    F. Hu, L. Yang, Y. Jiang, C. Duan, X. Wang, L. Zeng, X. Lv, D. Duan, Q. Liu, T. Kong, J. Jiang, R. Long, Y. Xiong, Angew. Chem. Int. Ed. 60 (2021) 26122−26127.
    [14]
    M. B. Ross, P. De Luna, Y. Li, C. T. Dinh, D. Kim, P. Yang, E. H. Sargent, Nature Catal. 2 (2019) 648−658.
    [15]
    L. R. L. Ting, O. Pique, S. Y. Lim, M. Tanhaei, F. Calle-Vallejo, B. S. Yeo, ACS Catal. 10 (2020) 4059−4069.
    [16]
    K. Yang, Y. Sun, S. Chen, M. Li, M. Zheng, L. Ma, W. Fan, Y. Zheng, Q. Li, J. Duan, Small. 19 (2023) 2301536.
    [17]
    D. Ren, J. Gao, L. Pan, Z. Wang, J. Luo, S. M. Zakeeruddin, A. Hagfeldt, M. Gratzel, Angew. Chem. Int. Ed. 58 (2019) 15036−15040.
    [18]
    F. Li, Y. Li, Z. Wang, J. Li, D. H. Nam, Y. Lum, M. Luo, X. Wang, A. Ozden, S. F. Hung, B. Chen, Y. Wang, J. Wicks, Y. Xu, Y. Li, C. M. Gabardo, C. T. Dinh, Y. Wang, T. Zhuang, D. Sinton, E. H. Sargent, Nature Catal. 3 (2020) 75−82.
    [19]
    J. Jiao, R. Lin, S. Liu, W. C. Cheong, C. Zhang, Z. Chen, Y. Pan, J. Tang, K. Wu, S. F. Hung, H. Chen, L. Zheng, Q. Lu, X. Yang, B. Xu, H. Xiao, J. Li, D. Wang, Q. Peng, C. Chen, Y. Li, Nature Chem. 11 (2019) 222−228.
    [20]
    J. Gao, H. Zhang, X. Guo, J. Luo, S. M. Zakeeruddin, D. Ren, M. Gratzel, J. Am. Chem. Soc. 141 (2019) 18704-18714.
    [21]
    H. Zhang, X. Chang, J. Chen, W. A Goddard III, B. Xu, M. J Cheng, Q. Lu, Nat. Commun. 10 (2019) 3340.
    [22]
    K. Sun, Y. Qian, H. Jiang, Angew. Chem. Int. Ed. 62 (2023) e202217565.
    [23]
    D. H. Nam, O. Shekhah, G. H. Lee, A. Mallick, H. Jiang, F. Li, B. Chen, J. Wicks, M. Eddaoudi, E. H. Sargent, J. Am. Chem. Soc. 142 (2020) 21513−21521.
    [24]
    J. S. Lee, X. Wang, H. Luo, S. Dai, Adv. Mater. 22 (2010) 1004−1007.
    [25]
    L. Liu, C. Zhao, H. Zhao, D. Pitts, Y. Li, Chem. Commun. 49 (2013) 3664−3666.
    [26]
    G. Zhou, Y. Shan, Y. Hu, X. Xu, L. Long, J. Zhang, J. Dai, J. Guo, J. Shen, S. Li, L. Liu, X. Wu, Nature Commun. 9 (2018) 3366.
    [27]
    Y. Yang, Z. Tang, B. Zhou, J. Shen, H. He, A. Ali, Q. Zhong, Y. Xiong, C. Gao, A. Alsaedi, Appl. Catal. B: Environ. 264 (2020) 118470.
    [28]
    L. Xiong. Y. Yang. Q. Deng. W. Dong. X. Zhang. J. Shen, Carbon. 218 (2023) 118715.
    [29]
    J. Dong, J. Zhao, X. Yan, L. Li, G. Liu, M. Ji, B. Wang, Y. She, H. Li, J. Xia, Appl. Catal. B: Environ. 351 (2024) 123993.
    [30]
    Q. Chen, S. Li, H. Xu, G. Wang, Y. Qu, P. Zhu, D. Wang, Chin. J. Catal. 41 (2020) 514−523.
    [31]
    P. Qiu, Y. Yao, S. Lu, L. Chen, Y. Chen, X. Liao, Fuel. 351 (2023) 129043.
    [32]
    M. Li, J. Yuan, G. Wang, L. Yang, J. Shao, H. Li, J. Lu, Sep. Purif. Technol. 298 (2022) 121658.
    [33]
    Y. Zhang, J. Luan, P. Li, L. Jiang, H. Yan, W. Liu, Z. Yan, Carbon. 228 (2024) 119430.
    [34]
    M. Zhang, J. Li, R. Wang, S. Zhao, S. Zang, T. C. W. Mak, Adv. Mater. 8 (2021) 2101884.
    [35]
    Y. Fu, T. Huang, L. Zhang, J. Zhu, X. Wang, Nanoscale. 7 (2015) 13723−13733.
    [36]
    P. Qiu, Y. Yao, S. Lu, L. Chen, Y. Chen, X. Liao, Fuel. 351 (2023) 129043.
    [37]
    X. Chen, X. Peng, L. Jiang, X. Yuan, J. Fei, W. Zhang, Chem. Engin. J. 427 (2022) 130945.
    [38]
    P. Karthik, A. R. M. Shaheer, A. Vinu, B. Neppolian, Small. 16 (2020) 1902990.
    [39]
    J. Jin, P. Li, D. Chun, B. Jin, K. Zhang, J. H. Park, Adv. Funct. Mater. 31 (2021) 2102511.
    [40]
    Y. Li, J. Tian, Z. Liu, Z. Liu, D. Dong, F. Wang, W. Wang, M. Liu, J. Dan, Y. Li, F. Yu, B. Dai, Y. Yu, Green Energy Environ. 8 (2023) 1102-1116.
    [41]
    M. Z. Hussain, Z. Yang, A. M. E. Khalil, S. Hussain, S. U. Awan, Q. Jia, R. A. Fischer, Y. Zhu, Y. Xia, J. Mater. Sci. Technol. 101 (2022) 49−59.
    [42]
    L. Jing, M. Xie, Y. Xu, C. Tong, X. Du, H. Zhao, N. Zhong, H. Li, J. Hu, Green Energy Environ. 9 (2024) 1159-1170.
    [43]
    F. Zelenak, M. Kovacova, Z. Moravec, M. Cernak, R. Krumpolec, Carbon. 215 (2023) 118436.
    [44]
    Y. Luo, A. Serrano-Lotina, F. F. Budihardjo, S. Taghipour, S. A. Ferdousi, L. Li, J. J. Delgado, A. Lopez-Buendia, R. Portela, W. Han, M. A. Banares, K. L. Yeung, Chem. Engin. J. 466 (2023) 143254.
    [45]
    M. Lan, R. Guo, Y. Dou, J. Zhou, A. Zhou, J. Li, Nano Energy. 33 (2017) 238−246.
    [46]
    L. Sun, C. Liu, J. Li, Y. Zhou, H. Wang, P. Huo, C. Ma, Y. Yan, Chin. J. Catal. 40 (2019) 80−94.
    [47]
    Y. Wu, Z. Liu, Y. Li, J. Chen, X. Zhu, P. Na, Chin. J. Catal. 40 (2019) 60−69.
    [48]
    X. Yang, F. Qian, G. Zou, M. Li, J. Lu, Y. Li, M. Bao, Appl. Catal. B: Environ. 193 (2016) 22−35.
    [49]
    J. Dong, Y. Zhang, L. Liu, X. Zhang, L. Li, G. Liu, H. Li, P. Yan, J. Xia, Chem. Commun. 61 (2025) 7125-7128.
    [50]
    S. Cao, B. Shen, T. Tong, J. Fu, J. Yu, Adv. Funct. Mater. 28 (2018) 1800136.
    [51]
    R. Zhang, H. Wang, S. Tang, C. Liu, F. Dong, H. Yue, B. Liang, ACS Catal. 8 (2018) 9280−9286.
    [52]
    W. Gao, S. Li, H. He, X. Li, Z. Cheng, Y. Yang, J. Wang, Q. Shen, X. Wang, Y. Xiong, Y. Zhou, Nature Commun. 12 (2021) 4747.
    [53]
    Y. Cao, L. Guo, M. Dan, D. E. Doronkin, C. Han, Z. Rao, Y. Liu, J. Meng, Z. Huang, K. Zheng, P. Chen, F. Dong, Y. Zhou, Nature Commun. 12 (2021) 1675.
    [54]
    J. Xu, Z. Ju, W. Zhang, Y. Pan, J. Zhu, J. Mao, X. Zheng, H. Fu, M. Yuan, H. Chen, R. Li, Angew. Chem. Int. Ed. 60 (2021) 8705−8709.
    [55]
    J. Hao, D. Yang, J. Wu, B. Ni, L. Wei, Q. Xu, Y. Min, H. Li, Chem. Engin. J. 423 (2021) 130190.
    [56]
    A. Du, S. Sanvito, S. C. Smith, Phys. Rev. Lett. 108 (2012) 197207.
    [57]
    Y. Liu, Y. Liu, Z. Yao, Z. Yu, H. Zhu, C. Xing, Y. Wang, X. Tan, Y. Huang, Y. Hou, S. Wang, Appl. Catal. B: Environ. 371 (2025) 125275.
    [58]
    P. Chen, B. Lei, X. Dong, H. Wang, J. Sheng, W. Cui, J. Li, Y. Sun, Z. Wang, F. Dong, ACS Nano. 14 (2020) 15841−15852.
    [59]
    Y. Shi, J. Li, C. Mao, S. Liu, X. Wang, X. Liu, S. Zhao, X. Liu, Y. Huang, L. Zhang, Nature Commun.12 (2021) 5923.
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