A new strategy for the fabrication of covalent organic framework-metal-organic framework hybrids via in-situ functionalization of ligands for improved hydrogen evolution reaction activity

doi:10.1016/S1872-2067(21)63892-5

Abstract

Abstract:

The development of novel porous materials have attracted significant attention owing to its possible application in several fields. In this study, we designed a novel covalent organic framework-metal-organic framework (COF-MOF) material through an in-situ ligand self-assembly method. The in-situ modified ligands not only act as nucleation sites to form Ti-MOF, but also as a channel to rapidly transfer photogenerated electrons without introducing additional chemical bonds. The photocatalytic hydrogen production rate achieved over B-CTF-Ti-MOF(1:1) was 1975 µmol·g^-1·h^-1 with an apparent quantum efficiency of 4.76%, which is 11.8 times higher than that of the pure CTF-1. In addition, compared with the sample prepared by separating the ligands (CTF-1/Ti-MOF), B-CTF-Ti-MOF shows excellent activity and stability. Finally, a reasonable photocatalytic mechanism was proposed using the results of electrochemical tests and spectral analyses. This study provides a universal method for the construction of highly efficient and stable COF/MOF materials with excellent properties.

Key words: Metal-organic frameworks, Covalent organic frameworks, COF/MOF hybrid, In-situ, Hydrogen evolution

Ling-Ling Zheng, Long-Shuai Zhang, Ying Chen, Lei Tian, Xun-Heng Jiang, Li-Sha Chen, Qiu-Ju Xing, Xiao-Zhen Liu, Dai-She Wu, Jian-Ping Zou. A new strategy for the fabrication of covalent organic framework-metal-organic framework hybrids via in-situ functionalization of ligands for improved hydrogen evolution reaction activity[J]. Chinese Journal of Catalysis, 2022, 43(3): 811-819.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63892-5

https://www.cjcatal.com/EN/Y2022/V43/I3/811

Figures/Tables 6

Scheme 1. Schematic of the B-CTF-Ti-MOF composite preparation process.

Fig. 1. SEM images of CTF-1 (a), Ti-MOF (b), and B-CTF-Ti-MOF (c); (d?f) TEM images of B-CTF-Ti-MOF; C, N, O, and Ti EDS maps (g), HRTEM image (h), and SAED pattern (i) of B-CTF-Ti-MOF.

Fig. 2. XRD patterns (a) and FTIR spectra (b) of Ti-MOF, CTF-1, B-CTF-1, and B-CTF-Ti-MOF; XPS spectra: survey (c), C 1s region (d), O 1s region (e), and Ti 2p region (f) for CTF-1, B-CTF-1, Ti-MOF, and B-CTF-Ti-MOF.

Fig. 3. Photocatalytic H2 production over the as-obtained samples under simulated sunlight irradiation: (a) without co-catalyst; (b) with 3 wt% Pt added as co-catalyst. (c) The wavelength dependence of the H2 evolution rate of B-CTF-Ti-MOF; (d) Recyclability of the H2 evolution over B-CTF-Ti-MOF and CTF-1/Ti-MOF irradiated under simulated sunlight.

Fig. 4. (a) UV-vis DRS spectra of the samples; Steady-state PL spectra (b), time-resolved fluorescence decay spectra (c), and electrochemical impedance spectra (d) of Ti-MOF, B-CTF-1, CTF-1/Ti-MOF, and B-CTF-Ti-MOF.

Scheme 2. Possible photocatalytic mechanism for the H2 evolution reaction over B-CTF-Ti-MOF under light irradiation.

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