Precisely decorating CdS on Zr-MOFs through pore functionalization strategy: A highly efficient photocatalyst for H2 production

doi:10.1016/S1872-2067(21)63949-9

Abstract

Abstract:

Different materials, such as metal sulphides, are often combined with metal-organic frameworks (MOFs) to develop multi-functional composites and improve their photocatalytic properties. However, the high interfacial energy barrier limits the formation and nano-assembly of the heterogeneous junctions between MOFs and metal sulphides. Herein, the heterostructured Zr-MOF-S@CdS are successfully constructed through a sequential synthesis method, in which the mesoporous Zr-MOF are firstly decorated with thioglycolic acid through pore functionalization, and followed by the S^2- anion exchange process resulting in the surface close attached growth of CdS onto Zr-MOF-S materials. Due to the presence of molecules linkers, the CdS can be precisely decorated onto Zr-MOF-S without aggregation, which can provide more active sites. Moreover, the intimate connections and the suitable band structures between two materials can also facilitate the photogenerated electron-hole pairs separation. Therefore, the resulting Zr-MOF-S@CdS with appropriate ratio exhibits high photocatalytic activity for water reduction, in which the H₂ evolution rate can reach up to 1861.7 μmol·g^‒1·h^‒1, 4.5 times higher than pure CdS and 2.3 times higher than of Zr-MOF/CdS, respectively. Considering the promising future of MOF-based photocatalysts, this work may provide an avenue for the further design and synthesis MOF-based composite photocatalysts for efficient H₂ evolution.

Key words: Zr-MOF, Pore functionalization, Photocatalytic H₂ production, Molecular linker, Junction

Haijun Hu, Kailai Zhang, Ge Yan, Litong Shi, Baohua Jia, Hongwei Huang, Yu Zhang, Xiaodong Sun, Tianyi Ma. Precisely decorating CdS on Zr-MOFs through pore functionalization strategy: A highly efficient photocatalyst for H₂ production[J]. Chinese Journal of Catalysis, 2022, 43(9): 2332-2341.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63949-9

https://www.cjcatal.com/EN/Y2022/V43/I9/2332

Figures/Tables 9

Scheme 1. Schematic illustration of the synthetic process of Zr-MOF-S@CdS.

Fig. 1. (a?c) SEM images of Zr-MOF, Zr-MOF-S and Zr-MOF-S@CdS(48). (d,e) TEM images of Zr-MOF and Zr-MOF-S. (f) HRTEM image of Zr-MOF-S@CdS(48). (g?l) the SEM-EDS images of Zr-MOF-S@CdS(48).

Fig. 2. N2 adsorption-desorption isotherms of prepared samples.

Fig. 3. (a) The survey XPS spectra of CdS, Zr-MOF-S@CdS(48), Zr-MOF-S and Zr-MOF. (b) Typical Zr 3d XPS spectra of Zr-MOF-S, Zr-MOF and Zr-MOF-S@CdS(48). (c) Typical Cd 3d XPS spectra of CdS and Zr-MOF-S@CdS(48). (d) Typical S 2p XPS spectra of CdS and Zr-MOF-S@CdS(48).

Fig. 4. (a) UV-Vis diffuse reflectance spectra for CdS, Zr-MOF, Zr-MOF-S and Zr-MOF-S@CdS composites with altered weight ratios of CdS. (b) Tauc plot of CdS and Zr-MOF-S. (c,d) Mott-Schottky plots for CdS and Zr-MOF-S in a 0.2 mol L?1 Na2SO4 aqueous solution (pH = 6.8).

Fig. 5. Schematic energy-band diagrams for CdS and Zr-MOF-S (VBM, CBM, Vac, HOMO, LUMO, Ef and W1, W2 denote valence band maximum, conduction band minimum, vacuum level, highest occupied molecular orbital, lowest unoccupied molecular orbital, Fermi level, Work function, respectively (in eV)).

Fig. 6. (a,b) Photocatalytic H2 evolution amount and H2 production rate of CdS, Zr-MOF and Zr-MOF-S@CdS composites with altered weight ratios of CdS. (c) Photocatalytic H2 evolution amount comparison for Zr-MOF-S@CdS(48) with different sacrificial agents. (d) The recycle tests of Zr-MOF-S@CdS(48).

Fig. 7. (a) The electrochemical impedance spectroscopy plots for CdS, Zr-MOF/CdS(48) and Zr-MOF-S@CdS composites with altered weight ratios of CdS. (b) Transient photocurrent responses for CdS, Zr-MOF/CdS(48), Zr-MOF-S and Zr-MOF-S@CdS composites with altered weight ratios of CdS.

Scheme 2. Energetic scheme that illustrates electron transfer dynamics from CdS to Zr-MOF-S.

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Precisely decorating CdS on Zr-MOFs through pore functionalization strategy: A highly efficient photocatalyst for H₂ production

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