Facile construction of highly efficient MOF-based Pd@UiO-66-NH2@ZnIn2S4 flower-like nanocomposites for visible-light-driven photocatalytic hydrogen production

doi:10.1016/j.jmst.2020.11.028

Abstract

Abstract:

Construction of metal-organic-frameworks-based composite photocatalysts has attracted much attention for the reasonable band gap and high surface areas to improve the photocatalytic activity. In this study, the ternary heterojunction Pd@UiO-66-NH₂@ZnIn₂S₄ nanocomposites were facilely prepared for the first time by a two-step method. The visible-light-promoted hydrogen production rate of 0.3 % Pd@UiO-66-NH₂@ZnIn₂S₄ reaches up to 5.26 mmol g^-1 h^-1, which is evidently much higher than pure UiO-66-NH₂, ZnIn₂S₄ and binary UiO-66-NH₂/ZnIn₂S₄ composites. Such a huge improvement in the photocatalytic performance is mainly attributed to the matched band gap of ZnIn₂S₄ and UiO-66-NH₂, and the introduction of Pd NPs into photocatalysts that broaden spectral response range and promote the photon induced charge carrier separation. This work may provide a feasible approach for the design and construction of metal-organic-frameworks-based photocatalytic materials.

Key words: Metal-organic frameworks (MOFs), UiO-66-NH₂, ZnIn₂S₄, Pd nanoparticles, Photocatalytic hydrogen production

Mengting Cao, Fengli Yang, Quan Zhang, Juhua Zhang, Lu Zhang, Lingfeng Li, Xiaohao Wang, Wei-Lin Dai. Facile construction of highly efficient MOF-based Pd@UiO-66-NH₂@ZnIn₂S₄ flower-like nanocomposites for visible-light-driven photocatalytic hydrogen production[J]. J. Mater. Sci. Technol., 2021, 76: 189-199.

Figures/Tables 14

Scheme 1. Schematic illustration of the synthetic process for Pd@UiO-66-NH2@ZnIn2S4 composites.

Fig. 1. XRD patterns of different photocatalysts.

Fig. 2. (a) TEM image of UN, (b) TEM image of PU, (c, d) SEM images of PUZ.

Fig. 3. (a, b) TEM, (c) HRTEM, (d) EDS pattern, and (e-l) mapping images of PUZ composites.

Fig. 4. FT-IR spectra of (a-c) PU-x and (d, e) PUZ-x catalysts.

Fig. 5. XPS spectra of UN, PU-3, ZIS and PUZ-3: (a) survey spectra, (b) C 1s, (c) Zr 3d, (d) Pd 3d, (e) In 3d, (f) Zn 2p, and (g) S 2p.

Fig. 6. (a) Nitrogen adsorption-desorption isotherms and (b) pore size distribution of UN, ZIS, UZ, and PUZ-3.

Table 1 The physical structural properties of UN, ZIS, UZ, and PUZ-3.

Sample	S_BET (m² g^-1)	Pore volume (cm³ g^-1)	Average pore size (nm)
UN	732.5	0.46	2.49
ZIS	74.4	0.10	12.2
UZ	162.8	0.11	11.9
PUZ-3	165.2	0.32	7.79

Fig. 7. (a) UV-vis. diffuse-re?ectance spectra and (b) Kubelka-Munk curves of different photocatalysts.

Fig. 8. (a) Photocatalytic hydrogen production under visible-light irradiation, (b, c) hydrogen production rates of various photocatalysts, and (d) reusability of PUZ-3 for the photocatalytic hydrogen production.

Table 2 The quantum efficiency (QE) for PUZ-3.

Wavelength (nm)	320	400	420	450
QE (%)	20.4	5.0	3.2	1.3

Fig. 9. (a) Photoluminescence emission spectra, (b) photocurrent, and (c) electrochemical impedance spectra of catalysts.

Fig. 10. (a) Electrochemical Mott-Schottky plots of ZIS, UZ and PUZ-3, (b) schematic illustration of band structures of UN, ZIS, UZ and PUZ-3.

Scheme 2. Schematic illustration of the mechanism of PUZ-3 during photocatalytic hydrogen evolution under sunlight irradiation.

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Facile construction of highly efficient MOF-based Pd@UiO-66-NH₂@ZnIn₂S₄ flower-like nanocomposites for visible-light-driven photocatalytic hydrogen production

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