Synthesis of ternary Ni2P@UiO-66-NH2/Zn0.5Cd0.5S composite materials with significantly improved photocatalytic H2 production performance

doi:10.1016/S1872-2067(21)63912-8

Abstract

Abstract:

abstract The design and construction of low-cost and high-performance hybrid materials for the photocatalytic hydrogen production reaction (HER) are extremely important for the large-scale application of hydrogen energy. Metal-organic frameworks (MOFs) are considered to be potential photocatalytic materials. Herein, monodisperse, small size, non-precious metal transition metal phosphide Ni₂P is encapsulated into a typical MOF (UiO-66-NH₂) as a hybrid core-shell cocatalyst to modify Zn_0.5Cd_0.5S for photocatalytic hydrogen production. Ni₂P is wrapped in UiO-66-NH₂ via an in situ solvothermal method, and Zn_0.5Cd_0.5S sulfide is decorated with a core-shell Ni₂P@UiO-66-NH₂cocatalyst to obtain ternary Ni₂P@UiO-66-NH₂/Zn_0.5Cd_0.5S composite materials. Photoelectric and chemical characterization confirms that the ternary composites have good kinetic hydrogen production performance. The hydrogen production rate of 10% 10 mg Ni₂P@UiO-66-NH₂/Zn_0.5Cd_0.5S reaches 40.91 mmol·g^-1·h^-1 with an apparent quantum efficiency at 420 nm of 13.57%. The addition of 10 mg Ni₂P@UiO-66-NH₂ increases the surface area of the ternary material, providing abundant reaction sites and forming an efficient charge transfer channel, which is conducive to efficient hydrogen production by the ternary photocatalysts. It is shown that the formation of a ternary composite system is beneficial to the occurrence of an efficient catalytic reaction. This study provides a new perspective for the construction of high-performance photocatalytic materials.

Key words: Ni₂P, UiO-66-NH₂, Zn_0.5Cd_0.5S, Hydrogen evolution, Ternary photocatalyst

Aixia Wang, Linhe Zhang, Xuli Li, Yangqin Gao, Ning Li, Guiwu Lu, Lei Ge. Synthesis of ternary Ni₂P@UiO-66-NH₂/Zn_0.5Cd_0.5S composite materials with significantly improved photocatalytic H₂ production performance[J]. Chinese Journal of Catalysis, 2022, 43(5): 1295-1305.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63912-8

https://www.cjcatal.com/EN/Y2022/V43/I5/1295

Figures/Tables 12

Fig. 1. XRD patterns of different samples. (a) Pure UiO-66-NH2 (U), 10 mg Ni2P@UiO-66-NH2 (10 N@U) and pure Ni2P (N); (b) Zn0.5Cd0.5S (ZCS), 10% 10mg Ni2P@UiO-66-NH2/Zn0.5Cd0.5S (10% 10 N@U/ZCS) and 20% 10mg Ni2P@UiO-66-NH2/Zn0.5Cd0.5S (20% 10 N@U/ZCS).

Fig. 2. (a) SEM result for UiO-66-NH2 (U); (b) SEM result for 10 mg Ni2P@UiO-66-NH2 (10 N@U); (c) TEM result for UiO-66-NH2 (U); TEM (d), HRTEM (e) results, and EDX mapping (f) of the 10mg Ni2P@UiO-66-NH2 (10 N@U) sample.

Fig. 3. (a) TEM result for Zn0.5Cd0.5S (ZCS) (HRTEM image in illustration); TEM (b) and HRTEM (c) images for 20% 10mg Ni2P@UiO-66-NH2/Zn0.5Cd0.5S (20% 10 N@U/ZCS).

Fig. 4. XPS spectra of the 10% 10mg Ni2P@UiO-66-NH2/Zn0.5Cd0.5S photocatalyst (10% 10 N@U/ZCS). (a) Zn 2p; (b) Cd 3d; (c) S 2p; (d) Zr 3d; (e) C 1s; (f) Ni 2p; (g) P 2p; (h) survey.

Fig. 5. Diffuse reflectance spectra of pure Zn0.5Cd0.5S (ZCS) and 10% 10 mg Ni2P@UiO-66-NH2/Zn0.5Cd0.5S (10% 10 N@U/ZCS). Inset: spectra of pure UiO-66-NH2 (U) and 10 mg Ni2P@UiO-66-NH2 (10 N@U).

Fig. 6. MS curves of pure Zn0.5Cd0.5S (ZCS) (a) and pure UiO-66-NH2 (U) (b).

Fig. 7. (a) Transient photocurrent diagrams for Zn0.5Cd0.5S (ZCS), 10% 10mg Ni2P@UiO-66-NH2/Zn0.5Cd0.5S (10% 10 N@U/ZCS) (with, inset, the transient photocurrent diagrams of UiO-66-NH2 (U), and 10mg Ni2P@UiO-66-NH2 (10 N@U)); (b) Electrochemical impedance diagrams for UiO-66-NH2 (U), 10mg Ni2P@UiO-66-NH2 (10 N@U), pure Zn0.5Cd0.5S (ZCS) and 10% 10mg Ni2P@UiO-66-NH2/Zn0.5Cd0.5S (10% 10 N@U/ZCS).

Fig. 8. SPV spectra of Zn0.5Cd0.5S (ZCS) and 10% 10mg Ni2P@UiO-66-NH2/ Zn0.5Cd0.5S (10% 10 N@U/ZCS).

Fig. 9. Hydrogen production rates under visible-light illumination. (a) With different contents of x mg Ni2P@UiO-66-NH2 (x N@U) catalysts; (b) x% 10mg Ni2P@UiO-66-NH2/Zn0.5Cd0.5S (x% 10 N@U/ZCS) with different contents of 10 N@U cocatalyst.

Fig. 10. Hydrogen production cycles (a) and quantum efficiency (b) at 420 nm for 10% 10mg Ni2P@UiO-66-NH2/Zn0.5Cd0.5S (10% 10 N@U/ZCS).

Fig. 11. ESR spectra of e- and h+ signals of pure Zn0.5Cd0.5S (ZCS) and 10% 10 mg Ni2P@UiO-66-NH2/Zn0.5Cd0.5S (10% 10 N@U/ZCS) ternary photocatalysts at room temperature: e- signal with light irradiation time of 0 min (a), 5 min (b) and 10 min (c); h+ signal with light irradiation time of 0 min (d), 5 min (e) and 10 min (f).

Fig. 12. Electron transfer and hydrogen production mechanism of N@U/ZCS under visible light irradiation.

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Synthesis of ternary Ni₂P@UiO-66-NH₂/Zn_0.5Cd_0.5S composite materials with significantly improved photocatalytic H₂ production performance

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