Direct Z-scheme photochemical hybrid systems: Loading porphyrin-based metal-organic cages on graphitic-C3N4 to dramatically enhance photocatalytic hydrogen evolution

doi:10.1016/S1872-2067(22)64109-3

Abstract

Abstract:

The rational design of photochemical molecular device (PMD) and its hybrid system has great potential in improving the activity of photocatalytic hydrogen production. A series of Pd₆L₃type metal-organic cages, denoted as MOC-Py-M (M = H, Cu, and Zn), are designed for PMDs by combining metalloporphyrin-based ligands with catalytically active Pd²⁺ centers. These metal-organic cages (MOCs) are first successfully hybridized with graphitic carbon nitride (g-C₃N₄) to form direct Z-scheme heterogeneous MOC-Py-M/g-C₃N₄ (M = H, Cu, and Zn) photocatalysts via π-π interactions. Benefiting from its better light absorption ability, the MOC-Py-Zn/g-C₃N₄ catalyst exhibits high H₂ production activity under visible light (10348 μmol g^-1 h^-1), far superior to MOC-Py-H/g-C₃N₄ and MOC-Py-Cu/g-C₃N₄. Moreover, the MOC-Py-Zn/g-C₃N₄ system obtains an enhanced turn over number (TON) value of 32616 within 100 h, outperforming the homogenous MOC-Py-Zn (TON of 507 within 100 h), which is one of the highest photochemical hybrid systems based on MOC for visible-light-driven hydrogen generation. This confirms the direct Z-scheme heterostructure can promote effective charge transfer, expand the visible light absorption region, and protect the cages from decomposition in MOC-Py-Zn/g-C₃N₄. This work presents a creative example that direct Z-scheme PMD-based systems for effective and persistent hydrogen generation from water under visible light are obtained by heterogenization approach using homogeneous porphyrin-based MOCs and g-C₃N₄ semiconductors.

Key words: Porphyrin-based metal-organic cage, g-C3N4, Photochemical molecular device, Direct Z-scheme heterostructure, Photocatalytic hydrogen evolution, from water

Yang Lei, Jian-Feng Huang, Xin-Ao Li, Chu-Ying Lv, Chao-Ping Hou, Jun-Min Liu. Direct Z-scheme photochemical hybrid systems: Loading porphyrin-based metal-organic cages on graphitic-C₃N₄ to dramatically enhance photocatalytic hydrogen evolution[J]. Chinese Journal of Catalysis, 2022, 43(8): 2249-2258.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64109-3

https://www.cjcatal.com/EN/Y2022/V43/I8/2249

Figures/Tables 10

Scheme 1. The chemical structure of TPyP and the construction of Pd-based cage MOC-Py-M (M = H, Cu, and Zn).

Fig. 1. The PXRD patterns of g-C3N4, MOC-Py-M/g-C3N4 and MOC-Py-M (M = H, Cu, and Zn).

Fig. 2. (a,b) SEM and TEM for g-C3N4. (c,d) SEM and TEM for MOC-Py-Zn/g-C3N4. (e) TEM elemental mapping images for MOC-Py-Zn/g-C3N4.

Fig. 3. (a) UV-vis absorption spectra of MOC-Py-M in ethanol solution. (b) UV-vis diffusion reflectance absorption spectra of MOC-Py-M/g-C3N4 (M = H, Cu, and Zn).

Fig. 4. H2 production curves of g-C3N4, MOC-Py-M, and MOC-Py-M/g-C3N4 (M = H, Cu, and Zn) (a), and g-C3N4, Pd/g-C3N4, ZnTPyP/g-C3N4, and ZnTPyP-Pd/g-C3N4 (b) in 100 mL H2O/TEOA (9:1, v/v) irradiated by a 300 W Xe lamp with a cut-off filter (λ > 420 nm).

Fig. 5. Photocurrent responses (a) and EIS Nyquist plots (b) of g-C3N4 and MOC-Py-M/g-C3N4 (M = Cu and Zn) with 0.2 V bias vs. Ag/AgCl under visible light illumination.

Fig. 6. (a) H2 production curves of MOC-Py-Zn and MOC-Py-Zn/g-C3N4 in 100 mL H2O/TEOA (9:1, v/v) under visible light irradiation (λ > 420 nm). (b) accumulated TONs and TOFs based on MOC-Py-Zn of MOC-Py-Zn and MOC-Py-Zn/g-C3N4 in 100 h.

Fig. 7. Schematic illustration for the separation and transfer of photoproduced charges in the MOC-Py-Zn/g-C3N4.

Fig. 8. (a) The Z-scheme electron transfer route for •OH generation of MOC-Py-Zn/g-C3N4. (b) PL spectra at 315 nm excitation for TA-OH produced by MOC-Py-Zn, g-C3N4, and MOC-Py-Zn/g-C3N4 in the presence of TA under visible light.

Fig. 9. PL spectra (a) and time-resolved PL decay curves (b) of g-C3N4, MOC-Py-Zn, and MOC-Py-Zn/g-C3N4 composites at 360 nm excitation.

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Direct Z-scheme photochemical hybrid systems: Loading porphyrin-based metal-organic cages on graphitic-C₃N₄ to dramatically enhance photocatalytic hydrogen evolution

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