Incorporating porphyrin-Pt in light-harvesting metal-organic frameworks for enhanced visible light-driven hydrogen production

doi:10.1016/S1872-2067(20)63738-X

Abstract

Abstract:

Molecular catalysts for H₂-evolution are of interest for their integration into light-harvesting complexes for photocatalytic water splitting. Here, we report the meso-tetra (4-carboxyphenyl) porphine [(TCPP)Pt ^II] complex as a molecular H₂-evolving photocatalyst using chloranilic acid (CA) as a sacrificial electron donor, the choice of which is critical to the stability of the photocatalyst. When triethanolamine was used, [(TCPP)Pt ^II] decomposed to form Pt nanoparticles. Density functional theory calculations together with evidence from electrochemical and spectroscopic analyses suggested that the catalysis was possibly initiated by a proton-coupled electron transfer (PCET) to form [(TCPP)Pt ^I]-N-H, followed by another electron injection and protonation to form a [(TCPP)Pt ^II-hydride]-N-H intermediate that can release H₂. As the whole catalytic cycle involves the injection of multiple electrons, a light-harvesting network should be helpful by providing multiple photo-induced electrons. Thus, we integrated this molecular catalyst into a light-harvesting metal-organic framework to boost its activity by ~830 times. This work presents a mechanistic study of the photocatalytic H₂ evolution and energy transfer and highlights the importance of a light-harvesting network for multiple electron injections.

Key words: Artificial photosynthesis, Hydrogen evolution reaction, Light-harvesting, Metal-organic frameworks, Molecular catalyst

Huihui Hu, Lingzhen Zeng, Zhe Li, Tianbao Zhu, Cheng Wang. Incorporating porphyrin-Pt in light-harvesting metal-organic frameworks for enhanced visible light-driven hydrogen production[J]. Chinese Journal of Catalysis, 2021, 42(8): 1345-1351.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63738-X

https://www.cjcatal.com/EN/Y2021/V42/I8/1345

Figures/Tables 4

Fig. 1. (a) Structure of Hf-[(TCPP)PtII]-MOF(PCN-223) with green polyhedrons representing Hf6O4OH4(COO)12 clusters and yellow balls representing Pt in the center of [(TCPP)PtII]; (b) Structure of Hf-[(TCPP)ZnII/PtII]-MOF(PCN-223) with green polyhedrons representing Hf6O4OH4(COO)12 clusters, purple balls representing Zn in the center of [(TCPP)ZnII], and yellow balls representing Pt in the center of [(TCPP)PtII]; (c) The photocatalytic hydrogen evolution by Hf-[(TCPP)PtII]-MOF(PCN-223) under visible-light irradiation, light source: 420 nm LED. (d) The photocatalytic hydrogen evolution by Hf-[(TCPP)ZnII/PtII]-MOF(PCN-223) under visible-light irradiation, light source: 420 nm LED.

Fig. 2. (a) SWVs of [(TCPP)PtII] in DMF with addition of TFA; (b) UV-Vis change in [(TCPP)PtII] with increasing reaction time.

Fig. 3. (a) Phosphorescence emission spectra of [(TCPP)PtII]; (b) Time-resolved phosphorescence spectra of [(TCPP)PtII]; (c) Time trace of nsTA at 460 nm of [(TCPP)PtII]; (d) Time trace of nsTA at 460 nm of Hf-[(TCPP)ZnII/PtII]-MOF (PCN-223).

Fig. 4. (a) Proposed catalytic cycle for the visible light-driven HER catalyzed by [(TCPP)PtII]; (b) Free energy profiles for HER by [(TCPP)PtII] in different possible reaction paths calculated by DFT.

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