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Developing Photosensitizer-Cobaloxime Hybrids for Solar-Driven H2 Production in Aqueous Aerobic Conditions

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Utilizing Metal-Thiocatecholate Functionalized UiO-66 Framework for Photocatalytic Hydrogen Evolution Reaction.

Hao Zhong¹, Song Chen¹, Zhixin Jiang¹

¹School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou, 510006, P. R. China.

Small (Weinheim an Der Bergstrasse, Germany)

|January 24, 2023

Summary

This study developed new metal-organic frameworks (MOFs) with well-defined active sites for efficient photocatalytic water splitting. The novel UiO-66-dcbdt-Cu material significantly enhances hydrogen evolution reactions, advancing clean energy solutions.

Keywords:

metal thiocatecholate metal-organic frameworks photocatalytic hydrogen evolution reaction post-synthetic modification

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Published on: June 23, 2023

Area of Science:

Materials Science
Chemistry
Sustainable Energy

Background:

Metal-organic frameworks (MOFs) are promising for photocatalysis due to their tunable properties and high porosity.
A key challenge in MOF design is incorporating unambiguous, metal-centered active sites for enhanced catalytic activity.
Sunlight-driven water splitting is a critical pathway for sustainable hydrogen production.

Purpose of the Study:

To synthesize a novel thiol-functionalized MOF (UiO-66-dcbdt) capable of anchoring transition metal ions.
To create well-defined metal-thiocatecholate active sites within the MOF structure for photocatalytic applications.
To investigate the efficiency of these MOF-based catalysts in the hydrogen evolution reaction (HER).

Main Methods:

Assembly of a Zr-Oxo cluster with 1,4-dicarboxylbenzene-2,3-dithiol (H2dcbdt) to form the UiO-66-dcbdt framework.
Chelation of transition metal ions (Fe, Ni, Cu) onto the thiol groups of the MOF to create UiO-66-dcbdt-M.
Photocatalytic hydrogen evolution reaction (HER) testing under irradiation, with and without external photosensitizers and heterojunctioning with TiO2.

Main Results:

UiO-66-dcbdt successfully anchored transition metal ions, forming unambiguous metal-thiocatecholate moieties.
UiO-66-dcbdt-Cu demonstrated the highest HER rate (4.18 mmol g⁻¹ h⁻¹) when paired with a Ru-polypyridyl photosensitizer.
Heterojunctioning UiO-66-dcbdt-Cu with TiO2 significantly boosted the HER rate to 12.63 mmol g⁻¹ h⁻¹, outperforming pristine TiO2 by 32.3 times.

Conclusions:

This work presents the first MOF assembly using H2dcbdt as a linker for subsequent metal ion chelation.
The developed MOFs provide well-defined active sites, crucial for efficient photocatalytic hydrogen evolution.
This strategy offers a new pathway for designing advanced MOF photocatalysts for clean energy applications.