Electron Injection from Photoexcited Metal-Organic Framework Ligands to Ru Secondary Building Units for Visible-Light-Driven Hydrogen Evolution

Overview

Journal J Am Chem Soc

Publisher American Chemical Society

Specialty Chemistry

Date 2018 Mar 27

PMID 29578703

Citations 8

Authors

Guangxu Lan

Yuan-Yuan Zhu

Samuel S Veroneau

Ziwan Xu

Daniel Micheroni

Wenbin Lin

Affiliations

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Abstract

We report the design of two new metal-organic frameworks (MOFs), Ru-TBP and Ru-TBP-Zn, based on Ru secondary building units (SBUs) and porphyrin-derived tetracarboxylate ligands. The proximity of Ru SBUs to porphyrin ligands (∼1.1 nm) facilitates multielectron transfer from excited porphyrins to Ru SBUs to enable efficient visible-light-driven hydrogen evolution reaction (HER) in neutral water. Photophysical and electrochemical studies revealed oxidative quenching of excited porphyrin by Ru SBUs as the initial step of the HER process and the energetics of key intermediates in the catalytic cycle. Our work provides a new strategy to building multifunctional MOFs with synergistic ligands and SBUs for efficient photocatalysis.

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