Hot π-Electron Tunneling of Metal–Insulator–COF Nanostructures for Efficient Hydrogen Production

Jintao Ming, Ai Liu, Jiwu Zhao, Pu Zhang, Haowei Huang, Huan Lin, Ziting Xu, Xuming Zhang, Xuxu Wang, Johan Hofkens, Maarten B.J. Roeffaers, Jinlin Long

Research output: Journal article publicationJournal articleAcademic researchpeer-review

23 Citations (Scopus)

Abstract

A metal–insulator–semiconductor (MIS) photosystem based on covalent organic framework (COF) semiconductors was designed for robust and efficient hydrogen evolution under visible-light irradiation. A maximal H2 evolution rate of 8.42 mmol h−1 g−1 and a turnover frequency of 789.5 h−1 were achieved by using a MIS photosystem prepared by electrostatic self-assembly of polyvinylpyrrolidone (PVP) insulator-capped Pt nanoparticles (NPs) with the hydrophilic imine-linked TP-COFs having =C=O−H−N= hydrogen-bonding groups. The hot π-electrons in the photoexcited n-type TP-COF semiconductors can be efficiently extracted and tunneled to Pt NPs across an ultrathin PVP insulating layer to reduce protons to H2. Compared to the Schottky-type counterparts, the COF-based MIS photosystems give a 32-fold-enhanced carrier efficiency, attributed to the combined enhancement of photoexcitation rate, charge separation, and oxidation rate of holes accumulated in the valence band of the TP-COF semiconductor.

Original languageEnglish
Pages (from-to)18290-18294
Number of pages5
JournalAngewandte Chemie - International Edition
Volume58
Issue number50
DOIs
Publication statusPublished - 9 Dec 2019

Keywords

  • covalent organic frameworks
  • hydrogen production
  • nanostructures
  • photocatalysis
  • semiconductors

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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