Visible-Light Photochemical Reduction of CO2 to CO Coupled to Hydrocarbon Dehydrogenation

Huijun Yu, Eynat Haviv, Ronny Neumann

Research output: Contribution to journalArticlepeer-review

7 Citations (Scopus)

Abstract

Research on the photochemical reduction of CO2, initiated already 40 years ago, has with few exceptions been performed by using amines as sacrificial reductants. Hydrocarbons are high-volume chemicals whose dehydrogenation is of interest, so the coupling of a CO2 photoreduction to a hydrocarbon-photodehydrogenation reaction seems a worthwhile concept to explore. A three-component construct was prepared including graphitic carbon nitride (g-CN) as a visible-light photoactive semiconductor, a polyoxometalate (POM) that functions as an electron acceptor to improve hole–electron charge separation, and an electron donor to a rhenium-based CO2 reduction catalyst. Upon photoactivation of g-CN, a cascade is initiated by dehydrogenation of hydrocarbons coupled to the reduction of the polyoxometalate. Visible-light photoexcitation of the reduced polyoxometalate enables electron transfer to the rhenium-based catalyst active for the selective reduction of CO2 to CO. The construct was characterized by zeta potential, IR spectroscopy, thermogravimetry, scanning electron microscopy (SEM) and energy dispersive X-ray spectroscopy (EDS). An experimental Z-scheme diagram is presented based on electrochemical measurements and UV/Vis spectroscopy. The conceptual advance should promote study into more active systems.

Original languageEnglish
JournalAngewandte Chemie - International Edition
DOIs
Publication statusAccepted/In press - Jan 1 2020

Keywords

  • carbon nitride
  • CO reduction
  • hydrocarbon dehydrogenation
  • photochemistry
  • polyoxometalate

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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