Photocatalytic Aqueous CO2Reduction to CO and CH4Sensitized by Ullazine Supramolecular Polymers

Oliver Dumele, Luka Dordević, Hiroaki Sai, Thomas J. Cotey, M. Hussain Sangji, Kohei Sato, Adam J. Dannenhoffer, Samuel I. Stupp*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

42 Scopus citations

Abstract

There has been rapid progress on the chemistry of supramolecular scaffolds that harness sunlight for aqueous photocatalytic production of hydrogen. However, great efforts are still needed to develop similar photosynthetic systems for the great challenge of CO2reduction especially if they avoid the use of nonabundant metals. This work investigates the synthesis of supramolecular polymers capable of sensitizing catalysts that require more negative potentials than proton reduction. The monomers are chromophore amphiphiles based on a diareno-fused ullazine core that undergo supramolecular polymerization in water to create entangled nanoscale fibers. Under 450 nm visible light these fibers sensitize a dinuclear cobalt catalyst for CO2photoreduction to generate carbon monoxide and methane using a sacrificial electron donor. The supramolecular photocatalytic system can generate amounts of CH4comparable to those obtained with a precious metal-based [Ru(phen)3](PF6)2sensitizer and, in contrast to Ru-based catalysts, retains photocatalytic activity in all aqueous media over 6 days. The present study demonstrates the potential of tailored supramolecular polymers as renewable energy and sustainability materials.

Original languageEnglish (US)
Pages (from-to)3127-3136
Number of pages10
JournalJournal of the American Chemical Society
Volume144
Issue number7
DOIs
StatePublished - Feb 23 2022

ASJC Scopus subject areas

  • General Chemistry
  • Biochemistry
  • Catalysis
  • Colloid and Surface Chemistry

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