Solar-Driven Lignin Oxidation via Hydrogen Atom Transfer with a Dye-Sensitized TiO2 Photoanode

Shuya Li, Zhi Jun Li, Hyun Yu, Marion Ryan Sytu, Yunxuan Wang, Debora Beeri, Weiwei Zheng, Benjamin D. Sherman, Chang Geun Yoo, Gyu Leem

Research output: Contribution to journalArticle

Abstract

Molecular-based dye-sensitized photoelectrochemical cells (DSPECs) have traditionally targeted solar-driven water splitting for the conversion of solar energy into fuels in aqueous media. This work reports the use of a DSPEC-type photoanode specifically designed to carry out chemoselective oxidation of benzylic alcohol moieties in lignin model compounds and real lignin in organic media. The TiO2-based photoanode incorporates a surface-bound Ru(II)-based photocatalyst and solution-dissolved hydrogen atom transfer (HAT) co-catalyst to perform solar-driven photocatalytic oxidation of the lignin substrates. Under aerobic conditions with simulated solar illumination, conversion efficiencies in excess of 90% are observed for the formation of the oxidized ketone product from model compounds. The DSPEC half-cell exhibited impressive long-term durability, sustaining photocatalytic oxidation of the lignin model compound over a net illumination period of 80 h. This photoelectrochemical heterogeneous catalytic process provides a unique foundation to perform selective C-O bond cleavage for real lignin conversion technologies.

Original languageEnglish (US)
Pages (from-to)777-784
Number of pages8
JournalACS Energy Letters
Volume5
Issue number3
DOIs
StatePublished - Mar 13 2020

ASJC Scopus subject areas

  • Chemistry (miscellaneous)
  • Renewable Energy, Sustainability and the Environment
  • Fuel Technology
  • Energy Engineering and Power Technology
  • Materials Chemistry

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    Li, S., Li, Z. J., Yu, H., Sytu, M. R., Wang, Y., Beeri, D., Zheng, W., Sherman, B. D., Yoo, C. G., & Leem, G. (2020). Solar-Driven Lignin Oxidation via Hydrogen Atom Transfer with a Dye-Sensitized TiO2 Photoanode. ACS Energy Letters, 5(3), 777-784. https://doi.org/10.1021/acsenergylett.9b02391