Efficient and Reversible Catalysis of Formic Acid-Carbon Dioxide Cycle Using Carbamate-Substituted Ruthenium-Dithiolate Complexes

Hui Min Tsai, Wan Hsiang Lien, Chi Hsuan Liao, Yi Ting Chen, Sheng Cih Huang, Feng Pai Chou, Chin-Yuan Chang, Jen-Shiang K. Yu, Ya-Ting Kao, Tung-Kung Wu*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

Abstract

It is important to develop viable technologies for efficient hydrogen (H2) production and carbon dioxide (CO2) conversion to realize the future supply of clean energy and reduction of global CO2 concentration. Herein, we report a series of carbamate-substituted ruthenium-dithiolate complexes 1–3, [Rux(CO)y(μ-SCH(NCO2(C(CH3)3))CH2CH2S)] (x=2, 3, 6 and y=6, 9, 20), which can effectively catalyze the reversible formic acid-carbon dioxide (FA-CO2/H2) cycle that can be used to convert CO2 and produce H2. Complex 2 effectively dehydrogenates FA to produce H2 with an unprecedented turnover frequency (TOF) of 1.15×106 h−1 under conditions of sunlight irradiation. Under conditions of high temperature and pressure, complex 3 hydrogenates CO2 to FA with a high initial TOF of 1.02×106 h−1, resulting in an efficient FA-CO2/H2 cycle. These results can potentially help provide the platform for the development of technologies that can be used in future to produce clean energy and control environmental threats.

Original languageAmerican English
Pages (from-to)4092-4098
Number of pages7
JournalChemCatChem
Volume13
Issue number19
DOIs
StatePublished - 7 Oct 2021

Keywords

  • Carbon dioxide
  • Carbon neutral cycle
  • Catalysis
  • Hydrogen
  • Ruthenium H-cluster
  • Solar energy

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