Formic Acid Dehydrogenation via an Active Ruthenium Pincer Catalyst Immobilized on Tetra-Coordinated Aluminum Hydride Species Supported on Fibrous Silica Nanospheres

Layal Yaacoub, Indranil Dutta, Baraa Werghi, Benjamin W.J. Chen, Jia Zhang, Edy Abou Hamad, Eleanor Pei Ling Ang, Eva Pump, Anissa Bendjeriou Sedjerari, Kuo Wei Huang*, Jean Marie Basset*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

16 Scopus citations

Abstract

The demand for harmless and efficient energy sources is remarkably expanding, particularly after the increased awareness of global warming, greenhouse gas emissions, immense fossil fuel consumption, and so forth. Formic acid is considered a potential candidate as an energy carrier for reversible hydrogen storage owing to its decomposition to hydrogen (H2) and carbon dioxide (CO2) in the presence of suitable catalysts. However, selective and efficient decomposition of formic acid using classical heterogeneous catalysis is still challenging because most heterogeneous catalysts which are known are ill defined. Herein, we report a promising heterogeneous approach toward formic acid dehydrogenation using a ruthenium PN3P pincer complex, [Ru-H(CO) (tBuPN3P)] (I), immobilized on a fibrous silica nanosphere, KCC-1, with a strong Lewis acid character [(Si-O-Si) (Si-O-)2Al-H]. The resulting heterogeneous catalyst, [Ru(H) (CO) (tBuPN3P)]@[(Si-O-Si) (Si-O-)2Al-H] (III), has been fully characterized by advanced solid-state characterization techniques. In this compound, Al is tetrahedrally coordinated. It is a single-site catalyst which exhibits good stability toward water, high pressures, and high temperatures as well as good activity in formic acid dehydrogenation. An excellent turnover number of 600,000 and a recyclability of up to 45 cycles are observed.

Original languageEnglish (US)
Pages (from-to)14408-14417
Number of pages10
JournalACS Catalysis
Volume12
Issue number22
DOIs
StatePublished - Nov 18 2022

Keywords

  • formic acid dehydrogenation
  • KCC-1
  • PNP pincer
  • ruthenium
  • single-site heterogeneous catalysis
  • SOMC

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry

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