Bis-Imidazole Methane Ligated Ruthenium(II) Complexes: Synthesis, Characterization, and Catalytic Activity for Hydrogen Production from Formic Acid in Water

Soumyadip Patra; Hemanta Deka; Sanjay K Singh

doi:10.1021/acs.inorgchem.1c01784

Bis-Imidazole Methane Ligated Ruthenium(II) Complexes: Synthesis, Characterization, and Catalytic Activity for Hydrogen Production from Formic Acid in Water

Inorg Chem. 2021 Sep 20;60(18):14275-14285. doi: 10.1021/acs.inorgchem.1c01784. Epub 2021 Aug 30.

Authors

Soumyadip Patra¹, Hemanta Deka¹, Sanjay K Singh¹

Affiliation

¹ Catalysis Group, Department of Chemistry, Indian Institute of Technology Indore, Simrol, Indore 453552, Madhya Pradesh, India.

PMID: 34461719
DOI: 10.1021/acs.inorgchem.1c01784

Abstract

A series of half sandwich arene-ruthenium complexes [(η⁶-arene)RuCl(κ²-L)]⁺ ([Ru]-1-[Ru]-10) containing bis-imidazole methane-based ligands {4,4'-(phenylmethylene)bis(2-ethyl-5-methyl-1H-imidazole)} (L1), {4,4'-((4-methoxyphenyl)methylene)bis(2-ethyl-5-methyl-1H-imidazole)} (L2), {4,4'-((2-methoxyphenyl)methylene)bis(2-ethyl-5-methyl-1H-imidazole)} (L3), {4,4'-((4-chlorophenyl)methylene)bis(2-ethyl-5-methyl-1H-imidazole)} (L4), and {4,4'-((2-chlorophenyl)methylene)bis(2-ethyl-5-methyl-1H-imidazole)} (L5) are synthesized. The synthesized and purified complexes ([Ru]-1-[Ru]-10) are further employed for hydrogen production from formic acid in aqueous medium. Among the investigated complexes, [(η⁶-p-cymene)RuCl(κ²-L2)]⁺ [Ru]-2, having Ru(II) coordinated 4-methoxy phenyl substituted bis-imidazole methane ligand (L2), outperformed over others, displaying a higher catalytic turnover of 8830 and high efficiency (TOF = 1545 h^-1) with appreciably high long-term stability for formic acid dehydrogenation in water.