Protic Ru(II)-NHC Pincer Catalyst for the Catalytic Hydrogenation of CO2 and Its Derivatives to Methanol DOI
Arindom Bhattacherya, Mandeep Kaur, Ravi Kumar

и другие.

Organometallics, Год журнала: 2024, Номер 44(1), С. 244 - 254

Опубликована: Дек. 10, 2024

Methanol production from CO2 offers an attractive alternative to developing a sustainable energy economy. In this work, phosphine-free Ru(II)-NHC pincer complex (1•PF6) bearing proton-responsive pyridyl(benzamide) appended on N-heterocyclic carbene (NHC) has been synthesized. The molecular structure of 1•PF6 reveals the deprotonated iminolic form ligand. acid–base equilibrium between iminolic-amide tautomer ligand scaffold was examined by 1H NMR and UV–vis spectra. catalytic efficacy for hydrogenation urea carbamates as derivatives, two most challenging carbonyl substrates, methanol (yield 74–90%) explored. Further, amine-assisted capture followed formamide its subsequent up 90%) were performed using catalyst 1•PF6. A maximum TON 1700 attained taking piperidine capturing agent. exhibits superior activity in comparison protonated form, revealing metal–ligand cooperation dihydrogen activation. Catalyst is air- moisture-stable thus operational simplicity. experiments suggest intermediacy [Ru–H/N–H]+ intermediate engaged proton hydride management pathway. plausible cycle proposed based informative mechanistic experiments.

Язык: Английский

Protic Ru(II)-NHC Pincer Catalyst for the Catalytic Hydrogenation of CO2 and Its Derivatives to Methanol DOI
Arindom Bhattacherya, Mandeep Kaur, Ravi Kumar

и другие.

Organometallics, Год журнала: 2024, Номер 44(1), С. 244 - 254

Опубликована: Дек. 10, 2024

Methanol production from CO2 offers an attractive alternative to developing a sustainable energy economy. In this work, phosphine-free Ru(II)-NHC pincer complex (1•PF6) bearing proton-responsive pyridyl(benzamide) appended on N-heterocyclic carbene (NHC) has been synthesized. The molecular structure of 1•PF6 reveals the deprotonated iminolic form ligand. acid–base equilibrium between iminolic-amide tautomer ligand scaffold was examined by 1H NMR and UV–vis spectra. catalytic efficacy for hydrogenation urea carbamates as derivatives, two most challenging carbonyl substrates, methanol (yield 74–90%) explored. Further, amine-assisted capture followed formamide its subsequent up 90%) were performed using catalyst 1•PF6. A maximum TON 1700 attained taking piperidine capturing agent. exhibits superior activity in comparison protonated form, revealing metal–ligand cooperation dihydrogen activation. Catalyst is air- moisture-stable thus operational simplicity. experiments suggest intermediacy [Ru–H/N–H]+ intermediate engaged proton hydride management pathway. plausible cycle proposed based informative mechanistic experiments.

Язык: Английский

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