Synergistic Effect of Pendant N Moieties for Proton Shuttling in the Dehydrogenation of Formic Acid Catalyzed by Biomimetic Ir(III)Complexes

2021-03-06 Hits:

Indexed by:期刊论文

Date of Publication:2021-03-06

Journal:CHEMSUSCHEM

Volume:13

Issue:18

Page Number:5015-5022

ISSN No.:1864-5631

Key Words:biomimetic complex; dehydrogenation; iridium; pendant base; proton shuttling

Abstract:Formic acid (FA) is among the most promising hydrogen storage materials. The development of efficient catalysts for the dehydrogenation of FA via molecular-level control and precise tuning remains challenging. A series of biomimetic Ir complexes was developed for the efficient dehydrogenation of FA in an aqueous solution without base addition. A high turnover frequency of 46510 h(-1)was achieved at 90 degrees C in 1 mFA solution with complex1bearing pendant pyridine. Experimental and mechanistic studies revealed that the integrated pendant pyridine and pyrazole moieties of complex1could act as proton relay and facilitate proton shuttling in the outer coordination sphere. This study provides a new strategy to control proton transfer accurately and a new principle for the design of efficient catalysts for FA dehydrogenation.

Date of Publication:2021-03-06