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论文类型：期刊论文

发表时间：2021-03-06

发表刊物：CHEMSUSCHEM

卷号：13

期号：18

页面范围：5015-5022

ISSN号：1864-5631

关键字：biomimetic complex; dehydrogenation; iridium; pendant base; proton shuttling

摘要：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.