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用于高效铱催化水氧化催化的供体柔性氮配体

Donor-Flexible Nitrogen Ligands for Efficient Iridium-Catalyzed Water Oxidation Catalysis.

作者信息

Navarro Miquel, Li Mo, Müller-Bunz Helge, Bernhard Stefan, Albrecht Martin

机构信息

Department of Chemistry & Biochemistry, University of Bern, Freiestrasse 3, 3012, Bern, Switzerland.

School of Chemistry and Chemical Biology, University College Dublin, Belfield, Dublin, 4, Ireland.

出版信息

Chemistry. 2016 May 10;22(20):6740-5. doi: 10.1002/chem.201600875. Epub 2016 Apr 5.

DOI:10.1002/chem.201600875
PMID:26919306
Abstract

A pyridylideneamide ligand with variable donor properties owing to a pronounced zwitterionic and a neutral diene-type resonance structure was used as a dynamic ligand at a Cp* iridium center to facilitate water oxidation catalysis, a reaction that requires the stabilization of a variety of different iridium oxidation states and that is key for developing an efficient solar fuel device. The ligand imparts high activity (nearly three-fold increase of turnover frequency compared to benchmark systems), and exceptionally high turnover numbers, which indicate a robust catalytic cycle and little catalyst degradation.

摘要

一种由于具有明显的两性离子和中性二烯型共振结构而具有可变供体性质的吡啶叉酰胺配体,被用作Cp*铱中心的动态配体,以促进水氧化催化反应,该反应需要稳定多种不同的铱氧化态,并且是开发高效太阳能燃料装置的关键。该配体具有高活性(与基准体系相比,周转频率提高了近三倍)和极高的周转数,这表明催化循环稳健且催化剂降解很少。

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