Direct Observation of a Hydroperoxide Surface Intermediate upon Visible Light-Driven Water Oxidation at an Ir Oxide Nanocluster Catalyst by Rapid-Scan FT-IR Spectroscopy

被引：118

作者：

Sivasankar, Narayanappa ^{[1
]}

Weare, Walter W. ^{[1
]}

Frei, Heinz ^{[1
]}

机构：

[1] Univ Calif Berkeley, Lawrence Berkeley Lab, Phys Biosci Div, Berkeley, CA 94720 USA

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2011年 / 133卷 / 33期

关键词：

IN-SITU FTIR; MESOPOROUS SILICA; OXYGEN EVOLUTION; IRIDIUM OXIDE; CLUSTERS; TIO2; COMPLEXES; SYSTEM; STATE;

D O I：

10.1021/ja205300a

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

A surface hydroperoxide intermediate has been detected upon oxidation of water at an Ir oxide nanocluster catalyst system under pulsed excitation of a [Ru(bpy)(3)](2+) visible light sensitizer by recording of the OO vibrational mode at 830 cm(-1). Rapid-scan FT-IR spectroscopy of colloidal H2O, D2O, and (D2O)-O-18 solutions in the attenuated total reflection mode allowed spectral assignment of IrOOH on the basis of an observed D shift of 30 cm(-1), and O-18 shifts of 24 cm(-1) ((OO)-O-16-O-18) and 46 cm(-1) ((OO)-O-18-O-18). The laser pulse response of the infrared band is consistent with the kinetic relevancy of the intermediate. This is the first observation of a surface intermediate of oxygen evolution at an Ir oxide multielectron catalyst.

引用

页码：12976 / 12979

页数：4

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