Promoting Photochemical Water Oxidation with Metallic Band Structures

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• 作者：Hongfei Liu ; René Moré ; Henrik Grundmann ; Chunhua Cui ; Rolf Erni ; Greta R. Patzke
• 刊名：Journal of the American Chemical Society
• 出版年：2016
• 出版时间：February 10, 2016
• 年：2016
• 卷：138
• 期：5
• 页码：1527-1535
• 全文大小：658K
• ISSN：1520-5126

文摘

The development of economic water oxidation catalysts is a key step toward large-scale water splitting. However, their current exploration remains empirical to a large extent. Elucidating the correlations between electronic properties and catalytic activity is crucial for deriving general and straightforward catalyst design principles. Herein, strongly correlated electronic systems with abundant and easily tunable electronic properties, namely La_1–xSr_xBO₃ perovskites and La_2-xSr_xBO₄ layered perovskites (B = Fe, Co, Ni, or Mn), were employed as model systems to identify favorable electronic structures for water oxidation. We established a direct correlation between the enhancement of catalytic activity and the insulator to metal transition through tuning the electronic properties of the target perovskite families via the La³⁺/Sr²⁺ ratio. Their improved photochemical water oxidation performance was clearly linked to the increasingly metallic character. These electronic structure–activity relations provide a promising guideline for constructing efficient water oxidation catalysts.