Construction of Mesoporous Aluminosilicate Thin Films on ITO Electrodes for Immobilizing a Cationic Ru(II) Water Oxidation Catalyst

IF 3.8 3区化学 Q2 CHEMISTRY, PHYSICAL ChemCatChem Pub Date : 2024-09-02 DOI:10.1002/cctc.202401199

Masaya Okamura, Shunpei Harada, Ayano Yamada, Narumi Nakano, Shiro Hikichi

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Abstract

Aluminosilicate (Al‐SiO2) thin films with vertically aligned mesochannels were successfully synthesized on ITO electrodes and employed for the immobilization of a cationic Ru(II) water oxidation catalyst without requiring linker groups. Optimal synthesis conditions yielded uniform mesoporous Al‐SiO2 films with tunable Al content, high surface area (568 m2/g), 3.94 nm pore size, and 155 nm thickness. Electrochemical studies confirmed the presence of the immobilized Ru complex undergoing diffusion‐controlled Ru(III/II) and Ru(IV/III) electron transfer. The Ru loading reached 4.71 nmol/cm2 at Si/Al = 9.6, with higher Al content enhancing loading amounts via cation exchange. The Ru‐modified electrode exhibited high electrocatalytic water oxidation activity, achieving 75.3% Faradaic efficiency and a turnover number of 298.6 for O2 evolution for 1 hour. This work provides a new approach to construct porous environments on an electrode surface to immobilize positively charged transition‐metal complexes as catalysts, offering potential applications in the development of electrocatalytic systems for energy conversion.

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在 ITO 电极上构建用于固定阳离子 Ru(II) 水氧化催化剂的介孔硅酸铝薄膜

在 ITO 电极上成功合成了具有垂直排列介孔的硅酸铝（Al-SiO2）薄膜，并用于固定阳离子 Ru(II) 水氧化催化剂，而无需连接基团。最佳合成条件产生了均匀的介孔 Al-SiO2 薄膜，其铝含量可调，具有高比表面积（568 m2/g）、3.94 nm 孔径和 155 nm 厚度。电化学研究证实，固定化的 Ru 复合物正在进行扩散控制的 Ru(III/II) 和 Ru(IV/III) 电子转移。在 Si/Al = 9.6 时，Ru 的负载量达到 4.71 nmol/cm2，铝含量越高，通过阳离子交换的负载量越大。Ru 改性电极具有很高的电催化水氧化活性，法拉第效率达到 75.3%，1 小时的氧气进化周转数为 298.6。这项工作提供了一种在电极表面构建多孔环境以固定带正电的过渡金属复合物作为催化剂的新方法，为开发用于能源转换的电催化系统提供了潜在应用。

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来源期刊

ChemCatChem 化学-物理化学

CiteScore

8.10

自引率

4.40%

发文量

511

审稿时长

1.3 months

期刊介绍： With an impact factor of 4.495 (2018), ChemCatChem is one of the premier journals in the field of catalysis. The journal provides primary research papers and critical secondary information on heterogeneous, homogeneous and bio- and nanocatalysis. The journal is well placed to strengthen cross-communication within between these communities. Its authors and readers come from academia, the chemical industry, and government laboratories across the world. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies, and is supported by the German Catalysis Society.