Cocatalyst Designing: A Regenerable Molybdenum-Containing Ternary Cocatalyst System for Efficient Photocatalytic Water Splitting

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• 作者：G. Wilma Busser ; Bastian Mei ; Philipp Weide ; Peter C. K. Vesborg ; Kai St眉hrenberg ; Matthias Bauer ; Xing Huang ; Marc-Georg Willinger ; Ib Chorkendorff ; Robert Schl枚gl ; Martin Muhler
• 刊名：ACS Catalysis
• 出版年：2015
• 出版时间：September 4, 2015
• 年：2015
• 卷：5
• 期：9
• 页码：5530-5539
• 全文大小：549K
• ISSN：2155-5435

文摘

Earth-abundant materials are required to facilitate upscaling of renewable hydrogen generation. Here, the synthesis of a novel oxidic ternary cocatalyst containing molybdenum, chromium, and copper, which has been found to be highly active in the overall photocatalytic splitting of water over gallium oxide, is described. With the noble metal-free system, requiring hydrogen evolution rates comparable to that of the well-established Rh_xCr_2鈥?i>xO₃/Ga₂O₃ water splitting cocatalyst is achieved. Although the stability of the as-prepared ternary cocatalyst system appeared to be poor, the cocatalyst can be easily regenerated and stabilized by an oxygen treatment under ambient conditions. Furthermore, higher MoO_x loadings were found to be more active and showed improved stability. By means of careful characterization using X-ray-based spectroscopy and TEM, the function of the individual cocatalyst compounds was closely examined, suggesting synergetic interactions of molybdena and chromia stabilizing CuO against photoreduction. Although stability issues should be further addressed, this work highlights that multicomponent systems, which are well-studied in industrial processes for heterogeneous reactions and commonly used in various other fields of research, can be used in solar water splitting. In particular, molybdena-containing materials are discovered as a new class of earth-abundant cocatalysts for overall water-splitting.