Influencing factors on heterogeneous water oxidation catalysis by di-μ-oxo dimanganese complex on mica as a synthetic model of photosystem II

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• 作者：Akinori Shoji (1)
  Masanari Hirahara (1)
  Hirosato Yamazaki (1)
  Masayuki Yagi (1) (2)
  
• 关键词：Water oxidation catalyst ; Di ; μ ; oxo dinuclear manganese complex ; Layer compounds ; Photosystem II
• 刊名：Research on Chemical Intermediates
• 出版年：2014
• 出版时间：November 2014
• 年：2014
• 卷：40
• 期：9
• 页码：3199-3208
• 全文大小：423 KB
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• 作者单位：Akinori Shoji (1)
  Masanari Hirahara (1)
  Hirosato Yamazaki (1)
  Masayuki Yagi (1) (2)
  
  1. Department of Materials Science and Technology, Faculty of Engineering and Center for Transdisciplinary Research, Niigata University, 8050 Ikarashi-2, Niigata, 950-2181, Japan
  2. Precursory Research for Embryonic Science and Technology (PRESTO), Japan Science and Technology Agency (JST), 4-1-8 Honcho, Kawaguchi, Saitama, 332-0012, Japan
  
• ISSN：1568-5675

文摘

The influencing factors on heterogeneous water oxidation catalysis (WOC) were investigated in a synthetic photosystem II model developed by adsorbing [(OH2)(terpy)MnIII(μ-O)2MnIV(terpy)(OH2)]3+ (terpy?=?2,2-6-2-terpyridine) (1) as an oxygen evolving center onto mica. For chemical WOC using a Ce4+ oxidant, the catalytic activity of 1 on mica increased by a factor of 2.3 or 1.4 by co-adsorption (0.015?mmol?g?) of redox-inactive trications of Al3+ or Ce3+ with 1 (0.15?mmol?g?), respectively, whereas it decreased by co-adsorption (0.25?mmol?g?) of excess Al3+ or Ce3+. The cooperative catalysis by two equivalents of the adsorbed 1 for water oxidation could be facilitated by enrichment of 1 by trications at their low co-adsorption conditions. The decreased catalytic activity at high trications co-adsorption conditions could be explained by impeded penetration of Ce4+ oxidant ions into a mica interlayer. For photochemical WOC containing a [Ru(bpy)3]2+ (bpy?=?2,2-bipyridine) photoexcitation center in mica, the drying treatment at 65?°C under the vacuum after 1 adsorption was required in adsorbate preparation, possibly to maintain favorable arrangement of 1 and [Ru(bpy)3]2+ in a mica interlayer. The drying treatment at 65?°C under the vacuum after [Ru(bpy)3]2+ adsorption inactivated the photochemical WOC. The proton-coupled electron transport from interior [Ru(bpy)3]2+ centers to ones near the surface in mica is considered to be suppressed by the drying treatment, which could be responsible for the inactivated photochemical WOC.