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首页> 外文期刊>Catalysis science & technology >Arrangement effect of the di-μ-oxo dimanganese catalyst and Ru(bpy)3~(2+) photoexcitation centers adsorbed on mica for visible-light-derived water oxidation
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Arrangement effect of the di-μ-oxo dimanganese catalyst and Ru(bpy)3~(2+) photoexcitation centers adsorbed on mica for visible-light-derived water oxidation

机译：Di-μ-oxo Dimanganese催化剂和RU（BPY）3〜（2+）光激发中心吸附在云母上的di-μoxooxo di-oxo

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A photosynthetic photosystem II (PS II) model was developed by adsorbing [(OH2)(terpy)Mnl"(n-0)2-Mn~(IV)(terpy)(OH2)]~(3+) (1, terpy = 2,2':6',2"-terpyridine) as an oxygen evolving center and Ru(bpy)3~(2+) (bpy = 2,2'-bipyridine) as a photoexcitation center onto mica. The mica adsorbates were prepared by three different methods; Adsorbate A was prepared by adsorption of 1 followed by Ru(bpy)3~(2+) on mica, and Adsorbates B and C were prepared by the opposite adsorption order and co-adsorption of 1 and Ru(bpy)3~(2+), respectively. The UV-visible diffuse reflectance (DR) spectroscopic data and emission decay measurements of the photoexcited Ru(bpy)3~(2+) suggested the different arrangements of 1 and Ru(bpy)3~(2+) among the three adsorbates in a mica interlayer. For Adsorbate A, Ru(bpy)3~(2+) could be adsorbed near the mica surface, being shallowly intercalated relative to 1. For Adsorbate B, 1 is adsorbed near the mica surface, Ru(bpy)3~(2+) being deeply intercalated relative to 1. For Adsorbate C, either 1 or Ru(bpy)3~(2+) could be randomly intercalated relative to the other adsorbates. In photochemical water oxidation experiments, a significant amount of O2 was evolved when visible light was used to irradiate an aqueous suspension of Adsorbate A containing a S208~(2-) electron acceptor in a liquid phase, whereas O2 was not evolved under the same conditions when using Adsorbates B and C. 1 is considered to work for photochemical water oxidation in Adsorbate A due to an efficient electron transport from deeply intercalated 1 to S2O8~(2-) ions in a liquid phase via Ru(bpy)3~(2+) photoexcitation near the mica adsorbate surface.
机译：通过吸附[（oh2）（terpy）mnl“（n-0）2-mn〜（iv）（iv）（terpy）（oh2）（oh2）]〜（1，terpy）（1，terpy） = 2,2'：6'，2“ - terpyridine）作为氧气进化中心，Ru（bpy）3〜（2+）（bpy = 2,2'-二吡啶）作为米卡的光激发中心。云母吸附物是通过三种不同的方法制备的。通过吸附1的吸附剂，然后在云母上的RU（BPY）3〜（2+）制备吸附物A，并通过相反的吸附顺序和1和RU（BPY）3〜（2 +），分别。紫外可见的弥散反射率（DR）光谱数据和光激发ru（bpy）3〜（2+）的发射衰减测量表明，1和RU（bpy）3〜（2+）的不同排列云母中间层。对于吸附物A，RU（BPY）3〜（2+）可以在云母表面附近吸附，相对于1.吸附物B，在云母表面附近被吸附1个，RU（BPY）3〜（2+（2+） ）相对于1的深度插入。对于吸附物C，可以随机插入1或RU（BPY）3〜（2+）相对于其他吸附物。在光化学水氧化实验中，当使用可见光来照射含有S208〜（2-）电子受体的吸附物A的水性悬浮液在液相中，而O2在相同的条件下未进化，则大量的O2进化。当使用吸附物B和C。1被认为可用于吸附A中的光化学水氧化，因为有效的电子从深度插入的1到S2O8〜（2-）离子在液相中通过RU（BPY）3〜（2）（2）（2） +）云母吸附材料表面附近的光激发。

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