Niobium Oxide Nanoscrolls as Building Blocks for Dye-Sensitized Hydrogen Production from Water under Visible Light Irradiation
Niobium Oxide Nanoscrolls as Building Blocks for Dye-Sensitized Hydrogen Production from Water under Visible Light Irradiation
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DOI：
10.1021/cm801807b
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发表时间：
2008-11-11
影响因子：
8.6
通讯作者：
Mallouk, Thomas E.
中科院分区：
文献类型：
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作者：
Maeda, Kazuhiko;Eguchi, Miharu;Mallouk, Thomas E.
研究了六铌酸钾纳米卷（NS-K4 Nb 6 O 17）作为可见光驱动的水制氢（λ> 420 nm）的结构单元，以三（2，2 '-联吡啶）氯化钌（Ru（bpy）（3）（2+））为敏化剂，乙二胺四乙酸（EDTA）为电子给体。NS-K4 Nb 6 O 17的表面在pH 3-11下带负电荷，使得阳离子Ru（bpy）（3）（2+）分子能够有效地吸附到表面上，允许快速激发态电子和随后的H-2释放，而敏化剂和氧化物表面之间没有任何化学键连接。可见光H-2的生产率在nanoscroll为基础的系统是10倍以上，类似敏化K4 Nb 6 O 17。这种差异可以主要归因于在纳米卷的情况下Ru（bpy）（3）（2+）的强吸附。最大的光催化反应性被发现在一个狭窄的范围内的pH值和Pt负载。这项研究强调了单晶氧化物纳米片作为可见光驱动的H-2从水中生产的光系统的组成部分的实用性。
Potassium hexaniobate nanoscrolls (NS-K4Nb6O17) formed by exfoliation of lamellar K4Nb6O17 were studied as building blocks for visible-light-driven H-2 production (lambda > 420 nm) from water using tris(2,2'-bipyridyl)ruthenium(II) chloride (Ru(bpy)(3)(2+)) as a sensitizer and ethylenediaminetetraacetic acid (EDTA) as an electron donor. The surface of NS-K4Nb6O17 is negatively charged at pH 3-11, enabling cationic Ru(bpy)(3)(2+) molecules to be efficiently adsorbed onto the surface, allowing for rapid excited-state electron and subsequent H-2 evolution without any chemical bond linkage between the sensitizer and the oxide surface. The rate of visible light H-2 production in the nanoscroll-based system is 10 times higher than that of similarly sensitized K4Nb6O17. The difference can be primarily attributed to the strong adsorption of Ru(bpy)(3)(2+) in the case of the nanoscrolls. The maximum photocatalytic reactivity is found over a narrow range of pH and Pt-loading. This study highlights the utility of single-crystalline oxide nanosheets as components of photosystems for visible-light-driven H-2 production from water.