Photochemical hydrogen evolution from aqueous triethanolamine solutions sensitized by binaphthol-modified titanium(IV) oxide under visible-light irradiation

Photochemical hydrogen evolution from aqueous triethanolamine solutions sensitized by binaphthol-modified titanium(IV) oxide under visible-light irradiation
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DOI:
10.1016/s1010-6030(03)00222-3
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发表时间:
2003-08-07
影响因子:
4.3
通讯作者:
Ohtani, B
Ohtani, B
中科院分区:
化学3区
文献类型:
--
作者:
Ikeda, S;Abe, C;Ohtani, B

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在回流乙醇溶液中,用具有阻转手性的双酚羟基二醇(bn(OH)(2))对二氧化钛(TiO 2)进行表面改性,形成深黄色的表面络合物,在波长低于约100 nm处有可见光吸收。550-600 nm。表面复合物的定量分析表明,在漫反射(DR)测量中在450 nm处的吸收强度几乎与其量成正比,并且其量强烈地依赖于TiO 2的表面羟基的量,但不依赖于TiO 2、金红石和金红石的晶体结构。BN(OH)(2)络合也适用于铂TiO 2驱动光催化分子氢(H-2)从脱气三乙醇胺溶液中的可见光照射下,波长甚至超过540 nm的演变。对于负载0.1 wt.%的BN(OH)(2)-改性的TiO 2(JRC-TiO-3),在450 nm处的光催化反应的光子效率估计为0.02铂金在这些实验结果的基础上,反应机理,其中包括可见光激发的表面络合物,从络合物的电子注入到TiO 2,和迁移的电子到铂沉积物,其中H+发生还原,得到H-2,被阐明。(C)2003 Elsevier Science B. V.保留所有权利。
Surface modification of titanium(IV) oxide (TiO2) powders with 1, 1-binaphthalene-2,2'-diol (bn(OH)(2)), having two phenolic hydroxyls and atropisomeric chirality, in refluxed ethanol led to the formation of a deep yellow-colored surface complex, giving visible-light absorption at a wavelength below ca. 550-600 nm. Quantitative analyses of the surface complex revealed that absorption intensity at 450 nm in diffuse reflection (DR) measurement was almost proportional to its amount and that its amount depended strongly on the amount of surface hydroxyl groups of TiO2 but not on the crystal structure of TiO2, anatase, and rutile. The bn(OH)(2) complexation was also applied to platinized TiO2 to drive photocatalytic molecular hydrogen (H-2) evolution from deaerated triethanolamine solutions under visible-light irradiation at a wavelength even longer than 540 nm. The photonic efficiency of the photocatalytic reaction at 450 nm was estimated to be 0.02% for bn(OH)(2)-modified TiO2 (JRC-TIO-3) loaded with 0.1 wt.% of platinum. On the basis of these experimental results, the reaction mechanism, which involves visible-light excitation of the surface complex, injection of electrons from the complex to TiO2, and migration of the electrons to platinum deposits, where reduction of H+ takes place to give H-2, was elucidated. (C) 2003 Elsevier Science B.V. All rights reserved.