Quantum yields for sacrificial hydrogen generation from saccharides over a Pt-loaded TiO2 photocatalyst
作者:Masahide Yasuda、Ryo Kurogi、Tomoko Matsumoto
DOI:10.1007/s11164-015-2253-5
日期:2016.4
Much attention is paid to sacrificial hydrogen generation from saccharides over a Pt-loaded titanium oxide (Pt/TiO2) from the viewpoint of being a renewable energy alternative to petroleum-based fuels. Here, monosaccharides such as glucose, gluconic acid, galactose, sorbose, fructose, mannose, and disaccharides such as sucrose and cellobiose as well as related compounds such as ascorbic acid and sugar alcohols (xylitol and sorbitol) were used as sacrificial agents (R–H) in order to determine quantum yields (Φ) for hydrogen evolution. From double-reciprocal plots of Φ to the concentration of R–H, we obtained the limiting quantum yield in an infinite concentration of R–H. The limiting quantum yields were determined to be of similar values (0.058–0.168) for monosaccharides. Moreover, the rate constant (k R) for the hydrogen abstraction by hydroxyl radical from saccharides were obtained from the double reciprocal plots. It was found that the k R value of glucose was larger compared to galactose, mannose, sorbose, and fructose, which were the stereo and structural isomers of glucose.
从可再生能源替代石油燃料的角度来看,针对负载铂的二氧化钛(Pt/TiO2)催化剂,牺牲性氢气生成反应受到广泛关注。本文使用了单糖(如葡萄糖、葡萄糖酸、半乳糖、山梨糖、果糖、甘露糖)和双糖(如蔗糖和纤维二糖),以及相关化合物(如抗坏血酸和糖醇,例如木糖醇与山梨醇)作为牺牲剂(R–H),以确定氢气释放的量子产率(Φ)。通过Φ与R–H浓度的双倒数图,我们得到了在无限浓度R–H下的极限量子产率。单糖的极限量子产率被确定为相似值(0.058–0.168)。此外,通过双倒数图获得了氢氧根自由基从糖类中抽取氢的速率常数(k R)。结果发现,葡萄糖的k R值大于半乳糖、甘露糖、山梨糖和果糖,这些是葡萄糖的立体异构体和结构异构体。