Kurnosenko Sergei A, Voytovich Vladimir V, Silyukov Oleg I, Rodionov Ivan A, Zvereva Irina A
Department of Chemical Thermodynamics and Kinetics, Institute of Chemistry, Saint Petersburg State University, 199034 Saint Petersburg, Russia.
Nanomaterials (Basel). 2022 Aug 7;12(15):2717. doi: 10.3390/nano12152717.
Nowadays, the efficient conversion of plant biomass components (alcohols, carbohydrates, etc.) into more energy-intensive fuels, such as hydrogen, is one of the urgent scientific and technological problems. The present study is the first one focused on the photoinduced hydrogen evolution from aqueous D-glucose and D-xylose using layered perovskite-like oxides HCaNbO, HLaTiO, and their organically modified derivatives that have previously proven themselves as highly active photocatalysts. The photocatalytic performance was investigated for the bare compounds and products of their surface modification with a 1 mass. % Pt cocatalyst. The photocatalytic experiments followed an innovative scheme including dark stages as well as the control of the reaction suspension's pH and composition. The study has revealed that the inorganic-organic derivatives of the layered perovskite-like oxides can provide efficient conversion of carbohydrates into hydrogen fuel, being up to 8.3 times more active than the unmodified materials and reaching apparent quantum efficiency of 8.8%. Based on new and previously obtained data, it was shown that the oxides' interlayer space functions as an additional reaction zone in the photocatalytic hydrogen production and the contribution of this zone to the overall activity is dependent on the steric characteristics of the sacrificial agent used.
如今，将植物生物质成分（醇类、碳水化合物等）高效转化为能量密度更高的燃料，如氢气，是紧迫的科技问题之一。本研究首次聚焦于使用层状钙钛矿型氧化物HCaNbO、HLaTiO及其有机改性衍生物从D - 葡萄糖和D - 木糖水溶液中光致产氢，这些材料此前已证明自身是高活性光催化剂。研究了裸化合物及其用1质量%铂助催化剂进行表面改性后的产物的光催化性能。光催化实验采用了一种创新方案，包括黑暗阶段以及对反应悬浮液pH值和组成的控制。研究表明，层状钙钛矿型氧化物的无机 - 有机衍生物能够实现碳水化合物向氢燃料的高效转化，活性比未改性材料高出8.3倍，表观量子效率达到8.8%。基于新获得的数据以及之前的数据表明，氧化物的层间空间在光催化产氢过程中起到额外反应区的作用，该区域对整体活性的贡献取决于所使用牺牲剂的空间特性。
