当前位置：
X-MOL 学术
›
J. Phys. Chem. C
›
论文详情
Our official English website, www.x-mol.net, welcomes your
feedback! (Note: you will need to create a separate account there.)
Tetrathiafulvalene Scaffold-Based Sensitizer on Hierarchical Porous TiO2: Efficient Light-Harvesting Material for Hydrogen Production
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2018-12-26 , DOI: 10.1021/acs.jpcc.8b08787 Amritanjali Tiwari 1 , Naresh Duvva , Vempuluru Navakoteswara Rao 2 , Shankar Muthukonda Venkatakrishnan 2 , Lingamallu Giribabu 1 , Ujjwal Pal 1
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2018-12-26 , DOI: 10.1021/acs.jpcc.8b08787 Amritanjali Tiwari 1 , Naresh Duvva , Vempuluru Navakoteswara Rao 2 , Shankar Muthukonda Venkatakrishnan 2 , Lingamallu Giribabu 1 , Ujjwal Pal 1
Affiliation
|
In this work, a photochemical device that contains thioalkyl-substituted tetrathiafulvalene dyes and hierarchical porous TiO2 has been designed and successfully employed in visible light-driven hydrogen production. The design strategy boosts up the desirable photophysical properties of catalysts and is well supported by optical, electrochemical, and computational studies. The introduction of thioalkyl-substituted tetrathiafulvalene dyes as light-harvesting sensitizers onto the porous TiO2 triggers unprecedented high rate of hydrogen evolution. This study focuses on the role of thiafulvalene scaffold, which can promote ultrafast interfacial electron injection from excited-state dye into the hierarchical porous TiO2 conduction band. The purposeful construction of this integrated composite G3T3 (dye content 1.0 μmol in 10 mg Pt-TiO2 composite) significantly increases the hydrogen production rate of 24 560 μmol h–1 gcat–1 with high apparent quantum yield ∼41%. In the study, the absorption onset of both sensitizers extends up to 500 nm in solution and 600 nm on hierarchical porous TiO2. Density functional theory in the present study described that the highest occupied molecular orbital levels are delocalized on anthracene as well as on tetrathiafulvalene donor units and that lowest unoccupied molecular orbital covers the carboxylate anchoring group in both dyes. This study unveiled for the first time that a tetrathiafulvalene scaffold in porous TiO2 attributes to positive synergistic effects in hydrogen production.
中文翻译：
四层多孔TiO 2上基于四硫富瓦烯骨架的增敏剂：高效的产氢光收集材料
在这项工作中，包含硫代烷基取代的四硫富瓦烯染料和分级多孔TiO 2的光化学装置已被设计并成功用于可见光驱动的制氢中。该设计策略提高了催化剂的理想光物理性能，并得到了光学，电化学和计算研究的充分支持。将硫代烷基取代的四硫富富瓦烯染料作为光敏敏化剂引入到多孔TiO 2上引发了前所未有的高氢释放速率。这项研究侧重于噻富瓦烯骨架的作用，该骨架可以促进从激发态染料到分级多孔TiO 2的超快速界面电子注入。导带。这种有目的的复合材料G3T3的构造（10 mg Pt-TiO 2复合物中的染料含量为1.0μmol ）显着提高了24 560μmolh –1 g cat –1的产氢率，表观量子产率高达〜41％。在研究中，两种增敏剂在溶液中的吸收起始延伸至500 nm，在分层多孔TiO 2上的吸收起始延伸至600 nm。。本研究中的密度泛函理论描述了在蒽以及四硫富瓦烯供体单元上最高占据的分子轨道水平是离域的，并且在两种染料中，最低的未占据分子轨道覆盖了羧酸盐锚定基团。这项研究首次揭示了多孔TiO 2中的四硫富瓦烯骨架在制氢中具有积极的协同作用。
更新日期：2018-12-28
中文翻译：
四层多孔TiO 2上基于四硫富瓦烯骨架的增敏剂：高效的产氢光收集材料
在这项工作中，包含硫代烷基取代的四硫富瓦烯染料和分级多孔TiO 2的光化学装置已被设计并成功用于可见光驱动的制氢中。该设计策略提高了催化剂的理想光物理性能，并得到了光学，电化学和计算研究的充分支持。将硫代烷基取代的四硫富富瓦烯染料作为光敏敏化剂引入到多孔TiO 2上引发了前所未有的高氢释放速率。这项研究侧重于噻富瓦烯骨架的作用，该骨架可以促进从激发态染料到分级多孔TiO 2的超快速界面电子注入。导带。这种有目的的复合材料G3T3的构造（10 mg Pt-TiO 2复合物中的染料含量为1.0μmol ）显着提高了24 560μmolh –1 g cat –1的产氢率，表观量子产率高达〜41％。在研究中，两种增敏剂在溶液中的吸收起始延伸至500 nm，在分层多孔TiO 2上的吸收起始延伸至600 nm。。本研究中的密度泛函理论描述了在蒽以及四硫富瓦烯供体单元上最高占据的分子轨道水平是离域的，并且在两种染料中，最低的未占据分子轨道覆盖了羧酸盐锚定基团。这项研究首次揭示了多孔TiO 2中的四硫富瓦烯骨架在制氢中具有积极的协同作用。
京公网安备 11010802027423号