Chen Xin, Krajewska Aleksandra M, McGuinness Cormac, Lynes Amy, McAteer David, Berner Nina, Duesberg Georg, Coleman Jonathan N, McDonald Aidan R
School of Chemistry, CRANN/AMBER Nanoscience Institute, Trinity College Dublin, The University of Dublin, College Green, Dublin, 2, Ireland.
School of Physics and CRANN/AMBER Nanoscience Institute, Trinity College Dublin, The University of Dublin, College Green, Dublin, 2, Ireland.
Chemistry. 2021 Jan 13;27(3):984-992. doi: 10.1002/chem.202002615. Epub 2020 Dec 7.
Covalently tethering photosensitizers to catalytically active 1T-MoS surfaces holds great promise for the solar-driven hydrogen evolution reaction (HER). Herein, we report the preparation of two new Ru -complex-functionalized MoS hybrids [Ru (bpy) (phen)]-MoS and [Ru (bpy) (py)Cl]-MoS . The influence of covalent functionalization of chemically exfoliated 1T-MoS with coordinating ligands and Ru complexes on the HER activity and photo-electrochemical performance of this dye-sensitized system was studied systematically. We find that the photo-electrochemical performance of this Ru -complex-sensitized MoS system is highly dependent on the surface extent of photosensitizers and the catalytic activity of functionalized MoS . The latter was strongly affected by the number and the kind of functional groups. Our results underline the tunability of the photovoltage generation in this dye-sensitized MoS system by manipulation of the surface functionalities, which provides a practical guidance for smart design of future dye-sensitized MoS hydrogen production devices towards improved the photofuel conversion efficiency.
将光敏剂共价连接到具有催化活性的1T-MoS表面对于太阳能驱动的析氢反应（HER）具有巨大潜力。在此，我们报告了两种新型Ru-配合物功能化的MoS杂化物[Ru(bpy)(phen)]-MoS和[Ru(bpy)(py)Cl]-MoS的制备。系统研究了用配位配体和Ru配合物对化学剥离的1T-MoS进行共价功能化对该染料敏化体系的HER活性和光电化学性能的影响。我们发现，这种Ru-配合物敏化的MoS体系的光电化学性能高度依赖于光敏剂的表面覆盖程度和功能化MoS的催化活性。后者受到官能团数量和种类的强烈影响。我们的结果强调了通过操纵表面功能来调节该染料敏化MoS体系中光电压产生的可能性，这为未来智能设计染料敏化MoS制氢装置以提高光燃料转换效率提供了实际指导。
