Sadigh Akbari Sina, Karadas Ferdi
Department of Chemistry, Faculty of Science, Bilkent University, 06800 Ankara, Turkey.
UNAM-National Nanotechnology Research Center, Institute of Materials Science and Nanotechnology, Bilkent University, 06800 Ankara, Turkey.
ACS Omega. 2024 Feb 9;9(7):8585-8593. doi: 10.1021/acsomega.4c00217. eCollection 2024 Feb 20.
Derivation of 3D coordination polymers to produce active catalysts has been a feasible strategy to achieve a precise coordination sphere for the catalytic site. This study demonstrates the partial conversion of a 3D cobalt dicyanamide coordination polymer, Co-dca, to a 2D layered hydroxide-oxyhydroxide structure under photocatalytic conditions. The catalyst exhibits an activity as high as 28.3 mmol h g in the presence of a [Ru(bpy)]/triethylamine (TEA) couple to maintain it for at least 12 h. Photocatalytic and characterization studies reveal that the dicyanamide ligand within the coordination polymer is crucial for governing modification and achieving a superior H evolution rate. Moreover, we observed the critical role of TEA as the hydrolyzing agent for the transformation process. This study displays that the metal dicyanamides can be utilized as templates for preparing active and robust catalysts.
衍生三维配位聚合物以制备活性催化剂一直是实现催化位点精确配位环境的可行策略。本研究表明，在光催化条件下，三维钴双氰胺配位聚合物Co-dca可部分转化为二维层状氢氧化物 - 羟基氧化物结构。在存在[Ru(bpy)]/三乙胺（TEA）对的情况下，该催化剂表现出高达28.3 mmol h g的活性，并能保持至少12小时。光催化和表征研究表明，配位聚合物中的双氰胺配体对于控制改性和实现优异的析氢速率至关重要。此外，我们观察到TEA作为转化过程中的水解剂的关键作用。本研究表明，金属双氰胺可作为制备活性和稳健催化剂的模板。
