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Cercosporin-Photocatalyzed [4+1]- and [4+2]-Annulations of Azoalkenes Under Mild Conditions
Published on: July 17, 2020
Naphthalene Monoanhydride and Perylene Composites for Efficient Photocatalytic Hydrogen Evolution and Metal-Free
Anita Kumari1, Raj Sekhar Roy1, Ujjal K Gautam1
1Department of Chemical Sciences, Indian Institute of Science Education and Research (IISER) Mohali, Knowledge City, Sector 81, P.O. Manauli, Mohali, Punjab 140306, India.
Abstract:
This study explores the synthesis of two visible light active organic chromophore-based composites using naphthalene monoanhydride (Np) and 1,7-dibromoperylene monoanhydride diester (PMDE). These chromophores feature favorable optical and electronic properties and polyaromatic skeletons with anhydride functionalities that facilitate π-π interactions between the chromophore and polymeric carbon nitride (CN) or covalent connections of chromophores with NH2 groups of CN. Accordingly, heterogeneous chromophore-CN composite photocatalysts namely, Np/(c) and PMDE/(c) were prepared by adopting in situ calcination (c) and composites (a) and PMDE/(a) were prepared by ex situ physical adsorption (a) methods. In situ prepared Np/(c) and PMDE/(c) composites exhibited H2 evolution rates (HER) of 1069 and 705 μmol h-1 g-1, respectively, which are significantly higher than ex situ Np/(a) and PMDE/(a) composites with HER of 465 and 252 μmol h-1 g-1, respectively. These rates are 10, 7, 4.8, and 2.5 times higher than the bulk-CN, indicating the potential of these composites for efficient photocatalytic H2 evolution. Surface area normalized HER enhancements were 3.8, 5.3, 6.6, and 4.2 times higher for Np/(c), PMDE/(c), Np/(a), and PMDE/(a) respectively compared to bulk-CN. These composite photocatalysts exhibited excellent stabilities under prolonged photoirradiation, with H2 evolution consistently increasing with the light exposure time. Additionally, these metal-free heterogeneous composites demonstrated efficient photocatalytic activities towards oxidative amidation of aromatic aldehydes, with up to 80% product yields, establishing the prospects of combining homogeneous and heterogeneous entities in a metal-free active material in solar energy harvesting.
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