Harnessing photocatalytic activity of mesoporous graphitic carbon nitride decorated by copper single-atom catalysts for oxidative dehydrogenation of N-heterocycles.

This work describes the application of Cu single-atom catalysts (SACs) for photocatalytic oxidative dehydrogenation of N-heterocyclic amines to the respective N-heteroaromatics through environmentally benign and sustainable pathways. The mesoporous graphitic carbon nitride (mpg-C3N4), prepared by the one-step pyrolysis method, possesses a lightweight material with a high surface area (95 m2 g-1) and an average pore diameter (3.6 nm). A simple microwave-assisted preparation method was employed to decorate Cu single-atom over mpg-C3N4 support. The Cu single-atom decorated on mpg-C3N4 support (Cu@mpg-C3N4) is characterized by various characterization techniques, including XRD, UV-visible spectrophotometry, HRTEM, HAADF-STEM with elemental mapping, AC-STEM, ICP-OES, XANES, EXAFS, and BET surface area. These characterization studies confirmed that the Cu@mpg-C3N4 catalyst exhibited high surface area, mesoporous nature, medium band gap, and low metal loading. The as-synthesized and well-characterized Cu@mpg-C3N4 single-atom photocatalyst is then evaluated for its efficacy in converting N-heterocycles into corresponding N-heteroaromatic compounds with excellent conversion and selectivity (>99 %). This transformation is achieved using water as a green solvent and a 30 W white light as a visible light source, demonstrating the catalyst's potential for sustainable and environmentally benign reactions.

Single-Atom Catalysts: A Sustainable Pathway for the Advanced Catalytic Applications.

A heterogeneous catalyst is a backbone of modern sustainable green industries; and understanding the relationship between its structure and properties is the key for its advancement. Recently, many upscaling synthesis strategies for the development of a variety of respectable control atomically precise heterogeneous catalysts are reported and explored for various important applications in catalysis for energy and environmental remediation. Precise atomic-scale control of catalysts has allowed to significantly increase activity, selectivity, and in some cases stability. This approach has proved to be relevant in various energy and environmental related technologies such as fuel cell, chemical reactors for organic synthesis, and environmental remediation. Therefore, this review aims to critically analyze the recent progress on single-atom catalysts (SACs) application in oxygen reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, and chemical and/or electrochemical organic transformations. Finally, opportunities that may open up in the future are summarized, along with suggesting new applications for possible exploitation of SACs.