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Published on: December 6, 2021
Enhancing Mass Transport and Charge Transfer in Carbon Nitride Photocatalysts for Efficient Benzylamine Oxidation
Zeming Chen1,2, Qiqi Sun1, Dandan Zheng1,2
1State Key Laboratory of Chemistry for NBC Hazards Protection, State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, China.
Abstract:
Polymeric carbon nitride is a promising photocatalyst for coupling benzylamine (BA) oxidation with hydrogen evolution. However, its efficiency is often limited by a low specific surface area, high defect density, inefficient charge separation, and poor mass transport. To address these challenges, we developed a hybrid template-molten salt strategy to synthesize crystalline mesoporous carbon nitride nanospheres (C-MCNs). The resulting C-MCNs architecture not only enhances mass transport but also reduces charge transfer losses, outperforming crystalline bulk carbon nitride (C-BCN) in mass transfer capability and exhibiting lower charge loss than amorphous mesoporous carbon nitride nanospheres (A-MCNs). The optimized C-MCNs exhibit exceptional photocatalytic performance, achieving N-benzylidenebenzylamine (NBI) production from BA with high selectivity (>99%) at a rate of 15.6 mmol g-1 h-1, alongside H2 generation at 15.9 mmol g-1 h-1. The hydrogen evolution rate with C-MCNs is 3.6 times and 8.2 times higher than that of C-BCN and A-MCNs, respectively. This work opens a pathway for the rational design of high-performance photocatalysts by introducing a hybrid template-molten salt strategy that enables synergistic control over crystallinity and nanostructure in carbon nitride.
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