One-Pot Synthesis of Hexamethylenetetramine Coupled with H2 Evolution from Methanol and Ammonia by a Pt/TiO2
Weikun Chen1, Xiaoying Liu1, Hui Zheng1
1State Key Laboratory of Physical Chemistry of Solid Surfaces, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
Abstract:
Utilization of solar energy for photocatalytic H2 evolution coupled with value-added chemical synthesis is a promising avenue to address energy and environmental crises. Here, we report the hexamethylenetetramine (HMT) synthesis and H2 evolution from methanol and ammonia in one pot using a nanophotocatalyst of the conventional semiconductor TiO2 (P25) loaded with Pt (Pt/P25). The addition of ammonia inhibits byproduct ethylene glycol formation, promotes H2 evolution, and obtains HMT with high selectivity (>99.0%). The Pt valence state is regulated by calcination and reduction treatment, indicating that Pt/P25 is a stable catalyst for the photocatalytic synthesis of HMT from methanol and ammonia. The optimized formation rates of H2 and HMT are 71.53 and 11.39 mmol gcat -1 h-1, respectively. This work provides a green and sustainable pathway for the photocatalytic HMT synthesis coupled with H2 evolution under mild conditions.
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