One-Pot Synthesis of Hexamethylenetetramine Coupled with H2 Evolution from Methanol and Ammonia by a Pt/TiO2 Nanophotocatalyst

Weikun Chen; Xiaoying Liu; Hui Zheng; Xiao Fu; Youzhu Yuan

doi:10.1021/acsomega.2c01323

One-Pot Synthesis of Hexamethylenetetramine Coupled with H₂ Evolution from Methanol and Ammonia by a Pt/TiO₂ Nanophotocatalyst

ACS Omega. 2022 Jun 6;7(23):19614-19621. doi: 10.1021/acsomega.2c01323. eCollection 2022 Jun 14.

Authors

Weikun Chen¹, Xiaoying Liu¹, Hui Zheng¹, Xiao Fu¹, Youzhu Yuan¹

Affiliation

¹ State 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 g_cat ^-1 h^-1, respectively. This work provides a green and sustainable pathway for the photocatalytic HMT synthesis coupled with H₂ evolution under mild conditions.