Solvent-free photocatalytic propane oxidation to acetone with heterogenized decatungstate #470
Authors
Yuhan Zhang, Jan Paul Menzel, Cristina Decavoli, Xingxu Yan, Rabiya Naveed, Muchun Fei, James R Wilkes, Min Li, Yucheng Yuan, Jier Huang, Xiaoqing Pan, Victor S Batista, Gary W Brudvig, Dunwei Wang
Abstract
The direct and selective oxidation of light alkanes into value-added liquid chemicals under mild conditions remains a long-standing challenge in catalysis. Here, we report a heterogeneous photocatalyst based on site-isolated decatungstate (DT) anions immobilized on SBA-15 via a silatrane linker (sil-DT). Under UV-light irradiation at room temperature and ambient pressure, the catalyst selectively oxidizes propane to acetone and exhibits an acetone production rate of 11.2 mmol gDT−1 h−1, a total liquid product selectivity of 89.0%, and an acetone fraction of 69.0% within the liquid products. In contrast, bulk sodium DT (NaDT) shows negligible activity under identical conditions. Spectroscopic and computational studies reveal that the high catalytic performance arises from the uniform dispersion and site isolation of DT species, which retain the photophysical properties of their homogeneous counterparts. This work demonstrates the critical role of molecular dispersion in enabling selective light-driven alkane oxidation and offers a sustainable route for propane valorization.