Selective C–H Bond Activation in Propane with Molecular Oxygen over Cu(I)-ZSM-5 at Ambient Conditions
Hai‐Sheng Su, Yiwei Liu, Hao Tian, Dinghui Chen, Qikai Shen, Xiaoxia Chang, Qi Lu, Bingjun Xu
Abstract
Selective activation of C–H bonds in light alkanes under mild conditions is challenging but holds the promise of efficient upgrading of abundant hydrocarbons. In this work, we report the conversion of propane to propylene with ∼95% selectivity on Cu(I)-ZSM-5 with O 2 at room temperature and pressure. The intraporous Cu(I) species was oxidized to Cu(II) during the reaction but could be regenerated with H 2 at 220 °C. Diffuse reflectance ultraviolet spectroscopy indicated the presence of both Cu + -O 2 and Cu 2 (μ-O 2 ) 2+ species in the zeolite pores during the reaction, and electron paramagnetic resonance results showed that propane activation occurred via a radical-mediated pathway distinct from that with H 2 O 2 as the oxidant. Correlation between spectroscopic and reactivity results on Cu(I)-ZSM-5 with different Cu loadings suggests that the isolated intraporous Cu(I) species is the main active species in propane activation.