Efficient propane mineralization over unsaturated Pd cluster/CeO2 with prominent C-C cleavage capacity driven by inherent oxygen activation ability

J Hazard Mater. 2024 Jan 5:461:132509. doi: 10.1016/j.jhazmat.2023.132509. Epub 2023 Sep 12.

Abstract

Light alkanes extensively presented in industrial exhausts have led tremendous harm to the atmospheric environment and human health. However, the catalytic destruction of light alkanes generally operates at elevated temperatures and the consequent reaction by-products are inevitably produced. It is therefore of great significance to engineer catalysts with superior thermal stability, internal activity and selectivity. Herein, we developed a Pd cluster/CeO2 catalyst (Pdn/CeO2) by a scalable deposition precipitation strategy, which demonstrates unexpected activity and thermal stability in the presence of 5% H2O attributing to abundant unsaturated Pd metal sites and excellent oxygen dissociation performance. Pdn/CeO2 possesses a highly efficient C-C cleavage capability due to the persistent formation of a large number of oxygen vacancies. In comparison, the Pd1/CeO2 catalyst, which is preferential for C-H bond cleavage and inactive for C-C bond cracking, produces remarkable hazardous organic by-products such as propyne and propylene, inhibiting the continuous decomposition of propane. The present study sheds critical insights into engineering efficient and stable catalysts for light alkane destruction.

Keywords: C-C bond dissociation; Oxygen vacancies; Propane destruction; Selectivity; Thermal stability.