Xie Yu, Cheng Jiawei, Wang Wangyang, Han Yaoyao, Fan Qiyuan, Li Hui, Cheng Kang, Zhang Qinghong, Wang Ye
State Key Laboratory of Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan, 030006, China.
Angew Chem Int Ed Engl. 2025 Jul;64(29):e202503767. doi: 10.1002/anie.202503767. Epub 2025 Apr 14.
The oxidative coupling of methane (OCM) is an attractive approach for methane transformations, but achieving a satisfactory combination of activity and selectivity remains challenging, even with the promising Mn-NaWO/SiO catalyst. Herein, we demonstrate that nanoscale separation of Mn-based and NaWO-based phases results in a highly efficient catalyst, achieving a remarkable 79% selectivity for C-C hydrocarbons at a 32% CH conversion at 775 °C, outperforming most previously reported catalysts. Our studies reveal that MnWO phases with adjustable surface Mn/W ratios and redox activities are more effective for the selective activation of O, thereby enhancing the OCM of CH. The assembly of MnWO and NaWO/SiO components in nanoscale proximity significantly promotes the formation of C-C hydrocarbons by suppressing deep oxidation. We propose a bifunctional mechanism involving the transfer of active oxygen species from MnWO to NaWO/SiO, which induces selective activation and coupling of CH on the NaWO/SiO surface.