Methane, the most stable alkane, is significantly more stable than its partial oxidation products. This renders the highly selective conversion of CH4 to CH3OH an extremely intractable challenge, especially when using molecular oxygen as the oxidant. In this work, we synthesized a bimetallic-modified zeolite composite catalyst (PdCo bimetallic nanoclusters supported on H-ZSM-5 molecular sieve, denoted as PdCo@H-ZSM-5) via a simple impregnation method. PdCo@H-ZSM-5 can efficiently activate H2 and O2 to highly selectively oxidize CH4 to CH3OH under mild conditions (70°C), achieving a remarkable CH3OH yield of 2349 µmol gcat -1 h-1 (249 mmol gPd -1 h-1). Significantly, PdCo@H-ZSM-5 is the sole catalyst reported to date that can achieve over 99% CH3OH selectivity in the oxidation of CH4 by molecular oxygen under mild conditions. This work is expected to inspire new technologies for industrial CH4 to CH3OH conversion, promoting more sustainable chemistry and engineering. Furthermore, the low-energy consumption, high-efficiency activated oxygen catalyst eliminates the necessity for transporting and storing highly concentrated hydrogen peroxide, serving as a foundation for other green oxidation reactions.
Wang et al. (Tue,) studied this question.