Affiliation:
1. School of Marine Science and Engineering, State Key Laboratory of Marine Resource Utilization in South China Sea Hainan University Haikou Hainan 570228 China
2. Guangxi Key Laboratory of Electrochemical Energy Materials, College of Chemistry and Chemical Engineering, State Key Laboratory of Processing for NonFerrous Metal and Featured Materials Guangxi University 100 Daxue Road Nanning Guangxi 530004 China
Abstract
Comprehensive SummaryThe direct oxidation of methane (CH4) into high‐valued C1 oxygenates production has garnered increased attention in effectively using vast CH4 and alleviating the global energy crisis. However, due to the high cleavage energy of C—H bond and low polarity of CH4 molecule, it is difficult to activate the first C—H bond. Furthermore, C1 oxygenates are readily inclined to be oxidized to CO2, because their weaker C—H bond comparing with CH4 molecule, resulting in poor selectivity. Herein, we designed ultrathin PdxAuy alloy NWs supported on ZSM‐5 (Z‐5) to investigate the direct oxidation of CH4 to high value‐added oxygenate under mild conditions. By precisely adjusting the molar ratio of Pd/Au and alloying degree, Pd9Au1NWs/Z‐5 showed an excellent yield of 11.57 mmol·g–l·h–1 and the outstanding selectivity of 95.1% for C1 oxygenates (CH3OH, CH3OOH and HCOOH). The in‐situ spectroscopic and mechanism analysis proved that the enhanced catalytic performance of Pd9Au1NWs/Z‐5 was ascribed to the stable one‐dimensional nanostructure and the strong synergy effect with high alloying PdAu, which could increase the adsorption capacity of CH4 molecules on Pd atoms to promote the CH4 conversion. This work offers valuable insights into the design concept of high‐efficient catalysts and the structure‐activity relationship for the direct oxidation of CH4.