Insights into elusive and cooperative multi-oxidant mechanisms in enabling catalytic methane-to-methanol conversion over atomically dispersed metals

• Published in: Inorganic chemistry frontiers Vol. 1; no. 6; pp. 1838 - 1851
• Main Authors: Zhang, Li-Long, Su, Yaqiong, Chen, Dandan, Wu, Hongguo, Xu, Feng, Li, Hu, Yang, Song
• Format: Journal Article
• Language: English
• Published: London Royal Society of Chemistry 14.03.2023
• Subjects: Catalytic converters; Conversion; Inorganic chemistry; Methane; Methanol; Nitrous oxide; Oxidation; Oxidizing agents
• ISSN: 2052-1553; 2052-1545; 2052-1553
• DOI: 10.1039/d3qi00079f

NO x is frequently invoked as an oxidant for direct selective conversion of methane into methanol (DSCMM), which has long been considered one of the holy grails in green chemistry. A challenge in studying the use of NO x in oxidizing methane is the interconversion of various NO x compounds as well as the easy formation of O 2 , rendering it difficult to draw firm conclusions on the oxidant. Here, we explicitly elucidate the strengths of using dual oxidants (NO and N 2 O) for DSCMM over various phosphotungstic acid-supported single-atom catalysts. A competitive but cooperative multi-functional protocol involving dual oxidants is proposed to enhance catalytic performance due to its overall strong CH 4 adsorption and thermodynamic favorability compared with normal mechanisms (single O 2 , N 2 O, or NO). The new cooperative multi-functional mechanism strategy is expected to motivate further research to elaborate on its potential advantages in DSCMM and other relevant catalytic systems. A cooperative multi-oxidant protocol was developed to be efficient for converting greenhouse gas (CH 4 ) and environmentally polluting gases (NO x ) into clean and renewable energy molecules (CH 3 OH).