Zhao Guofeng, Ni Jiayong, Si Jiaqi, Sun Weidong, Lu Yong
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, No. 3663 North Zhongshan Road, Shanghai, 200062, China.
Institute of Eco-Chongming, No. 20 Cuiniao Road, Shanghai, 202162, China.
Chemphyschem. 2022 Nov 18;23(22):e202200365. doi: 10.1002/cphc.202200365. Epub 2022 Sep 1.
Oxidative coupling of methane (OCM) catalyzed by MnO -Na WO -based catalysts has great industrial potential to convert CH directly to C products, but the high light-off temperature is a big challenge to OCM commercialization. The reaction mechanism studies disclosed that O /CH -activation relevant "Mn ↔Mn " redox cycle is tightly linked with the catalyst light-off. One concept is thus put forward that the OCM light-off temperature could be lowered once a "Mn ↔Mn " redox cycle was established to be triggered at low temperature over MnO -Na WO -based catalysts. The relevant studies in recent years are reviewed, showing that the establishment of low-temperature light-off "Mn ↔Mn " redox cycle over the MnO -Na WO -based catalysts indeed works effectively toward a low-temperature light-off OCM process. Moreover, three perspectives for the OCM industrialization are discussed based on this concept, including monolithic catalyst, fluidized-bed method and chemical-looping process.
由MnO-Na₂WO₄基催化剂催化的甲烷氧化偶联（OCM）在将CH₄直接转化为C₂产物方面具有巨大的工业潜力，但高起燃温度是OCM商业化面临的一大挑战。反应机理研究表明，与O₂/CH₄活化相关的“Mn³⁺↔Mn⁴⁺”氧化还原循环与催化剂的起燃紧密相关。因此提出了一个概念，即在MnO-Na₂WO₄基催化剂上，如果能在低温下建立并触发“Mn³⁺↔Mn⁴⁺”氧化还原循环，那么OCM的起燃温度就可以降低。本文综述了近年来的相关研究，结果表明在MnO-Na₂WO₄基催化剂上建立低温起燃的“Mn³⁺↔Mn⁴⁺”氧化还原循环确实对低温起燃的OCM过程有效。此外，基于这一概念讨论了OCM工业化的三个方向，包括整体式催化剂、流化床法和化学链过程。
