A convenient method for methane(CH_(4))direct conversion to methanol(CH_(3)OH)is of great significance to use methane-rich resources,especially clathrates and stranded shale gas resources located in remote regions.The...A convenient method for methane(CH_(4))direct conversion to methanol(CH_(3)OH)is of great significance to use methane-rich resources,especially clathrates and stranded shale gas resources located in remote regions.Theoretically,the activation of CH_(4) and the selectivity to the CH_(3)OH product are challenging due to the extreme stability of CH_(4) and relatively high reactivity of CH_(3)OH.The state-of-the-art‘methane reforming-methanol synthesis’process adopts a two-step strategy to avoid the further reaction of CH_(3)OH under the harsh conditions required for CH_(4) activation.In the electrochemical field,researchers are trying to develop conversion pathways under mild conditions.They have found suitable catalysts to activate the C–H bonds in methane with the help of external charge and have designed the electrode reactions to continuously generate certain active oxygen species.These active oxygen species attack the activated methane and convert it to CH_(3)OH,with the benefit of avoiding over-oxidation of CH_(3)OH,and thus obtain a high conversion efficiency of CH_(4) to CH_(3)OH.This mini-review focuses on the advantages and challenges of electrochemical conversion of CH4 to CH_(3)OH,especially the strategies for supplying electro-generated active oxygen species in-situ to react with the activated methane.展开更多
Ammonia, primarily made with Haber-Bosch process developed in 1909 and winning two Nobel prizes, is a promising noncarbon fuel for preventing global warming of 1.5 °C above pre-industrial levels. However,the unde...Ammonia, primarily made with Haber-Bosch process developed in 1909 and winning two Nobel prizes, is a promising noncarbon fuel for preventing global warming of 1.5 °C above pre-industrial levels. However,the undesired characteristics of the process, including high carbon footprint, necessitate alternative ammonia synthesis methods, and among them is chemical looping ammonia production(CLAP) that uses nitrogen carrier materials and operates at atmospheric pressure with high product selectivity and energy efficiency. To date, neither a systematic review nor a perspective in nitrogen carriers and CLAP has been reported in the critical area. Thus, this work not only assesses the previous results of CLAP but also provides perspectives towards the future of CLAP. It classifies, characterizes, and holistically analyzes the fundamentally different CLAP pathways and discusses the ways of further improving the CLAP performance with the assistance of plasma technology and artificial intelligence(AI).展开更多
基金support from National Science Foundation of China(No.22075012).
文摘A convenient method for methane(CH_(4))direct conversion to methanol(CH_(3)OH)is of great significance to use methane-rich resources,especially clathrates and stranded shale gas resources located in remote regions.Theoretically,the activation of CH_(4) and the selectivity to the CH_(3)OH product are challenging due to the extreme stability of CH_(4) and relatively high reactivity of CH_(3)OH.The state-of-the-art‘methane reforming-methanol synthesis’process adopts a two-step strategy to avoid the further reaction of CH_(3)OH under the harsh conditions required for CH_(4) activation.In the electrochemical field,researchers are trying to develop conversion pathways under mild conditions.They have found suitable catalysts to activate the C–H bonds in methane with the help of external charge and have designed the electrode reactions to continuously generate certain active oxygen species.These active oxygen species attack the activated methane and convert it to CH_(3)OH,with the benefit of avoiding over-oxidation of CH_(3)OH,and thus obtain a high conversion efficiency of CH_(4) to CH_(3)OH.This mini-review focuses on the advantages and challenges of electrochemical conversion of CH4 to CH_(3)OH,especially the strategies for supplying electro-generated active oxygen species in-situ to react with the activated methane.
基金supported by the DNL Cooperation Fund,CAS(DNL180402)the support from the University of Wyoming。
文摘Ammonia, primarily made with Haber-Bosch process developed in 1909 and winning two Nobel prizes, is a promising noncarbon fuel for preventing global warming of 1.5 °C above pre-industrial levels. However,the undesired characteristics of the process, including high carbon footprint, necessitate alternative ammonia synthesis methods, and among them is chemical looping ammonia production(CLAP) that uses nitrogen carrier materials and operates at atmospheric pressure with high product selectivity and energy efficiency. To date, neither a systematic review nor a perspective in nitrogen carriers and CLAP has been reported in the critical area. Thus, this work not only assesses the previous results of CLAP but also provides perspectives towards the future of CLAP. It classifies, characterizes, and holistically analyzes the fundamentally different CLAP pathways and discusses the ways of further improving the CLAP performance with the assistance of plasma technology and artificial intelligence(AI).