Green hydrogen is identified as one of the prime clean energy carriers due to its high energy density and a zero emission of CO_(2).A possible solution for the transport of H_(2)in a safe and low-cost way is in the fo...Green hydrogen is identified as one of the prime clean energy carriers due to its high energy density and a zero emission of CO_(2).A possible solution for the transport of H_(2)in a safe and low-cost way is in the form of liquid organic hydrogen carriers(LOHCs).As an alternative to loading LOHC with H_(2)via a two-step procedure involving preliminary electrolytic production of H_(2)and subsequent chemical hydrogenation of the LOHC,we explore here the possibility of electrochemical hydrogen storage(EHS)via conversion of proton of a proton donor into a hydrogen atom involved in covalent bonds with the LOHC(R)via a protoncoupled electron transfer(PCET)reaction:2nH^(+)+2ne^(-)+Rox■n H_(2)^(0)Rred.We chose 9-fluorenone/fluorenol(Fnone/Fnol)conversion as such a model PCET reaction.The electrochemical activation of Fnone via two sequential electron transfers was monitored with in-situ and operando spectroscopies in absence and in presence of different alcohols as proton donors of different reactivity,which enabled us to both quantify and get the mechanistic insight on PCET.The possibility of hydrogen extraction from the loaded carrier molecule was illustrated by chemical activation.展开更多
基金financially supported by the Swedish Research Council(grant 2016-05990)the Knut and Alice Wallenberg Foundation(H2O2 and Cellfion)the Swedish Government Strategic Research Area in Materials Science on Advanced Functional Materials at Link?ping University(Faculty Grant SFO-Mat-Li U No.200900971)。
文摘Green hydrogen is identified as one of the prime clean energy carriers due to its high energy density and a zero emission of CO_(2).A possible solution for the transport of H_(2)in a safe and low-cost way is in the form of liquid organic hydrogen carriers(LOHCs).As an alternative to loading LOHC with H_(2)via a two-step procedure involving preliminary electrolytic production of H_(2)and subsequent chemical hydrogenation of the LOHC,we explore here the possibility of electrochemical hydrogen storage(EHS)via conversion of proton of a proton donor into a hydrogen atom involved in covalent bonds with the LOHC(R)via a protoncoupled electron transfer(PCET)reaction:2nH^(+)+2ne^(-)+Rox■n H_(2)^(0)Rred.We chose 9-fluorenone/fluorenol(Fnone/Fnol)conversion as such a model PCET reaction.The electrochemical activation of Fnone via two sequential electron transfers was monitored with in-situ and operando spectroscopies in absence and in presence of different alcohols as proton donors of different reactivity,which enabled us to both quantify and get the mechanistic insight on PCET.The possibility of hydrogen extraction from the loaded carrier molecule was illustrated by chemical activation.
