Nitrate-methanol co-electrolysis involving the cathodic nitrate reduction reaction(NO_(3)RR)combined with the anodic methanol oxidation reaction(MOR)is a viable way to synchronously produce ammonia(NH_(3))and formate ...Nitrate-methanol co-electrolysis involving the cathodic nitrate reduction reaction(NO_(3)RR)combined with the anodic methanol oxidation reaction(MOR)is a viable way to synchronously produce ammonia(NH_(3))and formate via gentle,sustainable and energy-saving“E-refining”and“E-reforming”means.An efficient bifunctional catalyst for the NO_(3)RR and MOR is pivotal to achieve such a goal.In this work,a nitrogen-doped carbon-encapsulated nickel iron phosphide hybrid(Ni_(2)FeP@NC)was prepared as a bifunctional catalyst for the NO_(3)RR and MOR,and its electrochemical performance for nitrate-methanol co-electrolysis was investigated.The Ni_(2)FeP@NC catalyst exhibited a high NH_(3) yield(0.47 mmol h^(-1) cm^(-2) at-0.35 V)and faradaic efficiency(FE,93%at-0.15 V)for the NO_(3)RR and simultaneously demonstrated high MOR efficiency for formate production(yield of 1.62 mmol h^(-1) cm^(-2) at 1.7 V and FE of around 95%).The bifunctional catalytic features of the nitrate-methanol co-electrolysis system enabled the concurrent production of NH_(3) and formate at low input voltage.This work provides a viable paradigm for pairwise electrosynthesis of valuable chemicals via“E-refining”and“E-reforming”through the rational design of bifunctional catalysts.展开更多
基金supported by NSFC(No.51802084)the 111 Project(No.D17007)Henan Center for Outstanding Oversea Scientists(No.GZS_(2)022017).
文摘Nitrate-methanol co-electrolysis involving the cathodic nitrate reduction reaction(NO_(3)RR)combined with the anodic methanol oxidation reaction(MOR)is a viable way to synchronously produce ammonia(NH_(3))and formate via gentle,sustainable and energy-saving“E-refining”and“E-reforming”means.An efficient bifunctional catalyst for the NO_(3)RR and MOR is pivotal to achieve such a goal.In this work,a nitrogen-doped carbon-encapsulated nickel iron phosphide hybrid(Ni_(2)FeP@NC)was prepared as a bifunctional catalyst for the NO_(3)RR and MOR,and its electrochemical performance for nitrate-methanol co-electrolysis was investigated.The Ni_(2)FeP@NC catalyst exhibited a high NH_(3) yield(0.47 mmol h^(-1) cm^(-2) at-0.35 V)and faradaic efficiency(FE,93%at-0.15 V)for the NO_(3)RR and simultaneously demonstrated high MOR efficiency for formate production(yield of 1.62 mmol h^(-1) cm^(-2) at 1.7 V and FE of around 95%).The bifunctional catalytic features of the nitrate-methanol co-electrolysis system enabled the concurrent production of NH_(3) and formate at low input voltage.This work provides a viable paradigm for pairwise electrosynthesis of valuable chemicals via“E-refining”and“E-reforming”through the rational design of bifunctional catalysts.