The green synthesis of nitrate(NO_(3)^(−))via electrocatalytic nitrogen oxidation reaction(NOR)is a promising strategy for artificial nitrogen fixation,which shows great advantages than traditional nitrate synthesis b...The green synthesis of nitrate(NO_(3)^(−))via electrocatalytic nitrogen oxidation reaction(NOR)is a promising strategy for artificial nitrogen fixation,which shows great advantages than traditional nitrate synthesis based on Haber–Bosch and Ostwald processes.But the poor N_(2)absorption,high bond energy of N≡N(941 kJ·mol^(−1)),and competing multi-electron-transfer oxygen evolution reaction(OER)limit the activity and selectivity.Herein,we fabricated MXene-derived irregular TiO_(2)−x nanoparticles anchored Cu nanowires(Cu-NWs)electrode for efficient electrocatalytic nitrogen oxidation,which exhibits a NO_(3)−yield of 62.50μg·h^(−1)·mgcat^(−1)and a Faradaic efficiency(FE)of 22.04%,and a significantly enhanced NO_(3)−yield of 92.63μg·h^(−1)·mgcat^(−1),and a FE of 40.58%under vacuum assistance.The TiO_(2)−x/Cu-NWs electrode also shows excellent reproducibility and stability under optimal experimental conditions.Moreover,a Zn-N_(2)reaction device was assembled with TiO_(2−x)/Cu-NWs as an anode and Zn plate as a cathode,obtaining an extremely high NO_(3)−yield of 156.25μg·h^(−1)·mgcat^(−1).The Zn-nitrate battery shows an open circuit voltage(OCV)of 1.35 V.This work provides novel strategies for enhancing the performance of ambient N_(2)oxidation to obtain higher NO_(3)^(−)yield.展开更多
基金the Natural Science Foundation of Shandong Province(No.ZR2021MB075)the National Natural Science Foundation of China(No.51602297).
文摘The green synthesis of nitrate(NO_(3)^(−))via electrocatalytic nitrogen oxidation reaction(NOR)is a promising strategy for artificial nitrogen fixation,which shows great advantages than traditional nitrate synthesis based on Haber–Bosch and Ostwald processes.But the poor N_(2)absorption,high bond energy of N≡N(941 kJ·mol^(−1)),and competing multi-electron-transfer oxygen evolution reaction(OER)limit the activity and selectivity.Herein,we fabricated MXene-derived irregular TiO_(2)−x nanoparticles anchored Cu nanowires(Cu-NWs)electrode for efficient electrocatalytic nitrogen oxidation,which exhibits a NO_(3)−yield of 62.50μg·h^(−1)·mgcat^(−1)and a Faradaic efficiency(FE)of 22.04%,and a significantly enhanced NO_(3)−yield of 92.63μg·h^(−1)·mgcat^(−1),and a FE of 40.58%under vacuum assistance.The TiO_(2)−x/Cu-NWs electrode also shows excellent reproducibility and stability under optimal experimental conditions.Moreover,a Zn-N_(2)reaction device was assembled with TiO_(2−x)/Cu-NWs as an anode and Zn plate as a cathode,obtaining an extremely high NO_(3)−yield of 156.25μg·h^(−1)·mgcat^(−1).The Zn-nitrate battery shows an open circuit voltage(OCV)of 1.35 V.This work provides novel strategies for enhancing the performance of ambient N_(2)oxidation to obtain higher NO_(3)^(−)yield.
