Electrocatalytic nitrate reduction to ammonia(NRA)under ambient conditions is significant for carbonneutral synthetic fuels.Nevertheless,the lack of efficient electrocatalysts with tunable nanostructure for NRA remain...Electrocatalytic nitrate reduction to ammonia(NRA)under ambient conditions is significant for carbonneutral synthetic fuels.Nevertheless,the lack of efficient electrocatalysts with tunable nanostructure for NRA remains a grand challenge.Herein,Nb WO_(6)nanosheets with oxygen vacancy(NbWO_(6-x))was demonstrated via thermal treatment and exfoliation with NH_(3)selectivity of 86.8%and Faradaic efficiency of85.7%toward NRA.^(1)H nuclear magnetic resonance spectra coupled with^(15)N isotope labeling experiments proved that NH_(3)originated from NO_(3)^-.The function of oxygen vacancy was revealed by computational studies in NRA.Moreover,the reaction mechanism and pathway of NRA could be deduced based on the results of online differential electrochemical mass spectrometry(DEMS).This work provides a selective NH_(3)generation strategy to decarbonize the energy-chemical sector,bridging the gap between batteries and biofuels.展开更多
基金the supports from the National Natural Science Foundation of China(NSFC,Nos.22074104 and 51978491)National Program for Support of Top-notch Young Professionals+3 种基金the Fundamental Research Funds for the Central Universities(No.2022-4-ZD-07)“Shuguang Scholar Program”(No.17SG52)by Shanghai Education Development FoundationShanghai Municipal Education Commission,Liaoning Provincial Natural Science Fund Project(No.2019-ZD-0550)Scientific Research Foundation of Shanghai Institute of Technology(No.YJ2021-24)。
文摘Electrocatalytic nitrate reduction to ammonia(NRA)under ambient conditions is significant for carbonneutral synthetic fuels.Nevertheless,the lack of efficient electrocatalysts with tunable nanostructure for NRA remains a grand challenge.Herein,Nb WO_(6)nanosheets with oxygen vacancy(NbWO_(6-x))was demonstrated via thermal treatment and exfoliation with NH_(3)selectivity of 86.8%and Faradaic efficiency of85.7%toward NRA.^(1)H nuclear magnetic resonance spectra coupled with^(15)N isotope labeling experiments proved that NH_(3)originated from NO_(3)^-.The function of oxygen vacancy was revealed by computational studies in NRA.Moreover,the reaction mechanism and pathway of NRA could be deduced based on the results of online differential electrochemical mass spectrometry(DEMS).This work provides a selective NH_(3)generation strategy to decarbonize the energy-chemical sector,bridging the gap between batteries and biofuels.
