Direct electrolysis of seawater offers a transformative technology for sustainable hydrogen production,circumventing the constraint of freshwater scarcity.However,the serious electrode corrosion and competitive chlori...Direct electrolysis of seawater offers a transformative technology for sustainable hydrogen production,circumventing the constraint of freshwater scarcity.However,the serious electrode corrosion and competitive chloride oxidation reactions make oxygen evolution reaction(OER)in seawater extremely challenging.Herein,the low-cost and scalable CoFe layered double hydroxides with Cl^(-)intercalation and decorated with Ce(OH)_(3)(named as CoFe-Cl^(-)/Ce(OH)_(3))catalyst is synthesized via rapid electrodeposition under ambient conditions,which is quickly reconstructed into a CeO_(2)decorated and Cl^(-)intercalated CoFeOOH(CoFeOOH-Cl^(-)/CeO_(2))during OER.Theoretical investigation reveals that Cl^(-)intercalation weakens the adsorption ability of Cl^(-)on Co/Fe atoms and hinders unfavorable coupling with chloride,thereby preventing the chlorine corrosion process and enhancing catalytic stability and activity.The CeO_(2)with hard Lewis acidity preferentially binds to OH-with harder Lewis base to ensure the OH-rich microenvironment around catalyst even under high current operating conditions,thus further enhancing stability and improving OER activity.The functionalized CoFe-Cl^(-)/Ce(OH)_(3)delivers 1000 mA cm^(-2)current density at only 329 mV overpotential with excellent stability for 1000 h under alkaline seawater.Electrochemical experiments elucidate the OER catalytic mechanism in which CeO_(2)serves as a co-catalyst for enriching OH-and CoFeOOH-Cl^(-)is the active species.Our work is a substantial step towards achieving massive and sustainable production of hydrogen fuel from immense seawater.展开更多
Water-soluble nitrite(NO_(2)^(-))in wastewater from agricultural and industrial activities poses ecological and health risks,and its electroreduction shows promise for ammonia(NH3)production,but energy losses from the...Water-soluble nitrite(NO_(2)^(-))in wastewater from agricultural and industrial activities poses ecological and health risks,and its electroreduction shows promise for ammonia(NH3)production,but energy losses from the hydrogen evolution reaction(HER)limit its overall efficiency.In this work,we report the use of CoFe-layered double hydroxides on three-dimensional(3D)TiO_(2) array(TiO_(2)@CoFe-LDH)as an effective electrocatalyst for NO_(2)-reduction.By offering superior *H species supply and hydroprocessing capability,this catalyst achieves an NH_(3) yield of 1056.4μmol·h^(-1)·cm^(-2) with a 97.4% Faradaic efficiency(FE)at-0.6 V and sustains FE above 87% across a range of applied potentials.Additionally,a 60-h simulated wastewater treatment experiment demonstrates its practical application potential.展开更多
基金financial support from the National Natural Science Foundation of China(52372173,52072034)。
文摘Direct electrolysis of seawater offers a transformative technology for sustainable hydrogen production,circumventing the constraint of freshwater scarcity.However,the serious electrode corrosion and competitive chloride oxidation reactions make oxygen evolution reaction(OER)in seawater extremely challenging.Herein,the low-cost and scalable CoFe layered double hydroxides with Cl^(-)intercalation and decorated with Ce(OH)_(3)(named as CoFe-Cl^(-)/Ce(OH)_(3))catalyst is synthesized via rapid electrodeposition under ambient conditions,which is quickly reconstructed into a CeO_(2)decorated and Cl^(-)intercalated CoFeOOH(CoFeOOH-Cl^(-)/CeO_(2))during OER.Theoretical investigation reveals that Cl^(-)intercalation weakens the adsorption ability of Cl^(-)on Co/Fe atoms and hinders unfavorable coupling with chloride,thereby preventing the chlorine corrosion process and enhancing catalytic stability and activity.The CeO_(2)with hard Lewis acidity preferentially binds to OH-with harder Lewis base to ensure the OH-rich microenvironment around catalyst even under high current operating conditions,thus further enhancing stability and improving OER activity.The functionalized CoFe-Cl^(-)/Ce(OH)_(3)delivers 1000 mA cm^(-2)current density at only 329 mV overpotential with excellent stability for 1000 h under alkaline seawater.Electrochemical experiments elucidate the OER catalytic mechanism in which CeO_(2)serves as a co-catalyst for enriching OH-and CoFeOOH-Cl^(-)is the active species.Our work is a substantial step towards achieving massive and sustainable production of hydrogen fuel from immense seawater.
基金supported by the Sichuan Province Youth Fund Project(No.2025ZNSFSC0897).
文摘Water-soluble nitrite(NO_(2)^(-))in wastewater from agricultural and industrial activities poses ecological and health risks,and its electroreduction shows promise for ammonia(NH3)production,but energy losses from the hydrogen evolution reaction(HER)limit its overall efficiency.In this work,we report the use of CoFe-layered double hydroxides on three-dimensional(3D)TiO_(2) array(TiO_(2)@CoFe-LDH)as an effective electrocatalyst for NO_(2)-reduction.By offering superior *H species supply and hydroprocessing capability,this catalyst achieves an NH_(3) yield of 1056.4μmol·h^(-1)·cm^(-2) with a 97.4% Faradaic efficiency(FE)at-0.6 V and sustains FE above 87% across a range of applied potentials.Additionally,a 60-h simulated wastewater treatment experiment demonstrates its practical application potential.
