Combining urea oxidation reaction(UOR) with hydrogen evolution reaction(HER) is an effective method for energy saving and highly efficient electrocatalytic hydrogen production. Herein, molybdenumincorporated cobalt ca...Combining urea oxidation reaction(UOR) with hydrogen evolution reaction(HER) is an effective method for energy saving and highly efficient electrocatalytic hydrogen production. Herein, molybdenumincorporated cobalt carbonate hydroxide nanoarrays(CoxMoyCH) are designed and synthesized as a bifunctional catalyst towards UOR and HER. Benefiting from the Mo doping, the dispersed nanoarray structure and redistributed electron density, the CoxMoyCH catalyst display outstanding catalytic performance and durability for both HER and UOR, affording the overpotential of 82 m V for HER and delivering a low potential of the 1.33 V for UOR(vs. reversible hydrogen electrode, RHE) to attain a current density of 10 m A cm^(-2), respectively. Remarkably, when CoxMoyCH was applied as bifunctional catalyst in a twoelectrode electrolyzer, a working voltage of 1.40 V is needed in urea-assisted water electrolysis at10 m A cm^(-2) and without apparent decline for 40 h, outperforming the working voltage of 1.51 V in conventional water electrolysis.展开更多
The overall energy efficiency of electrochemical systems is severely hindered by the traditional anodic oxygen evolution reaction(OER).Utilizing urea oxidation reaction(UOR)with lower thermodynamic potential to replac...The overall energy efficiency of electrochemical systems is severely hindered by the traditional anodic oxygen evolution reaction(OER).Utilizing urea oxidation reaction(UOR)with lower thermodynamic potential to replace OER provides a promising strategy to enhance the energy efficiency.Amorphous and heterojunctions electrocatalysts have been aroused extensive studies owing to their unique physicochemical properties and outperformed activity.Herein,we report a simple method to construct a novel crystalline-amorphous NiO-CrO_(x)heterojunction grown on Ni foam for UOR electrocatalyst.The NiO-CrO_(x)electrocatalyst displays excellent UOR performance with an ultralow working potential of 1.32 V at 10 mA·cm^(−2)and ultra-long stability about 5 days even at 100 mA·cm^(−2).In-situ Raman analysis and temperature-programmed desorption(TPD)measurement verify that the presence of the amorphous CrO_(x)phase can boost the reconstruction from NiO to active NiOOH species and enhance adsorption ability of urea molecule.Besides,the unique crystalline-amorphous interfaces are also benefit to improving the UOR performance.展开更多
基金financially supported by the National Natural Science Foundation of China(52025013,22121005)the 111 Project(B12015)+1 种基金Haihe Laboratory of Sustainable Chemical Transformationsthe Fundamental Research Funds for the Central Universities。
文摘Combining urea oxidation reaction(UOR) with hydrogen evolution reaction(HER) is an effective method for energy saving and highly efficient electrocatalytic hydrogen production. Herein, molybdenumincorporated cobalt carbonate hydroxide nanoarrays(CoxMoyCH) are designed and synthesized as a bifunctional catalyst towards UOR and HER. Benefiting from the Mo doping, the dispersed nanoarray structure and redistributed electron density, the CoxMoyCH catalyst display outstanding catalytic performance and durability for both HER and UOR, affording the overpotential of 82 m V for HER and delivering a low potential of the 1.33 V for UOR(vs. reversible hydrogen electrode, RHE) to attain a current density of 10 m A cm^(-2), respectively. Remarkably, when CoxMoyCH was applied as bifunctional catalyst in a twoelectrode electrolyzer, a working voltage of 1.40 V is needed in urea-assisted water electrolysis at10 m A cm^(-2) and without apparent decline for 40 h, outperforming the working voltage of 1.51 V in conventional water electrolysis.
基金supported by the National Natural Science Foundation of China(Nos.52025013 and 22121005)the 111 Project(No.B12015),Haihe Laboratory of Sustainable Chemical Transformations,and the Fundamental Research Funds for the Central Universities.
文摘The overall energy efficiency of electrochemical systems is severely hindered by the traditional anodic oxygen evolution reaction(OER).Utilizing urea oxidation reaction(UOR)with lower thermodynamic potential to replace OER provides a promising strategy to enhance the energy efficiency.Amorphous and heterojunctions electrocatalysts have been aroused extensive studies owing to their unique physicochemical properties and outperformed activity.Herein,we report a simple method to construct a novel crystalline-amorphous NiO-CrO_(x)heterojunction grown on Ni foam for UOR electrocatalyst.The NiO-CrO_(x)electrocatalyst displays excellent UOR performance with an ultralow working potential of 1.32 V at 10 mA·cm^(−2)and ultra-long stability about 5 days even at 100 mA·cm^(−2).In-situ Raman analysis and temperature-programmed desorption(TPD)measurement verify that the presence of the amorphous CrO_(x)phase can boost the reconstruction from NiO to active NiOOH species and enhance adsorption ability of urea molecule.Besides,the unique crystalline-amorphous interfaces are also benefit to improving the UOR performance.