The electrochemical CO_(2)reduction reaction(ECO_(2)RR)to formate is perceived as a technoeconomic pathway for transforming renewable electricity into fuels.However,the indeterminate mechanism underlying structural se...The electrochemical CO_(2)reduction reaction(ECO_(2)RR)to formate is perceived as a technoeconomic pathway for transforming renewable electricity into fuels.However,the indeterminate mechanism underlying structural self-reconstruction obstructs the strategic design of a high-performance In catalyst for the ECO_(2)RR.In this study,we chose InOOH as the model catalyst to illustrate the dynamic structure of In-based catalysts during reconstruction in the ECO_(2)RR.The findings of the current study indicate that the in situ electrochemical reconstruction of crystalline InOOH results in the creation of crystalline In clusters/InOOH,followed by In/InOOH heterostructures,and finally,metallic In over time.The efficiencies of the different phases conformed to the sequence:In clusters/InOOH>In/InOOH heterostructures>metallic In.This progression leads to a continuous drop in maximum current density and Faradaic efficiency from 29.6 mA/cm2 and 87%to 6.3 mA/cm^(2) and 75%,respectively with time extending to 7200 s,at-1.0 V relative to the reversible hydrogen electrode.Our in situ characterization and theoretical studies highlighted the crucial role of the In-cluster/InOOH interface in CO_(2)activation and conversion.展开更多
Electrochemical reductive exfoliation of graphite to few layered graphene(FLG) in presence of 1-ethyl-2,3-dimethyl imidazolium bis(trifluoromethylsulfonyl) imide ionic liquid and redox ionic liquid based ferrocene has...Electrochemical reductive exfoliation of graphite to few layered graphene(FLG) in presence of 1-ethyl-2,3-dimethyl imidazolium bis(trifluoromethylsulfonyl) imide ionic liquid and redox ionic liquid based ferrocene has been investigated. Thus, by applying a mild negative potential(-2.7 V vs. Fc/Fc^+) to carbon electrode in ionic liquid graphene flakes could be generated. The generated materials have been characterized by X-ray photoelectron spectroscopy, Raman spectroscopy, high resolution transmission electron microscopy and atomic force microscopy. XPS and Raman analysis show that the electrochemical reductive exfoliation provides the formation of FLG. The thickness of the resulting FLG was found to be ranged between 4 and1 nm. HR-TEM images reveal the formation of few graphene layers and in some cases single graphene layer was observed.Moreover, this electrochemical route conduces to the formation of ionic liquid functionalized FLG. Finally, the reductive exfoliation was further investigated in the presence of redox ionic liquid. XPS and electrochemical measurements confirm the presence of ferrocene.展开更多
基金supported by the National Natural Science Foundation of China[22006044]External Cooperation Program of Science and Technology Planning of Fujian Province[2023I0018]+1 种基金National Engineering Laboratory for Mobile Source Emission Control Technology[NELMS2020A03]Scientific Research Funds of Huaqiao University[605-50Y200270001].
文摘The electrochemical CO_(2)reduction reaction(ECO_(2)RR)to formate is perceived as a technoeconomic pathway for transforming renewable electricity into fuels.However,the indeterminate mechanism underlying structural self-reconstruction obstructs the strategic design of a high-performance In catalyst for the ECO_(2)RR.In this study,we chose InOOH as the model catalyst to illustrate the dynamic structure of In-based catalysts during reconstruction in the ECO_(2)RR.The findings of the current study indicate that the in situ electrochemical reconstruction of crystalline InOOH results in the creation of crystalline In clusters/InOOH,followed by In/InOOH heterostructures,and finally,metallic In over time.The efficiencies of the different phases conformed to the sequence:In clusters/InOOH>In/InOOH heterostructures>metallic In.This progression leads to a continuous drop in maximum current density and Faradaic efficiency from 29.6 mA/cm2 and 87%to 6.3 mA/cm^(2) and 75%,respectively with time extending to 7200 s,at-1.0 V relative to the reversible hydrogen electrode.Our in situ characterization and theoretical studies highlighted the crucial role of the In-cluster/InOOH interface in CO_(2)activation and conversion.
基金supported by the European Community Seventh Framework Programme(266391)
文摘Electrochemical reductive exfoliation of graphite to few layered graphene(FLG) in presence of 1-ethyl-2,3-dimethyl imidazolium bis(trifluoromethylsulfonyl) imide ionic liquid and redox ionic liquid based ferrocene has been investigated. Thus, by applying a mild negative potential(-2.7 V vs. Fc/Fc^+) to carbon electrode in ionic liquid graphene flakes could be generated. The generated materials have been characterized by X-ray photoelectron spectroscopy, Raman spectroscopy, high resolution transmission electron microscopy and atomic force microscopy. XPS and Raman analysis show that the electrochemical reductive exfoliation provides the formation of FLG. The thickness of the resulting FLG was found to be ranged between 4 and1 nm. HR-TEM images reveal the formation of few graphene layers and in some cases single graphene layer was observed.Moreover, this electrochemical route conduces to the formation of ionic liquid functionalized FLG. Finally, the reductive exfoliation was further investigated in the presence of redox ionic liquid. XPS and electrochemical measurements confirm the presence of ferrocene.