In this study,we prepared Ti/IrO2–ZrO2 electrodes with different ZrO2 contents using zirconium-n-butoxide(C16H36O4Zr)and chloroiridic acid(H2IrCl6)via a sol–gel route.To explore the effect of ZrO2 content on the sur...In this study,we prepared Ti/IrO2–ZrO2 electrodes with different ZrO2 contents using zirconium-n-butoxide(C16H36O4Zr)and chloroiridic acid(H2IrCl6)via a sol–gel route.To explore the effect of ZrO2 content on the surface properties and electrochemical behavior of electrodes,we performed physical characterizations and electrochemical measurements.The obtained results revealed that the binary oxide coating was composed of rutile IrO2,amorphous ZrO2,and an IrO2–ZrO2 solid solution.The IrO2–ZrO2 binary oxide coatings exhibited cracked structures with flat regions.A slight incorporation of ZrO2 promoted the crystallization of the active component IrO2.However,the crystallization of IrO2 was hindered when the added ZrO2 content was greater than 30at%.The appropriate incorporation of ZrO2 enhanced the electrocatalytic performance of the pure IrO2 coating.The Ti/70at%IrO2–30at%ZrO2 electrode,with its large active surface area,improved electrocatalytic activity,long service lifetime,and especially,lower cost,is the most effective for promoting oxygen evolution in sulfuric acid solution.展开更多
IrO2 and IrRuOx(Ir:Ru 60:40 at%),supported by 50 wt%onto titania nanotubes(TNTs)and(3 at%Nb)Nb-doped titania nanotubes(Nb-TNTs),as electrocatalysts for the oxygen evolution reaction(OER),were synthesized and character...IrO2 and IrRuOx(Ir:Ru 60:40 at%),supported by 50 wt%onto titania nanotubes(TNTs)and(3 at%Nb)Nb-doped titania nanotubes(Nb-TNTs),as electrocatalysts for the oxygen evolution reaction(OER),were synthesized and characterized by means of structural,surface analytical and electrochemical techniques.Nb doping of titania significantly increased the surface area of the support from 145(TNTs)to 260 m2g-1(Nb-TNTs),which was significantly higher than those of the Nb-doped titania supports previously reported in the literature.The surface analytical techniques showed good dispersion of the catalysts onto the supports.The X-ray photoelectron spectroscopy analyses showed that Nb was mainly in the form of Nb(IV)species,the suitable form to behave as a donor introducing free electrons to the conduction band of titania.The redox transitions of the cyclic voltammograms,in agreement with the XPS results,were found to be reversible.Despite the supported materials presented bigger crystallite sizes than the unsupported ones,the total number of active sites of the former was also higher due to their better catalyst dispersion.Considering the outer and the total charges of the cyclic voltammograms in the range 0.1–1.4 V,stability and electrode potentials at given current densities,the preferred catalyst was Ir O2 supported on the Nb-TNTs.The electrode potentials corresponding to given current densities were between the smallest ones given in the literature despite the small oxide loading used in this work and its Nb doping,thus making the Nb-TNTs-supported IrO2 catalyst a promising candidate for the OER.The good dispersion of IrO2,high specific surface area of the Nb-doped supports,accessibility of the electroactive centers,increased stability due to Nb doping and electron donor properties of the Nb(IV)oxide species were considered the main reasons for its good performance.展开更多
基金financially supported by the National Natural Science Foundation of China (Nos. U1802253, 51974025 and 51674026)the Guangxi Innovation-Driven Development Project (No. AA18242042-1)+1 种基金the Beijing Natural Science Foundation of China (No. 2182040)the Fundamental Research Funds for the Central Universities (FRF22TT-19-001)
摘要In this study,we prepared Ti/IrO2–ZrO2 electrodes with different ZrO2 contents using zirconium-n-butoxide(C16H36O4Zr)and chloroiridic acid(H2IrCl6)via a sol–gel route.To explore the effect of ZrO2 content on the surface properties and electrochemical behavior of electrodes,we performed physical characterizations and electrochemical measurements.The obtained results revealed that the binary oxide coating was composed of rutile IrO2,amorphous ZrO2,and an IrO2–ZrO2 solid solution.The IrO2–ZrO2 binary oxide coatings exhibited cracked structures with flat regions.A slight incorporation of ZrO2 promoted the crystallization of the active component IrO2.However,the crystallization of IrO2 was hindered when the added ZrO2 content was greater than 30at%.The appropriate incorporation of ZrO2 enhanced the electrocatalytic performance of the pure IrO2 coating.The Ti/70at%IrO2–30at%ZrO2 electrode,with its large active surface area,improved electrocatalytic activity,long service lifetime,and especially,lower cost,is the most effective for promoting oxygen evolution in sulfuric acid solution.
摘要IrO2 and IrRuOx(Ir:Ru 60:40 at%),supported by 50 wt%onto titania nanotubes(TNTs)and(3 at%Nb)Nb-doped titania nanotubes(Nb-TNTs),as electrocatalysts for the oxygen evolution reaction(OER),were synthesized and characterized by means of structural,surface analytical and electrochemical techniques.Nb doping of titania significantly increased the surface area of the support from 145(TNTs)to 260 m2g-1(Nb-TNTs),which was significantly higher than those of the Nb-doped titania supports previously reported in the literature.The surface analytical techniques showed good dispersion of the catalysts onto the supports.The X-ray photoelectron spectroscopy analyses showed that Nb was mainly in the form of Nb(IV)species,the suitable form to behave as a donor introducing free electrons to the conduction band of titania.The redox transitions of the cyclic voltammograms,in agreement with the XPS results,were found to be reversible.Despite the supported materials presented bigger crystallite sizes than the unsupported ones,the total number of active sites of the former was also higher due to their better catalyst dispersion.Considering the outer and the total charges of the cyclic voltammograms in the range 0.1–1.4 V,stability and electrode potentials at given current densities,the preferred catalyst was Ir O2 supported on the Nb-TNTs.The electrode potentials corresponding to given current densities were between the smallest ones given in the literature despite the small oxide loading used in this work and its Nb doping,thus making the Nb-TNTs-supported IrO2 catalyst a promising candidate for the OER.The good dispersion of IrO2,high specific surface area of the Nb-doped supports,accessibility of the electroactive centers,increased stability due to Nb doping and electron donor properties of the Nb(IV)oxide species were considered the main reasons for its good performance.