Proton exchange membrane(PEM)water electrolysis represents a promising technology for green hydrogen production,but its widespread deployment is greatly hindered by the indispensable usage of platinum group metal cata...Proton exchange membrane(PEM)water electrolysis represents a promising technology for green hydrogen production,but its widespread deployment is greatly hindered by the indispensable usage of platinum group metal catalysts,especially iridium(Ir)based materials for the energy-demanding oxygen evolution reaction(OER).Herein,we report a new sequential precipitation approach to the synthesis of mixed Ir-nickel(Ni)oxy-hydroxide supported on antimony-doped tin oxide(ATO)nanoparticles(IrNiyO_(x)/ATO,20 wt.%(Ir+Ni),y=0,1,2,and 3),aiming to reduce the utilisation of scarce and precious Ir while maintaining its good acidic OER performance.When tested in strongly acidic electrolyte(0.1 M HClO_(4)),the optimised IrNi1Ox/ATO shows a mass activity of 1.0 mAµgIr^(−1) and a large turnover frequency of 123 s^(−1) at an overpotential of 350 mV,as well as a comparatively small Tafel slope of 50 mV dec^(−1),better than the IrOx/ATO control,particularly with a markedly reduced Ir loading of only 19.7µgIr cm^(−2).Importantly,IrNi1O_(x)/ATO also exhibits substantially better catalytic stability than other reference catalysts,able to continuously catalyse acidic OER at 10 mA cm^(−2) for 15 h without obvious degradation.Our in-situ synchrotron-based x-ray absorption spectroscopy confirmed that the Ir^(3+)/Ir^(4+)species are the active sites for the acidic OER.Furthermore,the performance of IrNi1Ox/ATO was also preliminarily evaluated in a membrane electrode assembly,which shows better activity and stability than other reference catalysts.The IrNi1Ox/ATO reported in this work is a promising alternative to commercial IrO_(2) based catalysts for PEM electrolysis.展开更多
基金supported by the National Innovation Agency of Portugal through the project Baterias 2030(Grant No.POCI-01-0247-FEDER-046109)J R E would like to acknowledge the Fundación General CSIC’s ComFuturo programme which has received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement No.101034263+2 种基金The authors appreciate Dr Laura Simonelli and Dr Vlad Martin Diaconescu for their assistance in XAS measurements at the beamline BL22-CLÆSS,ALBA synchrotron(experiment AV-2022025706)R M is grateful to the Portuguese Foundation for Science and Technology(FCT)for the doctoral grant(Grant No.2021.06496.BD)R M and A M are grateful for the financial support from:LA/P/0045/2020,UIDB/00511/2020 and UIDP/00511/2020,funded by the national funds through FCT/MCTES(PIDDAC)。
文摘Proton exchange membrane(PEM)water electrolysis represents a promising technology for green hydrogen production,but its widespread deployment is greatly hindered by the indispensable usage of platinum group metal catalysts,especially iridium(Ir)based materials for the energy-demanding oxygen evolution reaction(OER).Herein,we report a new sequential precipitation approach to the synthesis of mixed Ir-nickel(Ni)oxy-hydroxide supported on antimony-doped tin oxide(ATO)nanoparticles(IrNiyO_(x)/ATO,20 wt.%(Ir+Ni),y=0,1,2,and 3),aiming to reduce the utilisation of scarce and precious Ir while maintaining its good acidic OER performance.When tested in strongly acidic electrolyte(0.1 M HClO_(4)),the optimised IrNi1Ox/ATO shows a mass activity of 1.0 mAµgIr^(−1) and a large turnover frequency of 123 s^(−1) at an overpotential of 350 mV,as well as a comparatively small Tafel slope of 50 mV dec^(−1),better than the IrOx/ATO control,particularly with a markedly reduced Ir loading of only 19.7µgIr cm^(−2).Importantly,IrNi1O_(x)/ATO also exhibits substantially better catalytic stability than other reference catalysts,able to continuously catalyse acidic OER at 10 mA cm^(−2) for 15 h without obvious degradation.Our in-situ synchrotron-based x-ray absorption spectroscopy confirmed that the Ir^(3+)/Ir^(4+)species are the active sites for the acidic OER.Furthermore,the performance of IrNi1Ox/ATO was also preliminarily evaluated in a membrane electrode assembly,which shows better activity and stability than other reference catalysts.The IrNi1Ox/ATO reported in this work is a promising alternative to commercial IrO_(2) based catalysts for PEM electrolysis.