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
The production of hydrogen through water electrolysis(WE)from renewable electricity is set to revolutionise the energy sector that is at present heavily dependent on fossil fuels.However,there is still a pressing need...The production of hydrogen through water electrolysis(WE)from renewable electricity is set to revolutionise the energy sector that is at present heavily dependent on fossil fuels.However,there is still a pressing need to develop advanced electrocatalysts able to show high activity and withstand industrially-relevant operating conditions for a prolonged period of time.In this regard,high entropy materials(HEMs),including high entropy alloys and high entropy oxides,comprising five or more homogeneously distributed metal components,have emerged as a new class of electrocatalysts owing to their unique properties such as low atomic diffusion,structural stability,a wide variety of adsorption energies and multi-component synergy,making them promising catalysts for challenging electrochemical reactions,including those involved in WE.This review begins with a brief overview about WE technologies and a short introduction to HEMs including their synthesis and general physicochemical properties,followed by a nearly exhaustive summary of HEMs catalysts reported so far for the hydrogen evolution reaction,the oxygen evolution reaction and the overall water splitting in both alkaline and acidic conditions.The review concludes with a brief summary and an outlook about the future development of HEM-based catalysts and further research to be done to understand the catalytic mechanism and eventually deploy HEMs in practical water electrolysers.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.
基金the financial support of the Mobilizador Programme(via Baterias 2030 project,Grant No.POCI-010247-FEDER-046109)from the National Innovation Agency of Portugalpartially supported by the start-up project of the Songshan lake Materials Laboratory(Grant No.Y2D1051Z311).
文摘The production of hydrogen through water electrolysis(WE)from renewable electricity is set to revolutionise the energy sector that is at present heavily dependent on fossil fuels.However,there is still a pressing need to develop advanced electrocatalysts able to show high activity and withstand industrially-relevant operating conditions for a prolonged period of time.In this regard,high entropy materials(HEMs),including high entropy alloys and high entropy oxides,comprising five or more homogeneously distributed metal components,have emerged as a new class of electrocatalysts owing to their unique properties such as low atomic diffusion,structural stability,a wide variety of adsorption energies and multi-component synergy,making them promising catalysts for challenging electrochemical reactions,including those involved in WE.This review begins with a brief overview about WE technologies and a short introduction to HEMs including their synthesis and general physicochemical properties,followed by a nearly exhaustive summary of HEMs catalysts reported so far for the hydrogen evolution reaction,the oxygen evolution reaction and the overall water splitting in both alkaline and acidic conditions.The review concludes with a brief summary and an outlook about the future development of HEM-based catalysts and further research to be done to understand the catalytic mechanism and eventually deploy HEMs in practical water electrolysers.