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
Conducting nanocomposites of poly （methyl methacrylate） （PMMA） and antimony doped tin oxide （ATO） were prepared by solution blending. The influences of ATO content on the electrical conductivity, thermal stabili...Conducting nanocomposites of poly （methyl methacrylate） （PMMA） and antimony doped tin oxide （ATO） were prepared by solution blending. The influences of ATO content on the electrical conductivity, thermal stability, and mechanical properties of the nanocomposites were investigated. A homogeneous dispersion of silane coupling agent modified ATO was achieved in PMMA matrix as evidenced by scanning electron microscopy. The resultant PMMA/silane-ATO nanocomposites were electrically conductive with significant conductivity enhancement at 4 wt pct. It was found that the composition at 4 wt pct ATO gave the higher tensile strength. Furthermore, it gave the largest elongation at break value among all the compositions. Thermal stability of the nanocomposites was remarkably enhanced by the incorporation of silane-ATO.展开更多
Antimony doped tin oxide（ATO） thin films have been prepared by pulsed laser deposition（PLD） method.The intrinsic effect of Sb dopant,including the Sb content,transition degree between Sb（3＋） and Sb（5＋） and c...Antimony doped tin oxide（ATO） thin films have been prepared by pulsed laser deposition（PLD） method.The intrinsic effect of Sb dopant,including the Sb content,transition degree between Sb（3＋） and Sb（5＋） and crystallinity on the electrical and optical properties of the ATO thin films is mainly investigated.It is suggested that the transition degree of Sb（3＋） towards Sb（5＋）（Sb（5＋）/Sb（3＋） ratio） is determined by Sb content.When the Sb content is increased to 12 at%,the Sb（5＋）/Sb（3＋） ratio reaches the highest value of 2.05,corresponding to the resistivity of 2.70×10（-3） Ω·cm.Meanwhile,the Burstein-Moss effect caused by the increase of carrier concentration is observed and the band gap of the ATO thin films is broadened to 4.0 eV when the Sb content is increased to 12 at%,corresponding to the highest average optical transmittance of 92%.Comprehensively considering the combination of electrical and optical properties,the ATO thin films deposited with Sb content of 12 at%exhibit the best properties with the highest ＂figure of merit＂ of 3.85×10（-3） Ω（-1）.Finally,an antimony selenide（Sb_2Se_3） heterojunction solar cell prototype with the ATO thin film as the anode has been prepared,and a power conversion efficiency of 0.83%has been achieved.展开更多
The Ti/SnO2-Sb-Mo electrodes doped with different molar ratios of molybdenum（Mo） were prepared by sol—gel method in order to investigate the effect of Mo on the characterization of Ti/SnO2-Sb—Mo electrodes.X-ray d...The Ti/SnO2-Sb-Mo electrodes doped with different molar ratios of molybdenum（Mo） were prepared by sol—gel method in order to investigate the effect of Mo on the characterization of Ti/SnO2-Sb—Mo electrodes.X-ray diffraction（XRD）,field-emission scanning electron microscopy（FE-SEM）,energy dispersive spectrometry（EDS）,and linear scanning voltammetry（LSV） were used to scrutinize the coating material and the electrochemical activity.The concentration of phenol,the value of total organic carbon（TOC）,the mineralization current efficiency（MCE） and the ultraviolet—visible spectroscopy（UV-Vis） spectrum of phenol solution were measured over the electrochemical degradation process of phenol to confirm the phenol degradation characterization of Ti/SnO2-Sb-Mo electrodes.Results showed that the electrode at the Mo content of 1 at.%provided optimal catalytic activity for phenol degradation and the longest life time.The removal percentage of phenol and TOC were 99.62%and82.67%,respectively.The Ti/SnO2-Sb-Mo electrode with 1 at.%of Mo reached maximum MCE of phenol oxidation.The kinetic investigation of phenol and TOC degradation displayed the pseudo-first order reaction model.The Ti/SnO2-Sb-Mo electrode coating with 7 at.%Mo presented the highest oxygen evolution overpotential,indicating the diverse effects for different Mo molar ratio doping.展开更多
Surfactant-free and binder-free antimony-doped tin oxide （ATO） transparent conducting thin films were fabricated through spin coating and rapid annealing processes, in which nanosheets were assembled into a compact ...Surfactant-free and binder-free antimony-doped tin oxide （ATO） transparent conducting thin films were fabricated through spin coating and rapid annealing processes, in which nanosheets were assembled into a compact structure via self-contracting high pressure. The mechanism of this compact thin film for- mation was further proposed and analyzed. The compact ATO thin film had a low root mean square （RMS） roughness of 5.03 nm. This surfactant-free and binder-free compact ATO thin film delivered low resistivity of 3.04 × 10^-2 Ω cm, stable resistivity which only increased 13% after exposing in 65% RH air for half a month, high transmittance of 92.70% at 550 nm, and high band gap energy of 4.07 eV. This effective strategy will provide new insight into the synthesis of low-cost and high-performance compact thin films.展开更多
Developing efficient catalysts toward the oxygen evolution reaction(OER)is important for water splitting and rechargeable metal-air batteries.Although NiFe oxides are considered as potentially applicable catalysts in ...Developing efficient catalysts toward the oxygen evolution reaction(OER)is important for water splitting and rechargeable metal-air batteries.Although NiFe oxides are considered as potentially applicable catalysts in the alkaline media,there are still a limited numbers of researches working on membrane electrode assembly(MEA)fed with pure water due to their poor electrical conductivity.In this work,antimony doped tin oxide(ATO)has been employed as conductive supports where NiFe layered double hydroxide uniformly dispersed[named NiFe-LDH(layered double hydroxide)/ATO].The catalysts have been synthesized by a one-step co-precipitation method,and then NiFe-LDH/ATO-air plasma was obtained through mild air plasma treatment.According to XPS analysis,binding energies of Ni2p and Fe2p were shifted negatively.Moreover,a new signal of low oxygen coordination appeared on O1s spectrum after air plasma treatment.These XPS results indicated that oxygen vacancies(Ov)were generated after air plasma treatment.Electrochemical measurement indicated that the vacancy-rich NiFe-LDH/ATO-air plasma exhibited better performance than NiFe-LDH/ATO not only in 1 mol/L KOH solutions but also in an alkaline polymer electrolyte water electrolyzer(APEWE)fed with deionized water.This work provides a feasible way to design practical catalysts used in electrochemical energy conversion systems by choosing corrosion resistance supports and defect engineering.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.
文摘Conducting nanocomposites of poly （methyl methacrylate） （PMMA） and antimony doped tin oxide （ATO） were prepared by solution blending. The influences of ATO content on the electrical conductivity, thermal stability, and mechanical properties of the nanocomposites were investigated. A homogeneous dispersion of silane coupling agent modified ATO was achieved in PMMA matrix as evidenced by scanning electron microscopy. The resultant PMMA/silane-ATO nanocomposites were electrically conductive with significant conductivity enhancement at 4 wt pct. It was found that the composition at 4 wt pct ATO gave the higher tensile strength. Furthermore, it gave the largest elongation at break value among all the compositions. Thermal stability of the nanocomposites was remarkably enhanced by the incorporation of silane-ATO.
基金Funded by the International Science&Technology Cooperation Program of China(No.2011DFA52650)the"111"Project(No.B13035)+1 种基金the National Natural Science Foundation of China(No.51521001)the Fundamental Research Funds for the Central Universities
文摘Antimony doped tin oxide（ATO） thin films have been prepared by pulsed laser deposition（PLD） method.The intrinsic effect of Sb dopant,including the Sb content,transition degree between Sb（3＋） and Sb（5＋） and crystallinity on the electrical and optical properties of the ATO thin films is mainly investigated.It is suggested that the transition degree of Sb（3＋） towards Sb（5＋）（Sb（5＋）/Sb（3＋） ratio） is determined by Sb content.When the Sb content is increased to 12 at%,the Sb（5＋）/Sb（3＋） ratio reaches the highest value of 2.05,corresponding to the resistivity of 2.70×10（-3） Ω·cm.Meanwhile,the Burstein-Moss effect caused by the increase of carrier concentration is observed and the band gap of the ATO thin films is broadened to 4.0 eV when the Sb content is increased to 12 at%,corresponding to the highest average optical transmittance of 92%.Comprehensively considering the combination of electrical and optical properties,the ATO thin films deposited with Sb content of 12 at%exhibit the best properties with the highest ＂figure of merit＂ of 3.85×10（-3） Ω（-1）.Finally,an antimony selenide（Sb_2Se_3） heterojunction solar cell prototype with the ATO thin film as the anode has been prepared,and a power conversion efficiency of 0.83%has been achieved.
基金financial support from the China Environmental Protection Foundation,Geping Green ActionLiaoning Environmental Research and Education Fund "123 Project"(Grant No.CEPF2012-123-2-10)
文摘The Ti/SnO2-Sb-Mo electrodes doped with different molar ratios of molybdenum（Mo） were prepared by sol—gel method in order to investigate the effect of Mo on the characterization of Ti/SnO2-Sb—Mo electrodes.X-ray diffraction（XRD）,field-emission scanning electron microscopy（FE-SEM）,energy dispersive spectrometry（EDS）,and linear scanning voltammetry（LSV） were used to scrutinize the coating material and the electrochemical activity.The concentration of phenol,the value of total organic carbon（TOC）,the mineralization current efficiency（MCE） and the ultraviolet—visible spectroscopy（UV-Vis） spectrum of phenol solution were measured over the electrochemical degradation process of phenol to confirm the phenol degradation characterization of Ti/SnO2-Sb-Mo electrodes.Results showed that the electrode at the Mo content of 1 at.%provided optimal catalytic activity for phenol degradation and the longest life time.The removal percentage of phenol and TOC were 99.62%and82.67%,respectively.The Ti/SnO2-Sb-Mo electrode with 1 at.%of Mo reached maximum MCE of phenol oxidation.The kinetic investigation of phenol and TOC degradation displayed the pseudo-first order reaction model.The Ti/SnO2-Sb-Mo electrode coating with 7 at.%Mo presented the highest oxygen evolution overpotential,indicating the diverse effects for different Mo molar ratio doping.
文摘Surfactant-free and binder-free antimony-doped tin oxide （ATO） transparent conducting thin films were fabricated through spin coating and rapid annealing processes, in which nanosheets were assembled into a compact structure via self-contracting high pressure. The mechanism of this compact thin film for- mation was further proposed and analyzed. The compact ATO thin film had a low root mean square （RMS） roughness of 5.03 nm. This surfactant-free and binder-free compact ATO thin film delivered low resistivity of 3.04 × 10^-2 Ω cm, stable resistivity which only increased 13% after exposing in 65% RH air for half a month, high transmittance of 92.70% at 550 nm, and high band gap energy of 4.07 eV. This effective strategy will provide new insight into the synthesis of low-cost and high-performance compact thin films.
基金This work was supported by the National Natural Science Foundation of China(Nos.21872108,21633008)the National Key Research and Development Program of China(No.2016YFB0101203)the Fund of the Wuhan University Innovation Team,China(Nos.2042017kf0232,2042020kf1073,2042019kf0270).
文摘Developing efficient catalysts toward the oxygen evolution reaction(OER)is important for water splitting and rechargeable metal-air batteries.Although NiFe oxides are considered as potentially applicable catalysts in the alkaline media,there are still a limited numbers of researches working on membrane electrode assembly(MEA)fed with pure water due to their poor electrical conductivity.In this work,antimony doped tin oxide(ATO)has been employed as conductive supports where NiFe layered double hydroxide uniformly dispersed[named NiFe-LDH(layered double hydroxide)/ATO].The catalysts have been synthesized by a one-step co-precipitation method,and then NiFe-LDH/ATO-air plasma was obtained through mild air plasma treatment.According to XPS analysis,binding energies of Ni2p and Fe2p were shifted negatively.Moreover,a new signal of low oxygen coordination appeared on O1s spectrum after air plasma treatment.These XPS results indicated that oxygen vacancies(Ov)were generated after air plasma treatment.Electrochemical measurement indicated that the vacancy-rich NiFe-LDH/ATO-air plasma exhibited better performance than NiFe-LDH/ATO not only in 1 mol/L KOH solutions but also in an alkaline polymer electrolyte water electrolyzer(APEWE)fed with deionized water.This work provides a feasible way to design practical catalysts used in electrochemical energy conversion systems by choosing corrosion resistance supports and defect engineering.
