Low-platinum(Pt)alloy catalysts hold promising application in oxygen reduction reaction(ORR)electrocatalysis of protonexchange-membrane fuel cells(PEMFCs).Although significant progress has been made to boost the kinet...Low-platinum(Pt)alloy catalysts hold promising application in oxygen reduction reaction(ORR)electrocatalysis of protonexchange-membrane fuel cells(PEMFCs).Although significant progress has been made to boost the kinetic ORR mass activity at low current densities in liquid half-cells,little attention was paid to the performance of Pt-based catalysts in realistic PEMFCs particularly at high current densities for high power density,which remains poorly understood.In this paper,we show that,regardless of the kinetic mass activity at the low current density region,the high current density performance of the low-Pt alloy catalysts is dominantly controlled by the total Pt surface area,particularly in low-Pt-loading H_(2)–air PEMFCs.To this end,we propose two different strategies to boost the specific Pt surface area,the post-15-nm dealloyed nanoporous architecture and the sub-5-nm solid core–shell nanoparticles(NPs)through fluidic-bed synthesis,both of which bring in comparably high mass activity and high Pt surface area for large-current-density performance.At medium current density,the dealloyed porous NPs provide substantially higher H_(2)–air PEMFC performance compared to solid core–shell catalysts,despite their similar mass activity in liquid half-cells.Scanning transmission electron microscopy images combined with electron energy loss spectroscopic imaging evidence a previously unreported“semi-immersed nanoporous-Pt/ionomer”structure in contrast to a“fully-immersed core–shellPt/ionomer”structure,thus favoring O_(2) transport and improving the fuel cell performance.Our results provide new insights into the role of Pt nanostructures in concurrently optimizing the mass activity,Pt surface area and Pt/Nafion interface for high power density fuel cells.展开更多
In the present study,two Ni/YSZ anodes with different volume ratios of Ni and YSZ,30:70 and 45:55 vol%,are operated in dry methane under open circuit and polarized conditions.Three-dimensional(3D)Ni/YSZ microstructure...In the present study,two Ni/YSZ anodes with different volume ratios of Ni and YSZ,30:70 and 45:55 vol%,are operated in dry methane under open circuit and polarized conditions.Three-dimensional(3D)Ni/YSZ microstructures after carbon deposition are reconstructed by the focused ion beam-scanning electron microscopy(FIB-SEM)with the help of machine learning segmentation.From the reconstructed mircostructures,volume fraction,connectivity,three phase boundary(TPB)density,and tortuosity are quantified.In addition,local carbon microstructures are quantitatively reconstructed,and the effect of polarization on carbon morphology is investigated.It is demonstrated that Ni surface in the vicinity of active TPB near the electrolyte is free from carbon formation,while remaining Ni surface at some distances from TPB exhibits severe carbon deposition.In average,total amount of carbon deposition is larger near the electrolyte.These observations imply complex interplay between the electrochemical steam generation and methane cracking on Ni surface which take place very locally near the active TPB.展开更多
The performance of multi-layer （1 -x）La0.8Sr0.2MnO3/xYSZ graded composite cathodes was studied as electrode materials for intermediate solid oxide fuel cells （SOFC）. The thermal expansion coefficient, electrical c...The performance of multi-layer （1 -x）La0.8Sr0.2MnO3/xYSZ graded composite cathodes was studied as electrode materials for intermediate solid oxide fuel cells （SOFC）. The thermal expansion coefficient, electrical conductivity, and electrochemical performance of multi-layer composite cathodes were investigated. The thermal expansion coefficient and electrical conductivity decreased with the increase in YSZ content. The （1 -x）Lao.sSr0.EMnO3/xYSZ composite cathode greatly increased the length of the active triple phase boundary line （TPBL） among electrode, electrolyte, and gas phase, leading to a decrease in polarization resistance and an increase in polarization current density. The polarization current density of the triple-layer graded composite cathode （0.77 A/cm2） was the highest and that of the monolayer cathode （0.13 A/cm2） was the lowest. The polarization resistance （Rp） of the triple-layer graded composite cathode was only 0.182 Ω·cm2 and that of the monolayer composite cathode was 0.323 Ω·cm2. The power density of the triple-layer graded composite cathode was the highest and that of the monolayer composite cathode was the lowest. The triple-layer graded composite cathode had superior performance.展开更多
在能源日益匮乏的今天,氢能作为一种可再生、绿色环保的新型能源成为全球节能降碳的重要载体。传统的碱水电解(Alkaline water electrolysis,AWE)制氢要求较高pH的碱液作为电解液,而且只能在低电流密度下工作;质子交换膜电解水(Proton e...在能源日益匮乏的今天,氢能作为一种可再生、绿色环保的新型能源成为全球节能降碳的重要载体。传统的碱水电解(Alkaline water electrolysis,AWE)制氢要求较高pH的碱液作为电解液,而且只能在低电流密度下工作;质子交换膜电解水(Proton exchange membrane water electrolysis,PEMWE)制氢技术具有电流密度大、效率高的特点,被人们视为最有前景的电解水制氢技术,但是其昂贵的催化剂以及所需的高耐酸性部件成为制约PEMWE发展的重要因素。阴离子交换膜电解水(Anion exchange membrane water electrolysis,AEMWE)作为一种新兴的技术,可以实现低成本“绿氢”制备。相较于AWE,AEMWE避免了高浓度碱液的循环;相较于PEMWE,AEMWE则具有成本低、腐蚀性低等优势。离聚物作为关键部件膜电极(Membrane electrode assembly,MEA)中三相界面(Triple phase boundary,TPB)的重要组成部分,对AEMWE内部催化作用和水管理能力起着重要作用。本文首先围绕AEMWE技术原理和离聚物在AEMWE中的作用进行了概述,随后对常见的不同种类的阴离子离聚物结构及特点进行了总结,最后从结构、含量以及添加剂调控三种调控策略入手,针对如何调控离聚物以达到更加优异的电解性能进行了具体的分析总结。展开更多
La（0.4）Sr（0.6）Co（0.2）Fe（0.7）Nb（0.1）O（3-δ）（LSCFN）was applied as both anode and cathode for symmetrical solid oxide fuel cells（SSOFCs）with zirconia based electrolyte.The cell with LSCFN electrode was fa...La（0.4）Sr（0.6）Co（0.2）Fe（0.7）Nb（0.1）O（3-δ）（LSCFN）was applied as both anode and cathode for symmetrical solid oxide fuel cells（SSOFCs）with zirconia based electrolyte.The cell with LSCFN electrode was fabricated by tape-casting and screen printing.Fabrication process was optimized firstly by comparing co-sintering and separate-sintering of electrode and electrolyte.To further improve the LSCFN electrode properties,oxygen ionic conductor of Gd（0.1）Ce（0.9）O（2-δ）（GDC）was added into the LSCFN electrode.The preferred composition of LSCFN-GDC composite electrode was found to be 1：1 in weight ratio with polarization resistance of 0.16Ωcm^2at 800~℃.The maximum power densities of LSCFN-GDC｜｜GDC/YSZ/GDC｜｜LSCFN-GDC tested in H2and CH4with 3%H2O were 395 m W cm^（-2）and 124 m W cm^（-2）at 850~？C,respectively,which were much higher than that of LSCFN｜｜GDC/YSZ/GDC｜｜LSCFN cells at same condition,possibly due to the extension of the triple phase boundary induced by the addition of GDC.The cell showed reasonable stability using H2and CH4with 3%H2O as fuels and no significant power output degradation was observed after total 200 h operation.展开更多
基金supported by the National Natural Science Foundation of China(Nos.52173222,51622103 and 22109088)the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(No.2017BT01N111)+1 种基金Key Area Research and Development Program of Guangdong Province(No.2020B0909040003)Shenzhen Science and Technology Innovation Committee(Nos.WDZ20200819115243002 and JCYJ20190809172617313).
文摘Low-platinum(Pt)alloy catalysts hold promising application in oxygen reduction reaction(ORR)electrocatalysis of protonexchange-membrane fuel cells(PEMFCs).Although significant progress has been made to boost the kinetic ORR mass activity at low current densities in liquid half-cells,little attention was paid to the performance of Pt-based catalysts in realistic PEMFCs particularly at high current densities for high power density,which remains poorly understood.In this paper,we show that,regardless of the kinetic mass activity at the low current density region,the high current density performance of the low-Pt alloy catalysts is dominantly controlled by the total Pt surface area,particularly in low-Pt-loading H_(2)–air PEMFCs.To this end,we propose two different strategies to boost the specific Pt surface area,the post-15-nm dealloyed nanoporous architecture and the sub-5-nm solid core–shell nanoparticles(NPs)through fluidic-bed synthesis,both of which bring in comparably high mass activity and high Pt surface area for large-current-density performance.At medium current density,the dealloyed porous NPs provide substantially higher H_(2)–air PEMFC performance compared to solid core–shell catalysts,despite their similar mass activity in liquid half-cells.Scanning transmission electron microscopy images combined with electron energy loss spectroscopic imaging evidence a previously unreported“semi-immersed nanoporous-Pt/ionomer”structure in contrast to a“fully-immersed core–shellPt/ionomer”structure,thus favoring O_(2) transport and improving the fuel cell performance.Our results provide new insights into the role of Pt nanostructures in concurrently optimizing the mass activity,Pt surface area and Pt/Nafion interface for high power density fuel cells.
基金partly supported by the New Energy and Industrial Technology Development Organization(NEDO)by the Japan Society for the Promotion of Science KAKENHI(21K14090)+3 种基金the National Key R&D Program of China(2019YFE0122000)the Scientific Research Foundation of Graduate School of Southeast University(YBPY2106)the China Scholarship Councilby the Advanced Research Infrastructure for Materials and Nanotechnology in Japan(ARIM Japan)sponsored by the Ministry of Education,Culture,Sport,Science and Technology(MEXT),Japan。
文摘In the present study,two Ni/YSZ anodes with different volume ratios of Ni and YSZ,30:70 and 45:55 vol%,are operated in dry methane under open circuit and polarized conditions.Three-dimensional(3D)Ni/YSZ microstructures after carbon deposition are reconstructed by the focused ion beam-scanning electron microscopy(FIB-SEM)with the help of machine learning segmentation.From the reconstructed mircostructures,volume fraction,connectivity,three phase boundary(TPB)density,and tortuosity are quantified.In addition,local carbon microstructures are quantitatively reconstructed,and the effect of polarization on carbon morphology is investigated.It is demonstrated that Ni surface in the vicinity of active TPB near the electrolyte is free from carbon formation,while remaining Ni surface at some distances from TPB exhibits severe carbon deposition.In average,total amount of carbon deposition is larger near the electrolyte.These observations imply complex interplay between the electrochemical steam generation and methane cracking on Ni surface which take place very locally near the active TPB.
基金supported by the National Natural Science Foundation of China(11247012,11174070)Innovation Scientists and TechniciansTroop Construction Projects of Henan Province,China(104200510014)~~
基金This project is financially supported by the National Nature Science Foundation of China （No. 90510006）.
文摘The performance of multi-layer （1 -x）La0.8Sr0.2MnO3/xYSZ graded composite cathodes was studied as electrode materials for intermediate solid oxide fuel cells （SOFC）. The thermal expansion coefficient, electrical conductivity, and electrochemical performance of multi-layer composite cathodes were investigated. The thermal expansion coefficient and electrical conductivity decreased with the increase in YSZ content. The （1 -x）Lao.sSr0.EMnO3/xYSZ composite cathode greatly increased the length of the active triple phase boundary line （TPBL） among electrode, electrolyte, and gas phase, leading to a decrease in polarization resistance and an increase in polarization current density. The polarization current density of the triple-layer graded composite cathode （0.77 A/cm2） was the highest and that of the monolayer cathode （0.13 A/cm2） was the lowest. The polarization resistance （Rp） of the triple-layer graded composite cathode was only 0.182 Ω·cm2 and that of the monolayer composite cathode was 0.323 Ω·cm2. The power density of the triple-layer graded composite cathode was the highest and that of the monolayer composite cathode was the lowest. The triple-layer graded composite cathode had superior performance.
基金国家自然科学基金(22208376)青岛新能源山东省实验室开放课题项目(QNESL OP 202303)+2 种基金山东省自然科学基金创新发展联合基金(ZR2023LFG005)山东博士后科学基金(SDBX202302037)山西省留学人员科技活动择优资助项目(20230002)。
文摘在能源日益匮乏的今天,氢能作为一种可再生、绿色环保的新型能源成为全球节能降碳的重要载体。传统的碱水电解(Alkaline water electrolysis,AWE)制氢要求较高pH的碱液作为电解液,而且只能在低电流密度下工作;质子交换膜电解水(Proton exchange membrane water electrolysis,PEMWE)制氢技术具有电流密度大、效率高的特点,被人们视为最有前景的电解水制氢技术,但是其昂贵的催化剂以及所需的高耐酸性部件成为制约PEMWE发展的重要因素。阴离子交换膜电解水(Anion exchange membrane water electrolysis,AEMWE)作为一种新兴的技术,可以实现低成本“绿氢”制备。相较于AWE,AEMWE避免了高浓度碱液的循环;相较于PEMWE,AEMWE则具有成本低、腐蚀性低等优势。离聚物作为关键部件膜电极(Membrane electrode assembly,MEA)中三相界面(Triple phase boundary,TPB)的重要组成部分,对AEMWE内部催化作用和水管理能力起着重要作用。本文首先围绕AEMWE技术原理和离聚物在AEMWE中的作用进行了概述,随后对常见的不同种类的阴离子离聚物结构及特点进行了总结,最后从结构、含量以及添加剂调控三种调控策略入手,针对如何调控离聚物以达到更加优异的电解性能进行了具体的分析总结。
基金supported by the National Natural Science Foundation of China (No. 51402355)Natural Science Foundation of Beijing Project (Nos. LJ201531 and 2154056)+1 种基金Shanxi Province Project (No. MD2014-08)Guangdong Project (No. 201460720100025)
文摘La（0.4）Sr（0.6）Co（0.2）Fe（0.7）Nb（0.1）O（3-δ）（LSCFN）was applied as both anode and cathode for symmetrical solid oxide fuel cells（SSOFCs）with zirconia based electrolyte.The cell with LSCFN electrode was fabricated by tape-casting and screen printing.Fabrication process was optimized firstly by comparing co-sintering and separate-sintering of electrode and electrolyte.To further improve the LSCFN electrode properties,oxygen ionic conductor of Gd（0.1）Ce（0.9）O（2-δ）（GDC）was added into the LSCFN electrode.The preferred composition of LSCFN-GDC composite electrode was found to be 1：1 in weight ratio with polarization resistance of 0.16Ωcm^2at 800~℃.The maximum power densities of LSCFN-GDC｜｜GDC/YSZ/GDC｜｜LSCFN-GDC tested in H2and CH4with 3%H2O were 395 m W cm^（-2）and 124 m W cm^（-2）at 850~？C,respectively,which were much higher than that of LSCFN｜｜GDC/YSZ/GDC｜｜LSCFN cells at same condition,possibly due to the extension of the triple phase boundary induced by the addition of GDC.The cell showed reasonable stability using H2and CH4with 3%H2O as fuels and no significant power output degradation was observed after total 200 h operation.
