Leached Pt-Fe and Pt-Co catalysts were prepared by acid leaching the reduced catalysts in acid solution. Oxidation treatments of leached catalysts produced the structure o f metal oxides decorat-ing the surface of...Leached Pt-Fe and Pt-Co catalysts were prepared by acid leaching the reduced catalysts in acid solution. Oxidation treatments of leached catalysts produced the structure o f metal oxides decorat-ing the surface of nanoparticles. The fully oxidized Fe2O3 and Co3O4 species on Pt nanoparticle sur-faces result in the low performance of the CO complete oxidation （COOX） reaction. In contrast, un-saturated FeO and CoO surface species can be formed during exposure to the CO preferential oxida-tion （CO-PROX） reaction with an excess of H2, leading to a high O2 activation ability and enhancing the CO-PROX activity. The FeOx surface structures can be transformed between these two states by varying the reactive gas environments, exhibiting oscillating activity in these two reactions. Con-versely, the CoO surface structure formed in the H2 -rich atmosphere is stable when exposed to the COOX reaction and exhibits similar activity in these two reactions. It is hoped that this work may assist in understanding the important role of surface oxides in real reactions.展开更多
为提高质子交换膜燃料电池(PEMFC)电催化剂的催化活性,并降低其成本,利用循环伏安法电沉积制备Pt-Fe合金催化剂,并以其作为PEMFC阴极。通过X射线衍射仪(XRD)、循环伏安法(CV)、能谱仪(EDS)、扫描电子显微镜(SEM)测试技术对催化剂样品进...为提高质子交换膜燃料电池(PEMFC)电催化剂的催化活性,并降低其成本,利用循环伏安法电沉积制备Pt-Fe合金催化剂,并以其作为PEMFC阴极。通过X射线衍射仪(XRD)、循环伏安法(CV)、能谱仪(EDS)、扫描电子显微镜(SEM)测试技术对催化剂样品进行性能表征。通过循环伏安线性扫描法确定Pt-Fe合金的沉积电位,并探究了电沉积过程中电解液温度、电位和扫描速率对催化剂样品形貌以及电催化性能的影响。结果表明:电解液温度主要对催化剂沉积量及分散性起作用,对形貌影响不大,扫描速率主要对晶体生长产生影响;电位扫描范围为-0.4~0.6 V、扫描速率为100 m V/s,电解液温度为50℃时,电沉积得到的Pt-Fe合金催化剂的颗粒在碳布表面呈空心球状且分散均匀,与其他沉积电位制得的样品相比较,合金中Pt/Fe原子比相对较高,其具有最大的电化学活性表面积,为64.30 m2/g,电催化活性最佳。展开更多
The reduction behavior of Y-Al2O3 supported iron and platinum-iron catalysts was studied by TPR combined in situ 57Fe MBS. The results indicated that Fe3+ is highly dis-persed on the Y-Al2O3 surface for all the sample...The reduction behavior of Y-Al2O3 supported iron and platinum-iron catalysts was studied by TPR combined in situ 57Fe MBS. The results indicated that Fe3+ is highly dis-persed on the Y-Al2O3 surface for all the samples containing iron before the reduction. No Fe was found in the reduction process. The Fe3+ was reduced to Fe2+ in tetrahedral vacancy first in Pt-Fe/Y-Al2O3 sample in TPR process. The TPR processes of all supported iron samples are very different from those of α-Fe2O3.展开更多
低温(110～130K)下,将次表层Fe结构的Pt-Fe模型催化剂(即Pt/Fe/Pt(111)结构)暴露于不同量CO气体,经不同温度退火后,采用高分辨电子能量损失谱(HREELS)研究催化剂表面CO分子的振动谱。结果表明,当CO的暴露量低于0.2 L (Langmuir)时,Pt/Fe...低温(110～130K)下,将次表层Fe结构的Pt-Fe模型催化剂(即Pt/Fe/Pt(111)结构)暴露于不同量CO气体,经不同温度退火后,采用高分辨电子能量损失谱(HREELS)研究催化剂表面CO分子的振动谱。结果表明,当CO的暴露量低于0.2 L (Langmuir)时,Pt/Fe/Pt(111)表面只存在顶位吸附;当暴露量大于0.4L,除了顶位吸附外,桥位吸附开始出现;顶位吸附分子的C-O键振动峰随着暴露量的增加不断向高波数方向偏移。退火温度影响Pt/Fe/Pt(111)表面CO的吸附形式,低于255K时,顶位吸附分子的脱附速率大于桥位吸附分子;高于255 K时,桥位吸附分子的脱附速率较大,并先于顶位吸附的CO从表面完全脱附,其完全脱附温度比Pt(111)表面低50 K。展开更多
An electrochemical approach to fabricate a nanostructured Fe/Pt-Fe catalyst through electrodeposition followed by galvanic replacement is presented. An Fe/Pt-Fe nanostructured electrode was prepared by deposition of F...An electrochemical approach to fabricate a nanostructured Fe/Pt-Fe catalyst through electrodeposition followed by galvanic replacement is presented. An Fe/Pt-Fe nanostructured electrode was prepared by deposition of Fe-Zn onto a Fe electrode surface, followed by replacement of the Zn by Pt at open-circuit potential in a Pt-containing alkaline solution. Scanning electron microscopy and energy-dispersive X-ray techniques reveal that the Fe/Pt-Fe electrode is porous and contains Pt. The electrocatalytic activity of the Fe/Pt-Fe electrode for oxidation of methanol was examined by cyclic voltammetry and chronoamperometry. The electrooxidation current on the Fe/Pt-Fe catalyst is much higher than that on flat Pt and smooth Fe catalysts. The onset potential and peak potential on the Fe/Pt-Fe catalyst are more negative than those on flat Pt and smooth Fe electrodes for methanol electrooxidation. All results show that this nanostructured Fe/Pt-Fe electrode is very attractive for integrated fuel cell applications in alkaline media.展开更多
Porous Pt-Fe bimetallic nanocrystals have been synthesized via self-assembly and can effectively facilitate the synthesis of 2-propanol from acetone. The bimetallic catalyst has three--dimensional channels and shows t...Porous Pt-Fe bimetallic nanocrystals have been synthesized via self-assembly and can effectively facilitate the synthesis of 2-propanol from acetone. The bimetallic catalyst has three--dimensional channels and shows turnover frequencies （TOFs） of up to 972 h^-1 for a continuous process more than 50 h. Preliminary mechanistic studies suggest that the high reactivity is related to the interface consisting of a bimetallic Pt-Fe alloy and Fe2O3-x. An understanding of real catalytic behavior and the catalytic mechanism based on model systems has been shown to help fabricate an improved Pt/Fe3O4 catalyst with increased activity and lifetime which has great potential for large-scale industrial applications.展开更多
基金supported by the National Natural Science Foundation of China(21403004,21403003)~~
文摘Leached Pt-Fe and Pt-Co catalysts were prepared by acid leaching the reduced catalysts in acid solution. Oxidation treatments of leached catalysts produced the structure o f metal oxides decorat-ing the surface of nanoparticles. The fully oxidized Fe2O3 and Co3O4 species on Pt nanoparticle sur-faces result in the low performance of the CO complete oxidation （COOX） reaction. In contrast, un-saturated FeO and CoO surface species can be formed during exposure to the CO preferential oxida-tion （CO-PROX） reaction with an excess of H2, leading to a high O2 activation ability and enhancing the CO-PROX activity. The FeOx surface structures can be transformed between these two states by varying the reactive gas environments, exhibiting oscillating activity in these two reactions. Con-versely, the CoO surface structure formed in the H2 -rich atmosphere is stable when exposed to the COOX reaction and exhibits similar activity in these two reactions. It is hoped that this work may assist in understanding the important role of surface oxides in real reactions.
文摘为提高质子交换膜燃料电池(PEMFC)电催化剂的催化活性,并降低其成本,利用循环伏安法电沉积制备Pt-Fe合金催化剂,并以其作为PEMFC阴极。通过X射线衍射仪(XRD)、循环伏安法(CV)、能谱仪(EDS)、扫描电子显微镜(SEM)测试技术对催化剂样品进行性能表征。通过循环伏安线性扫描法确定Pt-Fe合金的沉积电位,并探究了电沉积过程中电解液温度、电位和扫描速率对催化剂样品形貌以及电催化性能的影响。结果表明:电解液温度主要对催化剂沉积量及分散性起作用,对形貌影响不大,扫描速率主要对晶体生长产生影响;电位扫描范围为-0.4~0.6 V、扫描速率为100 m V/s,电解液温度为50℃时,电沉积得到的Pt-Fe合金催化剂的颗粒在碳布表面呈空心球状且分散均匀,与其他沉积电位制得的样品相比较,合金中Pt/Fe原子比相对较高,其具有最大的电化学活性表面积,为64.30 m2/g,电催化活性最佳。
文摘The reduction behavior of Y-Al2O3 supported iron and platinum-iron catalysts was studied by TPR combined in situ 57Fe MBS. The results indicated that Fe3+ is highly dis-persed on the Y-Al2O3 surface for all the samples containing iron before the reduction. No Fe was found in the reduction process. The Fe3+ was reduced to Fe2+ in tetrahedral vacancy first in Pt-Fe/Y-Al2O3 sample in TPR process. The TPR processes of all supported iron samples are very different from those of α-Fe2O3.
文摘低温(110～130K)下,将次表层Fe结构的Pt-Fe模型催化剂(即Pt/Fe/Pt(111)结构)暴露于不同量CO气体,经不同温度退火后,采用高分辨电子能量损失谱(HREELS)研究催化剂表面CO分子的振动谱。结果表明,当CO的暴露量低于0.2 L (Langmuir)时,Pt/Fe/Pt(111)表面只存在顶位吸附;当暴露量大于0.4L,除了顶位吸附外,桥位吸附开始出现;顶位吸附分子的C-O键振动峰随着暴露量的增加不断向高波数方向偏移。退火温度影响Pt/Fe/Pt(111)表面CO的吸附形式,低于255K时,顶位吸附分子的脱附速率大于桥位吸附分子;高于255 K时,桥位吸附分子的脱附速率较大,并先于顶位吸附的CO从表面完全脱附,其完全脱附温度比Pt(111)表面低50 K。
基金supported by the Iranian Nanotechnology Society and the Office of the Vice-chancellor in Charge of Research at Malek-Ashtar University of Technology
文摘An electrochemical approach to fabricate a nanostructured Fe/Pt-Fe catalyst through electrodeposition followed by galvanic replacement is presented. An Fe/Pt-Fe nanostructured electrode was prepared by deposition of Fe-Zn onto a Fe electrode surface, followed by replacement of the Zn by Pt at open-circuit potential in a Pt-containing alkaline solution. Scanning electron microscopy and energy-dispersive X-ray techniques reveal that the Fe/Pt-Fe electrode is porous and contains Pt. The electrocatalytic activity of the Fe/Pt-Fe electrode for oxidation of methanol was examined by cyclic voltammetry and chronoamperometry. The electrooxidation current on the Fe/Pt-Fe catalyst is much higher than that on flat Pt and smooth Fe catalysts. The onset potential and peak potential on the Fe/Pt-Fe catalyst are more negative than those on flat Pt and smooth Fe electrodes for methanol electrooxidation. All results show that this nanostructured Fe/Pt-Fe electrode is very attractive for integrated fuel cell applications in alkaline media.
基金This work was supported by the National Basic Research Program of China （Nos. 2011CB932401, 2011CBA00500, and 2012CB224802）, and the National Natural Science Foundation of China （Nos. 21221062, 21171105, 21322107 and 21131004）.
文摘Porous Pt-Fe bimetallic nanocrystals have been synthesized via self-assembly and can effectively facilitate the synthesis of 2-propanol from acetone. The bimetallic catalyst has three--dimensional channels and shows turnover frequencies （TOFs） of up to 972 h^-1 for a continuous process more than 50 h. Preliminary mechanistic studies suggest that the high reactivity is related to the interface consisting of a bimetallic Pt-Fe alloy and Fe2O3-x. An understanding of real catalytic behavior and the catalytic mechanism based on model systems has been shown to help fabricate an improved Pt/Fe3O4 catalyst with increased activity and lifetime which has great potential for large-scale industrial applications.
