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一种新型直接甲醇燃料电池阳极添加剂的电化学研究 总被引:3,自引:0,他引:3
将磷钼酸(H4PMo12O40·xH2O,PMo12)作为一种添加剂,制备了直接甲醇燃料电池阳极Pt-Ru/C-PMo12复合催化剂,并对甲醇在含有此复合催化剂的阳极上的氧化进行了电化学研究.测试表明该添加剂降低了甲醇及其电氧化中间产物转化的活化能,改善了电极内部的质子传输状况,对甲醇的电化学氧化过程具有明显的促进作用,该复合催化剂与常规的Pt-Ru/C催化剂相比,甲醇的阳极氧化电流提高了46%.添加剂的这一效应可能与磷钼酸的Keggin结构有关. 相似文献
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直接甲醇燃料电池电催化剂性能衰减研究 总被引:1,自引:1,他引:1
通过单电池放电试验, 考察了直接甲醇燃料电池(DMFC)电催化剂的性能衰减情况. 透射电镜(TEM)和X射线衍射分析(XRD)结果表明, 放电试验后阳极电催化剂的粒径变化很小, 而阴极电催化剂的粒径则显著增大. DMFC内部的液相环境是促使Pt粒子聚结的主要原因. 阳极催化剂中Ru的存在抑制了Pt粒子的生长. 阳极和阴极电催化剂的电化学表面积(ECSA)在放电后都有所降低, 且下降幅度均高于比表面积(SSA)的下降幅度. 放电过程中阳极电催化剂发生了Ru的流失. 相似文献
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高分散直接甲醇燃料电池Pt/C阴极电催化剂的制备过程机理与表征 总被引:4,自引:1,他引:4
通过调变的多元醇法制备了40%Pt/C直接甲醇燃料电池阴极电催化剂,应用透射电镜(TEM)及X射线衍射(XRD)方法表征催化剂.结果表明,由该制备方法可得到高分散,金属粒子粒径分布窄的高载量贵金属催化剂.TEM统计结果表明,调变多元醇法制备的40%Pt/C催化剂的金属粒子平均粒径约为2.9nm.直接甲醇燃料电池单池性能测试表明,该方法制得的40%Pt/C的电催化氧还原能力比同型商品催化剂更好.另外,利用UV-Vis光谱研究了催化剂的制备过程.结果表明,在调变的多元醇法中,Pt4+的还原是一步完成的. 相似文献
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采用两步浸渍-还原法制备了一种具有高Pt利用效率,高性能的Pt修饰的Ru/C催化剂(Ru@Pt/C).对于甲醇的阳极氧化反应,该催化剂的单位质量铂的催化活性分别为Pt/C、自制PtRu/C和商业JMPtRu/C催化剂的1.9、1.5和1.4倍;其电化学活性比表面积分别为Pt/C和自制PtRu/C的1.6和1.3倍.尤为重要的是该催化剂对甲醇氧化中间体具有很好的去除能力,其正向扫描的氧化峰的峰电流密度(If)与反向扫描氧化峰的峰电流密度(Ib)之比可高达2.4,为Pt/C催化剂的If/Ib的2.7倍,表明催化剂具有很好的抗甲醇氧化中间体毒化的能力.另外,Ru@Pt/C催化剂的稳定性也高于Pt/C、自制PtRu/C和商业JMPtRu/C催化剂的稳定性.采用X射线衍射(XRD)、透射电镜(TEM)和X射线光电子能谱(XPS)对催化剂进行了表征,Pt在Ru表面的包覆结构得到了印证.Ru@Pt/C的高铂利用效率、高性能和高抗毒能力使其有望成为一种理想的直接甲醇燃料电池电催化剂. 相似文献
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直接甲醇燃料电池阳极催化剂PtRu/C的制备和表征 总被引:22,自引:2,他引:22
用三种方法制备了PtRu/C[Pt和Ru质量分数分别为20%和10%,记为PtRu/C(20%-10%)]甲醇阳极催化剂,通过X射线衍射(XRD)和透射电镜(TEM)考察了PtRu/C催化剂的粒子大小和晶格参数的变化,利用单电池实验考察了催化剂在直接甲醇燃料电池中的催化活性.结果表明,改变溶剂的组成提高了贵金属在活性炭表面的分散度,并改善了PtRu间的相互作用,用乙二醇/水/异丙醇混合溶剂制备的PtRu催化剂金属颗粒较小,PtRu间的相互作用较强,以该催化剂作甲醇阳极的直接甲醇燃料电池的性能较好. 相似文献
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Physical and electrochemical characterizations of microwave-assisted polyol preparation of carbon-supported PtRu nanoparticles 总被引:9,自引:0,他引:9
Liu Z Lee JY Chen W Han M Gan LM 《Langmuir : the ACS journal of surfaces and colloids》2004,20(1):181-187
PtRu nanoparticles supported on Vulcan XC-72 carbon and carbon nanotubes were prepared by a microwave-assisted polyol process. The catalysts were characterized by transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy (XPS). The PtRu nanoparticles, which were uniformly dispersed on carbon, were 2-6 nm in diameter. All PtRu/C catalysts prepared as such displayed the characteristic diffraction peaks of a Pt face-centered cubic structure, excepting that the 2theta values were shifted to slightly higher values. XPS analysis revealed that the catalysts contained mostly Pt(0) and Ru(0), with traces of Pt(II), Pt(IV), and Ru(IV). The electro-oxidation of methanol was studied by cyclic voltammetry, linear sweep voltammetry, and chronoamperometry. It was found that both PtRu/C catalysts had high and more durable electrocatalytic activities for methanol oxidation than a comparative Pt/C catalyst. Preliminary data from a direct methanol fuel cell single stack test cell using the Vulcan-carbon-supported PtRu alloy as the anode catalyst showed high power density. 相似文献
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采用乙醇为助磨剂,利用球磨的方法将5-15μm长的多壁碳纳米管切短成长度约为200nm,并且分布较为均匀的短碳纳米管(SCNT).以SCNT为载体,采用有机溶胶法制得了含铂20%(w)的Pt/SCNT及PtRu/SCNT催化剂.实验发现:对于甲醇的阳极电氧化过程,以切短碳纳米管为载体的Pt/SCNT催化剂具有比相同条件制得的Pt/CNT催化剂高得多的催化活性,前者甲醇氧化峰电流密度是后者的1.4倍,并且远远高于商品的Pt/C催化剂.同时我们发现添加了钌的PtRu/SCNT具有比不含钌的催化剂更好的活性.采用X射线衍射(XRD)、透射电镜(TEM)、比表面积分析(BET)等方法对催化剂进行表征,结果表明,切短碳纳米管的晶相结构并未改变,但Pt/SCNT和PtRu/SCNT催化剂的比表面积和电化学活性得到了显著的提高. 相似文献
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高负载率纳米Pt-Ru/C催化剂的制备和表征 总被引:2,自引:0,他引:2
以Vulcan XC-72R碳黑为载体, 通过在含十二烷基硫酸钠(SDS)的乙二醇溶液中直接还原氯铂酸和三氯化钌, 制备了负载率为60%的纳米PtRu/C催化剂. 透射电镜(TEM)和X射线衍射(XRD)分析结果表明, SDS的加入可显著改善PtRu纳米颗粒在载体表面分散性, 平均粒径达到2.7 nm. 电化学循环伏安法(CV)测试的结果显示, 利用这种方法制备的纳米PtRu/C催化剂对于甲醇氧化具有较强的抗中毒能力和较高的电催化活性. 相似文献
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Nanostructured PtRu/C as anode catalysts prepared in a pseudomicroemulsion with ionic surfactant for direct methanol fuel cell 总被引:2,自引:0,他引:2
Nanostructured PtRu/C catalysts have been prepared from a water-in-oil pseudomicroemulsion with the aqueous phase of a mixed concentrated solution of H(2)PtCl(6), RuCl(3), and carbon powder, oil phase of cyclohexane, ionic surfactant of sodium dodecylbenzene sulfonate (C(18)H(29)NaO(3)S), and cosurfactant n-butanol (C(4)H(10)O). Two different composing PtRu/C nanocatalysts (catalyst 1, Pt 20 wt %, Ru 15 wt %; catalyst 2, Pt 20 wt %, Ru 10 wt %) were synthesized. The catalysts were characterized by transmission electron microscopy, X-ray diffractometry, X-ray photoelectron spectroscopy, and thermogravimetric analysis, and the particles were found to be nanosized (2-4 nm) and inherit the Pt face-centered cubic structure with Pt and Ru mainly in the zero valance oxidation state. The ruthenium oxide and hydrous ruthenium oxide (RuO(x)()H(y)()) were also found in these catalysts. The cyclic voltammograms (CVs) and chronoamperometries for methanol oxidation on these catalysts showed that catalyst 1 with a higher Ru content (15 wt %) has a higher and more durable electrocatalytic activity to methanol oxidation than catalyst 2 with low Ru content (10 wt %). The CV results for catalysts 1 and 2 strongly support the bifunctional mechanism of PtRu/C catalysts for methanol oxidation. The data from direct methanol single cells using these two PtRu/C as anode catalysts show the cell with catalyst 1 has higher open circuit voltage (OCV = 0.75 V) and maximal power density (78 mW/cm(2)) than that with catalyst 2 (OCV = 0.70 V, P(max) = 56 mW/cm(2)) at 80 degrees C. 相似文献
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Carbon-supported PtRu nanoparticles (Ru/Pt: 0.25) were prepared by three different methods; simultaneous reduction of PtCl(4) and RuCl(3) (catalyst I) and changing the reduction order of PtCl(4) and RuCl(3) (catalysts II and III) to enhance the performance of the anodic catalysts for methanol and ethanol oxidation. Structure, microstructure and surface characterizations of all the catalysts were carried out by X-ray diffraction (XRD), transmission electron microscopy (TEM) coupled with energy dispersive X-ray spectroscopy (EDS) and X-ray photoelectron spectroscopy (XPS). The results of the XRD analysis showed that all catalysts had a face-centered cubic (fcc) structure with different and smaller lattice parameters than that of pure platinum, showing that the Ru incorporates into the Pt fcc structure by different ratios in all the catalysts. The typical particle sizes of all catalysts were in the range of 2-3 nm. The most active and stable catalyst for methanol and ethanol oxidation is catalyst III, in which a large amount (more than 90%) of PtRu alloy formation was observed. It has been found that this catalyst is about 8.0 and 33.4 times more active at ~0.60 V towards the methanol and ethanol oxidation reactions, respectively, compared to the commercial Pt catalyst. 相似文献
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Stoupin S Rivera H Li Z Segre CU Korzeniewski C Casadonte DJ Inoue H Smotkin ES 《Physical chemistry chemical physics : PCCP》2008,10(42):6430-6437
Sonochemically prepared PtRu (3 : 1) and Johnson Matthey PtRu (1 : 1) were analyzed by X-ray absorption spectroscopy in operating liquid feed direct methanol fuel cells. The total metal loadings were 4 mg cm(-2) unsupported catalysts at the anode and cathode of the membrane electrode assembly. Ex situ XRD lattice parameter analysis indicates partial segregation of the Ru from the PtRu fcc alloy in both catalysts. A comparison of the in situ DMFC EXAFS to that of the as-received catalyst shows that catalyst restructuring during DMFC operation increases the total metal coordination numbers. A combined analysis of XRD determined grain sizes and lattice parameters, ex situ and in situ EXAFS analysis, and XRF of the as-received catalysts enables determination of the catalyst shell composition. The multi-spectrum analysis shows that the core size increases during DMFC operation by reduction of Pt oxides and incorporation of Pt into the core. This increases the mole fraction of Ru in the catalyst shell structure. 相似文献
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Ermete Antolini Leonardo Giorgi Francesco Cardellini Enza Passalacqua 《Journal of Solid State Electrochemistry》2001,5(2):131-140
Platinum-ruthenium catalysts supported on carbon (PtRu/C) have been characterized by X-ray diffraction (XRD), transmission
electron microscopy (TEM), specific surface area analysis (BET), X-ray photoelectron spectroscopy (XPS) and in proton exchange
membrane (PEM) fuel cell tests. The results indicate the presence of strong metal-carbon interactions, which hinder the formation
of a single-phase face-centered cubic (fcc) PtRu alloy. The particle size of the PtRu/C catalysts was smaller than both carbon-supported
platinum (Pt/C) and ruthenium (Ru/C) catalysts. In the bimetallic electrocatalysts the intercrystallite distance decreased
with respect to pure Pt and Ru metals. PEM fuel cell tests in H2/air operation mode revealed a decrease of performance with increasing carbon content of the catalyst, at a fixed Pt loading.
In H2 + 100 ppm CO/air operation mode the maximum performance of the PEM fuel cell was attained at 0.63 atomic fraction Ru.
Received: 2 December 1999 / Accepted: 27 January 2000 相似文献
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Nanosized Pt, PtRu, and Ru particles were prepared by a novel process, the hydrosilylation reaction. The hydrosilylation reaction is an effective method of preparation not only for Pt particles but also for other metal colloids, such as Ru. Vulcan XC-72 was selected as catalyst support for Pt, PtRu, and Ru colloids, and TEM investigations showed nanoscale particles and narrow size distribution for both supported and unsupported metals. All Pt and Pt-rich catalysts showed the X-ray diffraction pattern of a face-centered cubic (fcc) crystal structure, whereas the Ru and Ru-rich alloys were more typical of a hexagonal close-packed (hcp) structure. As evidenced by XPS, most Pt and Ru atoms in the nanoparticles were zerovalent, except a trace of oxidation-state metals. The electrooxidation of liquid methanol on these catalysts was investigated at room temperature by cyclic voltammetry and chronoamperometry. The results concluded that some alloy catalysts showed higher catalytic activities and better CO tolerance than the Pt-only catalyst; Pt56Ru44/C have displayed the best electrocatalytic performance among all carbon-supported catalysts. 相似文献