采用简易方法合成直接乙醇固体氧化物燃料电池海胆状Pd催化层（英文）

在室温下,通过电位置换反应在固体氧化物燃料电池的Ni-YSZ(钇掺杂氧化锆)阳极表面制备海胆状Pd催化层。该催化层的结构和性能通过SEM、XRD和电化学等表征手段进行表征。结果表明,三维纳米花状Pd催化剂是由在Ni-YSZ阳极表面形成的多条纳米棒有序的组合而成。通过在Ni/YSZ阳极表面引入该催化层,相比与传统Ni-YSZ阳极,燃料电池的最高功率和稳定性都获得了很大的提升。该研究表明,电位置换反应是一种很高效的在传统Ni-YSZ阳极表面制备纳米抗积炭的功能层的方法。     

直接碳氢化合物固体氧化物燃料电池

直接碳氢化合物固体氧化物燃料电池（D-HC SOFC）具有能量密度高和运行成本低等特点,可望在便携式电源等方面得到广泛应用,已成为国际上SOFC领域的研究热点。本文对D-HC SOFC进行了热力学分析,综述了目前国际上在D—HCSOFC研究方面的现状,指出现有的D-HC SOFC研究工作绝大多数都是围绕着如何避免积碳进行。围绕着避免积碳的3条途径即降低工作温度、采用合适的催化剂和促进电化学氧化,对D-HC SOFC研究进行了阐述和讨论。文中还提到一些阳极反应机理方面的研究,并对今后的D-HC SOFC工作提出了作者的观点,认为应该在D-HC SOFC电池组方面和涉及到气体分布的阳极反应机理方面做更多工作。     

直接碳氢化合物固体氧化物燃料电池

直接碳氢化合物固体氧化物燃料电池(D-HC SOFC)具有能量密度高和运行成本低等特点,可望在便携式电源等方面得到广泛应用,已成为国际上SOFC领域的研究热点。本文对D-HC SOFC进行了热力学分析,综述了目前国际上在D-HC SOFC研究方面的现状,指出现有的D-HC SOFC研究工作绝大多数都是围绕着如何避免积碳进行。围绕着避免积碳的3条途径即降低工作温度、采用合适的催化剂和促进电化学氧化,对D-HC SOFC研究进行了阐述和讨论。文中还提到一些阳极反应机理方面的研究,并对今后的D-HC SOFC工作提出了作者的观点,认为应该在D-HC SOFC电池组方面和涉及到气体分布的阳极反应机理方面做更多工作。     

直接碳氢化合物固体氧化物燃料电池

直接碳氢化合物固体氧化物燃料电池(D-HC SOFC)具有能量密度高和运行成本低等特点,可望在便携式电源等方面得到广泛应用,已成为国际上SOFC领域的研究热点.本文对D-HC SOFC进行了热力学分析,综述了目前国际上在D-HC SOFC研究方面的现状,指出现有的D-HC SOFC研究工作绝大多数都是围绕着如何避免积碳进行.围绕着避免积碳的3条途径即降低工作温度、采用合适的催化剂和促进电化学氧化,对D-HC SOFC研究进行了阐述和讨论.文中还提到一些阳极反应机理方面的研究,并对今后的D-HC SOFC工作提出了作者的观点,认为应该在D-HC SOFC电池组方面和涉及到气体分布的阳极反应机理方面做更多工作.     

直接氨固体氧化物燃料电池

塑性挤压成型阳极支撑管,采用真空浸涂法在阳极表面制备了均一、致密的氧化钇稳定的氧化锆电解质层,然后在电解质表面刷涂上阴极层,成功制备了阳极支撑型管状固体氧化物燃料电池.分别以氢气和氨气为燃料,考察了该管状固体氧化物燃料电池的电池性能.在800℃操作时,以氢气和氨气为燃料的电池最大输出功率密度分别为202和200 mW/cm2.表明氨气可以作为固体氧化物燃料电池的替代燃料.     

钙钛矿型固体氧化物燃料电池阳极材料

固体氧化物燃料电池(SOFCs)作为一种高效、洁净的化学电源已经受到各国的重视.钙钛矿型复合氧化物由于其较高的混合导电性和对燃料气较好的催化活性及超强抗积碳能力而越来越被广泛地应用于直接烃类SOFCs的阳极材料中.本文对钙钛矿型固体氧化物燃料电池阳极材料的最新研究进展进行了较为全面的综述,从阳极的设计要求出发,着重比较了LaCrO3系列、SrTiO3系列和双钙钛矿等阳极材料的稳定性、电导率以及电催化活性,指出了其不足,并对其应用前景进行了展望.     

低温固体氧化物燃料电池

固体氧化物燃料电池作为新型的能源转换装置,具有高效、清洁、稳定性高、灵活多样等特点,有着良好的发展前景.它的中低温化对于商业应用具有十分重要的意义,现阶段的研究重点主要集中于将操作温度从传统的800-1000℃降低到600℃甚至以下.本文集中介绍了应用于600℃以下的中低温固体氧化物燃料电池,分别从低温电解质、阴极和阳...     

稀土改性固体氧化物燃料电池阳极催化材料的制备和表征

采用硝酸盐共分解法制备稀土改性固体氧化物燃料电池阳极催化材料NiOxREγOx。用x射线衍射（XRD）、程序升温还原（TPR）、扫描电镜（SEM）等表征手段考察了材料的物理化学性质。XRD结果表明,添加镧在800℃即会与氧化镍发生反应,而镨则在1400℃与氧化镍发生反应,钐和钆则在两种情况下都没有与氧化镍发生反应。通过添加稀土材料改性,大大降低了氧化镍的粒径,新型催化材料中氧化镍的还原峰向低温方向移动,而添加的稀土材料与氧化镍相互作用,形成一个温度较高的还原峰。结果表明,添加的稀土材料通过与氧化镍相互作用,阻止了制备过程中氧化镍颗粒的长大。     

镧改性镍基阳极固体氧化物燃料电池

研究了镧改性镍基阳极的组成与结构及其电化学性能.XRD结果显示,镧可以与氧化镍反应生成LaNiO3,在复合阳极中可以与氧化锆反应生成La2Zr2O7.SEM结果显示,当镧含量为10%（摩尔比）时,复合阳极的颗粒较小,分布均匀;添加镧可以较好地阻止镍与氧化钇稳定的氧化锆（YSZ）的烧结长大,而且很好地改善镍与YSZ的界面接触;镧改性阳极的微结构得到了明显的改善,大大降低了电池的极化电阻,提高了电池性能,电池在800℃时的最大功率密度由添加前的1.33W/cm2提高到1.61W/cm^2.但当添加过量的镧（20%摩尔比）时,因较多的La2Zr2O7生成,使电池的欧姆和极化电阻明显增加,电池性能降低.     

高温固体氧化物燃料电池

从材料选择、结构设计与技术经济诸方面评述了第三代燃料电池（ＳＯＦＣ）的发展历史和发展现状。由于第三代燃料电池中大量应用稀土及其固有的一系列优点，值得引起我国的重视。分析表明，在我国开展ＳＯＦＣ的研究与开发工作具有重要意义。同时，分析了发展ＳＯＦＣ过程中的材料选择与结构设计的原则。     

固体氧化物直接碳燃料电池阳极反应过程分析

以氧化钇稳定的氧化锆(YSZ)为电解质组装成直接碳燃料电池(DCFC),分别以活性炭(AC)、石墨(G)、神府半焦(SC)作为DCFC燃料,研究了碳燃料的特性、电池操作温度以及阳极反应气氛等对DCFC阳极反应过程的影响。结果表明,三种碳燃料在空气、CO₂气氛中氧化反应活性顺序为AC > SC > G,当三种碳材料作为DCFC燃料时,活性炭作为燃料的DCFC性能最好,半焦燃料次之,石墨作为燃料的DCFC性能最差,而且燃料反应活性与其表面含氧官能团、孔隙结构有关;DCFC的阳极反应过程存在碳燃料直接氧化为CO₂、CO₂与C反应转化为CO,以及CO氧化为CO₂等。     

A direct-methane solid oxide fuel cell with a double-layer anode

A tubular anode-supported solid oxide fuel cell with a double-layer anode for the direct conversion of CH₄ has been prepared and operated at 800 °C successfully. The double-layer anode was composed of NiO–YSZ and CoO–NiO–SDC acting as supporting layer and active reforming layer, respectively. At 800 °C, a maximum power density of 350 mW cm⁻² was obtained with CH₄ as fuel and air as oxidant. The time-dependent impedance spectra of the tubular cell were examined and discussed. No carbon deposition was observed on the surface of the anode when the cell was operated at a constant current density of 250 mA cm⁻².     

以椰壳生物质炭为燃料的直接炭固体氧化物燃料电池

通过热裂解制得椰壳炭,表征了其结构和组成,并将其用于电解质为钇稳定化氧化锆（YSZ）、电极材料为银和钆掺杂氧化铈（Ag-GDC）的固体氧化物燃料电池（SOFC）的燃料,对所构成的直接炭固体氧化物燃料电池（DC-SOFC）的性能进行了测试研究。结果表明,所制得的椰壳炭颗粒粒径在微米级别,具有介孔结构,而且椰壳炭中含有K、Ca等元素,可用作Boudouard反应催化剂。当使用椰壳炭作为DC-SOFC燃料时,在800 ℃下电池最大功率密度为255 mW/cm²;负载Fe催化剂后,最大功率密度提升为274 mW/cm²。以0.5 A/cm²的恒电流放电,0.5 g负载Fe椰壳炭燃料电池能够连续工作17.6 h,燃料利用率为39%,表明椰壳炭作为DC-SOFC燃料具有优异的性能和潜力。     

Promotional effect of nitrogen-doped and pore structure for the direct synthesis of hydrogen peroxide from hydrogen and oxygen by Pd/C catalyst at ambient pressure

Nitrogen-doped porous carbon is potential support for directly synthesizing H₂O₂ from H₂ and O₂. Here, density functional theory (DFT) was used to study the effect of N-doped porous carbon on H₂O₂ directly synthesized. The theoretical calculation results showed that N-doped improved H₂O₂ productivity and H₂ conversion by increasing the dispersion of Pd nanoparticles and the Pd⁰/Pd²⁺ ratio. However, N-doped decreased H₂O₂ selectivity by reducing oxygen's dissociation energies. The experimental results showed that adjusting the pore structure of N-doped porous carbon could improve the adverse effects of N-doping for H₂O₂ selectivity. The H₂O₂ productivity and selectivity of Pd/C catalyst with a macropore-mesoporous-microporous hierarchical porous structure were up to 328.4 mol_H2O2·kg_cat^-1·h^?1 and 71.9 %, respectively, at ambient pressure. The macropore structure enhances the transfer and diffusion performance of the catalyst and effectively inhibits the effect of N-doping on OO bond dissociation, which improves H₂O₂ productivity and selectivity. This research provides a possible solution for designing a high-performance Pd/C catalyst to directly synthesize H₂O₂ from H₂ and O₂ at ambient pressure.     

LSM-infiltrated LSCF cathodes for solid oxide fuel cells

Mixed ionic-electronic conductors in the family of La_xSr_1–xCo_yFe_1–yO_3–δ have been widely studied as cathode materials for solid oxide fuel cells (SOFCs). However, the long-term stability was a concern. Here we report our findings on the effect of a thin film coating of La_0.85Sr_0.15MnO_3–δ (LSM) on the performance of a porous La_0.6Sr_0.4Co_0.2Fe_0.8O_3–δ (LSCF) cathode. When the thicknesses of the LSM coatings are appropriate, an LSM-coated LSCF electrode showed better stability and lower polarization (or higher activity) than the blank LSCF cathode without LSM infiltration. An anode-supported cell with an LSM-infiltrated LSCF cathode demonstrated at 825 °C a peak power density of ～1.07 W/cm², about 24% higher than that of the same cell without LSM infiltration (～0.86 W/cm²). Further, the LSM coating enhanced the stability of the electrode; there was little degradation in performance for the cell with an LSM-infiltrated LSCF cathode during 100 h operation.     

新型碳纤维负载直接乙醇燃料电池Pt-SnO_2阳极催化剂的性能研究

采用静电纺丝技术制备了碳纤维基纳米Pt-SnO2阳极催化剂(Pt/Sn原子比为3)。通过X射线衍射(XRD)、红外光谱(FT-IR)、扫描电子显微镜(SEM)等技术对该催化剂进行了表征,并采用循环伏安法对其在乙醇燃料电池中的阳极催化活性进行了评价。结果表明,纳米Pt-SnO2催化剂均匀地分散在碳纤维骨架上;随着烧结温度的升高,碳纤维载体的致密度越高、导电性能越好。电催化性能测试表明,烧结温度为800℃时催化剂的峰电流密度最大,达到0.11 A/cm2,抗中毒能力也最强。单电池的发电性能表明,在一定的乙醇浓度下,1.0 mL/min进样流速具有最优的发电效率。     

Oxidation kinetics study of the iron-based steel for solid oxide fuel cell application

Kinetics of oxidation of Fe-Cr steel containing 25 wt.-percent Cr was studied as a function of temperature (1023–1173 K) for up to 480 h in flowing air, which corresponds to SOFC cathode environment operating conditions. The oxidation process was found to be a parabolic, suggesting that the diffusion of ionic defects in the scale is the slowest, rate determining step and it occurs predominantly by short-circuit diffusion paths. Comparison of the determined activation energy of oxidation of the studied steel with literature data indicates that at 1098–1173 K the chromia scale grows by the outward solid-state diffusion of chromium interstitials, whereas at 1023–1098 K — through a significant contribution of counter-current oxygen/chromium diffusion along Cr₂O₃ grain boundaries. The oxide scales were composed mainly of Cr₂O₃ with a continuous thin Mn_1.5Cr_1.5O₄ spinel layer on top of the chromia scale. The oxidation test results on Fe-25Cr steel demonstrate the applicability of the commercial type DIN 50049 stainless steel as interconnect for SOFC. This revised version was published online in July 2006 with corrections to the Cover Date.     

Microwave synthesis of polymer-embedded Pt-Ru catalyst for direct methanol fuel cell

Platinum-ruthenium nanoparticles stabilized within a conductive polymer matrix are prepared using microwave heating. Polypyrrole di(2-ethylhexyl) sulfosuccinate, or PPyDEHS, has been chosen for its known electrical conductivity, thermal stability, and solubility in polar organic solvents. A scalable and quick two-step process is proposed to fabricate alloyed nanoparticles dispersed in PPyDEHS. First a mixture of PPyDEHS and metallic precursors is heated in a microwave under reflux conditions. Then the nanoparticles are extracted by centrifugation. Physical characterization by TEM shows that crystalline and monodisperse alloyed nanoparticles with an average size of 2.8 nm are obtained. Diffraction data show that crystallite size is around 2.0 nm. Methanol electro-oxidation data allow us to propose these novel materials as potential candidates for direct methanol fuel cells (DMFC) application. The observed decrease in sulfur content in the polymer upon incorporation of PtRu nanoparticles may have adversely affected the measured catalytic activity by decreasing the conductivity of PPyDEHS. Higher concentration of polymer leads to lower catalyst activity. Design and synthesis of novel conductive polymers is needed at this point to enhance the catalytic properties of these hybrid materials.     

Neutron powder diffraction as a characterization tool of solid oxide fuel cell materials

Neutron diffraction is a powerful tool for the characterization of materials and, particularly, oxides. Oxide materials find applications in solid oxide fuel cells (SOFCs) as solid electrolytes as well as anode and cathode materials. As a structural probe, neutrons are specially suitable for the crystallographic study of oxides, given the comparable scattering factors of O and other heavier elements, allowing its precise localization in the crystal structure. Many problems can be addressed by neutrons, related to the octahedral tilting in perovskites, phase transitions, order–disorder phenomena, presence of anionic vacancies, etc. Neutrons make possible an accurate determination of the thermal factors and provide a visualization of the diffusion paths in ionic conductors. Neutrons allow the localization of light atoms such as hydrogen, and make possible the distinction between neighbouring elements, typically Fe and Mn. In this work we will describe some recent applications of this technique in the field of solid electrolytes and electrode materials, including some examples from our group.     

A sulfur-tolerant Pd/CeO2 catalyst for methanol synthesis from syngas

The catalytic activity of ceria-supported Pd for selective hydrogenation of CO is well preserved in the presence of 30 ppm H2S due to the parallel oxidation of sulfur by CeO2 under standard methanol synthesis conditions. The bifunctional nature of this catalyst opens a route for the conversion of sulfur-contaminated gas streams such as the integrated gasification combined cycle syngas or biogas into liquid fuels if desulfurization by conventional means is not practical.