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微量Co修饰的碳载超细Pt纳米粒子的制备及其在燃料电池氧还原催化中的应用(英文) 被引量:7
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作者 唐雪君 方达晖 +6 位作者 瞿丽娟 徐东彦 秦晓平 覃博文 宋微 邵志刚 衣宝廉 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2019年第4期504-514,M0002,共12页
质子交换膜燃料电池(PEMFC)具有清洁、高效等优点,是一种理想的汽车动力电源.然而,由于其阴极氧还原反应(ORR)速率缓慢,需要使用大量的Pt基催化剂,导致燃料电池成本居高不下,严重制约了PEMFC的商业化发展.将Pt与过渡金属Fe, Co, Ni等形... 质子交换膜燃料电池(PEMFC)具有清洁、高效等优点,是一种理想的汽车动力电源.然而,由于其阴极氧还原反应(ORR)速率缓慢,需要使用大量的Pt基催化剂,导致燃料电池成本居高不下,严重制约了PEMFC的商业化发展.将Pt与过渡金属Fe, Co, Ni等形成合金,对表面Pt原子的几何结构和电子结构进行调变,可以有效提高催化剂的活性,实现Pt用量和燃料电池成本的降低.但是目前合金催化剂多采用溶剂热、浸渍-高温退火等制备方法,使用有毒有害试剂和难清洗的表面活性剂,且过程复杂、能耗高,不利于大规模化生产.此外,合金中过渡金属占比高,在燃料电池工况下,大量过渡金属溶解,加速了膜的降解,导致实际PEMFC性能的降低.对此,我们探索了一种简便有效的方法制备高活性、高稳定性的碳载Pt-Co催化剂.在没有添加表面活性剂的情况下,采用硼氢化钠辅助乙二醇还原法合成了具有超小尺寸和均匀分布的Pt-Co纳米颗粒,后续酸刻蚀处理去除不稳定的Co原子,重组双金属纳米颗粒的表面结构形成富Pt壳层,进一步提高了催化剂的活性和稳定性.通过电感耦合等离子体、X射线粉末衍射、透射电子显微镜、高分辨透射电子显微镜、高角环形暗场-扫描透射-元素分布及光电子能谱等物理表征证实了微量Co改性的碳载超细铂合金纳米颗粒的组成和结构.进一步对催化剂进行旋转圆盘电极和单电池测试,结果表明, Pt_(36)Co/C具有明显高于商业化Pt/C的有效电化学活性面积和电池性能.此外,加速衰减测试和衰减前后的电镜图片表明, Pt_(36)Co/C催化剂的稳定性相较于Pt/C亦有所增强.分析Pt-Co/C催化性能提高的原因,主要归于以下三点:(1)催化剂纳米颗粒在载体上分布均匀,且具有超小的粒径尺寸,提供了大量的三相反应界面位点;(2)双金属配体和电子效应的协同作用,降低了氧化物质在催化表面的吸附能力,加速了ORR的电催化动力学;(3)酸蚀刻导致的不稳定Co的溶解及催化剂表面结构的重排,形成了富Pt壳层结构,有利于提高催化剂的稳定性.这种简单有效的合金制备方法可以在电催化领域推广使用. 展开更多
关键词 质子交换膜燃料电池 氧还原反应 超细Pt纳米粒子 微量Co修饰 改进的乙二醇还原法 酸刻蚀
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Effect of electrode Pt-loading and cathode flow-field plate type on the degradation of PEMFC 被引量:5
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作者 lijuan qu Zhiqiang Wang +5 位作者 Xiaoqian Guo Wei Song Feng Xie Liang He Zhigang Shao Baolian Yi 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2019年第8期95-103,I0005,共10页
The electrode Pt-loading has an effect on the number of active sites and the thickness of catalyst layer,which has huge influence on the mass transfer and water management during dynamic process in PEMFCs. In this stu... The electrode Pt-loading has an effect on the number of active sites and the thickness of catalyst layer,which has huge influence on the mass transfer and water management during dynamic process in PEMFCs. In this study, membrane electrode assemblies with different Pt-loadings were prepared, and PEMFCs were assembled using those membrane electrode assemblies with traditional solid plate and water transport plate as cathode flow-field plates, respectively. The performance and electrochemical surface area of cells were characterized to evaluate the membrane electrode assemblies degradation after rapid currentvariation cycles. Scanning electron microscope and transmission electron microscope were used to investigate the decay of catalyst layers and Pt/C catalyst. With the increase of Pt-loading, the performance degradation of membrane electrode assemblies will be mitigated. But higher Pt-loading means thicker catalyst layer, which leads to a longer pathway of mass transfer, and it may result in carbon material corrosion in membrane electrode assemblies. The decay of Pt/C catalyst in cathode is mainly caused by the corrosion of carbon support, and the degradation of anode Pt/C catalyst is a consequence of migration and aggregation of Pt particles. And using water transport plate is beneficial to alleviating the age of cathode Pt/C catalyst. 展开更多
关键词 PROTON exchange membrane fuel cell ELECTRODE PLATINUM LOADING Current-variation cycle Traditional solid PLATE Water transport PLATE
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Protein Globule Formation in the Liver Graft during Cold Preservation for Liver Transplantation: Its Clinical and Pathological Significance
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作者 Changyin Feng Tongmei He +4 位作者 Haijian Huang lijuan qu Yi Jiang Wenhua Zhang Zhiyong Zheng 《Open Journal of Pathology》 2013年第3期119-126,共8页
In liver transplantation, liver graft ischemia-reperfusion injury occurs mainly due to cold preservation and warm reperfusion. In this research, we study the affection of plasma protein of the donor on liver graft dur... In liver transplantation, liver graft ischemia-reperfusion injury occurs mainly due to cold preservation and warm reperfusion. In this research, we study the affection of plasma protein of the donor on liver graft during cold preservation and warm reperfusion. In this study, 34 liver transplantations were performed from 2007 to 2010, and the clinical data were collected retrospectively from the Dongfang Hospital database. 34 specimens were harvested from 34 liver grafts when graft trimming as Group A and 34 specimens harvested from the same 34 liver grafts during liver transplantation surgery but before abdominal closure as B group. All liver tissue specimens were fixed with 40 g/L neutral formalin, embedded in paraffin. Light microscopy, transmission electron microscopy, Periodic Acid-Schiff (PAS) stain and immunohistochemical stain of IgG, IgM, IgA, C3d, C4d, Fib, C1q, and CD61 were used. In this study, we found that eosinophilic bodies emerged in liver lobes during liver transplantation which had not been reported previously in the literature. 1) Protein globules were found exclusively in liver graft specimens. The globules were round or oval with sharp edges, measured approximately 1.59 to 9.41 μm in diameter, and were scattered in the liver sinusoids or space of Disse or hepatocyte cytoplasm, were stained with IgG, IgM, IgA, Fib, C3d by immunohistochemical staining;2) There was no statistical significant difference of protein globules number between A group and B group (P > 0.05);3) IRI score of B group was not correlated with protein globules number (P > 0.05). Protein globules contain plasma composition, and may form during cold preservation. 展开更多
关键词 HEPATITIS B Virus IMMUNOHISTOCHEMISTRY LIVER Transplantation LIVER ISCHEMIA-REPERFUSION Injury
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A Profile of Native Integration Sites Used by φC31 Integrase in the Bovine Genome 被引量:1
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作者 lijuan qu Qingwen Ma +5 位作者 Zaiwei Zhou Haiyan Ma Ying Huang Shuzhen Huang Fanyi Zeng Yitao Zeng 《Journal of Genetics and Genomics》 SCIE CAS CSCD 2012年第5期217-224,共8页
The Streptomyces phage φC31 integrase can efficiently target attB-bearing transgenes to endogenous pseudo attP sites within mammalian genomes. To better understand the activity of φC31 integrase in the bovine genome... The Streptomyces phage φC31 integrase can efficiently target attB-bearing transgenes to endogenous pseudo attP sites within mammalian genomes. To better understand the activity of φC31 integrase in the bovine genome, DNA sequences of 44 integration events were analyzed, and 32 pseudo attP sites were identified. The majority of these sites share a sequence motif that contains inverted repeats and has similarities to wild-type attP site. Genomic DNA flanking these sites typically contained repetitive sequence elements, such as short and long interspersed repetitive elements. These sequence features indicate that DNA sequence recognition plays an important role in guiding φC31-mediated site-specific integration. In addition, BF27 integration hotspot sites were identified in the bovine genome, which accounted for 13.6% of all isolated integration events and mapped to an intron of the deleted in liver cancer 1 (DLC1) gene. Also we found that the pseudo attP sites in the bovine genome had other features in common with those in the human genome. This study represents the first time that the sequence features of pseudo attP sites specific integrase system has great potential for applied modifications in the bovine genome were analyzed. We conclude that this site- of the bovine genome. 展开更多
关键词 φC31 integrase Pseudo attP sites Sequence motif Repetitive elements Bovine genome
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