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作 者:王娟[1] 秦海英[2] 刘嘉斌[3] 李爱国[1] 张继超[1] 闫帅[1] 何燕[1] 余笑寒[1]
机构地区:[1]中国科学院上海应用物理研究所,上海201204 [2]杭州电子科技大学材料与环境工程学院,杭州310018 [3]浙江大学应用力学研究所,杭州310027
出 处:《核技术》2013年第2期1-6,共6页Nuclear Techniques
基 金:国家自然科学基金(21006090;11075200);科技部973计划(2010CB934501);浙江省钱江人才计划(2012R10058)资助
摘 要:介绍了上海光源硬X射线微聚焦及应用线站的新型原位实验装置,可用于对直接硼氢化钠燃料电池(DBFC)中阴极催化剂进行原位X射线衍射和荧光模式的X射线吸收近边结构测试,为研究阴极催化剂催化氧还原反应(ORR)机理提供实时表征依据。为验证本原位装置的可行性,在DBFC(采用聚吡咯修饰的碳载氢氧化钴作为阴极催化剂)工作过程中对催化剂进行原位测试。结果表明,在DBFC放电过程中,催化剂中Co元素的价态和局域结构发生变化,催化反应过程中新相形成。表明该原位实验装置对于DBFC中阴极催化剂催化ORR机理的研究是可行的。Background: Identifying the natures of the active sites in the catalysts is one of the key issues for the catalytic mechanism research. However, no accurate conclusions regarding to the nature of the electrocatalytic site that active in oxygen reduction reaction (ORR) can be extracted based merely on ex situ data of the dry material. Purpose: A new kind of in situ experimental setup based on BL15U1 in Shanghai Synchrotron Radiation Facility (SSRF) is designed to study the catalytic mechanism deeply by in situ characterization which is expected to be the most direct and necessary method. Methods: The in situ X-ray Diffraction (XRD) and Fluorescent X-ray Absorption Near Edge Structure (XANES) measurements were performed for the cathode catalyst (polypyrrole modified carbon supported cobalt hydroxide) of DBFC on BL15U1 in SSRF. Results: A new phase was formed during DBFC discharging, and the valence state varieties of Co atoms in cathode were recorded. Conclusions: Part of the Co2+ transformation to Co3+ to form CO2+/Co3+ balance during the catalytic reaction, resulting in the formation of a new chemical phase. It is confirmed that, by the preliminary analysis, this setup can provide real time evidence which can be used to research the ORR catalytic mechanism of the direct borohydride fuel cell cathode catalyst.
关 键 词:原位实验装置 直接硼氢化钠燃料电池 氧还原反应机理
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