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Shaped Pt-Ni nanocrystals with an ultrathin Pt-enriched shell derived from one-pot hydrothermal synthesis as active electrocatalysts for oxygen reduction

ISSN号：1006-3471
期刊名称：《电化学》
时间：0
分类：TQ424.25[化学工程] TM911.4[电气工程—电力电子与电力传动]
作者机构：[1]Beijing National Laboratory for Molecular Science, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China, [2]State Key Laboratory of Silicon Materials, Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Province and School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, China
相关基金：We thank Prof. Dechun Zou and Mr. Ming Peng for their help with electrochemical characterization. This work was supported by the National Natural Science Foundation of China （Nos. 21025101, 21271011, and 21321001）. Y. W. Z. particularly appreciates the financial aid from the China National Funds for Distinguished Young Scientists from the National Natural Science Foundation of China （NSFC）. The work on micros- copy was partly carried out in the Center of Electron Microscopy of Zhejiang University, which was financially supported by the National Natural Science Foundation of China （No. 51222202）, the National Basic Research Program of China （No. 2014CB932500） and the Program for Innovative Research Teams in Universities of Ministry of Education of China （No. IRT13037） and the Fundamental Research Funds for the Central Universities （No. 2014XZZX003-07）.

作者： Jun Gu[1], Guangxu Lan[1], Yingying Jiang[2], Yanshuang Xu[1], Wei Zhu[1], Chuanhong Jin[2], Yawen Zhang[1]

关键词：水热合成, 氧还原反应, 纳米晶体, 电催化剂, 铂原子, 镍合金, 比活性, X射线光电子能谱分析, Pt-NiPt-Ni alloy nanocrystals,bimetallic catalysts,oxygen reduction reaction,dealloying,aqueous-phase synthesis

中文摘要：

有 3d 转变金属的磅的合金 nanocrystals (NC ) ，特别 Ni，是为氧减小反应(ORR ) 的优秀催化剂。在这个工作，第一次，我们表明了水阶段 Pt-M (M = Ni，公司和 Fe ) 的胶体的合成有通过一个灵巧的热水的方法的悦耳的作文和形态学的合金 NC。Pt-Ni 合金 NC 综合了，这个方法更好介绍了 ORR 活动比商业 Pt/C 催化剂。X 光检查精力印射技术的散系列(版本) 表明充实磅的壳在同样综合的 Pt-Ni 合金 NC 上存在。厚分层的充实磅的壳在磅上形成了的大约二个原子 < 潜水艇 class= “ a-plus-plus ” > 50 Ni < 潜水艇 class= “ a-plus-plus ” > 当 Ni 内容增加了， 50 NC 和充实磅的壳的厚度增加了。而且， X 光检查光电子光谱学分析表明 Pt-Ni 合金 NC 上的表面磅原子的氧化水平与一金属的磅 NC 相比减少了，暗示在表面磅原子的 oxophilicity 的减少。有表面磅原子的更低的 oxophilicity 的 Pt-Ni 合金 NC 给更高的 ORR 活动。最活跃的合金样品显示出高 13 倍的特定的活动和高六倍的质量在 0.9 V 对一个可逆的氢电极的活动什么时候与商业 Pt/C 相比。Pt-Ni 合金 NC 也在长期的 ORR 测试比商业 Pt/C 显示出更好的耐久性。

英文摘要：

Alloy nanocrystals （NCs） of Pt with 3d transition metals, especially Ni, are excellent catalysts for the oxygen reduction reaction （ORR）. In this work, we, for the first time, demonstrated the water phase colloidal synthesis of Pt-M （M = Ni, Co and Fe） alloy NCs with tunable composition and morphology through a facile hydrothermal method. Pt-Ni alloy NCs synthesized with this method presented better ORR activity than commercial Pt/C catalysts. The X-ray energy dispersive spectra （EDS） mapping technique revealed that Pt-enriched shells existed on the as-synthesized Pt-Ni alloy NCs. About two atom thick layered Pt-enriched shells formed on Pts0Nis0 NCs and the thickness of the Pt-enriched shells increased as the Ni content increased. Furthermore, X-ray photoelectron spectroscopy analysis revealed that the oxidation level of the surface Pt atoms on the Pt-Ni alloy NCs decreased compared with monometallic Pt NCs, implying a decrease in the oxophilicity of the surface Pt atoms. Pt-Ni alloy NCs with lower oxophilicity of the surface Pt atoms give higher ORR activity. The most active alloy sample showed 13 times higher specific activity and six times higher mass activity at 0.9 V vs. a reversible hydrogen electrode when compared with commercial Pt/C. Pt-Ni alloy NCs also showed better durability than commercial Pt/C in long term ORR tests.