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Facet-Controlled Synthesis of Platinum-Group-Metal Quaternary Alloys: The Case of Nanocubes and {100} Facets
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2022-12-28 , DOI: 10.1021/jacs.2c12368
Chenxiao Wang 1 , Zhennan Huang 2 , Yong Ding 3 , Minghao Xie 1 , Miaofang Chi 2 , Younan Xia 1, 4
Affiliation  

We report a robust method for the facet-controlled synthesis of nanocrystals with an ultrathin shell made of a nearly equimolar RuRhPdPt quaternary alloy. Our strategy involves the use of well-defined Rh cubic seeds, halide-free precursors, and a method for precisely controlling the reaction kinetics of different precursors. In the setting of dropwise addition, the precursors with different reactivities can be reduced at about the same pace for the generation of an alloy with a uniform and well-controlled composition. The core–shell nanocubes show greatly enhanced activity toward ethanol oxidation when benchmarked against Pd and Pt counterparts. Combining in situ and ex situ electron microscopy studies, we also demonstrate that the core–shell nanocubes possess good thermal and electrochemical stability in terms of both geometrical shape and elemental composition, with their cubic shape and alloy composition retained when annealing at 500 °C or after long-term electrochemical cycling. It is expected that the synthetic approach can be further extended to fabricate multimetallic catalysts with enhanced activities toward a variety of thermal and electrochemical reactions.

中文翻译:

铂族金属季合金的晶面控制合成:纳米立方体和 {100} 晶面的案例

我们报告了一种通过面控制合成纳米晶体的可靠方法,该纳米晶体具有由近等摩尔的 RuRhPdPt 四元合金制成的超薄壳。我们的策略涉及使用明确定义的 Rh 立方晶种、无卤化物前体,以及精确控制不同前体反应动力学的方法。在逐滴添加的设置中,具有不同反应性的前体可以以大约相同的速度被还原,以生成具有均匀且良好控制的成分的合金。当以 Pd 和 Pt 对应物为基准时,核壳纳米立方体显示出大大增强的乙醇氧化活性。就地异地相结合通过电子显微镜研究,我们还证明了核壳纳米立方体在几何形状和元素组成方面具有良好的热稳定性和电化学稳定性,在 500 °C 退火或长期电化学循环后,其立方体形状和合金成分保持不变. 预计该合成方法可以进一步扩展以制造对各种热和电化学反应具有增强活性的多金属催化剂。
更新日期:2022-12-28
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