Understanding galvanic replacement reactions: the case of Pt and Ag

Understanding galvanic replacement reactions: the case of Pt and Ag
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DOI:
10.1016/j.mtadv.2019.100037
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发表时间:
2020-03-01
影响因子:
10
通讯作者:
Puntes, V
Puntes, V
中科院分区:
材料科学2区
文献类型:
--
作者:
Merkoci, F.;Patarroyo, J.;Puntes, V

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纳米晶体(NCs)的合成尤其具有挑战性和难以控制,其中材料科学元素是用有机化学精密技术处理的。这种困难来自于矿化过程的复杂性增加和液固界面的产生。这些方面,以及对反应动力学的强烈敏感性,最终转化为可重复性和形态控制的严重挑战。通过系统地改变用于控制NCs形态的不同参数,包括络合剂、共还原剂和共氧化剂,可以绘制总体反应景观,并可以确定最稳定和可重复的配方。我们将这一概念应用于不混相Pt和Ag之间通过电替换反应形成空心Pt NCs的模型。在这项工作中,对648种合成配方进行了表征,并对每个重复进行了表征,从中分析了307种可控制形成空心nc的配方,以将反应条件与最终获得的结构和稳定性(再现性)联系起来。因此,我们提出了强大的通用合成方案,可用于特殊生产基于pt的空心nc,并可独立控制外壳厚度、空隙尺寸、表面粗糙度和孔隙度。(c) 2019年作者。Elsevier Ltd.出版。
Synthesis of nanocrystals (NCs), where material science elements are addressed with organic chemistry precision techniques, is especially challenging and difficult to control. This difficulty arises from the increased complexity of the mineralization processes and the generation of a liquid-solid interface. These aspects, along with a strong susceptibility to reaction kinetics, ultimately translate into serious challenges for reproducibility and morphological control. By systematically varying the different parameters used to control the morphology of NCs, including complexing agents, coreducers, and cooxidants, the general reaction landscape can be mapped and the most stable and reproducible recipes can be identified. We apply this concept to the model transmetallation reaction between immiscible Pt and Ag forming hollow Pt NCs by galvanic replacement reactions. In this work, 648 synthetic recipes were performed and characterized per duplicate, from which a subset of 307 recipes leading to the controlled formation of hollow NCs were further analyzed to correlate reaction conditions with the final obtained structure and stability (reproducibility). As a result, we present robust general synthetic protocols leading to the ad hoc production of Pt-based hollow NCs with independent control of shell thickness, void size, surface roughness, and degree of porosity. (c) 2019 The Authors. Published by Elsevier Ltd.