A model for the formation of gold nanoparticles in the citrate synthesis method
A model for the formation of gold nanoparticles in the citrate synthesis method
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DOI：
10.1016/j.ces.2018.06.046
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发表时间：
2018-12-14
影响因子：
4.7
通讯作者：
Mazzei, Luca
中科院分区：
文献类型：
--
作者：
Agunloye, Emmanuel;Panariello, Luca;Mazzei, Luca
本文提出了一种预测柠檬酸盐合成方法中金纳米粒子（GNP）粒径演变的新模型。在该方法中，前体是四氯金酸的酸性溶液，而还原剂是柠檬酸钠的碱溶液。溶液的酸碱性质影响合成过程中颗粒尺寸的变化。在文献中，已经提出了各种机械理论来解释这种演变。图尔克维奇等人。 (1951)率先提出了这种合成方法，并提出了“组织者理论”。 Kumar 等人对合成的这种机制描述进行了建模。 (2007)，但最近 Agunloye 等人。 （2017）表明，在一些情况下，该模型表现不佳，因为它没有考虑反应物的酸碱性质。在这项工作中，我们提出了一个基于 Wuithschick 等人提出的合成种子介导的机械描述的动力学模型。 （2015）。在本说明书中，前体同时还原成金原子并羟基化成钝化形式。然后金原子聚集成种子颗粒，最终在生长步骤中与前体的被动形式发生反应。我们使用在种子介导机制有效的条件下获得的文献实验数据验证了该模型。预测的国民生产总值最终规模与实验获得的结果非常吻合。 (C) 2018 Elsevier Ltd. 保留所有权利。
This paper presents a new model for predicting the evolution of the particle size of gold nanoparticles (GNPs) in the citrate synthesis method. In this method, the precursor is an acid solution of tetrachloroauric acid, while the reducing agent is a base solution of sodium citrate. The acid-base properties of the solutions influence how the size of the particles evolves during the synthesis. In the literature, various mechanistic theories have been proposed to explain this evolution. Turkevich et al. (1951), who pioneered this synthesis method, suggested the "organizer theory". This mechanistic description of the synthesis was modelled by Kumar et al. (2007), but recently Agunloye et al. (2017) showed that in several cases this model performed poorly, since it does not account for the acid-base properties of the reactants. In this work, we present a kinetic model based on the synthesis seed-mediated mechanistic description proposed by Wuithschick et al. (2015). In this description, the precursor concurrently reduces into gold atoms and hydroxylates into a passive form. The gold atoms then aggregate into seed particles, which finally react with the passive form of the precursor in a growth step. We validated the model using experimental data from the literature obtained for conditions in which the seed-mediated mechanism is valid. The predicted GNP final sizes closely agree with those obtained experimentally. (C) 2018 Elsevier Ltd. All rights reserved.