时间分辨SANS揭示粒子间配体交换动力学

IF 9.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2024-12-25 DOI:10.1021/acs.nanolett.4c04163

Sang-Jo Lee, Jong Dae Jang, Sung-Min Choi

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引用次数: 0

摘要

纳米粒子超晶格的形成过程中会发生粒子间配体交换，从而影响纳米粒子超晶格的对称性。在这里，我们报道了时间分辨小角中子散射（TR-SANS）测量不同温度下金纳米颗粒（AuNPs）中硫化物配体的颗粒间交换动力学。为了跟踪AuNPs之间的配体交换，分别用氢化和氘化十二硫醇对两组AuNPs进行功能化，然后将其混合在甲苯和氘化甲苯的溶剂混合物中进行壳对比。颗粒间配体交换在25℃条件下即使经过40 h也几乎没有发生，而在50℃、60℃和70℃条件下分别发生了11%、34%和74%的交换。在80℃下，20 h后交换达到饱和。交换过程符合一级动力学，其活化能估计为29.1 kcal/mol，支持配体脱附是一个速率决定步骤。这些发现可以作为有价值的参考数据，帮助设计和理解npsl。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Interparticle Ligand Exchange Kinetics Revealed by Time-Resolved SANS

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Interparticle Ligand Exchange Kinetics Revealed by Time-Resolved SANS

Interparticle ligand exchange can occur during the formation of nanoparticle superlattices (NPSLs), affecting the symmetry of the NPSLs. Here, we report time-resolved small-angle neutron scattering (TR-SANS) measurements of the interparticle exchange kinetics of thiolate ligands among gold nanoparticles (AuNPs) at different temperatures. To track the ligand exchange among AuNPs, two groups of AuNPs were functionalized with hydrogenated and deuterated dodecanethiol, respectively, and then mixed in a solvent mixture of toluene and deuterated toluene for shell contrast. The interparticle ligand exchange barely occurred at 25 °C even after 40 h, but 11%, 34%, and 74% occurred at 50, 60, and 70 °C, respectively. At 80 °C, the exchange saturated after 20 h. The exchange process follows first-order kinetics, and its activation energy is estimated to be 29.1 kcal/mol, supporting that ligand desorption is a rate-determining step. These findings can be used as valuable reference data, aiding in the design and understanding of NPSLs.

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.