Toward a Janus Cluster: Regiospecific Decarboxylation of Ag44(4-MBA)30@Ag Nanoparticles,The Journal of Physical Chemistry C

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Toward a Janus Cluster: Regiospecific Decarboxylation of Ag44(4-MBA)30@Ag Nanoparticles
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2016-07-12 00:00:00 , DOI: 10.1021/acs.jpcc.6b04769
Indranath Chakraborty ₁ , Anirban Som ₁ , Tuhina Adit Maark ₁ , Biswajit Mondal ₁ , Depanjan Sarkar ₁ , Thalappil Pradeep ₁

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The ligand shell structure of the aspicule Ag₄₄(4-MBA)₃₀ (MBA: mercaptobenzoic acid, in the thiolate form) was modified in a precise, site-specific manner. Laser irradiation at 633 nm of a monolayer assembly of plasmonic Ag nanoparticles (NPs) covered with Ag₄₄(4-MBA)₃₀ clusters leads to decarboxylation of 4-MBA ligands forming thiophenolate (TP) ligands. While the molecular identity and integrity of aspicules post laser irradiation were confirmed by ESI MS, time-dependent SERS spectra and computational studies suggest that the phenomenon of decarboxylation is limited to the 4-MBA ligands facing the NP surface. This creates modified Ag₄₄ clusters, with 4-MBA ligands on one side and TP ligands on the other, giving them a two-faced (Janus) ligand structure. The ligand distribution of such clusters gets equilibrated in solution. We show that such selective transformation can be used to create molecular patterns. Janus clusters may be important in chemistry at biphasic interfaces.

中文翻译：

向Janus群集：Ag ₄₄（4-MBA）₃₀ @Ag纳米粒子的区域特异性脱羧。

Ag ₄₄（4-MBA）₃₀（MBA：巯基苯甲酸，硫醇盐形式）的配体壳结构以精确的位点特异性方式进行了修饰。在633 nm的激光照射下，覆盖有Ag ₄₄（4-MBA）₃₀簇的等离子体Ag纳米粒子（NP）的单层组件导致4-MBA配体的脱羧形成硫代酚盐（TP）配体。虽然通过ESI MS证实了激光照射后的小分子的分子身份和完整性，但随时间变化的SERS光谱和计算研究表明，脱羧现象仅限于面对NP表面的4-MBA配体。这会产生修饰的Ag ₄₄团簇，一侧为4-MBA配体，另一侧为TP配体，使它们具有双面（Janus）配体结构。这些簇的配体分布在溶液中达到平衡。我们表明这种选择性转化可用于创建分子模式。Janus团簇在双相界面化学中可能很重要。

更新日期：2016-07-12

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