Quantum Dot Assembly Driven by Electrochemically Generated Metal-Ion Crosslinkers
Quantum Dot Assembly Driven by Electrochemically Generated Metal-Ion Crosslinkers
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DOI：
10.1021/acs.chemmater.1c00832
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发表时间：
2021-06-09
影响因子：
8.6
通讯作者：
Luo, Long
中科院分区：
文献类型：
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作者：
Hewa-Rahinduwage, Chathuranga C.;Silva, Karunamuni L.;Luo, Long
纳米颗粒组装的控制是制造能够实现复杂的系统级功能的纳米结构的关键使能器。在这里，我们报告了一个简单的电化学方法组装成介孔凝胶量子点（QD）直接到电极表面上使用本地化，原位生成的金属离子交联剂（Ni 2+，Co 2+，Ag+，或Zn 2+）内的金属硫族化物纳米粒子的胶体溶液与配位体具有悬垂羧酸基团。机理研究揭示了0.5个金属离子的临界化学计量：溶液中需要1个QD来触发金属离子介导的电凝胶化（ME-凝胶化），这表示金属离子的浓度比在整个溶液体积中引发交联所需的浓度低得多（>26个金属离子：溶液中1个QD）。ME凝胶化方法用于制造基于QD的电子器件的应用通过QD凝胶在印刷电路板芯片上的电化学图案化来证明。
Control of nanoparticle assembly is a critical enabler for fabricating nanostructures capable of complex, system-level functionality. Here, we report a facile electrochemical method for assembling quantum dots (QDs) into mesoporous gels directly onto an electrode surface using localized, in situ generated metal ion crosslinkers (Ni2+, Co2+, Ag+, or Zn2+) within a colloidal solution of metal chalcogenide nanoparticles capped with ligands featuring pendant carboxylate groups. A mechanistic study reveals a critical stoichiometry of 0.5 metal ions: 1 QD in solution is required to trigger metal ion-mediated electrogelation (ME-gelation), representing a much lower concentration of metal ions than is needed for initiating crosslinking throughout an entire volume of solution (>26 metal ions: 1 QD in solution). The application of the ME gelation approach for the fabrication of QD-based electronic devices is demonstrated by electrochemical patterning of QD gels onto a printed circuit board chip.