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发光碳点/ MoS 杂化材料中的电子相互作用及其对析氢反应的电催化活性。

Electronic Interactions in Illuminated Carbon Dot/MoS Ensembles and Electrocatalytic Activity towards Hydrogen Evolution.

机构信息

Theoretical and Physical Chemistry Institute, National Hellenic Research Foundation, 48 Vassileos Constantinou Avenue, 11635, Athens, Greece.

Instituto de Carboquímica (ICB-CSIC), Consejo Superior de Investigaciones Científicas, C/Miguel Luesma Castán 4, 50018, Zaragoza, Spain.

出版信息

Chemistry. 2018 Jul 20;24(41):10468-10474. doi: 10.1002/chem.201801425. Epub 2018 Jun 19.

Abstract

The preparation, characterization, and photophysical and electrocatalytic properties of carbon dot (CD)/MoS ensembles is reported. Based on electrostatic interactions, ammonium-functionalized MoS , which was prepared upon reaction of 1,2-dithiolane tert-butyl carbamate with MoS followed by acidic deprotection, was coupled with CDs bearing multiple carboxylates on their periphery, as derived upon microwave-assisted polycondensation of citric acid and ethylenediamine followed by alkaline treatment. Insights into electronic interactions between the two species within CD/MoS ensembles emanated from absorption and photoluminescence titration assays. Efficient fluorescence quenching of CDs by MoS was observed and attributed to photoinduced electron/energy transfer as the decay mechanism for the transduction of the singlet excited state of CDs. Finally, the electrocatalytic performance of the CD/MoS ensemble was assessed towards the hydrogen evolution reaction and found to be superior to that of individual CDs species.

摘要

报道了碳点(CD)/MoS 复合物的制备、表征以及光物理和电催化性质。基于静电相互作用,将 1,2-二硫代丁基氨基甲酸酯与 MoS 反应,然后进行酸性脱保护得到的铵功能化 MoS 与在微波辅助下柠檬酸和乙二胺缩聚,然后进行碱性处理得到的具有多个羧酸盐外围的 CD 偶联。通过吸收和光致荧光滴定分析深入了解了 CD/MoS 复合物中两种物质之间的电子相互作用。观察到 MoS 对 CDs 的有效荧光猝灭,并归因于光诱导电子/能量转移,这是 CD 的单重激发态转换的传输机制。最后,评估了 CD/MoS 复合物在析氢反应中的电催化性能,发现其优于单个 CD 物种。

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