Flow Alters the Interfacial Reactions of Upconversion Nanocrystals Probed by In Situ Sum Frequency Generation

Flow Alters the Interfacial Reactions of Upconversion Nanocrystals Probed by In Situ Sum Frequency Generation
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通过原位和频生成探测流动改变上转换纳米晶体的界面反应

DOI:
10.1002/admi.201902046
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发表时间:
2020-02
期刊:
Adv. Mater. Interfaces
影响因子:
--
通讯作者:
Lin Hongzhen
Lin Hongzhen
中科院分区:
其他
文献类型:
--
作者:
Yonglan Xi;Lin Hongzhen

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粒子运动是胶体纳米颗粒的一种基本现象,但其对界面相互作用的影响还远未阐明。通过模拟上转换氟纳米粒子在流动池中的粒子运动,采用原位和频与光致发光光谱相结合的方法,清楚地揭示了界面反应对胶体纳米粒子运动的高度依赖性。研究发现,颗粒运动会产生一个带正电荷的表面,从而引起吸附界面水的重排。更重要的是,除了通过增强的静电相互作用更容易吸附罗丹明B的带负电荷的羧基外,在pH为6.8的情况下移动的粒子还可以通过排斥带正电的二乙氨基来重新定向平行于NP表面的染料的黄环。因此,只需调节流量,就可以可逆地调制从上转换NPs到罗丹明B的荧光共振能量转移效率。这项工作为胶体纳米粒子的界面相互作用提供了新的视角,有望指导其表面修饰和实际应用。
Particle moving is a fundamental phenomenon of colloidal nanoparticles (NPs), but its influence on the interfacial interaction is far from been clarified. Herein, by mimicking the particle moving of upconverting fluoride NPs in a flowing cell, highly dependence of interfacial reactions on the particle moving of the colloidal NPs is clearly revealed by adopting combined in situ sum frequency generation and photoluminescence spectroscopies. It is found that particle moving can induce the rearrangement of the adsorbed interfacial water due to generating a more positively charged surface. More importantly, besides more prone to adsorb negatively charged carboxyl group of Rhodamine B via enhanced electrostatical interaction, particle moving at pH of 6.8 could reorient the xanthene ring of the dye parallel to the NP surface, via repelling the positively charged diethylamino groups. As a consequence, fluorescence resonance energy transfer efficiency from the upconverting NPs to Rhodamine B can be reversibly modulated by only tuning the flow. This work provides new insight into the interfacial interactions of the colloidal NPs, which are expected to guide their surface modification and practical applications.
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