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Reversible Modulation of the Electrostatic Potential of a Colloidal Quantum Dot through the Protonation Equilibrium of Its Ligands
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2017-09-28 00:00:00 , DOI: 10.1021/acs.jpclett.7b02101 Chen He 1 , Zhengyi Zhang 1 , Chen Wang 1 , Yishu Jiang 1 , Emily A. Weiss 1
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2017-09-28 00:00:00 , DOI: 10.1021/acs.jpclett.7b02101 Chen He 1 , Zhengyi Zhang 1 , Chen Wang 1 , Yishu Jiang 1 , Emily A. Weiss 1
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This Letter describes the reversible modulation of the electrostatic potential at the interface between a colloidal PbS quantum dot (QD) and solvent, through the protonation equilibrium of the QD’s histamine-derivatized dihydrolipoic acid (DHLA) ligand shell. The electrostatic potential is sensitively monitored by the yield of photoinduced electron transfer from the QD to a charged electron acceptor, 9,10-anthraquinone-2-sulfonate (AQ). The permeability of the DHLA coating to the AQ progressively increases as the average degree of protonation of the ligand shell increases from 0 to 92%, as quantified by 1H NMR, upon successive additions of p-toluenesulfonic acid; this increase results in a decrease in the photoluminescence (PL) intensity of the QDs by a factor of 6.7. The increase in permeability is attributable to favorable electrostatic interactions between the ligands and AQ. This work suggests the potential of the combination of near-IR-emitting QDs and molecular quenchers as robust local H+ sensors.
中文翻译：
胶体量子点通过其配体的质子平衡对静电势的可逆调制
这封信描述了通过QD组胺衍生化的二氢硫辛酸（DHLA）配体壳的质子化平衡，在胶体PbS量子点（QD）和溶剂之间的界面上对电势的可逆调制。静电势通过从QD转移到带电电子受体9,10-蒽醌-2-磺酸盐（AQ）的光诱导电子转移的产率来灵敏地监控。的DHLA涂布到AQ渗透性逐渐增大作为平均程度的配位体壳从0增加到92％的质子化的，如通过定量1 H NMR，在连续加入p-甲苯磺酸；这种增加导致QD的光致发光（PL）强度降低了6.7倍。渗透性的增加归因于配体与AQ之间的良好静电相互作用。这项工作表明，结合近红外发射的量子点和分子猝灭剂作为稳健的局部H +传感器的潜力。
更新日期：2017-09-29
中文翻译：
胶体量子点通过其配体的质子平衡对静电势的可逆调制
这封信描述了通过QD组胺衍生化的二氢硫辛酸（DHLA）配体壳的质子化平衡，在胶体PbS量子点（QD）和溶剂之间的界面上对电势的可逆调制。静电势通过从QD转移到带电电子受体9,10-蒽醌-2-磺酸盐（AQ）的光诱导电子转移的产率来灵敏地监控。的DHLA涂布到AQ渗透性逐渐增大作为平均程度的配位体壳从0增加到92％的质子化的，如通过定量1 H NMR，在连续加入p-甲苯磺酸；这种增加导致QD的光致发光（PL）强度降低了6.7倍。渗透性的增加归因于配体与AQ之间的良好静电相互作用。这项工作表明，结合近红外发射的量子点和分子猝灭剂作为稳健的局部H +传感器的潜力。
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