Single-Micelle and Single-Zinc-Particle Imaging Provides Insights into the Physical Processes Underpinning Organozinc Reactions in Water.
Single-Micelle and Single-Zinc-Particle Imaging Provides Insights into the Physical Processes Underpinning Organozinc Reactions in Water.
复制标题
单胶束和单锌粒子成像提供了对水中有机锌反应的物理过程的见解。
DOI：
10.1021/jacs.2c00421
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发表时间：
2022-02-23
影响因子：
15
通讯作者：
Blum SA
中科院分区：
文献类型：
--
作者：
Peacock H;Blum SA
单个金属锌颗粒表面上的胶束通过荧光显微镜成像，其灵敏度高达单个胶束。这些胶束通过掺入硼二吡咯亚甲基（BODIPY）荧光团作为代表性的有机分子“货物”而被制成荧光的以能够成像。突出了这种原位和灵敏的荧光技术的优点，通过非原位SEM/EDS分析不可见相同的胶束。检查胶束溶液与锌揭示了一个老化过程：胶束不立即粘附在锌表面混合后，而是随着时间的推移建立。此外，在较长的时间内，较小的锌颗粒变得完全包裹在胶束“壳”中。一旦粘附，胶束在成像实验的持续时间（>2小时）内保留在锌表面的局部区域中。单胶束在溶液中成像，其分子含量的特点。双色荧光交叉实验表明，胶束粘附在锌离子表面，与溶液中的胶束分子交换，约2.5 h达到分子交换平衡。独特的（非合奏平均）交换动力学显示在锌表面上的不同位置的胶束，与单胶束或小的局部胶束簇的交换动力学一致。的胶束溶液的老化和交换率，而在表面上的锌表明，胶束质量传递过程可能有助于整体反应障碍可持续的有机锌交叉偶联反应在胶束水中。所观察到的老化的系统表明路线的制备，实验室规模的合成反应，涉及胶束制备的有机锌化合物的改进。
Micelles on the surfaces of individual metallic zinc particles are imaged by fluorescence microscopy with sensitivity up to single micelles. These micelles are made fluorescent to enable imaging, through incorporation of boron dipyrromethene (BODIPY) fluorophores as representative organic molecular “cargo”. Highlighting an advantage of this in situ and sensitive fluorescence technique, the same micelles are not visible by ex situ SEM/EDS analysis. Examination of micellar solutions with zinc reveals an aging process: micelles do not immediately adhere to the zinc surfaces upon mixing but rather build up over time. Furthermore, at longer times, smaller zinc particles become fully encased in micelle “shells”. Once adhered, micelles remain in local regions of the zinc surface for the duration of the imaging experiments (>2 h). Single micelles are imaged in solution, and their molecular contents are characterized. Two-color fluorescence crossover experiments show that micelles adhered to the surface of the zinc exchange molecular contents with micelles in solution, achieving molecular exchange equilibrium in ~2.5 h. Unique (non-ensemble averaged) exchange kinetics are displayed by micelles at different locations on the zinc surface, consistent with exchange kinetics of single micelles or small local clusters of micelles. The aging of the micellar solutions and the rate of exchange while on the surface of the zinc suggest that micelle mass transport processes may contribute to overall reaction barriers in sustainable organozinc cross-coupling reactions in micellar water. The observed aging of the system suggests routes for improvement of preparative, bench-scale synthetic reactions involving micellar preparations of organozinc compounds.
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影响因子：
16.6
作者：
Krasovskiy, Arkady;Malakhov, Vladimir;Knochel, Paul
通讯作者：
Knochel, Paul
影响因子：
8
作者：
Ansari TN;Sharma S;Hazra S;Jasinski JB;Wilson AJ;Hicks F;Leahy DK;Handa S
通讯作者：
Handa S
DOI：
10.1002/chem.201504100
发表时间：
2015-12-14
期刊：
Chemistry (Weinheim an der Bergstrasse, Germany)
影响因子：
--
作者：
Boott CE;Laine RF;Mahou P;Finnegan JR;Leitao EM;Webb SE;Kaminski CF;Manners I
通讯作者：
Manners I
影响因子：
12.9
作者：
Bihani, Manisha;Ansari, Tharique N.;Handa, Sachin
通讯作者：
Handa, Sachin
影响因子：
3.9
作者：
Gapinski, Jacek;Szymanski, Jedrzej;Holyst, Robert
通讯作者：
Holyst, Robert