Label-assisted mass spectrometry for the acceleration of reaction discovery and optimization.
Label-assisted mass spectrometry for the acceleration of reaction discovery and optimization.
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DOI：
10.1038/nchem.1612
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发表时间：
2013-05
期刊：
影响因子：
21.8
通讯作者：
Kozmin SA
中科院分区：
文献类型：
--
作者：
Cabrera-Pardo JR;Chai DI;Liu S;Mrksich M;Kozmin SA
新反应的识别扩展了我们对化学反应性的了解，并使新的合成应用成为可能。加快这一发现进程的步伐仍然具有挑战性。我们描述了一个高效和简单的平台，用于筛选大量潜在的化学反应，以发现和优化以前未知的催化转化，从而揭示新的化学反应性。我们的策略是基于标记的反应物之一与聚芳族化学标签，它选择性地经历光电离-解吸过程，激光照射后，没有外部矩阵的协助下，使任何产品的快速质谱检测源自这样的标记的反应物在复杂的反应混合物中，没有任何色谱分离。该方法成功地用于高通量发现和随后的优化两个以前未知的benzannulation反应。
Identification of new reactions expands our knowledge of chemical reactivity and enables new synthetic applications. Accelerating the pace of this discovery process remains challenging. We describe a highly effective and simple platform for screening a large number of potential chemical reactions in order to discover and optimize previously unknown catalytic transformations thereby revealing new chemical reactivity. Our strategy is based on labeling one of the reactants with a polyaromatic chemical tag, which selectively undergoes photoionization-desorption process upon laser irradiation without the assistance of an external matrix and enables rapid mass spectrometric detection of any products originating from such labeled reactants in complex reaction mixtures without any chromatographic separation. This method was successfully employed for high-throughput discovery and subsequent optimization of two previously unknown benzannulation reactions.