An autonomous organic reaction search engine for chemical reactivity.
An autonomous organic reaction search engine for chemical reactivity.
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DOI：
10.1038/ncomms15733
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发表时间：
2017-06-09
影响因子：
16.6
通讯作者：
Cronin L
中科院分区：
文献类型：
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作者：
Dragone V;Sans V;Henson AB;Granda JM;Cronin L
探索新的反应性、反应和分子的化学空间受限于需要单独的后处理-分离步骤来寻找分子而不是反应性。在这里，我们提出了一个系统，可以自主评估化学反应的64个可能的反应组合的网络内，并针对新的反应性，而不是预定义的一组目标。该机器人系统将化学处理、在线光谱学和实时反馈与分析与算法相结合，该算法能够区分和选择最具反应性的途径，生成反应选择指数（RSI），而无需单独的后处理或纯化步骤。这允许化学网络的自动导航，导致以前未报告的分子，同时只需要在没有任何化学知识的情况下进行全部可能反应的一小部分。我们发现RSI与反应性相关，并且能够使用最具反应性的途径搜索化学空间。虽然自动化反应系统通常用于合成预定义的分子，但发现反应性的自动化系统更具挑战性。在这里，作者报告了一个自主的有机反应搜索引擎，允许在多试剂，多步骤反应系统中发现最具反应性的途径。
The exploration of chemical space for new reactivity, reactions and molecules is limited by the need for separate work-up-separation steps searching for molecules rather than reactivity. Herein we present a system that can autonomously evaluate chemical reactivity within a network of 64 possible reaction combinations and aims for new reactivity, rather than a predefined set of targets. The robotic system combines chemical handling, in-line spectroscopy and real-time feedback and analysis with an algorithm that is able to distinguish and select the most reactive pathways, generating a reaction selection index (RSI) without need for separate work-up or purification steps. This allows the automatic navigation of a chemical network, leading to previously unreported molecules while needing only to do a fraction of the total possible reactions without any prior knowledge of the chemistry. We show the RSI correlates with reactivity and is able to search chemical space using the most reactive pathways. While automated reaction systems typically work for the synthesis of pre-defined molecules, automated systems to discover reactivity are more challenging. Here the authors report an autonomous organic reaction search engine that allows discovery of the most reactive pathways in a multi-reagent, multistep reaction system.