通过高吞吐量实验和机器学习来对1,2-二碳烯的恩和区域选择性单降解进行一般性驱动的优化
Terim Seo1, Donghun Kim2, Shinwon Ham1
1Department of Chemistry, Sungkyunkwan University, Suwon, 16419, Republic of Korea.
Angewandte Chemie (International ed. in English)
|November 3, 2025
概括
这项研究引入了一种高通量选策略,用于使用性氧化玻利离子 (COBI) 催化剂对1,2-二碳酸进行不对称的减少. 机器学习模型确定了有效的催化剂,使有价值的性化合物的高效合成成为可能.
科学领域:
- 有机化学 有机化学
- 催化剂是一种催化剂.
- 高通量试验 高通量试验
背景情况:
- 为各种基质优化单一的催化剂是不可预测的和低效的.
- 开发1,2-二碳烯的一般不对称还原方法仍然是一个挑战.
研究的目的:
- 开发一种实用的多基板选策略,用于1,2-二碳烯的不对称单降解.
- 为了确定有效的性氧化玻利离子 (COBI) 催化剂,以实现广泛的基板适用性.
主要方法:
- 利用高通量实验 (HTE) 进行快速催化剂和基质选.
- 使用定量1H NMR和19F NMR进行聚合反应混合物的加速分析.
- 利用机器学习模型与冷凝反应图 (CGR) 描述符用于催化剂预测.
- 引入了用于SMILES预处理的各种替代品 (ARMS) 系统的自动反应映射.
主要成果:
- 在八个基板上选了31个COBI变体,实现了八倍的工作流加速.
- 确定了用于不对称还原的高效催化剂,产生奇拉性α-silyloxy子 (>99%的产量,>99% ee).
- 机器学习模型成功地预测了催化剂,而不需要量子化学计算.
结论:
- 开发的HTE策略和ML方法为发现一般不对称的还原催化剂提供了有效的方法.
- 合成的性α-silyloxy类作为有价值的前体,用于高价值化合物,如 (S) -bupropion.
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