Optically Controlled Recovery and Recycling of Homogeneous Organocatalysts Enabled by Photoswitches
Optically Controlled Recovery and Recycling of Homogeneous Organocatalysts Enabled by Photoswitches
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通过光开关实现均相有机催化剂的光控回收和再循环
DOI：
10.1002/anie.202300723
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发表时间：
2023
期刊：
影响因子：
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通讯作者：
Han, Grace G. D.
中科院分区：
文献类型：
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作者：
Qiu, Qianfeng;Sun, Zhenhuan;Joubran, Danielle;Li, Xiang;Wan, Joshua;Schmidt‐Rohr, Klaus;Han, Grace G. D.
我们解决了一个关键的挑战，回收和循环均相有机催化剂，通过设计光开关催化剂结构，显示可逆的溶解度变化，响应于光。最初不溶的催化剂被UV转换为可溶的异构体状态，其催化反应，然后在反应完成后反异构化为不溶状态，以进行过滤和再循环。揭示了允许异构体状态之间超过10倍的剧烈溶解度变化、通过光诱导沉淀的87%回收率和多轮催化剂循环的分子设计原理。这一概念验证将为开发高度可回收的均相催化剂提供机会，这些催化剂对于合成各个行业的关键化合物非常重要，预计将显著降低环境影响和成本。
We address a critical challenge of recovering and recycling homogeneous organocatalysts by designing photoswitchable catalyst structures that display a reversible solubility change in response to light. Initially insoluble catalysts are UV‐switched to a soluble isomeric state, which catalyzes the reaction, then back‐isomerizes to the insoluble state upon completion of the reaction to be filtered and recycled. The molecular design principles that allow for the drastic solubility change over 10 times between the isomeric states, 87 % recovery by the light‐induced precipitation, and multiple rounds of catalyst recycling are revealed. This proof of concept will open up opportunities to develop highly recyclable homogeneous catalysts that are important for the synthesis of critical compounds in various industries, which is anticipated to significantly reduce environmental impact and costs.