Polyketones from Carbon Dioxide and Ethylene by Integrating Electrochemical and Organometallic Catalysis
Polyketones from Carbon Dioxide and Ethylene by Integrating Electrochemical and Organometallic Catalysis
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DOI：
10.1021/acscatal.3c00769
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发表时间：
2023-03-09
期刊：
影响因子：
12.9
通讯作者：
Miller, Alexander J. M.
中科院分区：
文献类型：
--
作者：
Dodge, Henry M.;Natinsky, Benjamin S.;Miller, Alexander J. M.
在聚合物合成中利用二氧化碳对于可持续材料来说是一个有吸引力的策略。电化学二氧化碳还原将为生产单体提供一个天然的起点，但电催化的条件通常与配位插入聚合的条件截然不同。本文报道了一种耦合电化学和有机金属催化剂的策略，该策略能够在单个多室反应器中从二氧化碳和乙烯合成聚酮。以这种方式可以制备由 CO2 衍生的高达 50 wt% 的聚酮材料。对产生 CO 的催化剂进行恒电位控制，可以控制低压 CO 的生成，与膦磺酸钯有机金属催化剂相结合，可以共聚为非交替聚酮，并根据所施加的电流密度调整 CO 含量。
The utilization of carbon dioxide in polymer synthesis is an attractive strategy for sustainable materials. Electrochemical CO2 reduction would offer a natural starting point for producing monomers, but the conditions of electrocatalysis are often drastically different from the conditions of coordination-insertion polymerization. Reported here is a strategy for coupling electrochemical and organometallic catalysts that enables polyketone synthesis from CO2 and ethylene in a single multicompartment reactor. Polyketone materials that are CO2- derived up to 50 wt % can be prepared in this way. Potentiostatic control over the CO-producing catalyst enables the controlled generation of low-pressure CO, which in conjunction with a palladium phosphine sulfonate organometallic catalyst enables copolymerization to nonalternating polyketones with the CO content tuned based on the applied current density.