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Lanthanide Complexes Supported by a Trizinc Crown Ether as Catalysts for Alternating Copolymerization of Epoxide and CO2: Telomerization Controlled by Carboxylate Anions
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2018-01-17 , DOI: 10.1002/anie.201709218 Haruki Nagae 1 , Ryota Aoki 1 , Shin-nosuke Akutagawa 1 , Julian Kleemann 2 , Risa Tagawa 1 , Tobias Schindler 2 , Gyeongshin Choi 1 , Thomas P. Spaniol 2 , Hayato Tsurugi 1 , Jun Okuda 2 , Kazushi Mashima 1
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2018-01-17 , DOI: 10.1002/anie.201709218 Haruki Nagae 1 , Ryota Aoki 1 , Shin-nosuke Akutagawa 1 , Julian Kleemann 2 , Risa Tagawa 1 , Tobias Schindler 2 , Gyeongshin Choi 1 , Thomas P. Spaniol 2 , Hayato Tsurugi 1 , Jun Okuda 2 , Kazushi Mashima 1
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A new family of heterometallic catalysts based on trimetalated macrocyclic tris(salen) ligands and rare‐earth metals was prepared and structurally characterized. The LaZn3 system containing anionic ligands such as acetate plays a critical role in catalyzing the alternating copolymerization of cyclohexene oxide (CHO) and CO2 with a high proportion of carbonate linkages. Among the lanthanide metals, the CeZn3 system exhibits high catalytic activity with a turnover frequency (TOF) of over 370 h−1. NMR analysis of the complex and end‐group analysis of the polymer suggest that the acetate ligands are rapidly exchanged, not only among coordinated acetates, but also between coordinated acetates and added carboxylate anions. These unique properties make this the first example of telomerization for the copolymerization of CHO and CO2.
中文翻译：
Trizinc冠醚支持的镧系元素络合物作为环氧和CO2交替共聚的催化剂：羧酸根阴离子控制的端粒化
基于三金属化的大环三（salen）配体和稀土金属制备了新的杂金属催化剂家族，并对其结构进行了表征。包含阴离子配体（如乙酸盐）的LaZn 3系统在催化环己烯氧化物（CHO）和具有高比例碳酸盐键的CO 2交替共聚中起关键作用。在镧系金属中，CeZn 3体系表现出高催化活性，周转频率（TOF）超过370 h -1。聚合物的复杂和端基分析的NMR分析表明，不仅在配位的乙酸酯之间，而且在配位的乙酸酯和添加的羧酸根阴离子之间，乙酸酯配体都可以快速交换。这些独特的特性使它成为CHO和CO 2共聚的端粒化的第一个例子。
更新日期：2018-01-17
中文翻译：
Trizinc冠醚支持的镧系元素络合物作为环氧和CO2交替共聚的催化剂：羧酸根阴离子控制的端粒化
基于三金属化的大环三（salen）配体和稀土金属制备了新的杂金属催化剂家族，并对其结构进行了表征。包含阴离子配体（如乙酸盐）的LaZn 3系统在催化环己烯氧化物（CHO）和具有高比例碳酸盐键的CO 2交替共聚中起关键作用。在镧系金属中，CeZn 3体系表现出高催化活性，周转频率（TOF）超过370 h -1。聚合物的复杂和端基分析的NMR分析表明，不仅在配位的乙酸酯之间，而且在配位的乙酸酯和添加的羧酸根阴离子之间，乙酸酯配体都可以快速交换。这些独特的特性使它成为CHO和CO 2共聚的端粒化的第一个例子。
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