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将二氧化碳有效且可逆地插入铈唑盐中。

Effective and Reversible Carbon Dioxide Insertion into Cerium Pyrazolates.

作者信息

Bayer Uwe, Werner Daniel, Maichle-Mössmer Cäcilia, Anwander Reiner

机构信息

Institut für Anorganische Chemie, Eberhard Karls Universität Tübingen, Auf der Morgenstelle 18, 72076, Tübingen, Germany.

出版信息

Angew Chem Int Ed Engl. 2020 Mar 27;59(14):5830-5836. doi: 10.1002/anie.201916483. Epub 2020 Jan 30.

DOI:10.1002/anie.201916483
PMID:31916355
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC7155069/
Abstract

The homoleptic pyrazolate complexes [Ce (Me pz) ] and [Ce (Me pz) ] quantitatively insert CO to give [Ce (Me pz⋅CO ) ] and [Ce (Me pz⋅CO ) ], respectively (Me pz=3,5-dimethylpyrazolato). This process is reversible for both complexes, as observed by in situ IR and NMR spectroscopy in solution and by TGA in the solid state. By adjusting the molar ratio, one molecule of CO per [Ce (Me pz) ] complex could be inserted to give trimetallic [Ce (Me pz) (Me pz⋅CO ) (thf)]. Both the cerous and ceric insertion products catalyze the formation of cyclic carbonates from epoxides and CO under mild conditions. In the absence of epoxide, the ceric catalyst is prone to reduction by the co-catalyst tetra-n-butylammonium bromide (TBAB).

摘要

同配吡唑盐配合物[Ce(Me pz)₃]和[Ce(Me pz)₄]能定量插入CO，分别生成[Ce(Me pz)₃(CO)]和[Ce(Me pz)₄(CO)]（Me pz = 3,5 - 二甲基吡唑基）。如通过溶液中的原位红外光谱和核磁共振光谱以及固态热重分析所观察到的，该过程对这两种配合物而言都是可逆的。通过调节摩尔比，每个[Ce(Me pz)₄]配合物可插入一个CO分子，生成三金属配合物[Ce(Me pz)₃(Me pz·CO)(thf)]。亚铈和铈的插入产物在温和条件下均能催化环氧化物与CO反应生成环状碳酸酯。在没有环氧化物的情况下，铈催化剂易于被助催化剂四正丁基溴化铵（TBAB）还原。

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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b8b6/7155069/65ce8be92355/ANIE-59-5830-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b8b6/7155069/65b29a028f32/ANIE-59-5830-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b8b6/7155069/73f132bab041/ANIE-59-5830-g004.jpg
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