Reduction of CO2 and Related Compounds with a Low‐Valent CaI Synthon

The reduction of CO2 with low‐valent s‐block metal complexes is limited to MgI reducing agents. Herein, the reduction of a series of CX2 reagents (X = O, S, NiPr) with the CaI synthon [(BDI)Ca(THP)]2(N2) (VI) is described, which is a CaII complex that reacts like the hypothetical CaI complex (BDI)Ca...

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Main Authors: Stefan Thum, Jonathan Mai, Neha Patel, Jens Langer, Sjoerd Harder
Format: Article
Language:English
Published: Wiley-VCH 2025-07-01
Series:ChemistryEurope
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Online Access:https://doi.org/10.1002/ceur.202500080
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author Stefan Thum
Jonathan Mai
Neha Patel
Jens Langer
Sjoerd Harder
author_facet Stefan Thum
Jonathan Mai
Neha Patel
Jens Langer
Sjoerd Harder
author_sort Stefan Thum
collection DOAJ
description The reduction of CO2 with low‐valent s‐block metal complexes is limited to MgI reducing agents. Herein, the reduction of a series of CX2 reagents (X = O, S, NiPr) with the CaI synthon [(BDI)Ca(THP)]2(N2) (VI) is described, which is a CaII complex that reacts like the hypothetical CaI complex (BDI)CaCa(BDI); BDI = HC[(Me)‐N(DIPeP)]2, DIPeP = 2,6‐Et2CH‐phenyl, THP = tetrahydropyran. Reaction of VI with excess CO2 led to crystallization of a carbonate complex with a Ca4(CO3)24+ core. The stabilizing BDI ligands also react by nucleophilic addition of CO2 at the backbone γ‐C atom. Reaction with only two equivalents of CO2 gave the presumed carbonite (CO22−) intermediate, but this could not be confirmed by X‐ray diffraction. Reaction with CS2 gave the first unique s‐block metal complex with a CS22− anion. This anion bridges between two (BDI)Ca+ cations by CaC and CaS bonding. The reduction of iPrN=C=NiPr with VI gave C–C coupling to a [(iPrN)2C–C(NiPr)2]2− dianion. An intermediate with a C(NiPr)22− dianion could not be isolated.
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spelling doaj-art-c0b89b7a63024e0cbb1d004340b8f2bc2025-08-20T03:30:19ZengWiley-VCHChemistryEurope2751-47652025-07-0134n/an/a10.1002/ceur.202500080Reduction of CO2 and Related Compounds with a Low‐Valent CaI SynthonStefan Thum0Jonathan Mai1Neha Patel2Jens Langer3Sjoerd Harder4Inorganic and Organometallic Chemistry Friedrich‐Alexander Universität Erlangen‐Nürnberg Egerlandstraße 1 91058 Erlangen GermanyInorganic and Organometallic Chemistry Friedrich‐Alexander Universität Erlangen‐Nürnberg Egerlandstraße 1 91058 Erlangen GermanyInorganic and Organometallic Chemistry Friedrich‐Alexander Universität Erlangen‐Nürnberg Egerlandstraße 1 91058 Erlangen GermanyInorganic and Organometallic Chemistry Friedrich‐Alexander Universität Erlangen‐Nürnberg Egerlandstraße 1 91058 Erlangen GermanyInorganic and Organometallic Chemistry Friedrich‐Alexander Universität Erlangen‐Nürnberg Egerlandstraße 1 91058 Erlangen GermanyThe reduction of CO2 with low‐valent s‐block metal complexes is limited to MgI reducing agents. Herein, the reduction of a series of CX2 reagents (X = O, S, NiPr) with the CaI synthon [(BDI)Ca(THP)]2(N2) (VI) is described, which is a CaII complex that reacts like the hypothetical CaI complex (BDI)CaCa(BDI); BDI = HC[(Me)‐N(DIPeP)]2, DIPeP = 2,6‐Et2CH‐phenyl, THP = tetrahydropyran. Reaction of VI with excess CO2 led to crystallization of a carbonate complex with a Ca4(CO3)24+ core. The stabilizing BDI ligands also react by nucleophilic addition of CO2 at the backbone γ‐C atom. Reaction with only two equivalents of CO2 gave the presumed carbonite (CO22−) intermediate, but this could not be confirmed by X‐ray diffraction. Reaction with CS2 gave the first unique s‐block metal complex with a CS22− anion. This anion bridges between two (BDI)Ca+ cations by CaC and CaS bonding. The reduction of iPrN=C=NiPr with VI gave C–C coupling to a [(iPrN)2C–C(NiPr)2]2− dianion. An intermediate with a C(NiPr)22− dianion could not be isolated.https://doi.org/10.1002/ceur.202500080calciumcarbodiimideCO2CS2low‐valent
spellingShingle Stefan Thum
Jonathan Mai
Neha Patel
Jens Langer
Sjoerd Harder
Reduction of CO2 and Related Compounds with a Low‐Valent CaI Synthon
ChemistryEurope
calcium
carbodiimide
CO2
CS2
low‐valent
title Reduction of CO2 and Related Compounds with a Low‐Valent CaI Synthon
title_full Reduction of CO2 and Related Compounds with a Low‐Valent CaI Synthon
title_fullStr Reduction of CO2 and Related Compounds with a Low‐Valent CaI Synthon
title_full_unstemmed Reduction of CO2 and Related Compounds with a Low‐Valent CaI Synthon
title_short Reduction of CO2 and Related Compounds with a Low‐Valent CaI Synthon
title_sort reduction of co2 and related compounds with a low valent cai synthon
topic calcium
carbodiimide
CO2
CS2
low‐valent
url https://doi.org/10.1002/ceur.202500080
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