Hydrogenation of CO2\n-Derived Carbonates and Polycarbonates to Methanol and Diols by Metal-Ligand Cooperative Manganese Catalysis

Viktoriia Zubar; Yury Lebedev; Luis Azofra Mesa; Luigi Cavallo; Osama El-Sepelgy; Magnus Rueping

doi:10.1002/anie.201805630

Hydrogenation of CO2\n-Derived Carbonates and Polycarbonates to Methanol and Diols by Metal-Ligand Cooperative Manganese Catalysis

Viktoriia Zubar, Yury Lebedev, Luis Azofra Mesa, Luigi Cavallo, Osama El-Sepelgy, Magnus Rueping

Research output: Contribution to journal › Article › peer-review

160 Scopus citations

Abstract

The first base-metal-catalysed hydrogenation of CO2 -derived carbonates to alcohols is presented. The reaction proceeds under mild conditions in the presence of a well-defined manganese complex with a loading as low as 0.25 mol %. The non-precious-metal homogenous catalytic system provides an indirect route for the conversion of CO2 into methanol with the co-production of value-added (vicinal) diols in yields of up to 99 %. Experimental and computational studies indicate a metal-ligand cooperative catalysis mechanism.

Original language	English (US)
Pages (from-to)	13439-13443
Number of pages	5
Journal	Angewandte Chemie International Edition
Volume	57
Issue number	41
DOIs	https://doi.org/10.1002/anie.201805630 https://doi.org/10.1002/ange.201805630
State	Published - Sep 3 2018

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: L.M.A. and L.C. thank King Abdullah University of Science and Technology (KAUST) for support. Gratitude is also due to the KAUST Supercomputing Laboratory for providing computational resources and granting access to the supercomputer Shaheen II.

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title = "Hydrogenation of CO2\n-Derived Carbonates and Polycarbonates to Methanol and Diols by Metal-Ligand Cooperative Manganese Catalysis",

abstract = "The first base-metal-catalysed hydrogenation of CO2 -derived carbonates to alcohols is presented. The reaction proceeds under mild conditions in the presence of a well-defined manganese complex with a loading as low as 0.25 mol %. The non-precious-metal homogenous catalytic system provides an indirect route for the conversion of CO2 into methanol with the co-production of value-added (vicinal) diols in yields of up to 99 %. Experimental and computational studies indicate a metal-ligand cooperative catalysis mechanism.",

author = "Viktoriia Zubar and Yury Lebedev and {Azofra Mesa}, Luis and Luigi Cavallo and Osama El-Sepelgy and Magnus Rueping",

note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: L.M.A. and L.C. thank King Abdullah University of Science and Technology (KAUST) for support. Gratitude is also due to the KAUST Supercomputing Laboratory for providing computational resources and granting access to the supercomputer Shaheen II.",

year = "2018",

month = sep,

day = "3",

doi = "10.1002/anie.201805630",

language = "English (US)",

volume = "57",

pages = "13439--13443",

journal = "Angewandte Chemie International Edition",

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publisher = "John Wiley and Sons Ltd",

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Zubar, V, Lebedev, Y, Azofra Mesa, L, Cavallo, L, El-Sepelgy, O & Rueping, M 2018, 'Hydrogenation of CO2\n-Derived Carbonates and Polycarbonates to Methanol and Diols by Metal-Ligand Cooperative Manganese Catalysis', Angewandte Chemie International Edition, vol. 57, no. 41, pp. 13439-13443. https://doi.org/10.1002/anie.201805630, https://doi.org/10.1002/ange.201805630

TY - JOUR

T1 - Hydrogenation of CO2\n-Derived Carbonates and Polycarbonates to Methanol and Diols by Metal-Ligand Cooperative Manganese Catalysis

AU - Zubar, Viktoriia

AU - Lebedev, Yury

AU - Azofra Mesa, Luis

AU - Cavallo, Luigi

AU - El-Sepelgy, Osama

AU - Rueping, Magnus

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: L.M.A. and L.C. thank King Abdullah University of Science and Technology (KAUST) for support. Gratitude is also due to the KAUST Supercomputing Laboratory for providing computational resources and granting access to the supercomputer Shaheen II.

PY - 2018/9/3

Y1 - 2018/9/3

N2 - The first base-metal-catalysed hydrogenation of CO2 -derived carbonates to alcohols is presented. The reaction proceeds under mild conditions in the presence of a well-defined manganese complex with a loading as low as 0.25 mol %. The non-precious-metal homogenous catalytic system provides an indirect route for the conversion of CO2 into methanol with the co-production of value-added (vicinal) diols in yields of up to 99 %. Experimental and computational studies indicate a metal-ligand cooperative catalysis mechanism.

AB - The first base-metal-catalysed hydrogenation of CO2 -derived carbonates to alcohols is presented. The reaction proceeds under mild conditions in the presence of a well-defined manganese complex with a loading as low as 0.25 mol %. The non-precious-metal homogenous catalytic system provides an indirect route for the conversion of CO2 into methanol with the co-production of value-added (vicinal) diols in yields of up to 99 %. Experimental and computational studies indicate a metal-ligand cooperative catalysis mechanism.

UR - http://hdl.handle.net/10754/628519

UR - https://onlinelibrary.wiley.com/doi/full/10.1002/anie.201805630

UR - http://www.scopus.com/inward/record.url?scp=85053385750&partnerID=8YFLogxK

U2 - 10.1002/anie.201805630

DO - 10.1002/anie.201805630

M3 - Article

C2 - 30102010

SN - 1433-7851

VL - 57

SP - 13439

EP - 13443

JO - Angewandte Chemie International Edition

JF - Angewandte Chemie International Edition

IS - 41

ER -

Hydrogenation of CO2\n-Derived Carbonates and Polycarbonates to Methanol and Diols by Metal-Ligand Cooperative Manganese Catalysis

Abstract

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CCDC 1876010: Experimental Crystal Structure Determination : tricarbonyl-(2-(diphenylphosphino)-N-[(pyridin-2-yl)methyl]ethan-1-amine)-manganese bromide dichloromethane solvate

CCDC 1876010: Experimental Crystal Structure Determination : tricarbonyl-(2-(diphenylphosphino)-N-[(pyridin-2-yl)methyl]ethan-1-amine)-manganese bromide dichloromethane solvate

Cite this

Hydrogenation of CO2\n-Derived Carbonates and Polycarbonates to Methanol and Diols by Metal-Ligand Cooperative Manganese Catalysis

Abstract

Bibliographical note

Access to Document

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Datasets

CCDC 1876010: Experimental Crystal Structure Determination : tricarbonyl-(2-(diphenylphosphino)-N-[(pyridin-2-yl)methyl]ethan-1-amine)-manganese bromide dichloromethane solvate

CCDC 1876010: Experimental Crystal Structure Determination : tricarbonyl-(2-(diphenylphosphino)-N-[(pyridin-2-yl)methyl]ethan-1-amine)-manganese bromide dichloromethane solvate

Cite this