N-Heterocyclic Carbene Modified Palladium Catalysts for the Direct Synthesis of Hydrogen Peroxide

Richard J. Lewis; Maximilian Koy; Margherita Macino; Mowpriya Das; James H. Carter; David J. Morgan; Thomas E. Davies; Johannes B. Ernst; Simon J. Freakley; Frank Glorius; Graham J. Hutchings

doi:10.1021/jacs.2c04828

N-Heterocyclic Carbene Modified Palladium Catalysts for the Direct Synthesis of Hydrogen Peroxide

Richard J. Lewis, Maximilian Koy, Margherita Macino, Mowpriya Das, James H. Carter, David J. Morgan, Thomas E. Davies, Johannes B. Ernst, Simon J. Freakley, Frank Glorius, Graham J. Hutchings

Department of Chemistry

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

9 Citations (SciVal)

Abstract

Heterogeneous palladium catalysts modified by N-heterocyclic carbenes (NHCs) are shown to be highly effective toward the direct synthesis of hydrogen peroxide (H2O2), in the absence of the promoters which are typically required to enhance both activity and selectivity. Catalytic evaluation in a batch regime demonstrated that through careful selection of the N-substituent of the NHC it is possible to greatly enhance catalytic performance when compared to the unmodified analogue and reach concentrations of H2O2 rivaling that obtained by state-of-the-art catalysts. The enhanced performance of the modified catalyst, which is retained upon reuse, is attributed to the ability of the NHC to electronically modify Pd speciation.

Original language	English
Pages (from-to)	15431-15436
Number of pages	6
Journal	Journal of the American Chemical Society
Volume	144
Issue number	34
Early online date	17 Aug 2022
DOIs	https://doi.org/10.1021/jacs.2c04828
Publication status	Published - 31 Aug 2022

ASJC Scopus subject areas

Catalysis
Chemistry(all)
Biochemistry
Colloid and Surface Chemistry

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10.1021/jacs.2c04828Licence: CC BY

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@article{19caaad460b6458a899a17a601046ace,

title = "N-Heterocyclic Carbene Modified Palladium Catalysts for the Direct Synthesis of Hydrogen Peroxide",

abstract = "Heterogeneous palladium catalysts modified by N-heterocyclic carbenes (NHCs) are shown to be highly effective toward the direct synthesis of hydrogen peroxide (H2O2), in the absence of the promoters which are typically required to enhance both activity and selectivity. Catalytic evaluation in a batch regime demonstrated that through careful selection of the N-substituent of the NHC it is possible to greatly enhance catalytic performance when compared to the unmodified analogue and reach concentrations of H2O2 rivaling that obtained by state-of-the-art catalysts. The enhanced performance of the modified catalyst, which is retained upon reuse, is attributed to the ability of the NHC to electronically modify Pd speciation. ",

author = "Lewis, {Richard J.} and Maximilian Koy and Margherita Macino and Mowpriya Das and Carter, {James H.} and Morgan, {David J.} and Davies, {Thomas E.} and Ernst, {Johannes B.} and Freakley, {Simon J.} and Frank Glorius and Hutchings, {Graham J.}",

note = "Funding Information: R.J.L., J.H.C., D.J.M., T.E.D., and G.J.H. gratefully acknowledge Cardiff University and the Max Planck Centre for Fundamental Heterogeneous Catalysis (FUNCAT) for financial support. M.K., M.D., J.B.E., and F.G. gratefully acknowledge the University of M{\"u}nster and the Deutsche Forschungsgemeinschaft (Leibniz Award, SFB 858) for generous financial support. M.M. acknowledges the MAXNET Energy consortium for funding. J.B.E. acknowledges financial support by the Fonds der Chemischen Industrie. S.J.F. acknowledges the award of a Prize Research Fellowship from the University of Bath. ",

year = "2022",

month = aug,

day = "31",

doi = "10.1021/jacs.2c04828",

language = "English",

volume = "144",

pages = "15431--15436",

journal = "Journal of the American Chemical Society",

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TY - JOUR

T1 - N-Heterocyclic Carbene Modified Palladium Catalysts for the Direct Synthesis of Hydrogen Peroxide

AU - Lewis, Richard J.

AU - Koy, Maximilian

AU - Macino, Margherita

AU - Das, Mowpriya

AU - Carter, James H.

AU - Morgan, David J.

AU - Davies, Thomas E.

AU - Ernst, Johannes B.

AU - Freakley, Simon J.

AU - Glorius, Frank

AU - Hutchings, Graham J.

N1 - Funding Information: R.J.L., J.H.C., D.J.M., T.E.D., and G.J.H. gratefully acknowledge Cardiff University and the Max Planck Centre for Fundamental Heterogeneous Catalysis (FUNCAT) for financial support. M.K., M.D., J.B.E., and F.G. gratefully acknowledge the University of Münster and the Deutsche Forschungsgemeinschaft (Leibniz Award, SFB 858) for generous financial support. M.M. acknowledges the MAXNET Energy consortium for funding. J.B.E. acknowledges financial support by the Fonds der Chemischen Industrie. S.J.F. acknowledges the award of a Prize Research Fellowship from the University of Bath.

PY - 2022/8/31

Y1 - 2022/8/31

N2 - Heterogeneous palladium catalysts modified by N-heterocyclic carbenes (NHCs) are shown to be highly effective toward the direct synthesis of hydrogen peroxide (H2O2), in the absence of the promoters which are typically required to enhance both activity and selectivity. Catalytic evaluation in a batch regime demonstrated that through careful selection of the N-substituent of the NHC it is possible to greatly enhance catalytic performance when compared to the unmodified analogue and reach concentrations of H2O2 rivaling that obtained by state-of-the-art catalysts. The enhanced performance of the modified catalyst, which is retained upon reuse, is attributed to the ability of the NHC to electronically modify Pd speciation.

AB - Heterogeneous palladium catalysts modified by N-heterocyclic carbenes (NHCs) are shown to be highly effective toward the direct synthesis of hydrogen peroxide (H2O2), in the absence of the promoters which are typically required to enhance both activity and selectivity. Catalytic evaluation in a batch regime demonstrated that through careful selection of the N-substituent of the NHC it is possible to greatly enhance catalytic performance when compared to the unmodified analogue and reach concentrations of H2O2 rivaling that obtained by state-of-the-art catalysts. The enhanced performance of the modified catalyst, which is retained upon reuse, is attributed to the ability of the NHC to electronically modify Pd speciation.

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IS - 34

ER -

N-Heterocyclic Carbene Modified Palladium Catalysts for the Direct Synthesis of Hydrogen Peroxide

Abstract

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