Artificial Metalloenzymes as Catalysts for Oxidative Lignin Degradation

Megan V. Doble; Amanda G. Jarvis; Andrew C. C. Ward; Jonathan D. Colburn; Jan P. Götze; Michael Bühl; Paul C. J. Kamer

doi:10.1021/acssuschemeng.8b03568

Artificial Metalloenzymes as Catalysts for Oxidative Lignin Degradation

Megan V. Doble, Amanda G. Jarvis, Andrew C. C. Ward, Jonathan D. Colburn, Jan P. Götze, Michael Bühl, Paul C. J. Kamer

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

Abstract / Description of output

We report novel artificial metalloenzymes (ArMs), containing tris(pyridylmethyl)amine (TPA), for the atom economic oxidation of lignin β-O-4 model compounds, using hydrogen peroxide. The protein scaffold alters the selectivity of the reaction from a low yielding cleavage reaction when using the parent Fe-tpa complex to a high yielding benzylic alcohol oxidation when using the complex incorporated into a protein scaffold, SCP-2L A100C. Engineering the protein scaffold to incorporate glutamic acid was found to improve the ArM activity, showing that rational design of the protein environment using metal binding amino acids can be a first step towards improving the overall activity of an artificial metalloenzyme.

Original language	English
Journal	ACS Sustainable Chemistry & Engineering
Early online date	10 Oct 2018
DOIs	https://doi.org/10.1021/acssuschemeng.8b03568
Publication status	E-pub ahead of print - 10 Oct 2018

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10.1021/acssuschemeng.8b03568

20182910 Jarvis ACS Sus Chem 2018Accepted author manuscript, 477 KBLicence: Creative Commons: Attribution Non-Commercial (CC-BY-NC)

http://pubs.acs.org/doi/10.1021/acssuschemeng.8b03568

EASTBIO: EASTBIO East of Scotland BioScience Doctoral Training Partnership studentship - Research Training Grant BB/J01446X/1
Smith, S.
1/09/12 → 30/09/18
Project: Other (Non-Funded/Miscellaneous)

Cite this

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title = "Artificial Metalloenzymes as Catalysts for Oxidative Lignin Degradation",

abstract = "We report novel artificial metalloenzymes (ArMs), containing tris(pyridylmethyl)amine (TPA), for the atom economic oxidation of lignin β-O-4 model compounds, using hydrogen peroxide. The protein scaffold alters the selectivity of the reaction from a low yielding cleavage reaction when using the parent Fe-tpa complex to a high yielding benzylic alcohol oxidation when using the complex incorporated into a protein scaffold, SCP-2L A100C. Engineering the protein scaffold to incorporate glutamic acid was found to improve the ArM activity, showing that rational design of the protein environment using metal binding amino acids can be a first step towards improving the overall activity of an artificial metalloenzyme. ",

author = "Doble, {Megan V.} and Jarvis, {Amanda G.} and Ward, {Andrew C. C.} and Colburn, {Jonathan D.} and G{\"o}tze, {Jan P.} and Michael B{\"u}hl and Kamer, {Paul C. J.}",

year = "2018",

month = oct,

day = "10",

doi = "10.1021/acssuschemeng.8b03568",

language = "English",

journal = "ACS Sustainable Chemistry & Engineering",

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AU - Doble, Megan V.

AU - Jarvis, Amanda G.

AU - Ward, Andrew C. C.

AU - Colburn, Jonathan D.

AU - Götze, Jan P.

AU - Bühl, Michael

AU - Kamer, Paul C. J.

PY - 2018/10/10

Y1 - 2018/10/10

N2 - We report novel artificial metalloenzymes (ArMs), containing tris(pyridylmethyl)amine (TPA), for the atom economic oxidation of lignin β-O-4 model compounds, using hydrogen peroxide. The protein scaffold alters the selectivity of the reaction from a low yielding cleavage reaction when using the parent Fe-tpa complex to a high yielding benzylic alcohol oxidation when using the complex incorporated into a protein scaffold, SCP-2L A100C. Engineering the protein scaffold to incorporate glutamic acid was found to improve the ArM activity, showing that rational design of the protein environment using metal binding amino acids can be a first step towards improving the overall activity of an artificial metalloenzyme.

AB - We report novel artificial metalloenzymes (ArMs), containing tris(pyridylmethyl)amine (TPA), for the atom economic oxidation of lignin β-O-4 model compounds, using hydrogen peroxide. The protein scaffold alters the selectivity of the reaction from a low yielding cleavage reaction when using the parent Fe-tpa complex to a high yielding benzylic alcohol oxidation when using the complex incorporated into a protein scaffold, SCP-2L A100C. Engineering the protein scaffold to incorporate glutamic acid was found to improve the ArM activity, showing that rational design of the protein environment using metal binding amino acids can be a first step towards improving the overall activity of an artificial metalloenzyme.

U2 - 10.1021/acssuschemeng.8b03568

DO - 10.1021/acssuschemeng.8b03568

M3 - Article

SN - 2168-0485

JO - ACS Sustainable Chemistry & Engineering

JF - ACS Sustainable Chemistry & Engineering

ER -

Artificial Metalloenzymes as Catalysts for Oxidative Lignin Degradation

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Projects

EASTBIO: EASTBIO East of Scotland BioScience Doctoral Training Partnership studentship - Research Training Grant BB/J01446X/1

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