Publisher: American Chemical Society (ACS)

Issue: 11

License:

Publication date(s): 2018/11/05 (print) 2018/10/10 (online)

Pages: 15100-15107

Volume: 6 Issue: 11

Journal: ACS Sustainable Chemistry & Engineering

Link: https://pubs.acs.org/doi/pdf/10.1021/acssuschemeng.8b03568

URL: http://dx.doi.org/10.1021/acssuschemeng.8b03568

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 toward improving the overall activity of an artificial metalloenzyme.