Artificial Metalloenzymes as Catalysts for Oxidative Lignin Degradation

被引：20

作者：

Doble, Megan V. ^{[1
]}

Jarvis, Amanda G. ^{[1
,2
]}

Ward, Andrew C. C. ^{[1
]}

Colburn, Jonathan D. ^{[1
]}

Gotze, Jan P. ^{[1
]}

Buhl, Michael ^{[1
]}

Kamer, Paul C. J. ^{[1
,3
]}

机构：

[1] Univ St Andrews, Sch Chem, St Andrews KY16 9ST, Fife, Scotland

[2] Univ Edinburgh, Sch Chem, Joseph Black Bldg,David Brewster Rd,Kings Bldg, Edinburgh EH9 3FJ, Midlothian, Scotland

[3] Leibniz Inst Catalysis, Bioinspired Homo & Heterogeneous Catalysis, Albert Einstein Str 29a, D-18059 Rostock, Germany

来源：

ACS SUSTAINABLE CHEMISTRY & ENGINEERING | 2018年 / 6卷 / 11期

基金：

欧盟地平线“2020”; 英国工程与自然科学研究理事会; 英国生物技术与生命科学研究理事会;

关键词：

Lignin; Artificial metalloenzymes; Catalytic oxidation; O BOND-CLEAVAGE; ALCOHOL OXIDATION; HIGHLY EFFICIENT; ENZYME; IDENTIFICATION; VALORIZATION; DYNAMICS; MOLECULE; BIOMASS; DESIGN;

D O I：

10.1021/acssuschemeng.8b03568

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

We report novel artificial metalloenzymes (ArMs), containing tris(pyridylmethyl)amine (TPA), for the atom economic oxidation of lignin beta-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.

引用

页码：15100 / 15107

页数：15

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