Artificial Metalloenzymes as Catalysts for Oxidative Lignin Degradation
Artificial Metalloenzymes as Catalysts for Oxidative Lignin Degradation
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DOI：
10.1021/acssuschemeng.8b03568
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发表时间：
2018-11-05
影响因子：
8.4
通讯作者：
Kamer, Paul C. J.
中科院分区：
文献类型：
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作者：
Doble, Megan V.;Jarvis, Amanda G.;Kamer, Paul C. J.
我们报道了一种新型的人工金属酶(ARMS)，它含有三(吡啶甲基)胺(TPA)，用于木质素β-O-4模型化合物的过氧化氢原子经济氧化。该蛋白质支架将反应的选择性从使用母体Fe-TPA络合物时的低产率切割反应改变为当使用该络合物并入蛋白支架SCP-2L A100C时的高产率的苯甲醇氧化反应。研究发现，将谷氨酸引入蛋白质支架可以提高手臂的活性，这表明使用金属结合氨基酸合理设计蛋白质环境可以是提高人工金属酶整体活性的第一步。
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.