Structure- and Data-Driven Protein Engineering of Transaminases for Improving Activity and Stereoselectivity

被引:24
作者
Ao, Yu-Fei [1 ,2 ,3 ]
Pei, Shuxin [4 ]
Xiang, Chao [1 ]
Menke, Marian J. [1 ]
Shen, Lin [4 ,6 ]
Sun, Chenghai [1 ]
Dorr, Mark [1 ]
Born, Stefan [5 ]
Hohne, Matthias [1 ,7 ]
Bornscheuer, Uwe T. [1 ]
机构
[1] Univ Greifswald, Inst Biochem, Dept Biotechnol & Enzyme Catalysis, Felix Hausdorff Str 4, D-17487 Greifswald, Germany
[2] Chinese Acad Sci, Inst Chem, Beijing Natl Lab Mol Sci, CAS Key Lab Mol Recognit & Funct, Zhongguancun North First St 2, Beijing 100190, Peoples R China
[3] Univ Chinese Acad Sci, Yuquan Rd 19A, Beijing 100049, Peoples R China
[4] Beijing Normal Univ, Coll Chem, Key Lab Theoret & Computat Photochem, Minist Educ, Xinjiekouwai St 19, Beijing 100875, Peoples R China
[5] Tech Univ Berlin, Chair Bioproc Engn, Ackerstr 76, D-13355 Berlin, Germany
[6] Yantai Jingshi Inst Mat Genome Engn, Nanchang Rd 48, Yantai 265505, Shandong, Peoples R China
[7] Tech Univ Berlin, Dept Chem Biocatalysis, Muller Breslau Str 10, D-10623 Berlin, Germany
基金
中国国家自然科学基金;
关键词
Biocatalysis; Catalytic Activity; Machine Learning; Stereoselectivity; Transaminases; AMINE TRANSAMINASE; DIRECTED EVOLUTION; ASYMMETRIC-SYNTHESIS; PREDICTION;
D O I
10.1002/anie.202301660
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Amine transaminases (ATAs) are powerful biocatalysts for the stereoselective synthesis of chiral amines. Machine learning provides a promising approach for protein engineering, but activity prediction models for ATAs remain elusive due to the difficulty of obtaining high-quality training data. Thus, we first created variants of the ATA from Ruegeria sp. (3FCR) with improved catalytic activity (up to 2000-fold) as well as reversed stereoselectivity by a structure-dependent rational design and collected a high-quality dataset in this process. Subsequently, we designed a modified one-hot code to describe steric and electronic effects of substrates and residues within ATAs. Finally, we built a gradient boosting regression tree predictor for catalytic activity and stereoselectivity, and applied this for the data-driven design of optimized variants which then showed improved activity (up to 3-fold compared to the best variants previously identified). We also demonstrated that the model can predict the catalytic activity for ATA variants of another origin by retraining with a small set of additional data.
引用
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页数:9
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