title: Significant improvement of oxidase activity through the genetic incorporation of a redox-active unnatural amino acid.
abstract: While nature employs various covalent and non-covalent strategies to modulate tyrosine (Y) redox potential and pKain order to optimize enzyme activities, such approaches have not been systematically applied for the design of functional metalloproteins. Through the genetic incorporation of 3-methoxytyrosine (OMeY) into myoglobin, we replicated important features of cytochrome c oxidase (CcO) in this small soluble protein, which exhibits selective O2reduction activity while generating a small amount of reactive oxygen species (ROS). These results demonstrate that the electron donating ability of a tyrosine residue in the active site is important for CcO function. Moreover, we elucidated the structural basis for the genetic incorporation of OMeY into proteins by solving the X-ray structure of OMeY specific aminoacyl-tRNA synthetase complexed with OMeY.
authors.affiliation: Center of Biophysics and Computational Biology and Department of Chemistry , University of Illinois at Urbana-Champaign , Urbana , Illinois 61801 , USA . Email: yi-lu@illinois.edu.
authors.forename: Yang
authors.initials: Y
authors.lastname: Yu
authors.affiliation: Laboratory of RNA Biology , Institute of Biophysics , Chinese Academy of Sciences , 15 Datun Road, Chaoyang District , Beijing , 100101 , China . Email: jwang@ibp.ac.cn.
authors.forename: Qing
authors.initials: Q
authors.lastname: Zhou
authors.affiliation: School of Life Sciences , University of Science and Technology of China , Hefei , Anhui 230026 , China.|Laboratory of RNA Biology , Institute of Biophysics , Chinese Academy of Sciences , 15 Datun Road, Chaoyang District , Beijing , 100101 , China . Email: jwang@ibp.ac.cn.
authors.forename: Li
authors.initials: L
authors.lastname: Wang
authors.affiliation: Laboratory of RNA Biology , Institute of Biophysics , Chinese Academy of Sciences , 15 Datun Road, Chaoyang District , Beijing , 100101 , China . Email: jwang@ibp.ac.cn.
authors.forename: Xiaohong
authors.initials: X
authors.lastname: Liu
authors.affiliation: Laboratory of RNA Biology , Institute of Biophysics , Chinese Academy of Sciences , 15 Datun Road, Chaoyang District , Beijing , 100101 , China . Email: jwang@ibp.ac.cn.
authors.forename: Wei
authors.initials: W
authors.lastname: Zhang
authors.affiliation: Laboratory of RNA Biology , Institute of Biophysics , Chinese Academy of Sciences , 15 Datun Road, Chaoyang District , Beijing , 100101 , China . Email: jwang@ibp.ac.cn.
authors.forename: Meirong
authors.initials: M
authors.lastname: Hu
authors.affiliation: Laboratory of RNA Biology , Institute of Biophysics , Chinese Academy of Sciences , 15 Datun Road, Chaoyang District , Beijing , 100101 , China . Email: jwang@ibp.ac.cn.
authors.forename: Jianshu
authors.initials: J
authors.lastname: Dong
authors.affiliation: School of Life Sciences , University of Science and Technology of China , Hefei , Anhui 230026 , China.|Laboratory of RNA Biology , Institute of Biophysics , Chinese Academy of Sciences , 15 Datun Road, Chaoyang District , Beijing , 100101 , China . Email: jwang@ibp.ac.cn.
authors.forename: Jiasong
authors.initials: J
authors.lastname: Li
authors.affiliation: Laboratory of RNA Biology , Institute of Biophysics , Chinese Academy of Sciences , 15 Datun Road, Chaoyang District , Beijing , 100101 , China . Email: jwang@ibp.ac.cn.
authors.forename: Xiaoxuan
authors.initials: X
authors.lastname: Lv
authors.affiliation: Center of Biophysics and Computational Biology and Department of Chemistry , University of Illinois at Urbana-Champaign , Urbana , Illinois 61801 , USA . Email: yi-lu@illinois.edu.
authors.forename: Hanlin
authors.initials: H
authors.lastname: Ouyang
authors.affiliation: Laboratory of RNA Biology , Institute of Biophysics , Chinese Academy of Sciences , 15 Datun Road, Chaoyang District , Beijing , 100101 , China . Email: jwang@ibp.ac.cn.
authors.forename: Han
authors.initials: H
authors.lastname: Li
authors.affiliation: Laboratory of RNA Biology , Institute of Biophysics , Chinese Academy of Sciences , 15 Datun Road, Chaoyang District , Beijing , 100101 , China . Email: jwang@ibp.ac.cn.
authors.forename: Feng
authors.initials: F
authors.lastname: Gao
authors.affiliation: Laboratory of RNA Biology , Institute of Biophysics , Chinese Academy of Sciences , 15 Datun Road, Chaoyang District , Beijing , 100101 , China . Email: jwang@ibp.ac.cn.
authors.forename: Weimin
authors.initials: W
authors.lastname: Gong
authors.affiliation: Center of Biophysics and Computational Biology and Department of Chemistry , University of Illinois at Urbana-Champaign , Urbana , Illinois 61801 , USA . Email: yi-lu@illinois.edu.
authors.forename: Yi
authors.initials: Y
authors.lastname: Lu
authors.affiliation: Laboratory of RNA Biology , Institute of Biophysics , Chinese Academy of Sciences , 15 Datun Road, Chaoyang District , Beijing , 100101 , China . Email: jwang@ibp.ac.cn.
authors.forename: Jiangyun
authors.initials: J
authors.lastname: Wang