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- Title
Modifying the Steric Properties in the Second Coordination Sphere of Designed Peptides Leads to Enhancement of Nitrite Reductase Activity.
- Authors
Koebke, Karl J.; Yu, Fangting; Salerno, Elvin; Van Stappen, Casey; Tebo, Alison G.; Penner‐Hahn, James E.; Pecoraro, Vincent L.
- Abstract
Abstract: Protein design is a useful strategy to interrogate the protein structure‐function relationship. We demonstrate using a highly modular 3‐stranded coiled coil (TRI‐peptide system) that a functional type 2 copper center exhibiting copper nitrite reductase (NiR) activity exhibits the highest homogeneous catalytic efficiency under aqueous conditions for the reduction of nitrite to NO and H2O. Modification of the amino acids in the second coordination sphere of the copper center increases the nitrite reductase activity up to 75‐fold compared to previously reported systems. We find also that steric bulk can be used to enforce a three‐coordinate CuI in a site, which tends toward two‐coordination with decreased steric bulk. This study demonstrates the importance of the second coordination sphere environment both for controlling metal‐center ligation and enhancing the catalytic efficiency of metalloenzymes and their analogues.
- Subjects
NITRITE reductase; NITROREDUCTASES; PROTEIN engineering; MASS spectrometry; X-ray diffraction
- Publication
Angewandte Chemie, 2018, Vol 130, Issue 15, p4018
- ISSN
0044-8249
- Publication type
Article
- DOI
10.1002/ange.201712757