Detail publikace

Catalytic mechanism for Renilla-type luciferases

Schenkmayerova, A. Toul, M. Pluskal, D. Baatallah, R. Gagnot, G. Pinto, GP. Santana, VT. Stuchla, M. Neugebauer, P. Chaiyen, P. Damborsky, J. Bednar, D. Janin, YL. Prokop, Z. Marek, M.

Originální název

Catalytic mechanism for Renilla-type luciferases

Typ

článek v časopise ve Web of Science, Jimp

Jazyk

angličtina

Originální abstrakt

The widely used coelenterazine-powered Renilla luciferase was discovered over 40 years ago, but the oxidative mechanism by which it generates blue photons remains unclear. Here we decipher Renilla-type catalysis through crystallographic, spectroscopic and computational experiments. Structures of ancestral and extant luciferases complexed with the substrate-like analogue azacoelenterazine or a reaction product were obtained, providing molecular snapshots of coelenterazine-to-coelenteramide oxidation. Bound coelenterazine adopts a Y-shaped conformation, enabling the deprotonated imidazopyrazinone component to attack O-2 via a radical charge-transfer mechanism. A high emission intensity is secured by an aspartate from a conserved proton-relay system, which protonates the excited coelenteramide product. Another aspartate on the rim of the catalytic pocket fine-tunes the electronic state of coelenteramide and promotes the formation of the blue light-emitting phenolate anion. The results obtained also reveal structural features distinguishing flash-type from glow-type bioluminescence, providing insights that will guide the engineering of next-generation luciferase-luciferin pairs for ultrasensitive optical bioassays.

Klíčová slova

CYPRIDINA LUCIFERIN; PROTEIN CRYSTALLIZATION; BIOLUMINESCENCE; RENIFORMIS; LIGHT; CHEMILUMINESCENCE; COELENTERAZINE; STABILITY; LUMINESCENCE; SPECIFICITY

Autoři

Schenkmayerova, A.; Toul, M.; Pluskal, D.; Baatallah, R.; Gagnot, G.; Pinto, GP.; Santana, VT.; Stuchla, M.; Neugebauer, P.; Chaiyen, P.; Damborsky, J.; Bednar, D.; Janin, YL.; Prokop, Z.; Marek, M.

Vydáno

1. 1. 2023

Nakladatel

NATURE PORTFOLIO

Místo

BERLIN

ISSN

2520-1158

Periodikum

Nature Catalysis

Ročník

6

Číslo

1

Stát

Spojené království Velké Británie a Severního Irska

Strany od

23

Strany do

38

Strany počet

16

URL

https://www.nature.com/articles/s41929-022-00895-z

BibTex

@article{BUT183685,
  author="Schenkmayerova, A. and Toul, M. and Pluskal, D. and Baatallah, R. and Gagnot, G. and Pinto, GP. and Santana, VT. and Stuchla, M. and Neugebauer, P. and Chaiyen, P. and Damborsky, J. and Bednar, D. and Janin, YL. and Prokop, Z. and Marek, M.",
  title="Catalytic mechanism for Renilla-type luciferases",
  journal="Nature Catalysis",
  year="2023",
  volume="6",
  number="1",
  pages="23--38",
  doi="10.1038/s41929-022-00895-z",
  issn="2520-1158",
  url="https://www.nature.com/articles/s41929-022-00895-z"
}