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Serial crystallography captures dynamic control of sequential electron and proton transfer events in a flavoenzyme.

Maestre-Reyna M, Yang CH, Nango E, Huang WC, Ngurah Putu EPG, Wu WJ, Wang PH, Franz-Badur S, Saft M, Emmerich HJ, Wu HY, Lee CC, Huang KF, Chang YK, Liao JH, Weng JH, Gad W, Chang CW, Pang AH, Sugahara M, Owada S, Hosokawa Y, Joti Y, Yamashita A, Tanaka R, Tanaka T, Luo F, Tono K, Hsu KC, Kiontke S, Schapiro I, Spadaccini R, Royant A, Yamamoto J, Iwata S, Essen LO, Bessho Y, Tsai MD
Nat Chem 14 677-685 (2022)
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Cited: 5 times
EuropePMC logo PMID: 35393554

Abstract

Flavin coenzymes are universally found in biological redox reactions. DNA photolyases, with their flavin chromophore (FAD), utilize blue light for DNA repair and photoreduction. The latter process involves two single-electron transfers to FAD with an intermittent protonation step to prime the enzyme active for DNA repair. Here we use time-resolved serial femtosecond X-ray crystallography to describe how light-driven electron transfers trigger subsequent nanosecond-to-microsecond entanglement between FAD and its Asn/Arg-Asp redox sensor triad. We found that this key feature within the photolyase-cryptochrome family regulates FAD re-hybridization and protonation. After first electron transfer, the FAD•- isoalloxazine ring twists strongly when the arginine closes in to stabilize the negative charge. Subsequent breakage of the arginine-aspartate salt bridge allows proton transfer from arginine to FAD•-. Our molecular videos demonstrate how the protein environment of redox cofactors organizes multiple electron/proton transfer events in an ordered fashion, which could be applicable to other redox systems such as photosynthesis.

Articles citing this publication (5)

  1. Time-resolved serial femtosecond crystallography on fatty-acid photodecarboxylase: lessons learned. Hadjidemetriou K, Coquelle N, Barends TRM, De Zitter E, Schlichting I, Colletier JP, Weik M. Acta Crystallogr D Struct Biol 78 1131-1142 (2022)
  2. Understanding Cysteine Chemistry Using Conventional and Serial X-Ray Protein Crystallography. Smith N, Wilson MA. Crystals (Basel) 12 1671 (2022)
  3. A deazariboflavin chromophore kinetically stabilizes reduced FAD state in a bifunctional cryptochrome. Hosokawa Y, Morita H, Nakamura M, Yamamoto J. Sci Rep 13 16682 (2023)
  4. Mimicking reductive dehalogenases for efficient electrocatalytic water dechlorination. Min Y, Mei SC, Pan XQ, Chen JJ, Yu HQ, Xiong Y. Nat Commun 14 5134 (2023)
  5. Remote stereocontrol with azaarenes via enzymatic hydrogen atom transfer. Li M, Harrison W, Zhang Z, Yuan Y, Zhao H. Nat Chem (2023)


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