The Elusive 5′-Deoxyadenosyl Radical: Captured and Characterized by EPR and ENDOR Spectroscopies
Publication
, Journal Article
Yang, H; McDaniel, E; Impano, S; Byer, A; Jodts, R; Yokoyama, K; Broderick, W; Broderick, J; Hoffman, B
June 10, 2019
The 5'-deoxyadenosyl radical (5'-dAdo•) abstracts a substrate H-atom as the first step in radical-based transformations catalyzed by adenosylcobalamin-dependent and radical S-adenosyl-l-methionine (RS) enzymes. Notwithstanding its central biological role, 5'-dAdo• has eluded characterization despite efforts spanning more than a half-century. Here we report generation of 5'-dAdo• in a RS enzyme active site at 12 K, using a novel approach involving cryogenic photoinduced electron transfer from the [4Fe-4S]+cluster to the coordinated S-adenosylmethionine (SAM) to induce homolytic S-C' bond cleavage.
Duke Scholars
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Yang, H., McDaniel, E., Impano, S., Byer, A., Jodts, R., Yokoyama, K., … Hoffman, B. (2019). The Elusive 5′-Deoxyadenosyl Radical: Captured and Characterized by EPR and ENDOR Spectroscopies. https://doi.org/10.26434/chemrxiv.8244596.v1
Yang, Hao, Elizabeth McDaniel, Stella Impano, Amanda Byer, Richard Jodts, Kenichi Yokoyama, William Broderick, Joan Broderick, and Brian Hoffman. “The Elusive 5′-Deoxyadenosyl Radical: Captured and Characterized by EPR and ENDOR Spectroscopies,” June 10, 2019. https://doi.org/10.26434/chemrxiv.8244596.v1.
Yang H, McDaniel E, Impano S, Byer A, Jodts R, Yokoyama K, et al. The Elusive 5′-Deoxyadenosyl Radical: Captured and Characterized by EPR and ENDOR Spectroscopies. 2019 Jun 10;
Yang, Hao, et al. The Elusive 5′-Deoxyadenosyl Radical: Captured and Characterized by EPR and ENDOR Spectroscopies. June 2019. Epmc, doi:10.26434/chemrxiv.8244596.v1.
Yang H, McDaniel E, Impano S, Byer A, Jodts R, Yokoyama K, Broderick W, Broderick J, Hoffman B. The Elusive 5′-Deoxyadenosyl Radical: Captured and Characterized by EPR and ENDOR Spectroscopies. 2019 Jun 10;