The E. coli class Ia ribonucleotide reductase (RNR) achieves forward and reverse proton-coupled electron transfer (PCET) over a pathway of redox-active amino acids (β-Y122 ⇌ β-Y356 ⇌ α-Y731 ⇌ α-Y730 ⇌ α-C439) spanning ~35 Å and two subunits every time it turns over. We have developed photoRNRs that allow radical transport to be phototriggered at tyrosine (Y) or fluorotyrosine (FnY) residues along the PCET pathway. We now report a new photoRNR in which photooxidation of a tryptophan (W) residue replacing Y356 within the α/β subunit interface proceeds by a stepwise ETPT (electron transfer then proton transfer) mechanism and provides an orthogonal spectroscopic handle with respect to radical pathway residues Y731/Y730 in α. This construct displays a ~3-fold enhancement in photochemical yield of W• relative to F3Y• and a ~7-fold enhancement relative to Y•. Photogeneration of the W• radical occurs with a rate constant of 4.4 ± 0.2 × 105 s−1, which obeys a Marcus correlation for radical generation at the RNR subunit interface. Despite the fact that the Y → W variant displays no enzymatic activity in the absence of light, photogeneration of W• within the subunit interface results in 20% activity for turnover relative to wt-RNR under the same conditions.
Although reproductive injustices and reproductive health disparities are well-documented in the United States, recent studies have begun to explore the health care professional's role in their perpetuation. We hypothesized that obstetrics and gynecology residents would observe reproductive injustices during their training. Thus, using a national survey, we asked obstetrics and gynecology residents to share clinical cases in which discrimination, bias, inequity, or injustice was involved in a patient's reproductive health care and queried their preparedness to respond. Through qualitative analysis, we found that respondents shared cases involving racism, discrimination, and structural barriers to care and that they felt poorly equipped to handle injustice. We call for clinician educators to combat reproductive injustice through three key changes to obstetrics and gynecology residency training: 1) incorporate reproductive justice training into formal residency education; 2) create safe spaces for residents to collectively debrief about their experiences with injustice and collaborate on care improvement; and 3) teach community engagement and advocacy skills that identify, center, and elevate local reproductive health priorities.
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