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87 mA·cm -2 and turnover frequency of 1,962 h -1 at a mild overpotential of 620 mV for CO formation with 97% Faradic efficiency. © 2020 WILEY-VCH Verlag GmbH Co. KGaA, Weinheim.The understanding of biomolecular function is coupled to knowledge about the structure and dynamics of these biomolecules, preferably acquired under native conditions. In this regard, pulsed dipolar EPR spectroscopy (PDS) in conjunction with site-directed spin labeling (SDSL) is an important method in the toolbox of biophysical chemistry. However, the curren