We demonstrate that applied electric fields at interfaces can control the oxidative addition/reductive elimination equilibria of surface-attached molecular catalysts without any synthetic modification. Density functional theory (DFT) calculations show that the oxidative addition of HCl to a Co complex is "field switchable", being favorable under negative fields but unfavorable under sufficiently positive fields. Extending the analysis to different substrates (O, H) and metal centers (Rh, Ir) reveals consistent trends in the magnitude of the electric field effect: Co > Rh ≈ Ir and HCl > O > H. Our analysis indicates that these field-dependent effects are driven by changes in the permanent dipole moment, offering key insights for the design of field-controllable catalytic systems. This framework presents a novel strategy to overcome the "Goldilocks problem" of balancing competing catalytic steps by leveraging applied electric fields to dynamically tune catalytic reactivity in situ.
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