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9.1.3.3 Quasirreversible and Irreversible Multistep Processes If a multistep process is neither Nerstian nor at equilibrium, the details of the kinetics influence its behavior in electrochemical experiments, and one can use the results to diagnose the mechanism and to quantify kinetic parameters. As in the study of homogeneous kinetics, one proceeds by devising a hypothesis about the mechanism, predicting experimental behavior on the basis of the hypothesis, and comparing the predictions against the results. In the electrochemical sphere, an important part of predicting behavior is developing the current-potential characteristic in terms of controllable parameters, such as the concentrations of participating species. If the RDS is a heterogeneous electron-transfer step, then the current-potential characteristic has the form of (9.38). For most mechanisms, this equation is of limited direct utility, because O’ and R’ are intermediates, whose concentration cannot be controlled directly. Still, (9.38) can serve as the basis for a more practical current-potential relationship, because one can use the presumed mechanism to re-express CO’(0,t) and CR’(0,t) in terms of the concentrations of more controllable species, such as O and R. Unfortunately, the results can easily become too complex for practical application. For example, consider the simple mechanism in (9.35)-(9.37), where the pre- and postreactions are assumed to be kinetically facile enough to remain in local equilibrium. The overall Nerstian relationships connect the surface concentrations of O and R to those of O’ and R’. Thus, the current-potential characteristic, (9.38), can be expressed in terms of the surface concentrations of the initial reactant, O, and the final product, R. This relationship can be rewritten as where (9.45) (9.46) (9.47) (9.48) 227PDF Image | Redox Flow Batteries Vanadium to Earth Quinones
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