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The intensification of an electrochemical process by forced periodic operation was studied for the first time using the computer-aided Nonlinear Frequency Response method. This method enabled the automatic generation of frequency response functions and the DC components (Faradaic rectification) of the cost (overpotential) and benefit (current density) indicators. The case study, oxygen reduction reaction, was investigated both experimentally and theoretically. The results of the cost-benefit indicator analysis show that forced periodic change of electrode potential can be superior when compared to the steady-state regime for specific operational parameters. When the electrode rotation rate is changed periodically, the process will always deteriorate as the dynamic operation will inevitably lead to the thickening of the diffusion layer. This phenomenon is explained both from a mathematical and a physical point of view.

The Nonlinear Frequency Response (NFR) method is a useful Process Systems Engineering tool for developing experimental techniques and periodic processes that exploit the system nonlinearity. The basic and most time-consuming step of the NFR method is the derivation of frequency response functions (FRFs). The computer-aided Nonlinear Frequency Response (cNFR) method, presented in this work, uses a software application for automatic derivation of the FRFs, thus making the NFR analysis much simpler, even for systems with complex dynamics. The cNFR application uses an Excel user-friendly interface for defining the model equations and variables, and MATLAB code which performs analytical derivations. As a result, the cNFR application generates MATLAB files containing the derived FRFs in a symbolic and algebraic vector form. In this paper, the software is explained in detail and illustrated through: (1) analysis of periodic operation of an isothermal continuous stirred-tank reactor with a simple reaction mechanism, and (2) experimental identification of electrochemical oxygen reduction reaction.

BACKGROUND Oscillatory baffled reactors have good prospect for use in batch to continuous transition for many industries. For reliable design and scale up it is essential to mathematically describe mixing and flow pattern of oscillatory flow. The aim of this study is to investigate the effects of operating conditions on residence time distribution (RTD) of liquid phase in a continuous oscillatory baffled reactor (COBR) and to propose a correlation that accurately describes the flow pattern. RESULTS Analysis of results obtained for a wide variety of operating conditions in two geometrically similar reactors show that increase of oscillation frequency and amplitude both decrease axial dispersion, with a more prominent effect of amplitude. Proposed power‐law correlation is in very good agreement with all performed experiments. Peclet numbers predicted by this correlation are in reasonably good agreement with the literature experimental data and is much better than the ones obtained by the commonly used correlation, which contains more fitting parameters. CONCLUSION Results show that relatively high amplitudes, low frequencies and low to moderate secondary non‐oscillatory flow should be used to ensure effective mixing with a low net flow in COBR. Developed correlation offers a simple, yet reliable way to predict the macroscopic flow pattern of liquid in COBR. © 2017 Society of Chemical Industry