Modeling and Simulation of the Spatial and Light-Intensity Dependence of Product Distributions in an Integrated Photoelectrochemical CO2 Reduction System

A multiphysics model that accounts for the performance of electrocatalysts and triple-junction light absorbers, as well as for the transport properties of the electrolyte and dissolved CO 2, was used to evaluate the spatial and light-intensity dependence of product distributions in an integrated photoelectrochemical CO 2 reduction (CO 2 R) cell. Different sets of band gap combinations of triple-junction light absorbers were required to accommodate the optimal total operating current density relative to the optimal partial current density for CO 2 R. The simulated product distribution was highly nonuniform along the width of the electrode and depended on the electrode dimensions as well as the illumination intensity. To achieve the same product selectivity as in a potentiostatic, “half-cell” configuration, the electrocatalyst must retain its selectivity over a range of cathode potentials, and this range is dependent on the transport losses and current–voltage relationship of the light absorbers, the geometric parameters of the cell, and the illumination intensity.