Axiomatic Design for Analysis and Noniterative Engineering of Photoelectrochemical Cells for CO2 Conversion at High Photon to Product Yield

Artificial photosynthesis., vol. 1, pp. 237–250

Abstract

High Resolution Image Download MS PowerPoint Slide An Axiomatic Design (AD) theoretical protocol is proposed for the analysis and noniterative engineering of photoelectrochemical (PEC) cells that can convert CO 2 toward C 2+ products. AD provides criteria for identifying and selecting materials based on data commonly available in the literature. In addition, it establishes a design order for how to achieve optimal integration of materials for catalysis and light-induced charge separation with a proton-transporting membrane in a noniterative manner by matching relevant fluxes with concentration at interfaces across the design. For a hypothetical tandem PEC flow cell reactor for ethylene as an example, the AD protocol predicts an upper bound of 31 μmol h –1 cm –2 at 12% solar-to-product efficiency following PEC process optimization with a design path comprising five steps, starting from data for an O(II)D-Cu CO 2 reduction reaction (CO 2 RR) catalyst and including current concentration to tailor the overpotential. The computational procedure provides models with high yield and robustness by balancing high selectivity with low overpotential and a broad operation range of 0.5–1.2 Sun with a dual absorber with bandgaps of 1.90 and 1.35 eV and a fill factor of 0.85. The procedures are implemented in Python and use a decoupled design matrix that eliminates interdependencies between components.

Authors 3

1. Suzanne Assen Aachen Leiden Institute of Chemistry

   Leiden University

   Affiliation as printed

   Leiden Institute of Chemistry, Leiden University Einsteinweg 55, 2300 RA, Leiden, The Netherlands

2. G. J. A. Sevink Aachen Leiden Institute of Chemistry

   Leiden University

   Affiliation as printed

   Leiden Institute of Chemistry, Leiden University Einsteinweg 55, 2300 RA, Leiden, The Netherlands

3. Huub J. M. de Groot corresponding Aachen Leiden Institute of Chemistry

   Leiden University

   Affiliation as printed

   Leiden Institute of Chemistry, Leiden University Einsteinweg 55, 2300 RA, Leiden, The Netherlands