Optimized tandem catalyst patterning for CO$_2$ reduction flow reactors

TL;DR

This paper demonstrates a method to optimize the patterning of tandem catalysts in flow reactors for electrochemical CO$_2$ reduction, significantly enhancing high-value product formation through integrated modeling and design optimization.

Contribution

It introduces a combined continuum transport modeling and adjoint-based optimization approach for designing catalyst patterns in CO$_2$ reduction reactors.

Findings

Optimized catalyst patterns increase ethylene current density by up to 65%.

Design optimization is more effective at higher negative voltages.

Minimized low CO concentration zones correlate with improved performance.

Abstract

Tandem catalysis involves two or more catalysts arranged in proximity within a single reaction vessel, with the aim of synergistically aligning the catalysts' reaction pathways to maximize overall system performance. This study presents a proof of concept showing the integration of continuum transport modeling with design optimization in a simplified two-dimensional flow reactor setup for electrochemical CO$_2$ reduction. Ag catalysts provide the CO$_2$ $\rightarrow$ CO reaction capability, and Cu catalysts provide the CO $\rightarrow$ high-value products reaction capability. Given a set of input parameters, the optimization algorithm uses adjoint methods to modify the Ag/Cu surface patterning in order to maximize the current density toward high-value products, such as ethylene. The optimized designs yield significant performance enhancement especially at more negative applied voltages (i.e., stronger surface reactions) and for larger numbers of patterning sections. For an applied voltage of $-1.7$ V vs. SHE, the $12$-section optimized design increases the current density towards ethylene by up to $65$% compared to the unoptimized $2$-section design. For the optimized cases, observed differences in the production and consumption of CO (the key intermediate species) and minimized zones of low CO reactant surface concentration on Cu sections explain the improved reactor performance.