A Reaction-Advection-Diffusion Model to describe Non-Uniformities in Colorimetric Sensing using Thin Porous Substrates

TL;DR

This paper develops a reaction-advection-diffusion model to understand and predict non-uniform color patterns in paper-based sensors, revealing mechanisms behind ring formations and guiding sensor design improvements.

Contribution

It introduces a novel two-stage model capturing mass transport and reaction dynamics in porous substrates, explaining pattern formation without evaporation effects and validating with experimental data.

Findings

Ring-like patterns can form without evaporation.

Decreasing analyte-reagent ratio shifts color inward.

Thicker substrates improve uniformity but reduce intensity.

Abstract

Non-uniform product (color) distribution in colorimetric paper-based sensors affects the accuracy and reliability of measurements. The underlying mechanisms responsible for this are still unclear. The coffee ring effect explains the ring-formation at the periphery. However, ring-like patterns can also be found at intermediate radial positions in these sensors. In this work, we study the influence of mass transport and reaction dynamics within porous/paper substrates on the spatial product distribution. We consider one reactant embedded in a porous substrate, which reacts with another delivered through a sessile droplet. The process is modeled in two stages. In Stage 1, droplet imbibition creates two distinct flow domains in the substrate with moving boundaries. Stage 2 commences after complete penetration. Species-substrate interactions are addressed by including a mobility factor. The developed model is used to analyze the effects of different parameters on the product distribution for two configurations, Reagent-Embedded (RE) and Analyte-Embedded (AE). Our work demonstrates ring-like patterns can form even without evaporation effects. With decreasing analyte-reagent concentration ratio, the profile shifts inward. Thicker, more porous substrates yield greater uniformity but reduce color intensity. Immobilization of embedded species enhances uniformity in RE configuration with mobile product, and in AE configuration with immobile product. The model is validated with lead and nitrite detection experiments for RE and AE configurations respectively. It successfully captures three spatial color variations observed experimentally. This study also explains the emergence of multiple rings in these systems. The insights gained are useful for optimizing sensor design and protocols for colorimetry