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Non-injective gas sensor arrays: identifying undetectable composition changes.

Metal-organic frameworks (MOFs) are nanoporous materials with good prospects as recognition elements for gas sensors owing to their adsorptive sensitivity and selectivity. A gravimetric, MOF-based sensor functions by measuring the mass of gas adsorbed in a MOF. Changes in the gas composition are expected to produce detectable changes in the mass of gas adsorbed in the MOF. In practical settings, multiple components of the gas adsorb into the MOF and contribute to the sensor response. As a result, there are typically many distinct gas compositions that produce the same single-sensor response. The response vector of a gas sensor array places more constraints on the gas composition. Still, if the number of degrees of freedom in the gas composition is greater than the number of MOFs in the sensor array, the map from gas compositions to response vectors will be non-injective (many-to-one). Here, we outline a mathematical method to determine undetectable changes in gas composition to which non-injective gas sensor arrays are unresponsive. This is important for understanding their limitations and vulnerabilities. We focus on gravimetric, MOF-based gas sensor arrays. Our method relies on a mixed-gas adsorption model in the MOFs comprising the sensor array, which gives the mass of gas adsorbed in each MOF as a function of the gas composition. The singular value decomposition of the Jacobian matrix of the adsorption model uncovers (i) the unresponsive directions and (ii) the responsive directions, ranked by sensitivity, in gas composition space. We illustrate the identification of unresponsive subspaces and ranked responsive directions for gas sensor arrays based on Co-MOF-74 and HKUST-1 aimed at quantitative sensing of CH4/N2/CO2/C2H6mixtures relevant to natural gas sensing.