Optimal permeance ratio, flux direction and layer distribution in composite asymmetric membranes composed of sequences of layers obeying real-power flux laws

Abstract

In this study, the optimal permeance ratio and layers distribution in multilayer membranes and thin films in which each layer obeys the following real-power law: Flux=πi(P1,ini−P2,ini) are determined for any positive real values of ni. Such an exponent has a physical meaning in several cases, such as: diffusion-controlled permeation of hydrogen in metal membranes i) under infinite-dilution conditions (n = 0.5), and ii) under higher-concentration ones (0.5 < n < 1.5), iii) desorption-limited permeation (n = 1) in the same type of membranes, Knudsen-type diffusional mechanism (n = 1) and viscous flow (n = 2) in microporous membranes. Furthermore, n is equal to 4 in radiation-driven thermal flux. The work considers two generic layers of different thicknesses and exponents, for which it is proven the existence of a general optimal permeance ratio π1/π2 maximising the flux ratio, which is found to be equal to the inverse of the ratio between the respective maximum theoretical driving forces that can be established in each layer. Such an optimal permeance ratio is also proven to be a global optimum. Afterwards, we provide a theoretical generalisation of this optimality to whatever types of driving forces. Then, we provide a demonstration that the highest species permeating flux is always established when feeding it from the layer side with the highest exponent independently of the permeance ratio. As an important consequence, to maximise flux, a multilayer membrane/thin film should be fabricated by depositing the layers in cascade according to the ascending or descending exponents, and should be used in a configuration in which the flux flows from the layer with the highest pressure exponent to the layer with the lowest one. It is also shown that there exists an optimal value of the lower exponent n1 that maximizes the flux ratio keeping constant the other parameters. Finally, we showed that a virial-type linear combination of polynomial driving forces can be approximated by the empirical flux law investigated. Overall, our results are valid not only for whatever type of composite membranes and thin films (metallic, ceramic, polymeric and hybrid ones), but also for any sequential system involving a flux of whatever physical entity obeying the aforementioned law, such as heat transfer in the presence of radiation, non-linear electrical resistances and possible others.