The performance of an adsorption-based separation process is dictated by the choices of the solid sorbent and the process configuration. Often screening of materials and process configuration is performed using digital twins that mimic a real adsorption process. In typical studies, either several materials are screened for a specific process configuration to find the best candidate or the performance of several process configurations is evaluated for a specific material. However, it has long been suggested that to truly maximize the potential of a given material, it should be "married" to processes. In this work, we address the "marriage" of materials and processes through three dedicated goals. First, to develop a modeling framework for an all-encompassing pressure swing adsorption cycle composed of several process configurations. Second, to develop an optimization framework, drawing inspiration from superstructures, to select the optimal process configuration from the all-encompassing cycle to reach a given process target. Third, to highlight the importance and relevance of such an approach that enables each material to truly maximize its potential, by varying both the process configuration and the corresponding operating conditions. To address these goals, we have developed a computational framework composed of a process model and a process optimizer. Subsequently, using this computational framework, we have evaluated the performance of several real and hypothetical materials. Our computational studies led to two key outcomes, namely, (1) to employ an integrated material-process optimization approach to maximize the true potential of any material when screening for a given application and when evaluating the performance under different feed conditions; and (2) not to generalize the observations regarding the best process configuration from one material to every other material.

The performance of an adsorption-based separation process is dictated by the choices of the adsorbent and the process configuration. In typical studies, either several materials are screened for a specific process configuration to find the best candidate, or the performance of several process configurations is evaluated for a specific material. However, it has long been suggested that to truly maximize the potential of a given material, it should be “married” to processes. Here, we have developed a modeling framework for a hybrid adsorption cycle composed of several process configurations and a unified optimization approach to select the optimal material-process combination. We have shown through several case studies that (1) one needs to employ an integrated optimization approach to maximize the potential of any material when screening for a given application; (2) one should not generalize the observations regarding the best process configuration from one material to every other material.