SPICE_MARS: A Process Synthesis Framework for Membrane-Assisted Reactive Separations

Abstract

A membrane reactor (MR) combines reaction and separation phenomena in a single unit and offers an energy-efficient, cost-effective, compact, modular, and sustainable design compared to conventional designs. A systematic design framework can yield such benefits of MRs and increase their adoption in the chemical process industry. To this end, we present SPICE_MARS (synthesis and process intensification of chemical enterprises involving membrane-assisted reactive separations), a software prototype for conceptual design, simulation, synthesis, and optimization of MRs for different process applications. At the conceptual level, we can determine whether MR is desired or not and select which species to convert/separate. At the equipment level, we obtain optimal MR configurations considering different flow arrangements, intensification strategies, membrane types, sweep gases, reactor lengths, membrane areas, and catalyst amounts. Additionally, we can generate rank-ordered lists of optimal reactor configurations for different design objectives. These enabling capabilities are demonstrated using two case studies involving methanol synthesis and methane partial oxidation. In both cases, novel MR designsachieving drastic improvement compared to current industrial practiceare found.

Computer‐aided process intensification of natural gas to methanol process

“…Compared to the conventional MeOH reactor, the intensified MeOH_MR operates at a lower pressure. Because of the in situ removal of the product methanol and water, the membrane reactor can produce the same amount of methanol at a lower pressure 48 . The permeate side of the MeOH_MR operates at 1 bar with air as the sweep gas.…”

“…For WGS and MeOH reactor blocks, this upper limit is 1000 and 1504 kg, respectively. The maximum amount of catalyst that each of the POX and the MeOH reactor blocks can accommodate is estimated based on a previous study 48 . The maximum membrane surface area for the POX membrane, the CO 2 membrane, and the MeOH membrane are 94.25, 100, and 163.35 m 2 /block, respectively.…”

“…The maximum amount of catalyst that each of the POX and the MeOH reactor blocks can accommodate is estimated based on a previous study. 48 The maximum membrane surface area for the POX membrane, the CO 2 membrane, and the MeOH membrane are 94.25, 100, and 163.35 m 2 /block, respectively. These maximum membrane surface areas for membranes are estimated based on the reactor geometry.…”

“…Several kinetic models (e.g., Graaf et al, 42 Slotboom et al, 43 Lacerda et al, 44 Bisotti et al, 45 among others) are available for the MeOH reaction. We employ the Bussche and Froment model 46 as it shows good agreement with industrial reactor data 47,48 . The detailed reaction kinetics for all three reactions are presented in the Supporting Information (Section S5).…”

Advancements in Optimization and Control Techniques for Intensifying Processes

“…This approach was applied for several cases, including a reactive distillation process to produce ethylene glycol from ethylene oxide and water [49]. Recent works include the synthesis and intensification for the separation of a ternary mixture consisting of benzene, toluene, and o-xylene [50], the generation of various flowsheets from the block superstructure including the hydrodealkylation of toluene to produce benzene, the generation of products C and D from reactants A and B, and the methanol production from biogas [51], the synthesis of water integration, a heat exchanger network, and simultaneous water and heat integration [52], the integration and intensification for the production of ethylene glycol where heat integration outperforms reactive distillation-based processes [13], the synthesis of separation/reaction distillation intensified processes for the production of ethylene glycol [27], the synthesis of membrane reactors for the production of methanol from syngas and the partial oxidation of methane to generate syngas [53], and the synthesis and intensification of membrane-based processes for the separation of methane from nitrogen, vapor permeation for the separation of methanol/water, and gas permeation for the separation of syngas [54].…”