Thermodynamic limits of countercurrent reactor systems, with examples in membrane reactors and the ceria redox cycle
Literature Information
Countercurrent reactors can be utilized in chemical reaction systems which involve either a reaction between flows of different phases, or reactions between flows separated by a selective permeable membrane. This idea is quite similar in nature to a countercurrent heat exchanger, where the inlet of one participating flow is exposed to the outlet of the opposite flow. A countercurrent configuration can therefore improve the reaction conversion extent and transport properties. Here we formulate a straightforward approach in terms of an exchange coordinate, in order to determine an upper bound of species exchange in such systems, subject to the second law of thermodynamics and conservation of mass. The methodology is independent of the specifics of reactor design and can be generally applied to determine the maximum thermodynamic benefit of using a countercurrent reactor. We then demonstrate the analysis for a number of thermochemical fuel production routes; membrane thermolysis of carbon dioxide, dry methane reforming across a membrane, reverse water gas shift across a membrane, and the thermochemical ceria cycle.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.











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