A systematic design and synthesis framework for multi-step, multi-mode and periodic sorption-enhanced reaction processes (SERP) is presented. The formulated nonlinear algebraic and partial differential equation (NAPDE)-based model simultaneously identifies optimal SERP cycle configurations, design specifications and operating conditions. Key modeling contributions include a generalized boundary-condition formulation and a representation that enables the selection of discrete operation modes and flow directions using continuous pressure variables. A simulation-based constrained grey-box optimization strategy is employed to obtain optimal cycles and design parameters. The framework has been used for designing two SERP systems, namely sorption-enhanced steam methane reforming (SE-SMR) and sorption-enhanced water gas shift reaction (SE-WGSR), for maximizing hydrogen productivity and minimizing hydrogen-production cost. Specifically, a cyclic SE-SMR process is designed that obtains 95% pure hydrogen from natural gas with 35% higher productivity and 10.86% lower cost compared to existing small-scale, distributed systems. The developed synthesis framework can also be applied for other applications.

提出了一种用于多步，多模式和周期性吸附增强反应过程（SERP）的系统设计和合成框架。制定的基于非线性代数和偏微分方程（NAPDE）的模型可同时确定最佳的SERP循环配置，设计规格和工作条件。建模的主要贡献包括广义的边界条件公式化和表示法，该表示法能够使用连续的压力变量选择离散的操作模式和流向。采用基于仿真的约束灰箱优化策略来获得最佳周期和设计参数。该框架已用于设计两个SERP系统，即吸附增强型蒸汽甲烷重整（SE-SMR）和吸附增强型水煤气变换反应（SE-WGSR），用于最大化氢气生产率和最小化氢气生产成本。具体而言，设计了一种循环SE-SMR工艺，与现有的小型分布式系统相比，该工艺可从天然气中获得95％的纯氢，从而生产率提高了35％，成本降低了10.86％。开发的综合框架也可以应用于其他应用程序。