A novel model is presented for the estimation of natural CaO-based sorbents carbonation reactivity decay during Calcium Looping carbonation-calcination cycles. The model consists of a cyclic framework of two sub-models, the Overlapping Grain Model and the novel proposed modified Rate Theory for the Pore Size Distribution model. The model was implemented in gPROMS ModelBuilder® and parameter estimation was used for model validation using experimental data from three CaO-based sorbent precursors. The carbonation profile for the three sorbents was simulated with average deviations under 5%. The calcination sub-model predicted the evolution of total porous volume and total surface area for the calcination and sintering of dolomite, with an error of 3%. The cyclic framework successfully predicted the carbonation behavior of dolomite for 20 carbonation-calcination cycles. The model can be used for other CaO-based sorbents and the flexible modular structure allows the integration of other modules or approaches.

提出了一种新的模型，用于估计钙环碳酸化-煅烧循环过程中基于天然CaO的吸附剂的碳酸化反应性衰减。该模型由两个子模型的循环框架组成，即重叠颗粒模型和针对孔隙尺寸分布模型提出的新颖的改进速率理论。该模型在gPROMSModelBuilder®中实现，并且使用来自三种基于CaO的吸附剂前体的实验数据，将参数估计值用于模型验证。模拟了三种吸附剂的碳酸化曲线，其平均偏差在5％以下。煅烧子模型预测了白云石的煅烧和烧结的总孔体积和总表面积的变化，误差为3％。该循环框架成功地预测了20个碳化-煅烧循环中白云石的碳化行为。该模型可用于其他基于CaO的吸附剂，并且灵活的模块化结构允许集成其他模块或方法。