Adsorption for efficient low carbon hydrogen production: part 1—adsorption equilibrium and breakthrough studies for H2/CO2/CH4 on zeolite 13X
Adsorption for efficient low carbon hydrogen production: part 1—adsorption equilibrium and breakthrough studies for H2/CO2/CH4 on zeolite 13X
复制标题
高效低碳制氢的吸附：第 1 部分——H2/CO2/CH4 在 13X 沸石上的吸附平衡和突破性研究
DOI：
10.1007/s10450-021-00306-y
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发表时间：
2021
期刊：
影响因子：
3.3
通讯作者：
M. Mazzotti
中科院分区：
文献类型：
--
作者：
A. Streb;M. Mazzotti
化石燃料的重整与碳捕获和储存相结合，有可能以大规模和低成本生产低碳H2。吸附是一种潜在的有前途的技术，用于该过程中的两个关键分离任务：H2纯化和CO2捕获。在这项工作中，我们提出了平衡吸附数据的H2和CH 4沸石13 X，除了已经建立的CO2等温线。此外，我们进行了二元（CO2-CH 4）和三元（H2-CO2-CH 4）的突破实验，在不同的压力和温度下，以估计传输参数，评估我们的一维柱模型的预测能力，并比较不同的多组分吸附模型。CO_2在13 X沸石上吸附较强，CH_4吸附较少，H_2吸附很少。因此，H2首先突破，CH 4其次（在二元突破实验中第一个），CO2最后。线性驱动力（LDF）的传质系数估计的基础上，一个单一的突破实验和传质被发现是快速的H2，CH 4较慢，CO2最慢。LDF参数可以以预测的方式用于在不同的压力、温度、流量、甚至成分（尽管精度较低）下的突破实验。列内的传热描述以及与文献相关，从而产生一个很好的协议之间的模拟和测量柱温。理想和真实的吸附溶液理论（IAST和RAST，分别）都模型所观察到的突破组合物的配置文件，而扩展等温线是劣质的预测CH 4和CO2吸附之间的竞争行为。该研究为全循环试验及其模拟提供了必要的基础。
Reforming of fossil fuels coupled with carbon capture and storage has the potential to produce low-carbon H2 at large scale and low cost. Adsorption is a potentially promising technology for two key separation tasks in this process: H2 purification and CO2 capture. In this work, we present equilibrium adsorption data of H2 and CH4 on zeolite 13X, in addition to the already established CO2 isotherms. Further, we carry out binary (CO2–CH4) and ternary (H2–CO2–CH4) breakthrough experiments at various pressures and temperatures to estimate transport parameters, assess the predictive capacity of our 1D column model, and compare different multi-component adsorption models. CO2 adsorbs strongly on zeolite 13X, CH4 adsorbs less, and H2 adsorbs very little. Thus, H2 breaks through first, CH4 second (first in the binary breakthrough experiments) and CO2 last. Linear driving force (LDF) mass transfer coefficients are estimated based on a single breakthrough experiment and mass transfer is found to be fast for H2, slower for CH4, and slowest for CO2. The LDF parameters can be used in a predictive manner for breakthrough experiments at varying pressures, temperatures, flows, and, though with lower accuracy, even compositions. Heat transfer inside the column is described well with a literature correlation, thus yielding an excellent agreement between simulated and measured column temperatures. Ideal and real adsorbed solution theories (IAST and RAST, respectively) both model the observed breakthrough composition profiles well, whereas extended isotherms are inferior for predicting the competitive behavior between CH4 and CO2 adsorption. This study provides the groundwork necessary for full cyclic experiments and their simulation.