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A Strong Test of Atomically Detailed Models of Molecular Adsorption in Zeolites Using Multilaboratory Experimental Data for CO2 Adsorption in Ammonium ZSM-5.
The Journal of Physical Chemistry Letters ( IF 5.7 ) Pub Date : 2020-01-03 , DOI: 10.1021/acs.jpclett.9b02986
Hanjun Fang 1 , John Findley 1 , Giovanni Muraro 2 , Peter I Ravikovitch 2 , David S Sholl 1
Affiliation  

A recent international interlaboratory study led by the U.S. National Institute of Standards (NIST) reported CO2 adsorption isotherms measured independently by 11 groups on reference material RM 8852, an ammonium ZSM-5 zeolite. Good reproducibility and high reliability of this experimental data provide a strong test for the ability of atomically detailed models to predict adsorption of CO2 in zeolites. We developed force fields for CO2 in ammonium zeolites based on first-principles calculations and also independently performed experiments with RM 8852 by microcalorimetry. At low pressures good agreement was obtained between predictions and experiments. At high pressures, however, deviations were observed. We show that the charge-balancing cations in the experimental material are the predominant source of the discrepancy between simulation and experiment at high pressures; the experimental sample treatment causes deammoniation. In addition, accounting for a small amount of noncrystalline mesoporosity in the zeolite brings predictions into much better agreement with experiments.

中文翻译:

使用多实验室实验数据对ZSM-5铵中CO2的吸附,对沸石分子吸附的原子详细模型进行了强有力的测试。

由美国国家标准研究院(NIST)领导的最新国际实验室间研究报告,由11组在参考材料RM 8852(ZSM-5铵沸石)上独立测量了CO2吸附等温线。此实验数据的良好重现性和高可靠性为原子详细模型预测沸石中CO2吸附的能力提供了有力的检验。我们根据第一性原理计算得出了铵沸石中CO2的力场,并通过微量量热法对RM 8852进行了独立实验。在低压下,预测和实验之间获得了良好的一致性。然而,在高压下,观察到偏差。我们表明,实验材料中的电荷平衡阳离子是高压下模拟与实验之间差异的主要来源。实验样品处理会导致脱氨。另外,考虑到沸石中少量的非晶体介孔性,使预测与实验更好地吻合。
更新日期:2020-01-04
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