4.7 Article

Water adsorption and hydrothermal stability of CHA zeolites with different Si/Al ratios and compensating cations

期刊

CATALYSIS TODAY
卷 390, 期 -, 页码 99-108

出版社

ELSEVIER
DOI: 10.1016/j.cattod.2021.11.042

关键词

Molecular sieves; CHA; Hydrothermal aging; Water adsorption; Si/Al

资金

  1. Petrobras (Brazil) [2018/00130-5]
  2. CAPES (Brazil) [CAPES/Print 88887.311867/2018-00]
  3. Ministerio de Ciencia, Innovacion y Universidades (Spain) [RTI2018-099668-BC22]
  4. Junta de Andalucia (Spain) [UMA18-FEDERJA-126]
  5. FEDER (E.U.) funds
  6. AEI (Spain)
  7. FEDER (E.U.) [RTI2018-101784-B-I00, SEV-2016-0683]
  8. MCIU (Spain)

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Zeolites are crystalline aluminosilicates used in processes such as natural gas drying. This study investigated the effects of thermal aging on chabazite zeolite samples with different Si/Al ratios and compensating cations. It was found that aged materials had decreased adsorption capacity for CO2 and water vapor, and that a higher Si/Al ratio and the presence of potassium provided thermal stability and protection against aging.
Zeolites are well known crystalline aluminosilicates, which may be used in processes that take advantage of their molecular sieving effect, such as natural gas drying. They are often used in cyclic processes that swing pressure and/or temperature to perform adsorption and desorption steps. It is recognized that thermal stress may decrease process performance upon prolonged use. In this work, chabazite (CHA) zeolite with two different Si/Al ratios and compensating cations was investigated by thermally aging the samples using a laboratory-scale protocol. A Premature Aging Protocol - PAP was proposed that took into account the conditions which the adsorbent is exposed to in Temperature Swing Adsorption (TSA) process for natural gas drying. The sample was previously saturated with water and n-heptane vapors (as a reference hydrocarbon) followed by pressurization (30 bar) and heating (573 K) with a mixture of CO2 and CH4 (1:4, v/v). The Si/Al ratios of the CHA samples under study were 2 and 5 and the compensating cations were Na and K. Aged materials presented a lower CO2 and water vapor adsorption capacity with an increasing content of carbon in the bulk composition. The sample with higher Si/Al ratio (approximate to 5) had a larger pore volume but adsorbed less water. Despite having the highest carbon content after aging and modest acidity, it was the most thermally stable sample, together with the sample containing potassium. Even with a lower Si/Al ratio (approximate to 2), the presence of potassium provided the sample a protective effect against aging.

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