STUDY ON SO2 ADSORPTION PERFORMANCE OF HY MOLECULAR SIEVES

Abstract

Abstract: Three HY molecular sieves HY-1，HY-2，HY-3 with different ratios of Si/Al were used as adsorbents to perform experiments of SO2 adsorption in a fixed bed device. The relationship between saturation adsorption capacity and Si-Al ratios of the sieves was investigated. Physicochemical properties of HY molecular sieves were characterized by BET，XRD，XRF，CO2/O2-TPD techniques and correlated with SO2 saturated adsorption capacity. It was shown by the results that with the increase of Si/Al ratio, the SO2 penetration time of molecular sieves HY-1, HY-2 and HY-3 decreased in turn, and the saturated adsorption capacity decreased in turn, indicating that increasing Si/Al ratio is not conducive to adsorption of SO2 by HY molecular sieves and that the SO2 saturation adsorption capacity of HY molecular sieve was directly proportional to the basic content on its surface. It was found that the adsorption performance of molecular sieve for SO2 is directly related to the species and content of oxygen on its surface. With the increase of Si/Al ratio, the content of chemically adsorbed oxygen on HY molecular sieve surface decreased in turn for the three sieves, and the amount of chemically adsorbed SO2 decreased in turn.

Key words: HY molecular sieve, adsorption, SO2, Si/Al ratio, adsorption capacity

References

[1]REZAEI F，ROWNAGHI A A，MONJEZI S，et al. SOx/NOx Removal from Flue Gas Streams by Solid Adsorbents：A Review of Current Challenges and Future Directions [J]. Energy & Fuels，2015，29(9)： 5467-5486.
[2]GAUDIN P，DORGE S，NOUALI H，et al. Synthesis of CuO/SBA-15 adsorbents for SOx removal
applications，using different impregnation methods [J]. Comptes Rendus Chimie，2015，18(10)： 1013-1029.
[3]DEO A V，DALLA LANA I G，HABGOOD H W. Infrared studies of the adsorption and surface reactions of
hydrogen sulfide and sulfur dioxide on some aluminas and zeolites[J]. Journal of Catalysis，1971，21(3)：
270-281.
[4]MARCU I C，SANDULESCU I. Study of sulfur dioxide adsorption on Y zeolite[J]. JOURNAL-SERBIAN
CHEMICAL SOCIETY，2004，69(7)：563-570.
[5]NASLUZOV V A，SHOR A M，N?RTEMANN F，et al. Density functional study of SO2 adsorption in HY
zeolites[J]. Journal of Molecular Structure：THEOCHEM，1999，466(1-3)：235-244.
[6]SAKURAI Y，TAKAHASHI Y，MAKINO T. Laboratory measurement of absorption and oxidation of sulphur
dioxide by zeolite[J]. Journal of Geochemical Exploration，1998，64(1-3)：315-319.
[7]LANIECKI M，ZIOLEK M，KARGE H G. Effect of water on the formation of bisulfite ions upon sulfur
dioxide adsorption onto faujasite-type zeolites[J]. Journal of Physical Chemistry，1987，91(1)：4-6.
[8]Kirschhock C E A，Sultana A，Godard E，et al. Adsorption chemistry of sulfur dioxide in hydrated Na-Y
zeolite[J]. Angewandte Chemie International Edition，2004，43(28)：3722-3724.
[9]Srinivasan A，Grutzeck M W. The adsorption of SO2 by zeolites synthesized from fly ash[J]. Environmental
science & technology，1999，33(9)：1464-1469.
[10]Dragan G. The individual adsorption of carbon dioxide and sulphur dioxide by Y zeolites[J]. Rev Chim，2010，
61：897-902.
[11]DENG S G，LIN Y S. Sulfur dioxide sorption properties and thermal stability of hydrophobic zeolites[J].
Industrial & engineering chemistry research，1995，34(11)：4063-4070.
[12]郭大为，李倩，陈西岩，等. 烟气脱硫，脱氮吸附剂再生过程的考察[J]. 石油炼制与化工，2012 (2012
年02)：9-14.
[13]郭大为，张久顺，梁彬，等. 催化裂化烟气脱硫，脱氮吸附剂的初步研究[J]. 石油学报(石油加工)，2011，
27(2)：192-197.
[14]郭大为，张久顺，龙军，等.脱除烟气中硫氧化物和/或氮氧化物的方法及烃油裂化方法：中国，
CN101209391A[P] .2008.
[15]RAYMUNDO-PINERO E，CAZORLA-AMORóS D，DE LECEA C S M，et al. Factors controling the SO2 removal by porous carbons：relevance of the SO2 oxidation step[J]. Carbon，2000，38(3)：335-344.
[16]BARTHOMEUF D. Conjugate acid-base pairs in zeolites[J]. The Journal of Physical Chemistry，1984，88(1)：
42-45.
[17]XIE J，HUANG M，KALIAGUINE S. Zeolite basicity characterized by chloroform chemisorption. An infrared
study[J]. Reaction Kinetics and Catalysis Letters，1996，58(2)：217-227.
[18]MARSAL A，ROSSINYOL E，BIMBELA F，et al. Characterisation of LaOCl sensing materials using
CO2-TPD，XRD，TEM and XPS [J]. Sensors and Actuators B: Chemical，2005，109(1)：38-43.
[19]PI Z，SHEN B，ZHAO J，et al. CuO，CeO2 Modified Mg–Al Spinel for Removal of SO2 from Fluid Catalytic
Cracking Flue Gas [J]. Industrial & Engineering Chemistry Research，2015，54(43)：10622-10628.
[20]LEE K M，LIM Y H，JO Y M. Evaluation of moisture effect on low-level CO2 adsorption by ion-exchanged
zeolite [J]. Environmental technology，2012，33(1)：77-84.
[21]WORAYINGYONG A，KANGVANSURA P，KITYAKARN S. Schiff base complex sol–gel method for LaCoO3 perovskite preparation with high-adsorbed oxygen [J]. Colloids and Surfaces A：Physicochemical and Engineering Aspects，2008，320(1-3)：123-129.
[22]KLEPEL O，HUNGER B. Temperature-programmed desorption (TPD) of carbon dioxide on alkali-metal cation-exchanged faujasite type zeolites[J]. Journal of thermal analysis and calorimetry，2005，80(1)：201-206.
[23]FANG X，XIA L，PENG L，et al. Ln2Zr2O7 compounds (Ln = La，Pr，Sm，Y) with varied rare earth A sites for low temperature oxidative coupling of methane [J]. Chinese Chemical Letters，2019，30(6)：1141-1146.
[24]MA C，WANG D，XUE W，et al. Investigation of formaldehyde oxidation over Co3O4-CeO2 and Au/Co3O4-CeO2 catalysts at room temperature：effective removal and determination of reaction mechanism [J]. Environmental science & technology，2011，45(8)：3628-3634.
[25]LU S，WANG F，CHEN C，et al. Catalytic oxidation of formaldehyde over CeO2 -Co3O4 catalysts [J]. Journal of Rare Earths，2017，35(9)：867-874.