石油化工高等学校学报
石油化工高等學校學報
석유화공고등학교학보
JOURNAL OF PETROCHEMICAL UNIVERSITIES
2013年
4期
21-26
,共6页
孙月桥%张圆圆%杜夏梅%金英杰
孫月橋%張圓圓%杜夏梅%金英傑
손월교%장원원%두하매%금영걸
沸石合成%ZSM-22%竞争相%ZSM-5%方石英%相对结晶度%相纯度
沸石閤成%ZSM-22%競爭相%ZSM-5%方石英%相對結晶度%相純度
비석합성%ZSM-22%경쟁상%ZSM-5%방석영%상대결정도%상순도
Zeolite synthesis%ZSM-22%Competing phase%ZSM-5%Cristobalite%Relative crystallinity%Phase purity
在SiO2-Al2 O3-K2 O-DAH-H2 O(1,6-己二胺,DAH)体系中,研究水热合成条件对ZSM-22沸石相对结晶度和相纯度的影响。采用X射线衍射(XRD)和电感耦合等离子体(ICP)技术表征合成产物的结构、物相及化学组成。结果表明,合成胶 n(SiO2)/n(Al2 O3)在80~110,n(OH -)/n(SiO2)在0.33~0.35和433~438 K条件下,合成出系列相纯度较高的ZSM-22沸石。产物相对结晶度和相纯度依赖于合成胶硅铝物质的量比、碱度和晶化温度。适当升高晶化温度有利于提高产物的相纯度和相对结晶度;n(SiO2)/n(Al2 O3)在80~110之外,合成胶硅铝物质的量比的降低或提高分别导致ZSM-5或方石英相分率的逐渐增加。此外,纯ZSM-22骨架 n(Si)/n(Al)分布于41.8~53.4;与 n(SiO2)/n(Al2 O3)关联可知,n(Si)/n(Al)比值向该区间中心呈收敛趋势。
在SiO2-Al2 O3-K2 O-DAH-H2 O(1,6-己二胺,DAH)體繫中,研究水熱閤成條件對ZSM-22沸石相對結晶度和相純度的影響。採用X射線衍射(XRD)和電感耦閤等離子體(ICP)技術錶徵閤成產物的結構、物相及化學組成。結果錶明,閤成膠 n(SiO2)/n(Al2 O3)在80~110,n(OH -)/n(SiO2)在0.33~0.35和433~438 K條件下,閤成齣繫列相純度較高的ZSM-22沸石。產物相對結晶度和相純度依賴于閤成膠硅鋁物質的量比、堿度和晶化溫度。適噹升高晶化溫度有利于提高產物的相純度和相對結晶度;n(SiO2)/n(Al2 O3)在80~110之外,閤成膠硅鋁物質的量比的降低或提高分彆導緻ZSM-5或方石英相分率的逐漸增加。此外,純ZSM-22骨架 n(Si)/n(Al)分佈于41.8~53.4;與 n(SiO2)/n(Al2 O3)關聯可知,n(Si)/n(Al)比值嚮該區間中心呈收斂趨勢。
재SiO2-Al2 O3-K2 O-DAH-H2 O(1,6-기이알,DAH)체계중,연구수열합성조건대ZSM-22비석상대결정도화상순도적영향。채용X사선연사(XRD)화전감우합등리자체(ICP)기술표정합성산물적결구、물상급화학조성。결과표명,합성효 n(SiO2)/n(Al2 O3)재80~110,n(OH -)/n(SiO2)재0.33~0.35화433~438 K조건하,합성출계렬상순도교고적ZSM-22비석。산물상대결정도화상순도의뢰우합성효규려물질적량비、감도화정화온도。괄당승고정화온도유리우제고산물적상순도화상대결정도;n(SiO2)/n(Al2 O3)재80~110지외,합성효규려물질적량비적강저혹제고분별도치ZSM-5혹방석영상분솔적축점증가。차외,순ZSM-22골가 n(Si)/n(Al)분포우41.8~53.4;여 n(SiO2)/n(Al2 O3)관련가지,n(Si)/n(Al)비치향해구간중심정수렴추세。
The effect of hydrothermal synthesis conditions on both relative crystallinity and phase purity of ZSM-22 zeolites was investigated in SiO2-Al2 O3-K2 O-DAH-H2 O system , hereby DAH referring to 1 ,6-diaminohexane as template . The resulting samples were characterized by powder X-ray diffraction (XRD) and inductively coupled plasma (ICP) analyses in order to examine the structure ,XRD phase ,and chemical composition .As a result ,several ZSM-22 zeolites with the higher phase purity were synthesized at respective temperatures from 433 K up to 438 K by use of the different gels which involved SiO2/Al2 O3 molar ratios of 80~100 and OH - /SiO2 molar ratios of 0 .33~0 .35 .It is found that the relative crystallinity and phase purity of ZSM-22 zeolites markedly varied as a function of crystallization temperature ,SiO 2/Al2 O3 and OH - /SiO2 molar ratios . In fact , an adequate increase in crystallization temperature improves on ZSM-22 phase purity , followed a significant enhancement of relative crystallinity .Although the ZSM-5 crystal growth takes place predominantly in the solid phase ,the decrease in the range of SiO2/Al2 O3 ratio less than 80 leads to a gradual increase in the ZSM-5 phase fraction while the increase in SiO2/Al2 O3 ratio larger than 110 also enhances the phase fraction of cristobalite .Furthermore ,Si/Al atomic ratios in ZSM-22 framework located the range of 41 .8~53 .4 ,and by correlating the Si/Al ratio of ZSM-22 framework with the SiO2/Al2 O3 ratio of alumino-silicate gels ,it is noted that the nominal ratios in ZSM-22 framework tended to shift towards the center of the Si/Al ratio interval mentioned above .