工业催化
工業催化
공업최화
INDUSTRIAL CATALYSIS
2015年
7期
520-526
,共7页
王媛%范素兵%张建利%赵天生
王媛%範素兵%張建利%趙天生
왕원%범소병%장건리%조천생
催化剂工程%HZSM-5分子筛%直接合成%晶化条件
催化劑工程%HZSM-5分子篩%直接閤成%晶化條件
최화제공정%HZSM-5분자사%직접합성%정화조건
catalyst engineering%HZSM-5 molecular sieve%direct synthesis%crystallization conditions
考察了SiO2-Al2 O3-TPABr-NH3·H2 O-H2 O体系晶化时间、晶化温度和原料用量等对合成HZSM-5性能的影响。当n( SiO2):n( Al2 O3)=100、n( TPABr):n( SiO2)=0.1、n( NH3):n(SiO2)=1.5、n(H2O):n(SiO2)=22和晶种添加质量分数为4%时,180℃静态晶化72 h,合成收率与相对结晶度分别为10.1%和99.8%,对应理论收率为11.4%,合成收率与理论收率比为0.89。当投料n(SiO2):n(Al2O3)从50增加到400,合成收率与结晶度分别超过8.9%和82.8%,合成收率与理论收率比为0.76~0.89;样品酸量随着n( SiO2):n( Al2 O3)的增加逐渐减小,比表面积为405 m2·g-1,合成样品HZSM-5对甲醇制烯烃反应具有良好的酸催化活性。设定反应条件,采用投料n( SiO2):n( Al2 O3)=250的样品,甲醇转化率、丙烯选择性和C2=~C4=选择性分别为100%、39.27%和62.01%。
攷察瞭SiO2-Al2 O3-TPABr-NH3·H2 O-H2 O體繫晶化時間、晶化溫度和原料用量等對閤成HZSM-5性能的影響。噹n( SiO2):n( Al2 O3)=100、n( TPABr):n( SiO2)=0.1、n( NH3):n(SiO2)=1.5、n(H2O):n(SiO2)=22和晶種添加質量分數為4%時,180℃靜態晶化72 h,閤成收率與相對結晶度分彆為10.1%和99.8%,對應理論收率為11.4%,閤成收率與理論收率比為0.89。噹投料n(SiO2):n(Al2O3)從50增加到400,閤成收率與結晶度分彆超過8.9%和82.8%,閤成收率與理論收率比為0.76~0.89;樣品痠量隨著n( SiO2):n( Al2 O3)的增加逐漸減小,比錶麵積為405 m2·g-1,閤成樣品HZSM-5對甲醇製烯烴反應具有良好的痠催化活性。設定反應條件,採用投料n( SiO2):n( Al2 O3)=250的樣品,甲醇轉化率、丙烯選擇性和C2=~C4=選擇性分彆為100%、39.27%和62.01%。
고찰료SiO2-Al2 O3-TPABr-NH3·H2 O-H2 O체계정화시간、정화온도화원료용량등대합성HZSM-5성능적영향。당n( SiO2):n( Al2 O3)=100、n( TPABr):n( SiO2)=0.1、n( NH3):n(SiO2)=1.5、n(H2O):n(SiO2)=22화정충첨가질량분수위4%시,180℃정태정화72 h,합성수솔여상대결정도분별위10.1%화99.8%,대응이론수솔위11.4%,합성수솔여이론수솔비위0.89。당투료n(SiO2):n(Al2O3)종50증가도400,합성수솔여결정도분별초과8.9%화82.8%,합성수솔여이론수솔비위0.76~0.89;양품산량수착n( SiO2):n( Al2 O3)적증가축점감소,비표면적위405 m2·g-1,합성양품HZSM-5대갑순제희경반응구유량호적산최화활성。설정반응조건,채용투료n( SiO2):n( Al2 O3)=250적양품,갑순전화솔、병희선택성화C2=~C4=선택성분별위100%、39.27%화62.01%。
In SiO2-Al2 O3-TPABr-NH3 · H2 O-H2 O system,the effects of hydrothermal crystallization time and temperatures,and raw material amounts on the yields and properties of as-synthesized HZSM-5 molecular sieve were investigated. The results showed that the yield and relative crystallinity of as-synthesized samples were 10. 1% and 99. 8%,respectively,under the condition as follows:n( SiO2 ): n( Al2 O3 )=100, n(TPABr):n(SiO2)=0.1,n(NH3):n(SiO2)=1. 5,n(H2O):n(SiO2)=22,seed crystal amount 4%, crystallization temperature 180 ℃ and crystallization time 72 h. The corresponding theoretical yield was 11 . 4%,and the ratio of the yield of as-synthesized samples to the theoretical yield was 0 . 89 . As n(SiO2):n(Al2O3)of the raw material enhanced from 50 to 400,the yield and crystallinity of the as-synthesized samples remained more than 8. 9% and 82. 8%,respectively,and the ratio of as-synthesized sample yield to the theoretical yield was 0 . 76 -0 . 89 . The acid amount of the as-synthesized samples decreased gradually with the increase of n( SiO2 ): n( Al2 O3 )of the raw material. The as-synthesized HZSM-5 molecular sieve with BET surface area of 405 m2 ·g-1 exhibited good acid catalytic activity for methanol-to-olefins reaction. At the set condition,methanol conversion,the selectivity to propylene and C2=-C4= light olefins were 100%,39. 27% and 62. 01%,respectively,using HZSM-5 molecular sieve catalyst prepared with the raw material of n(SiO2):n(Al2O3)=250.