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다양한 입자크기와 산성도를 지닌 MTT 제올라이트의 합성 및 촉매특성 연구
박성준,장회구,조성준,Park, Sung Jun,Jang, Hoi-Gu,Cho, Sung June 한국화학공학회 2018 Korean Chemical Engineering Research(HWAHAK KONGHA Vol.56 No.4
다양한 Si/Al 몰비를 지닌 MTT 제올라이트를 합성하여 methanol-to-olefin(MTO) 반응에서 촉매의 산성도가 미치는 영향을 조사하였다. Si/Al 몰비를 조절하기 위해 N,N,N',N'-테트라메틸-1,3-디아미노프로판을 구조유도물질(SDA)로 사용하였으며, 알루민산나트륨의 함량을 달리하여 $20SiO_2$ : 30SDA : x (=0.25~1.25)$NaAlO_2$ : 2NaOH : $624H_2O$ 조성으로 모액을 제조한 후 433 K에서 4일 동안 수열 합성하였다. 알루민산나트륨의 함량이 감소함에 따라 MTT 제올라이트의 입자 크기가 증가하였으며 또한 산점의 양도 감소하였다. 제조한 MTT 제올라이트의 촉매 활성을 평가하기 위해 673 K에서 공간속도(WHSV)가 $1.2h^{-1}$인 조건으로 MTO 반응을 수행한 결과, Si/Al 몰비가 24인 H-MTT (1.00Al) 촉매가 900분까지 90% 이상의 전환율을 유지함을 확인하였다. The influence of acidity in MTT zeolite of different Si/Al molar ratio's on the catalyst activity in methanol-to-olefin (MTO) reaction has been investigated. The Si/Al ratio was controlled with the Al content in the gel when N,N,N',N'-tetramethyl-1,3-diaminopropane was used as a structure directing agent (SDA). The gel composition was controlled to $20SiO_2$ : 30SDA : x (=0.25~1.25)$NaAlO_2$ : 2NaOH : $624H_2O$, which was subject to the hydrothermal synthesis at 433 K for 4 days. As the composition of sodium aluminate decreased, the particle size of MTT zeolite increased, and also the amount of acid sites decreased. To investigate the catalytic performance, MTO reaction was carried out at 673 K with $1.2h^{-1}$ WHSV. It was found that the H-MTT (1.00Al) catalyst with a Si/Al molar ratio of 24 maintained the methanol conversion over 90% for 900 min.
UZM-9 제올라이트에서 메탄올의 올레핀으로 전환반응: 전이금속 이온 교환이 촉매의 활성저하에 미치는 영향
서곤 ( Gon Seo ),김선중 ( Sun Jung Kim ),장회구 ( Hoi Gu Jang ) 한국화학공학회 2013 Korean Chemical Engineering Research(HWAHAK KONGHA Vol.51 No.2
The effect of transition metal ion exchange into UZM-9 zeolite with LTA framework on its deactivation in methanol-to-olefin (MTO) conversion was discussed. The ion exchange of copper, cobalt, nickel, and iron did not induce any notable change in the crystallinity, crystal morphology, and acidity of UZM-9. The small cage entrance of UZM-9 caused the high selectivity to lower olefins in the MTO conversion, while its large cages allowed the rapid further cyclecondensation of active intermediates, polymethylbenzenes including hexamethylbenzene, resulting in a rapid deactivation. The UZM-9 containing copper and cobalt ions showed considerably slow deactivations. The interaction between transition metal ions and polymethylbenzene cation radicals, the active intermediates, generated in the MTO conversion stabilized the radicals and slowed down the deactivation of UZM-9.