化工学报
化工學報
화공학보
JOURNAL OF CHEMICAL INDUSY AND ENGINEERING (CHINA)
2015年
8期
3098-3105
,共8页
沸石%催化剂%反应%碱处理%多级孔
沸石%催化劑%反應%堿處理%多級孔
비석%최화제%반응%감처리%다급공
zeolite%catalyst%reaction%alkaline treatment%hierarchical pores
采用不同后处理手段(碱处理、水汽处理以及碱处理-水汽处理)对HZSM-5沸石的孔结构和酸性质进行了调变,并对其丁烯裂解性能进行了研究。运用N2吸脱附、扫描电镜(SEM)、X射线衍射(XRD)以及吡啶吸附红外(Py-IR)对后处理改性前后的沸石样品的物理化学性质进行了表征。碱处理后HZSM-5的质子酸量增加,在5~20 nm处具有分布较宽的介孔,其反应活性升高,丙烯选择性下降,但失活速率没有加快。单独水汽处理在2~4 nm处产生介孔,但介孔体积较小。碱处理-水汽处理在2~4和5~20 nm处具有双分布介孔,前者分布较集中,后者分布较宽。单独水汽处理和碱处理-水汽处理的样品可以提高HZSM-5的丙烯选择性,主要归功于酸量的降低;反应2.5 h后具有较稳定的丙烯收率(高碱浓度处理-水汽处理的样品除外)。
採用不同後處理手段(堿處理、水汽處理以及堿處理-水汽處理)對HZSM-5沸石的孔結構和痠性質進行瞭調變,併對其丁烯裂解性能進行瞭研究。運用N2吸脫附、掃描電鏡(SEM)、X射線衍射(XRD)以及吡啶吸附紅外(Py-IR)對後處理改性前後的沸石樣品的物理化學性質進行瞭錶徵。堿處理後HZSM-5的質子痠量增加,在5~20 nm處具有分佈較寬的介孔,其反應活性升高,丙烯選擇性下降,但失活速率沒有加快。單獨水汽處理在2~4 nm處產生介孔,但介孔體積較小。堿處理-水汽處理在2~4和5~20 nm處具有雙分佈介孔,前者分佈較集中,後者分佈較寬。單獨水汽處理和堿處理-水汽處理的樣品可以提高HZSM-5的丙烯選擇性,主要歸功于痠量的降低;反應2.5 h後具有較穩定的丙烯收率(高堿濃度處理-水汽處理的樣品除外)。
채용불동후처리수단(감처리、수기처리이급감처리-수기처리)대HZSM-5비석적공결구화산성질진행료조변,병대기정희렬해성능진행료연구。운용N2흡탈부、소묘전경(SEM)、X사선연사(XRD)이급필정흡부홍외(Py-IR)대후처리개성전후적비석양품적물이화학성질진행료표정。감처리후HZSM-5적질자산량증가,재5~20 nm처구유분포교관적개공,기반응활성승고,병희선택성하강,단실활속솔몰유가쾌。단독수기처리재2~4 nm처산생개공,단개공체적교소。감처리-수기처리재2~4화5~20 nm처구유쌍분포개공,전자분포교집중,후자분포교관。단독수기처리화감처리-수기처리적양품가이제고HZSM-5적병희선택성,주요귀공우산량적강저;반응2.5 h후구유교은정적병희수솔(고감농도처리-수기처리적양품제외)。
The structure and acidity of HZSM-5 zeolites were modified using different post treatment methods: alkaline treatment, steam treatment, and alkaline-steaming treatment. The catalytic performances of modified zeolites were tested in 1-butene catalytic cracking. Their physicochemical properties were characterized by N2 adsorption, scanning electron microscopy (SEM), X-ray diffraction (XRD), and infrared spectroscopy with pyridine adsorption (Py-IR). The acidities of zeolites increased after the alkaline treatment, and as a result, the activity of butene cracking increased and the selectivity of propylene decreased. However, the deactivation rate of alkaline-treated zeolites had no significant change. There was a pronounced development of mesopores (5—20 nm) with a broad pore-size distribution in alkaline-treated ZSM-5 zeolites. Mesopores (2—4 nm) with a narrow distribution is observed after steaming treatment, while the mesopore volume is low. Zeolites after alkaline- and steaming-treatment showed two kinds of mesopore distributions, 2—4 nm (narrow) and 5—20 nm (broad). Due to the decrease of Br?nsted acidic sites, the selectivity of propylene increased over ZSM-5 zeolites with any of the post treatments; a relatively stable propylene yield was obtained after the reaction of 2.5 h (except for zeolites treated with high concentration of alkaline followed by steaming treatment).