燃料化学学报
燃料化學學報
연료화학학보
JOURNAL OF FUEL CHEMISTRY AND TECHNOLOGY
2014年
9期
1128-1134
,共7页
马健%刘冬梅%魏民%王海彦%王坤%张晶卫
馬健%劉鼕梅%魏民%王海彥%王坤%張晶衛
마건%류동매%위민%왕해언%왕곤%장정위
碱处理%Na2 CO3%微-介孔%ZSM-5%硫醚化
堿處理%Na2 CO3%微-介孔%ZSM-5%硫醚化
감처리%Na2 CO3%미-개공%ZSM-5%류미화
alkail treatment%Na2 CO3%mci ro and me soporuo s%ZSM-5%thioetherfication
采用Na2 CO3溶液对ZSM-5分子筛进行碱处理,考察了处理温度和处理时间对ZSM-5分子筛结构特征和物化性能的影响。利用XRD、N2吸附-脱附、XRF、SEM及NH3-TPD表征对处理前后样品进行分析。以正丁硫醇和异戊二烯组成的模型化合物为原料,对碱处理后含微-介孔HZSM-5分子筛制得的Ni-Mo/HZSM-5催化剂进行硫醚化活性评价。结果表明, Na2 CO3溶液处理没有破坏原分子筛晶体形貌,保持微孔结构的同时,适当的提高处理温度和延长处理时间有利于ZSM-5分子筛比表面积、外比表面积、介孔孔容和平均孔径的增大,并调节了酸性质。但过长的处理时间并不利于介孔的生成和酸性的调变。经90℃的Na2 CO3溶液处理5 h得到催化剂表现较高硫醚化活性,正丁硫醇和异戊二烯转化率分别可达92.36%和97.33%。由此,Na2 CO3溶液处理可提高催化剂硫醚化活性,且改性过程温和可控。
採用Na2 CO3溶液對ZSM-5分子篩進行堿處理,攷察瞭處理溫度和處理時間對ZSM-5分子篩結構特徵和物化性能的影響。利用XRD、N2吸附-脫附、XRF、SEM及NH3-TPD錶徵對處理前後樣品進行分析。以正丁硫醇和異戊二烯組成的模型化閤物為原料,對堿處理後含微-介孔HZSM-5分子篩製得的Ni-Mo/HZSM-5催化劑進行硫醚化活性評價。結果錶明, Na2 CO3溶液處理沒有破壞原分子篩晶體形貌,保持微孔結構的同時,適噹的提高處理溫度和延長處理時間有利于ZSM-5分子篩比錶麵積、外比錶麵積、介孔孔容和平均孔徑的增大,併調節瞭痠性質。但過長的處理時間併不利于介孔的生成和痠性的調變。經90℃的Na2 CO3溶液處理5 h得到催化劑錶現較高硫醚化活性,正丁硫醇和異戊二烯轉化率分彆可達92.36%和97.33%。由此,Na2 CO3溶液處理可提高催化劑硫醚化活性,且改性過程溫和可控。
채용Na2 CO3용액대ZSM-5분자사진행감처리,고찰료처리온도화처리시간대ZSM-5분자사결구특정화물화성능적영향。이용XRD、N2흡부-탈부、XRF、SEM급NH3-TPD표정대처리전후양품진행분석。이정정류순화이무이희조성적모형화합물위원료,대감처리후함미-개공HZSM-5분자사제득적Ni-Mo/HZSM-5최화제진행류미화활성평개。결과표명, Na2 CO3용액처리몰유파배원분자사정체형모,보지미공결구적동시,괄당적제고처리온도화연장처리시간유리우ZSM-5분자사비표면적、외비표면적、개공공용화평균공경적증대,병조절료산성질。단과장적처리시간병불리우개공적생성화산성적조변。경90℃적Na2 CO3용액처리5 h득도최화제표현교고류미화활성,정정류순화이무이희전화솔분별가체92.36%화97.33%。유차,Na2 CO3용액처리가제고최화제류미화활성,차개성과정온화가공。
ZSM-5 zeolites were treated by alkali Na2 CO3 solution;the effect of treatment temperature and time on the structural feature and physical and chemical properties of ZSM-5 zeolites were investigated.The ZSM-5 samples before and after alkali treatment were characterized by XRD, N2 sorption, XRF, SEM and NH3-TPD. With n-butyl mercaptan and isoprene as the model compounds for thioetherfication, the acit viyt of Ni-Mo/HZSM-5 prepared from alkali treated HZSM-5 ez olites with micro-and meso-porous strcu ture were evaluated. The results show that the original zeolite frame structure is rees rev da fter Na2C O3 solution treatment; moreover, the performance of the Ni-Mo/HZSM-5 catalyst in thioetherfications is improved and the modification process was gentel and controllable. An appropriate increase of the treatment temperature and treatment time w as beneficial to the incrae se of surface area, meso-pore volume and average pore size,a s well as ht e regulation of the acid properties without affecting the microporous structure.However, excessive long treatment time was disadvantageous to the formation of mesopores and the modulation of acidity.The Ni-Mo/HZSM-5 catalyst from ZSM-5 treated with Na2 CO3 solution at 90℃for 5 h exhibits high thioetherfication performance;the conversions of n-butyl mercaptan and isoprene reach 92 .36%and 97 .33%, respectively.