石油学报(石油加工)
石油學報(石油加工)
석유학보(석유가공)
Acta Petrolei Sinica (Petroleum Processing Section)
2015年
5期
1057-1062
,共6页
薛冰%吴晟%宋小%柳娜%苏进%李永昕
薛冰%吳晟%宋小%柳娜%囌進%李永昕
설빙%오성%송소%류나%소진%리영흔
对二甲苯%择形催化%磷酸三乙酯%HMCM-22
對二甲苯%擇形催化%燐痠三乙酯%HMCM-22
대이갑분%택형최화%린산삼을지%HMCM-22
p-Xylene%shape-selective catalysis%triethyl phosphate%HMCM-22
以磷酸三乙酯为磷氧化物前驱物,采用浸渍法制备了一系列磷改性 HMCM‐22催化剂,在固定床反应器上考察了它们在甲苯与碳酸二甲酯烷基化合成对二甲苯反应中的择形催化性能。采用 N2吸附‐脱附、N H3‐T PD和Py‐IR手段对催化剂进行了表征,并考察了反应温度、空速及反应时间对甲苯烷基化反应的影响。结果表明,以磷酸三乙酯为磷氧化物的前驱物制备的磷改性 HMCM‐22催化剂在甲苯烷基化合成对二甲苯反应中,不仅表现出优异的择形性能,而且还保持了较高的催化活性。这主要是由于磷酸三乙酯有较大的分子尺寸,浸渍过程中可覆盖分子筛外表面酸性位,并可保证分子筛孔内的酸性位不受影响。
以燐痠三乙酯為燐氧化物前驅物,採用浸漬法製備瞭一繫列燐改性 HMCM‐22催化劑,在固定床反應器上攷察瞭它們在甲苯與碳痠二甲酯烷基化閤成對二甲苯反應中的擇形催化性能。採用 N2吸附‐脫附、N H3‐T PD和Py‐IR手段對催化劑進行瞭錶徵,併攷察瞭反應溫度、空速及反應時間對甲苯烷基化反應的影響。結果錶明,以燐痠三乙酯為燐氧化物的前驅物製備的燐改性 HMCM‐22催化劑在甲苯烷基化閤成對二甲苯反應中,不僅錶現齣優異的擇形性能,而且還保持瞭較高的催化活性。這主要是由于燐痠三乙酯有較大的分子呎吋,浸漬過程中可覆蓋分子篩外錶麵痠性位,併可保證分子篩孔內的痠性位不受影響。
이린산삼을지위린양화물전구물,채용침지법제비료일계렬린개성 HMCM‐22최화제,재고정상반응기상고찰료타문재갑분여탄산이갑지완기화합성대이갑분반응중적택형최화성능。채용 N2흡부‐탈부、N H3‐T PD화Py‐IR수단대최화제진행료표정,병고찰료반응온도、공속급반응시간대갑분완기화반응적영향。결과표명,이린산삼을지위린양화물적전구물제비적린개성 HMCM‐22최화제재갑분완기화합성대이갑분반응중,불부표현출우이적택형성능,이차환보지료교고적최화활성。저주요시유우린산삼을지유교대적분자척촌,침지과정중가복개분자사외표면산성위,병가보증분자사공내적산성위불수영향。
A series of phosphorous modified HMCM‐22 catalysts were prepared by impregnation with triethyl phosphate(TEP) as the precursor of phosphorous oxide .The catalytic performance of the phosphorous modified HMCM‐22 catalysts in the synthesis of p‐xylene(PX) by alkylation of toluene with dimethyl carbonate was investigated in a fixed bed reactor . The catalysts were characterized by means of N2 adsorption‐desorption ,NH3‐TPD and Py‐IR .The effects of reaction temperature ,M HSV and time‐on‐stream on the catalytic toluene alkylation were also investigated . The results indicated that the phosphorous modified HMCM‐22 catalysts prepared by using TEP as the precursor of phosphorous oxide exhibited an excellent shape‐selectivity along with a high catalytic activity ,which could be attributed to the large molecular size of TEP .The TEP molecules could not diffuse into the pores of HMCM‐22 zeolite due to their large size and only well covered the acid sites on the external surface of HMCM‐22 zeolite .