物理化学学报
物理化學學報
물이화학학보
ACTA PHYSICO-CHIMICA SINICA
2012年
4期
928-934
,共7页
薛蒙伟%周钰明%张一卫%黄力%刘旋%段永正
薛矇偉%週鈺明%張一衛%黃力%劉鏇%段永正
설몽위%주옥명%장일위%황력%류선%단영정
Mg%Sn-ZSM-5%丙烷脱氢%催化性能%催化剂
Mg%Sn-ZSM-5%丙烷脫氫%催化性能%催化劑
Mg%Sn-ZSM-5%병완탈경%최화성능%최화제
Mg%Sn-ZSM-5%Propane dehydrogenation%Catalytic performance%Catalyst
通过X射线衍射(XRD)、N2吸附、透射电镜(TEM)、NH3程序升温脱附(NH3-TPD)、H2程序升温还原(H2-TPR)和O2程序升温氧化(O2-TPO)等多种表征手段及催化反应性能评价,研究了镁助剂的添加对PtNa/Sn-ZSM-5催化丙烷脱氢反应性能的影响.结果表明:适量Mg的添加(0.3%和0.5%,质量分数)能促进催化剂表面金属粒子的分散,减少反应过程中积碳的产生.Mg的引入能有效抑制催化剂中Sn组分的还原,使更多量的Sn组分以氧化态形式存在,有利于丙烷脱氢反应的进行.但是,过量Mg的加入导致催化剂表面金属颗粒易于发生团聚,高温下Sn组分易于被还原,不利于反应的进行.在本实验中,0.5%Mg加入后PtNa/Sn-ZSM-5催化剂显示出最佳的反应性能,反应7h后,丙烷转化率仍然高达38.7%,对应的丙烯选择性能够维持在95%以上.
通過X射線衍射(XRD)、N2吸附、透射電鏡(TEM)、NH3程序升溫脫附(NH3-TPD)、H2程序升溫還原(H2-TPR)和O2程序升溫氧化(O2-TPO)等多種錶徵手段及催化反應性能評價,研究瞭鎂助劑的添加對PtNa/Sn-ZSM-5催化丙烷脫氫反應性能的影響.結果錶明:適量Mg的添加(0.3%和0.5%,質量分數)能促進催化劑錶麵金屬粒子的分散,減少反應過程中積碳的產生.Mg的引入能有效抑製催化劑中Sn組分的還原,使更多量的Sn組分以氧化態形式存在,有利于丙烷脫氫反應的進行.但是,過量Mg的加入導緻催化劑錶麵金屬顆粒易于髮生糰聚,高溫下Sn組分易于被還原,不利于反應的進行.在本實驗中,0.5%Mg加入後PtNa/Sn-ZSM-5催化劑顯示齣最佳的反應性能,反應7h後,丙烷轉化率仍然高達38.7%,對應的丙烯選擇性能夠維持在95%以上.
통과X사선연사(XRD)、N2흡부、투사전경(TEM)、NH3정서승온탈부(NH3-TPD)、H2정서승온환원(H2-TPR)화O2정서승온양화(O2-TPO)등다충표정수단급최화반응성능평개,연구료미조제적첨가대PtNa/Sn-ZSM-5최화병완탈경반응성능적영향.결과표명:괄량Mg적첨가(0.3%화0.5%,질량분수)능촉진최화제표면금속입자적분산,감소반응과정중적탄적산생.Mg적인입능유효억제최화제중Sn조분적환원,사경다량적Sn조분이양화태형식존재,유리우병완탈경반응적진행.단시,과량Mg적가입도치최화제표면금속과립역우발생단취,고온하Sn조분역우피환원,불리우반응적진행.재본실험중,0.5%Mg가입후PtNa/Sn-ZSM-5최화제현시출최가적반응성능,반응7h후,병완전화솔잉연고체38.7%,대응적병희선택성능구유지재95%이상.
The effects of Mg addition on the catalytic performance of PtNa/Sn-ZSM-5 in propane dehydrogenation was investigated using catalytic reaction performance tests and physicochemical characterizations such as X-ray diffraction (XRD),nitrogen adsorption,transmission electron microscopy (TEM),NH3 temperature-programmed desorption (NH3-TPD),H2 temperature-programmed reduction (H2-TPR),and O2 temperature-programmed oxidation (O2-TPO).It was found that addition of appropriate amounts of Mg (0.3% and 0.5%,mass fraction) promoted the dispersion of metallic particles and decreased carbon deposition.In these cases,the presence of Mg in the PtMgNa/Sn-ZSM-5 catalyst could inhibit reduction of Sn species,thus more Sn could exist in oxidized states,which is advantageous to the reaction.However,when the content of Mg was excessive,the metallic particles were not well distributed and the particles agglomerated more easily.Moreover,the reduction of Sn species at high temperatures is relatively easy,which is disadvantageous to the reaction.In our experiments,the addition of 0.5% Mg to the PtNa/Sn-ZSM-5 catalyst gave the best catalytic performance.After reaction for 7 h,higher than 95% selectivity toward propene was achieved with a corresponding propane conversion value of 38.7%.