化工进展
化工進展
화공진전
CHEMICAL INDUSTRY AND ENGINEERING PROGRESS
2012年
12期
2714-2719
,共6页
田静%宋月芹%冯敏超%金亚清%周晓龙
田靜%宋月芹%馮敏超%金亞清%週曉龍
전정%송월근%풍민초%금아청%주효룡
活化条件%铂%SO42%ZrO2-Al2O3%正己烷%异构化
活化條件%鉑%SO42%ZrO2-Al2O3%正己烷%異構化
활화조건%박%SO42%ZrO2-Al2O3%정기완%이구화
activation condition%Pt%SO42-/ZrO2-Al2O3%n-hexane%isomerization
采用浸渍法制备了Pt改性的Pt/SO42/ZrO2-Al2O3(PSZA)催化剂,考察了活化条件对PSZA催化剂正己烷异构化活性的影响,采用程序升温氧化(TPO-MS)、氮气-程序升温处理(TPN-MS)、程序升温还原(TPR-MS)对催化剂进行表征。异构化反应在连续流动的固定床微型反应器中进行。结果表明,200℃以上的高温氮气中活化预处理后的PSZA几乎没有异构化活性;空气气氛中、200~500℃高温条件下活化预处理的PSZA表现出了较高的异构化活性,正己烷初始转化率均在85%以上。在高于300℃的氢气中活化预处理,PSZA表现出较低的异构化活性。空气气氛中预处理除脱水之外,由于氧气的存在对催化剂的表面起到再氧化作用,导致高的异构化活性。氢气气氛中高温活化预处理导致了PSZA上硫物种的损失,进而引起异构化活性的下降。PSZA适宜的预处理条件为:空气气氛、300~500℃活化,250℃氢气中还原。
採用浸漬法製備瞭Pt改性的Pt/SO42/ZrO2-Al2O3(PSZA)催化劑,攷察瞭活化條件對PSZA催化劑正己烷異構化活性的影響,採用程序升溫氧化(TPO-MS)、氮氣-程序升溫處理(TPN-MS)、程序升溫還原(TPR-MS)對催化劑進行錶徵。異構化反應在連續流動的固定床微型反應器中進行。結果錶明,200℃以上的高溫氮氣中活化預處理後的PSZA幾乎沒有異構化活性;空氣氣氛中、200~500℃高溫條件下活化預處理的PSZA錶現齣瞭較高的異構化活性,正己烷初始轉化率均在85%以上。在高于300℃的氫氣中活化預處理,PSZA錶現齣較低的異構化活性。空氣氣氛中預處理除脫水之外,由于氧氣的存在對催化劑的錶麵起到再氧化作用,導緻高的異構化活性。氫氣氣氛中高溫活化預處理導緻瞭PSZA上硫物種的損失,進而引起異構化活性的下降。PSZA適宜的預處理條件為:空氣氣氛、300~500℃活化,250℃氫氣中還原。
채용침지법제비료Pt개성적Pt/SO42/ZrO2-Al2O3(PSZA)최화제,고찰료활화조건대PSZA최화제정기완이구화활성적영향,채용정서승온양화(TPO-MS)、담기-정서승온처리(TPN-MS)、정서승온환원(TPR-MS)대최화제진행표정。이구화반응재련속류동적고정상미형반응기중진행。결과표명,200℃이상적고온담기중활화예처리후적PSZA궤호몰유이구화활성;공기기분중、200~500℃고온조건하활화예처리적PSZA표현출료교고적이구화활성,정기완초시전화솔균재85%이상。재고우300℃적경기중활화예처리,PSZA표현출교저적이구화활성。공기기분중예처리제탈수지외,유우양기적존재대최화제적표면기도재양화작용,도치고적이구화활성。경기기분중고온활화예처리도치료PSZA상류물충적손실,진이인기이구화활성적하강。PSZA괄의적예처리조건위:공기기분、300~500℃활화,250℃경기중환원。
Pt/SO42-/ZrO2-Al2O3(PSZA) catalyst was prepared by impregnating SO42-/ZrO2-Al2O3with H2PtCl6.The effect of activation condition on n-hexane isomerization activity of PSZA catalyst was investigated.The catalyst was characterized by temperature-programmed oxidation(TPO-MS),temperature-programmed nitrogen treatment(TPN-MS) and temperature-programmed reduction(TPR-MS).The n-hexane isomerization activity of the catalyst was evaluated in a continuous flow fixed bed reactor.The experiment results showed that the conversion of n-hexane over PSZA was about 85% when it was activated in air at the temperature ranging from 200 ℃ to 500 ℃.However,the catalyst hardly possessed the isomerization activity when PSZA was activated in nitrogen at above 300 ℃.The reduction pretreatment at a high temperature above 300 ℃ led to the great decrease in catalytic activity.It was proposed that the role of activation in air at a high temperature was not only removal of water on the catalyst,but also re-oxidation of catalyst surface,which led to high catalytic activity.However,the pre-treatment in hydrogen gas at a high temperature led to the loss of sulfur species over PSZA,resulting in significant decrease in catalytic activity.The suitable activation condition was as follows:pretreatment in air at the temperature ranging from 300 ℃ to 500 ℃ and reduction in hydrogen gas at 250 ℃.