FAU分子筛催化γ-戊内酯脱羧制丁烯研究  

SELECTIVE PRODUCTION OF BUTENE FROM γ-VALEROLACTONE DECARBOXYLATION OVER FAU ZEOLITE

作　　者：乔堉锴 张新宝 李俊杰 于伟伟 安杰[1] 徐仕睿 朱向学[1] 徐龙伢[1] 李秀杰[1] Qiao Yukai;Zhang Xinbao;Li Junjie;Yu Weiwei;An Jie;Xu Shirui;Zhu Xiangxue;Xu Longya;Li Xiujie(Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,Liaoning 116023;University of Chinese Academy of Sciences;Fushun Dongke Fine Chemical Co.,Ltd.)

机构地区：[1]中国科学院大连化学物理研究所,辽宁大连116023 [2]中国科学院大学 [3]抚顺东科精细化工有限公司

出　　处：《石油炼制与化工》2024年第10期109-117,共9页Petroleum Processing and Petrochemicals

基　　金：国家自然科学基金资助项目(U20A20120,22172162,22372167);大连市重点领域创新团队项目(2020RT06)。

摘　　要：生物质基γ-戊内酯脱羧制备丁烯反应为碳四烯烃的可持续生产提供了一条新的途径。针对现有无定形SiO_(2)-Al_(2)O_(3)催化剂只能在低空速下运转的现状,开发了一种高效的NaY分子筛催化剂。因其丰富的Lewis酸与适宜的碱性,可在高空速下实现原料γ-戊内酯的100%转化,同时丁烯选择性高达99.6%。NaY分子筛催化剂显示出良好的反应稳定性和反应-再生循环性能,在连续运转1320 min后,丁烯收率保持在99.4%;经历5次反应-再生循环后,丁烯收率保持在99.2%。在此基础上,通过离子交换法制备LiY,KY,CaY分子筛,对比研究分子筛中金属阳离子种类对分子筛催化脱羧性能的影响。结果表明:NaY分子筛因其适宜的酸碱匹配度,脱羧性能最好;LiY分子筛和KY分子筛次之;CaY分子筛因存在强Br nsted酸位,催化性能最低。The decarboxylation of biomass-based γ-valerolactone(GVL)provides a new pathway for the sustainable production of butene.However,due to the low acidity of the commonly used amorphous SiO_(2)-Al_(2)O_(3) catalyst,this reaction could only be operated at low weight hourly space velocity(WHSV)condition,which limited its industrial scale-up.An efficient NaY catalyst was developed to address this challenge,which could achieve 100%GVL conversion and 99.6% butene selectivity at high WHSV.After 1320 minutes on stream,the yield of butene remained at 99.4%.In addition,the yield of butene remained at 99.2% after 5 cycles of regeneration.Furthermore,LiY,KY and CaY were prepared by ion exchange to investigate the effect of metal cations on catalytic performance.The results indicated that NaY showed the best performance due to its balanced acid and base sites,and CaY exhibited poor performance due to the existence of strong Br nsted acid sites.

关 键 词：γ-戊内酯 脱羧 丁烯 NAY分子筛 离子交换 生物质 

分 类 号：O643.36[理学—物理化学] TQ221.213[理学—化学]