Catalytic conversion of biomass derivative γ-valerolactone to aromatics over Zn/ZSM-5 catalyst
-
摘要: 应用浸渍法在ZSM-5沸石分子筛孔道中引入过渡金属Zn物种,制备了具有不同Zn含量的Zn/ZSM-5。考察了反应温度、催化剂用量、催化剂的酸性性质等条件对γ-戊内酯芳构化产物组成(气、液、固产物)及其液体成分含量的影响。实验结果表明,ZSM-5分子筛孔道中引入Zn后,可以有效改变液体产物成分以及影响气体和固体产物收率。当ZSM-5分子筛孔道中引入Zn物种后,能够明显提高液体产物中苯、甲苯、乙苯、萘等芳香类化合物的含量,表明Zn物种能促进γ-戊内酯芳构化反应的进行。Abstract: Zn/ZSM-5 zeolite catalysts with different Zn contents were prepared by impregnating method. The influence of reaction temperature, reaction time, catalyst dosage, and the acidic properties of catalysts on the conversion of γ-valerolactone to aromatic compounds was investigated.The results show that the introduction of Zn into H-ZSM-5 channel could effective modify the components of liquid product and influence the yields of gas, liquid, and solid as compared to H-ZSM-5 catalyst and non-catalytic conversion of γ-valerolactone. Zn/ZSM-5 catalyst affords the higher contents of aromatic compound compared to H-ZSM-5 and silica catalysts in the liquid product under identical reaction conditions. Therefore, Zn species of Zn/ZSM-5 can not only effectively improve the conversion of γ-valerolactone, but also enhance the formation of aromatic compounds, suggesting that Zn species play a very key role in the formation of these aromatic compounds.
-
Key words:
- γ-valerolactone /
- aromatization /
- Zn/ZSM-5 /
- Zn species
-
蒋剑春. 生物质热化学转化制液体燃料的研究进展[J]. 生物质化学工程, 2007, 41(5): 45-51.(JIANG Jian-chun. Research progress on thermo-chemical conversion of biomass into liquid fuels in China[J]. Biomass Chem Eng, 2007, 41(5): 45-51.) 蒋剑春. 生物质能源应用研究现状与发展前景[J]. 林产化学与工业, 2002, 22(2): 75-80.(JIANG Jian-chun. Research progress and development prospect of biomass energy[J]. Chem Ind For Prod, 2002, 22(2): 75-80.) 郑志锋, 蒋剑春, 戴伟娣, 孙云娟. 生物质能源转化技术与应用[J]. 生物质化学工程, 2007, 41(5): 67-77.(ZHENG Zhi-feng, JIANG Jian-chun, DAI Wei-di, SUN Yun-juan. Conversion technology and utilization of biomass energy[J]. Biomass Chem Eng, 2007, 41(5): 67-77.) 李海滨, 袁振宏, 马骁茜. 现代生物质能利用技术[M] . 北京: 化学工业出版社, 2012, 330-331.(LI Hai-bing, YUAN Zhen-hong, MA Xiao-qian. Utilization technology of modern biomass energy[M]. Beijing: Chemical Industry Press, 2012, 330-331.) 龙向东, 李泽龙, 高广, 夏春谷, 李福伟. 乙酰丙酸催化加氢制备γ -戊内酯的研究进展[J]. 分子催化, 2014, 28(4): 384-392.(LONG Xiang-dong, LI Ze-long, GAO Guang, XIA Chun-gu, LI Fu-wei. Research progress of hydrogenation of levulinic acid into γ-valerolactone[J]. J Mol Catal, 2014, 28(4): 384-392.) ZHAO Y, FU Y, GUO Q X. Production of aromatic hydrocarbons through catalytic pyrolysis of γ-valerolactone from biomass[J]. Bioresour Technol, 2012, 114: 740-744. 张建伟, 樊金龙, 吴卫泽. 乙酰丙酸加氢生成γ-戊内酯的反应动力学[J]. 北京化工大学学报(自然科学版), 2010, 37(5): 25-29.(ZHANG Jian-wei, FAN Jin-long, WU Wei-ze. The reaction kinetic of hydrogenation of levulinic acid into γ-valerolactone[J]. J Beijing Univ Chem Technol (Nat Sci), 2010, 37(5): 25-29.) WILLIAM R H, PALKOVITS R. Development of heterogeneous catalysts for the conversion of levulinic acid to γ-valerolactone[J]. ChemSusChem, 2012, 5(9): 1567-1577. BOND J Q, ALONSO D M, WANG D, WEST R M, DUMESIC J A. Integrated catalytic conversion of γ-valerolactone to liquid alkenes for transportation fuels[J]. Science, 2010, 327(5969): 1110-1114. CHENG Y T, JAE J, SHI J, FAN W, HUBER G W. Production of renewable aromatic compounds by catalytic fast pyrolysis of lignocellulosic biomass with bifunctional Ga/ZSM-5 catalysts[J]. Angew Chem Int Ed, 2012, 51(6): 1387-1390. SAMI M T, BRAHIM M, PIETER C M, MAGUSIN M, PIDKO E A, HENSEN E J M. Structure and reactivity of Zn-modified ZSM-5 zeolites: The importance of clustered cationic Zn complexes[J]. ACS Catal, 2012, 2(1): 71-83. YU L, HUANG S, ZHANG S, LIU Z, XIN W, XIE S, XU L. Transformation of isobutyl alcohol to aromatics over zeolite-based catalysts[J]. ACS Catal, 2012, 2(6): 1203-1210. 夏海岸, 王秀聪, 徐然然, 吴品, 吴义珠, 杨莉, 左宋林. 分子筛基Brønsted 酸和路易斯酸性位对纤维素热解行为的影响[J]. 林产化学与工业, 2013, 33(6): 29-36.(XIA Hai-an, WANG Xiu-chong, XU Ran-ran, WU Pin, WU Yi-zhu, YANG Li, ZUO Song-lin, Influence of Brønsted and lewis acid sites on pyrolytic behaviors of cellulose over zeolite-based catalysts[J]. Chem Ind For Prod, 2013, 33(6): 29-36.) XIA H, SUN K, FENG Z, LI C. The inhibiting effect of H2O on N2O decomposition over the bi-nuclear Fe sites in Fe/ZSM-5[J]. J Phys Chem C, 2011, 115(2): 542-548. XIA H, SUN K, LIU Z, FENG Z, YING P, LI C. The promotional effect of NO on N2O decomposition over the bi-nuclear Fe sites in Fe/ZSM-5[J]. J Catal, 2010, 270(1): 103-109.
点击查看大图
计量
- 文章访问数: 400
- HTML全文浏览量: 26
- PDF下载量: 351
- 被引次数: 0