焙烧温度对SO2-4/TiO2固体超强酸抗水稳定性的影响

李力成; 扈翟; 赵学娟; 钱祺; 王磊; 宋珊珊; 俞思凡; 严俊; 李小保

doi:10.3969/j.issn.1000-2006.2016.06.020

焙烧温度对SO^2-₄/TiO₂固体超强酸抗水稳定性的影响

李力成,扈翟,赵学娟,钱祺,王磊,宋珊珊,俞思凡,严俊,李小保

南京林业大学学报（自然科学版） ›› 2016, Vol. 40 ›› Issue (06) : 129-134.

PDF(1739711 KB)

国家林草科技领军期刊
中国精品科技期刊
中国高校百佳科技期刊
江苏省新闻出版政府奖期刊奖
RCCSE林学权威期刊（A+）
CSCD核心期刊
Scopus数据库收录期刊
中文核心期刊
SCD核心期刊

作者加群：102861116

微信公众号：南京林业大学学报

高级检索

PDF(1739711 KB)

南京林业大学学报（自然科学版） ›› 2016, Vol. 40 ›› Issue (06) : 129-134. DOI: 10.3969/j.issn.1000-2006.2016.06.020

研究论文

焙烧温度对SO^2-₄/TiO₂固体超强酸抗水稳定性的影响

李力成¹,扈翟¹,赵学娟²,钱祺¹,王磊¹,宋珊珊¹,俞思凡¹,严俊¹,李小保¹

作者信息 +

Influence of calcination temperature on the water-resistant stability of SO^2-₄/TiO₂ solid superacid

LI Licheng¹, HU Di¹, ZHAO Xuejuan², QIAN Qi¹, WANG Lei¹, SONG Shanshan¹, YU Sifan¹, YAN Jun¹, LI Xiaobao¹

Author information +

文章历史 +

摘要

通过水预处理方法对比研究了不同焙烧温度制备的SO^2-₄/TiO₂固体超强酸的抗水稳定性,借助XRD、NH₃-TPD、FT-IR、TG和BET等表征技术分析材料的结构特征。结果表明,当焙烧温度在500 ℃以下时,所制得的SO^2-₄/TiO₂固体超强酸具有相近的优异酯化性能; 当焙烧温度提升至600 ℃以上时,SO^2-₄/TiO₂的孔结构坍塌,SO^2-₄含量下降,酯化性能显著下降。经过水预处理后,所有固体超强酸酯化活性降低,主要与其SO^2-₄脱落和酸量明显减小有关。相比之下,400 ℃制备的SO^2-₄/TiO₂固体超强酸催化剂具有较好的稳定性。

Abstract

A water pretreatment method was used to evaluate the water-resistant stability of SO^2-₄/TiO₂ solid superacid prepared by calcination under different temperatures. The structural properties of samples were characterized by the X-ray diffraction(XRD), NH₃-TPD, fourier transform-infrared(FT-IR)spectroscopy, thermogravimetric(TG)analysis, and BET surface area analysis. The results showed that, when the calcination temperature did not exceed 500 ℃, the obtained SO^2-₄/TiO₂ solid superacid had similar esterification performances. However, the pore structure of solid superacid collapsed and its SO^2-₄ content decreased when the calcination temperature exceeded 600 ℃. In this case, the esterification performance of the solid superacid was poor. After the water pretreatment, the esterification performances of all solid superacids descended, which was mainly attributed to the removal of SO^2-₄ and the decrease of acid amount. In a comparison, SO^2-₄/TiO₂ solid superacid prepared at a calcination temperature of 400 ℃ had the optimum water-resistant stability.

引用本文

EndNote

Ris (Procite)

Bibtex

导出引用

李力成,扈翟,赵学娟,钱祺,王磊,宋珊珊,俞思凡,严俊,李小保. 焙烧温度对SO^2-₄/TiO₂固体超强酸抗水稳定性的影响[J]. 南京林业大学学报（自然科学版）. 2016, 40(06): 129-134 https://doi.org/10.3969/j.issn.1000-2006.2016.06.020

LI Licheng, HU Di, ZHAO Xuejuan, QIAN Qi, WANG Lei, SONG Shanshan, YU Sifan, YAN Jun, LI Xiaobao. Influence of calcination temperature on the water-resistant stability of SO^2-₄/TiO₂ solid superacid[J]. JOURNAL OF NANJING FORESTRY UNIVERSITY. 2016, 40(06): 129-134 https://doi.org/10.3969/j.issn.1000-2006.2016.06.020

中图分类号： TQ 032.4

参考文献

[1] 张盛明, 刘亮, 马艳丽, 等. SO^2-₄/ZrO₂固体超强酸催化碱木质素氢还原反应[J]. 林产化学与工业, 2014, 34(5): 15-21. Zhang S M, Liu L, Ma Y L, et al. Hydrogen reduction of straw alkali lignin catalyzed by solid superacid SO^2-₄/ZrO₂ [J]. Chemistry and Industry of Forest Products, 2014, 34(5): 15-21.
[2] 王琳, 谈继淮, 朱新宝. 固体酸催化剂在缩醛反应中的研究进展 [J]. 化学与黏合, 2014(5): 374-377. Wang L, Tan J H, Zhu X B. Progress in research on solid acid catalysts applied in acetalization [J]. Chemistry and Adhesion, 2014(5): 374-377.
[3] 马允. SO^2-₄/M_xO_y型固体超强酸催化剂的研究进展 [J]. 应用化工, 2014, 43(10): 1879-1883. Ma Y. Advances in SO^2-₄/M_xO_y solid superacid catalysts [J]. Applied Chemical Industry, 2014, 43(10): 1879-1883.
[4] 罗金岳, 倪传根, 王志国, 等. 固体超强酸SO^2-₄/ZrO₂催化α-蒎烯异构反应 [J]. 南京林业大学学报(自然科学版), 2004, 28(3):51-54. Doi:10.3969/j.issn.1000-2006.2004.03.013. Luo J Y, Ni C G, Wang Z G, et al. Study on α-pineneisomerization catalyzed by SO^2-₄/ZrO₂ solid superacid [J]. Journal of Nanjing Forestry University(Natural Sciences Editioin), 2004, 28(3):51-54.
[5] Reddy B M, Patil M K. Organic syntheses and transformations catalyzed by sulfated zirconia [J]. Chemical Reviews, 2009, 109(6): 2185-2208.Doi:10.1021/cr 90008m.
[6] Klose-Schubert B S, Jentoft R E, Jentoft F C. The balance between reactivity and stability of modified oxide surfaces illustrated by the behavior of sulfated zirconia catalysts [J]. Topics in Catalysis, 2011, 54(5): 398-414.Doi:10.1007/s11244-011-9670-5.
[7] Li X, Nagaoka K, Lercher J A. Labile sulfates as key components in active sulfated zirconia for n-butane isomerization at low temperatures [J]. Journal of Catalysis, 2004, 227(1): 130-137.Doi:10.1016/j.jcat.2004.07.003.
[8] Hua W, Xia Y, Yue Y, et al. Promoting effect of Al on SO^2-₄/M_xO_y(M= Zr, Ti, Fe)catalysts [J]. Journal of Catalysis, 2000, 196(1): 104-114.Doi:10.1006/jcat.2001.3032.
[9] 宋华, 杨东明, 李锋, 等. SO^2-₄/M_xO_y型固体超强酸催化剂的研究进展 [J]. 化工进展, 2007, 26(2): 145-151.Doi:10.3321/j.issn.1000-6613.2007.02.001. Song H, Yang D M, Li F, et al. Progress in SO^2-₄/M_xO_y solid superacid catalysts [J]. Chemical Industry and Engineering Progress, 2007, 26(2): 145-151.
[10] 钱祺, 王丹雅, 王磊, 等. 硫酸促进型固体超强酸在水预处理条件下的稳定性对比 [J]. 化工学报, 2015, 67(4): 1610-1617. Qian Q, Wang D Y, Wang L, et al. A comparison on the stability of the sulfated solid superacid with water pretreatment [J]. Ciesc Journal, 2015, 67(4): 1610-1617.
[11] 于荟, 朱银华, 刘畅, 等. 新型介孔SO^2-₄/TiO₂固体酸的制备及其催化酯化性能 [J]. 催化学报, 2009, 30(3): 265-271.Doi:10.3321/j.issn.0253-9837.2009.03.017. Yu H, Zhu Y H, Liu C, et al. Preparation of novel mesoporous SO^2-₄/TiO₂ solid acid catalyst and its catalytic activity for esterification [J]. Chinese Journal of Catalysis, 2009, 30(3): 265-271.
[12] 雷海琴, 朱春华, 陈家富, 等. SO^2-₄/TiO₂催化合成甲基丙烯酸甲氧基乙酯 [J]. 化学反应工程与工艺, 2010, 26(1): 19-23. Lei H Q, Zhu C H, Chen J F, et al. Synthesis of 2-methoxyethyl methaerylate catalyzed over SO^2-₄/TiO₂ [J]. Chemical Reaction Engineering and Technology, 2010, 26(1): 19-23.
[13] Li L, Wang Y, Shi K, et al. Preparation and characterization of mesoporous MoO₃/TiO₂ composite with high surface area by self-supporting and ammonia method [J]. Catalysis Letters, 2012, 142(4): 480-485.Doi:10.1007/s10562-012-0768-6.
[14] Zhang J, Li M, Feng Z, et al. UV Raman spectroscopic study on TiO₂. I. Phase transformation at the surface and in the bulk [J]. Journal of Physical Chemistry B, 2006, 110(2): 927-935.Doi:10.1021/jp0552473.
[15] Zhu C H, Guo M C, Zhu X B, et al. Probing the catalytic center of TiO₂/SO^2-₄solid superacid catalyst by X-band in situ high-temperature EPR spectroscopy[J]. Applied Megnetic Resonance, 2011, 42(3): 313-320.Doi:10.1007/s00723-011-0277-6.
[16] 陈建民, 缪长喜, 华伟明, 等. SO^2-₄/ZrO₂固体超强酸储存稳定性研究 [J]. 高等学校化学学报, 1996, 17(5): 797-799. Chen J M, Miao C X, Hua W M, et al. Studies on the storage stability of ZrO₂ solid superacid [J]. Chemical Research in Chinese Universities, 1996, 17(5): 797-799.
[17] Babou F, Coudurier G, Vedrine J C. Acidic properties of sulfated zirconia: an infrared spectroscopic study [J]. Journal of Catalysis, 1995, 152(2): 341-349.Doi:10.1006/jcat.1995.1088.
[18] Li L, Zhu Y, Lu X, et al. Carbon heterogeneous surface modification on a mesoporous TiO₂-supported catalyst and its enhanced hydrodesulfurization performance [J]. Chemical Communications, 2012, 48(94): 11525-11527.Doi:10.1039/c2cc36157d.
[19] 蒋平平, 卢冠忠. 固体超强酸催化剂改性研究进展 [J]. 现代化工, 2002, 22(7): 13-17. Jiang P P, Lu G Z. Advances in modif ication of solid superacid catalysts [J]. Modern Chemical Industry, 2002, 22(7): 13-17.
[20] Fu B, Gao L, Niu L, et al. Biodiesel from waste cooking oil via heterogeneous superacid catalyst SO^2-₄/ZrO₂ [J]. Energy & Fuels, 2008, 23(1): 569-572.Doi:10.1021/ef800751z.

基金

基金项目:国家自然科学基金项目(21406118,91434109,91334202); 南京林业大学人才启动基金项目(GXL2014036); 江苏省双创计划,科技副总(企业创新岗)特聘专家项目; 南京林业大学大学生创新训练计划项目(2015sjcx032); 江苏高校优势学科建设工程资助项目(PAPD)
第一作者:李力成(llc0024@yahoo.com),讲师,博士。
引文格式:李力成,扈翟,赵学娟,等. 焙烧温度对SO^2-₄/TiO₂固体超强酸抗水稳定性的影响[J]. 南京林业大学学报(自然科学版),2016,40(6):129-134.