Citation: LIANG Li-Ping, ZHU Qing, ZHAO Yong-Xiang, LIU Dian-Sheng. Effects of Heat Treatment on the Structure and Properties of the Tungstophosphoric Acid-Modified Zirconia Aerogel Solid Acids[J]. Acta Physico-Chimica Sinica, ;2011, 27(08): 1933-1940. doi: 10.3866/PKU.WHXB20110829 shu

Effects of Heat Treatment on the Structure and Properties of the Tungstophosphoric Acid-Modified Zirconia Aerogel Solid Acids

1.
1. Engineering Research Center for Fine Chemicals of Ministry of Education, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, P. R. China;
2. School of Materials Science and Engineering, Taiyuan University of Science and Technology, Taiyuan 030024, P. R. China

Received Date: 30 January 2011
Available Online: 24 June 2011
Fund Project: 山西省科技攻关计划项目(20090321059) (20090321059)山西省发改委产业技术开发项目(2009164)资助 (2009164)

Based on detailed experimental results, the effects of heat treatment on the structure, acidity, and catalytic performance of the 12-tungstophosphoric acid (TPA) modified zirconia aerogel (ZA) (TPZA) solid acids were investigated. TPZA samples, with TPA mass fraction of 25% and heat-treated at 120- 750 °C, were characterized by N₂ physical adsorption, X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, FTIR spectroscopy of adsorbed pyridine (Py-FTIR), and temperature programmed desorption of NH₃ (NH₃-TPD). And they were used as catalysts in the polymerization of tetrahydrofuran (THF). The results show that, although the heat treatment might greatly influence both the surface density and type of tungsten species, the TPZA materials with the TPA loading of 25% could acquire suitable Brönsted and Lewis acidity and accordingly acceptable catalytic activities over the wide temperature ranges of 120-300 °C and 550-750 °C. In the TPZA samples treated at 120-300 °C, the presence of Brönsted acid sites can be associated with the presence of highly dispersed and somewhat distorted but intact Keggin-anions, whereas the Brönsted acid sites in the samples treated at 550-750 °C might originate from the zirconia-anchored, highly polymerized tungstate surface species. Moreover, all the samples show obvious Lewis acidity, which is associated with the presence of coordinatively unsaturated Zr⁴⁺ and phosphorous oxide produced by the decomposition of TPA.
- Zirconia aerogel,
- Tungstophosphoric acid,
- Polytungstate,
- Tetrahydrofuran,
- Polymerization
1. [1]
  
  (1) Rafiee, E.; Joshaghani, M.; Tork, F.; Fakhri, A.; Eavani, S. J. Mol. Catal. A-Chem. 2008, 283, 1.
2. [2]
  (2) Guo,Y.; Li, K.; Yu, X.; Clark, J. H. Appl. Catal. B-Environ. 2008, 81, 182.
3. [3]
  (3) Kumbar, S. M.; Shanbhag, G. V.; Lefebvre, F.; Halligudi, S. B. J. Mol. Catal. A-Gen. 2006, 256, 324.
4. [4]
  (4) Bachiller-Baeza, B.; Anderson, J. A. J. Catal. 2004, 228, 225.
5. [5]
  (5) Yadav, G. D.; Pimparkar, K. P. J. Mol. Catal. A-Chem. 2007, 264, 179.
6. [6]
  (6) Obal?, Z.; Do?u, T. Chem. Eng. J. 2008, 138, 548.
7. [7]
  (7) Bhatt, N.; Patel, A. Catal. Lett. 2007, 113 (3-4), 99.
8. [8]
  (8) Bhatt, N.; Patel, A. J. Mol. Catal. A-Chem. 2007, 264, 214.
9. [9]
  (9) Bhatt, N.; Sharma, P.; Patel, A.; Selvam, P. Catal. Commun. 2008, 9, 1545.
10. [10]
  (10) Sharma, P.; Patel, A. Appl. Surf. Sci. 2009, 255, 7635.
11. [11]
  (11) Parida, K. M.; Mallick, S. J. Mol. Catal. A-Chem. 2007, 275, 77.
12. [12]
  (12) Parida, K. M.; Mallick, S.; Pradhan, G. C. J. Mol. Catal. AChem. 2009, 297, 93.
13. [13]
  (13) Devassy, B. M.; Halligudi, S. B. J. Catal. 2005, 236, 313.
14. [14]
  (14) Devassy, B. M.; Lefebvre, F.; Halligudi, S. B. J. Catal. 2005, 231, 1.
15. [15]
  (15) Sawant, D. P.; Vinu, A.; Jacob, N. E.; Lefebvre, F.; Halligudi, S. B. J. Catal. 2005, 235, 341.
16. [16]
  (16) Devassy, B. M.; Halligudi, S. B. J. Mol. Catal. A-Chem. 2006, 253, 8.
17. [17]
  (17) Sunita, G.; Devassy, B. M.; Vinu, A.; Sawant, D. P.; Balasubramanian, V. V.; Halligudi, S. B. Catal. Commun. 2008, 9, 696.
18. [18]
  (18) Lucas, N.; Bordoloi, A.; Amrute, A. P.; Kasinathan, P.; Vinu, A.; Bohringer,W.; Fletcher, J. C. Q.; Halligudi, S. B. Appl. Catal. A-Gen. 2009, 352, 74.
19. [19]
  (19) López-Salinas, E.; Hernández-Cortéz, J. G.; Schifter, I.; Torres- García, E.; Navarrete, J.; Gutiérrez-Carrillo, A.; López, T.; Lottici, P. P.; Bersani, D. Appl. Catal. A-Gen. 2000, 193, 215.
20. [20]
  (20) Liang, L. P.; Dang, S.;Wu, D.; Sun, Y. H. J. Mater. Sci. Technol. 2004, 20, 435.
21. [21]
  (21) Zhao, M.; Jia, Z. Q.; Zhao, L. L.; Sun, Z. J.; Liu, X.W.;Wang, P. F.; Gao, C. G. J. Mol. Catal. 2010, 24, 117. [赵敏, 贾志奇, 赵丽丽, 孙自瑾, 刘新文, 王鹏飞, 高春光, 赵永祥. 分子催化, 2010, 24, 117.]
22. [22]
  (22) Wachs, I. E.; Kim, T.; Ross, E. I. Catal. Today 2006, 116, 162.
23. [23]
  (23) Damyanova, S.; Fierro, J. L. G.; Sobrados, I.; Sanz, J. Langmuir 1999, 15, 469.
24. [24]
  (24) Zhu, Q.; Liang, L. P.; Jia, Z. Q.; Gao, C. G.; Zhao, Y. X. Acta Phys. -Chim. Sin. 2011, 27, 491. [朱晴, 梁丽萍, 贾志奇, 高春光, 赵永祥. 物理化学学报, 2011, 27, 491.]
25. [25]
  (25) Onfroy, T.; Clet, G.; Houalla, M. J. Phys. Chem. B 2005, 109, 3345.
26. [26]
  (26) Cortés-Jácome, M. A.; Toledo, J. A.; Angeles-Chavez, C.; Aguilar, M.;Wang, J. A. J. Phys. Chem. B 2005, 109, 22730.
27. [27]
  (27) Lebarbier, V.; Clet, G.; Houalla, M. J. Phys. Chem. B 2006, 110, 13905.
28. [28]
  (28) López, D. E.; Suwannakarn, K.; Bruce, D. A.; odwin J. G. Jr., J. Catal. 2007, 247, 43.
29. [29]
  (29) Reddy, B. M.; Patil, M. K.; Reddy, G. K.; Reddy, B. T.; Rao, K. N. Appl. Catal. A-Gen. 2007, 332, 183.
30. [30]
  (30) Kozhevnikov, I. V. Catalysis by Polyoxometalates (Catalysis for Fine Chemical Synthesis); Chemical Industry Press: Beijing, 2005; pp 17-20; Translated by Tang, P. K., li, X. G.,Wang, S. R. [Kozhevnikov, I. V. 精细化学品的合成: 多酸化合物及其催化. 唐培堃, 李祥高, 王世荣, 译. 北京: 化学工业出版社, 2005: 17-20.]
31. [31]
  (31) Xia, Q. H.; Hidajat, K; Kawi, S. J. Catal. 2002, 205, 318.
1. [1]
  Laiying Zhang , Yinghuan Wu , Yazi Yu , Yecheng Xu , Haojie Zhang , Weitai Wu . Innovation and Practice of Polymer Chemistry Experiment Teaching for Non-Polymer Major Students of Chemistry: Taking the Synthesis, Solution Property, Optical Performance and Application of Thermo-Sensitive Polymers as an Example. University Chemistry, 2024, 39(4): 213-220. doi: 10.3866/PKU.DXHX202310126
2. [2]
  Peiyu Zhang , Aixin Song , Jingcheng Hao , Jiwei Cui . 高频超声法制备聚多巴胺薄膜综合实验. University Chemistry, 2025, 40(6): 210-214. doi: 10.12461/PKU.DXHX202407081
3. [3]
  Zhengyu Zhou , Huiqin Yao , Youlin Wu , Teng Li , Noritatsu Tsubaki , Zhiliang Jin . Synergistic Effect of Cu-Graphdiyne/Transition Bimetallic Tungstate Formed S-Scheme Heterojunction for Enhanced Photocatalytic Hydrogen Evolution. Acta Physico-Chimica Sinica, 2024, 40(10): 2312010-0. doi: 10.3866/PKU.WHXB202312010
4. [4]
  Ran Yu , Chen Hu , Ruili Guo , Ruonan Liu , Lixing Xia , Cenyu Yang , Jianglan Shui . Catalytic Effect of H₃PW₁₂O₄₀ on Hydrogen Storage of MgH₂. Acta Physico-Chimica Sinica, 2025, 41(1): 100001-0. doi: 10.3866/PKU.WHXB202308032
5. [5]
  Jianan Hong , Chenyu Xu , Yan Liu , Changqi Li , Menglin Wang , Yanwei Zhang . Decoding the interfacial competition between hydrogen evolution and CO₂ reduction via edge-active-site modulation in photothermal catalysis. Acta Physico-Chimica Sinica, 2025, 41(9): 100099-0. doi: 10.1016/j.actphy.2025.100099
6. [6]
  Ke Qiu , Fengmei Wang , Mochou Liao , Kerun Zhu , Jiawei Chen , Wei Zhang , Yongyao Xia , Xiaoli Dong , Fei Wang . A Fumed SiO₂-based Composite Hydrogel Polymer Electrolyte for Near-Neutral Zinc-Air Batteries. Acta Physico-Chimica Sinica, 2024, 40(3): 2304036-0. doi: 10.3866/PKU.WHXB202304036
7. [7]
  Xiao SANG , Qi LIU , Jianping LANG . Synthesis, structure, and fluorescence properties of Zn(Ⅱ) coordination polymers containing tetra-alkenylpyridine ligands. Chinese Journal of Inorganic Chemistry, 2024, 40(11): 2124-2132. doi: 10.11862/CJIC.20240158
8. [8]
  Zijian Zhao , Yanxin Shi , Shicheng Li , Wenhong Ruan , Fang Zhu , Jijun Jiang . A New Exploration of the Preparation of Polyacrylic Acid by Free Radical Polymerization Based on the Concept of Green Chemistry. University Chemistry, 2024, 39(5): 315-324. doi: 10.3866/PKU.DXHX202311094
9. [9]
  Ruiying WANG , Hui WANG , Fenglan CHAI , Zhinan ZUO , Benlai WU . Three-dimensional homochiral Eu(Ⅲ) coordination polymer and its amino acid configuration recognition. Chinese Journal of Inorganic Chemistry, 2025, 41(5): 877-884. doi: 10.11862/CJIC.20250052
10. [10]
  Zizheng LU , Wanyi SU , Qin SHI , Honghui PAN , Chuanqi ZHAO , Chengfeng HUANG , Jinguo PENG . Surface state behavior of W doped BiVO₄ photoanode for ciprofloxacin degradation. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 591-600. doi: 10.11862/CJIC.20230225
11. [11]
  Junjie Zhang , Yue Wang , Qiuhan Wu , Ruquan Shen , Han Liu , Xinhua Duan . Preparation and Selective Separation of Lightweight Magnetic Molecularly Imprinted Polymers for Trace Tetracycline Detection in Milk. University Chemistry, 2024, 39(5): 251-257. doi: 10.3866/PKU.DXHX202311084
12. [12]
  Fanpeng Meng , Fei Zhao , Jingkai Lin , Jinsheng Zhao , Huayang Zhang , Shaobin Wang . Optimizing interfacial electric fields in carbon nitride nanosheet/spherical conjugated polymer S-scheme heterojunction for hydrogen evolution. Acta Physico-Chimica Sinica, 2025, 41(8): 100095-0. doi: 10.1016/j.actphy.2025.100095
13. [13]
  Bo YANG , Gongxuan LÜ , Jiantai MA . Nickel phosphide modified phosphorus doped gallium oxide for visible light photocatalytic water splitting to hydrogen. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 736-750. doi: 10.11862/CJIC.20230346
14. [14]
  Yongzhi LI , Han ZHANG , Gangding WANG , Yanwei SUI , Lei HOU , Yaoyu WANG . A two-dimensional metal-organic framework for the determination of nitrofurantoin and nitrofurazone in aqueous solution. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 245-253. doi: 10.11862/CJIC.20240307
15. [15]
  Xiaoli Sun , Xiang Wu , Li Gan , Wenming Wan . Barbier Polymerization: A New Teaching Case for Step-Growth Polymerization. University Chemistry, 2025, 40(4): 113-118. doi: 10.12461/PKU.DXHX202406102
16. [16]
  Xiaoning TANG , Shu XIA , Jie LEI , Xingfu YANG , Qiuyang LUO , Junnan LIU , An XUE . Fluorine-doped MnO₂ with oxygen vacancy for stabilizing Zn-ion batteries. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1671-1678. doi: 10.11862/CJIC.20240149
17. [17]
  Qiang Zhang , Yuanbiao Huang , Rong Cao . Imidazolium-Based Materials for CO₂ Electroreduction. Acta Physico-Chimica Sinica, 2024, 40(4): 2306040-0. doi: 10.3866/PKU.WHXB202306040
18. [18]
  Yanhui Guo , Li Wei , Zhonglin Wen , Chaorong Qi , Huanfeng Jiang . Recent Progress on Conversion of Carbon Dioxide into Carbamates. Acta Physico-Chimica Sinica, 2024, 40(4): 2307004-0. doi: 10.3866/PKU.WHXB202307004
19. [19]
  Zhiquan Zhang , Baker Rhimi , Zheyang Liu , Min Zhou , Guowei Deng , Wei Wei , Liang Mao , Huaming Li , Zhifeng Jiang . Insights into the Development of Copper-Based Photocatalysts for CO₂ Conversion. Acta Physico-Chimica Sinica, 2024, 40(12): 2406029-0. doi: 10.3866/PKU.WHXB202406029
20. [20]
  Hailang JIA , Pengcheng JI , Hongcheng LI . Preparation and performance of nickel doped ruthenium dioxide electrocatalyst for oxygen evolution. Chinese Journal of Inorganic Chemistry, 2025, 41(8): 1632-1640. doi: 10.11862/CJIC.20240398

Get Citation

PDF

XML

Metrics

PDF Downloads(973)
Abstract views(2576)
HTML views(22)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142