Citation: CHEN Ao-Ang, XU Xiang-Sheng, HUA Yan-Xiang, GU Hui-Zi, YAN Xin-Huan. Fe3O4 Modified Alumina Supported Ruthenium Catalyst for Novel In-situ Liquid Phase Catalytic Hydrogenation[J]. Acta Physico-Chimica Sinica doi: 10.3866/PKU.WHXB201302052 shu

Fe3O4 Modified Alumina Supported Ruthenium Catalyst for Novel In-situ Liquid Phase Catalytic Hydrogenation

1.
State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology, Zhejiang University of Technology, Hangzhou 310014, P. R. China

Received Date: 18 December 2012
Available Online: 5 February 2013
Fund Project: 国家自然科学基金(20676124, 21076197) (20676124, 21076197) 浙江省自然科学基金(Y4090440) (Y4090440)浙江省钱江人才项目(2010R10038)资助 (2010R10038)

Ru-Fe₃O₄/γ-Al₂O₃ was synthesized by stepwise impregnation method and applied to the in-situ liquid phase selective hydrogenation of 3,4-dichloronitrobenzene (3,4-DCNB). The nanoparticle size and distribution, metallic crystalline constitution, surface structure parameters, and adsorption species were systematically characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, N₂ adsorption-desorption (BET), and X-ray photoelectron spectroscopy (XPS). The Ru-Fe₃O₄/γ-Al₂O₃ catalyst was investigated using the in-situ liquid phase hydrogenation of 3,4-DCNB as probe reaction, the effect of different reaction conditions and different synthetic factors on the catalytic properties was studied. Experimental results showed that the catalytic properties of the Ru-Fe₃O₄/γ-Al₂O₃ catalyst were significantly influenced by its Fe₃O₄ content, under the optimum condition of 473 K, 3.0 MPa, 2% (w) 3,4-DCNB concentration with 75% ethanol and 25% water, the Ru-Fe₃O₄/γ-Al₂O₃ catalyst with Ru and Fe mass fractions of 2% and 6% exhibited the highest activity and stability, with 100% conversion of 3,4-DCNB, 96.4% selectivity of 3,4-dichloroaniline (3,4-DCAN), and this catalyst could be stabilized for more than 200 h. The main reason for the deactivation of the catalyst is CO coverage on active centers, and the poisoning-deactivated catalysts were regenerated by water-gasshift (WGS) reaction and Fischer-Tropsch synthesis (FTS), which employ Fe₃O₄ modified Ru/Al₂O₃ as catalyst due to its high efficiency of CO transformation. Carbon deposition on the catalyst surface is the reason second only to carbon monoxide poisoning, and this could be removed through calcination. Crystalline phase change and nanoparticles aggregation may cause partial deactivation, and investigation of the mechanism and catalyst regeneration are in progress.
- Ruthenium,
- Iron oxide,
- Catalytic stability,
- 3,4-Dichloronitrobenzene,
- In-situ liquid phase hydrogenation,
- CO poisoning deactivation
1. [1]
  
  (1) Hao, Y. Z.; Li, Z. X.; Tian, J. L. J. Mol. Catal. A-Chem. 2007,265, 258. doi: 10.1016/j.molcata.2006.09.045
2. [2]
  (2) Ma, L.; Chen, S.; Lu, C. S.; Zhang, Q. F.; Li, X. N. Catal.Today 2011, 173, 62. doi: 10.1016/j.cattod.2011.06.011
3. [3]
  (3) Zhou, L.; Gu, H. Z.; Yan, X. H. Catal. Lett. 2009, 132, 16. doi: 10.1007/s10562-009-0036-6
4. [4]
  (4) Jiang, L.; Zhu, Y. F.; Xiang, Y. Z.; Li, X. N. Chin. J. Catal.2007, 28, 281. [姜莉, 祝一锋, 项益智, 李小年. 催化学报,2007, 28, 281.]
5. [5]
  (5) Yang, F.; Xu, X. S.; Gu, H. Z.; Chen, A. A.; Yan, X. H. ActaPhys. -Chim. Sin. 2012, 28, 2141. [杨芳, 许响生, 顾辉子,陈傲昂, 严新焕. 物理化学学报, 2012, 28, 2141.] doi: 10.3866/PKU.WHXB201206201
6. [6]
  (6) Fang, Y. B.; Yan, X. H.; Sun, J. Q.; Xu, Z. Y.;Wang,W. J. Chin.J. Catal. 2005, 26, 233. [房永彬, 严新焕, 孙军庆, 徐振元,王文静. 催化学报, 2005, 26, 233.]
7. [7]
  (7) Han, X. X.; Zhou, R. X.; Lai, G. H.; Zheng, X. M. React. Kinet.Catal. 2004, 83, 51.
8. [8]
  (8) Kratky, V.; Kralik, M.; Mecarova, M.; Stolcova, M.; Zalibera,L.; Hronec, M. Appl. Catal. A-Gen. 2002, 235, 225. doi: 10.1016/S0926-860X(02)00274-0
9. [9]
  (9) Tijani, A.; Coq, B.; Figueras, F. Appl. Catal. 1991, 76, 255. doi: 10.1016/0166-9834(91)80051-W
10. [10]
  (10) Yan, X.; Liu, M. H.; Liu, H. F.; Liew, K. Y. J. Mol. Catal.A-Chem. 2001, 170, 223. doi: 10.1016/S1381-1169(01)00067-X
11. [11]
  (11) Tu,W. X.; Liu, H. F.; Tang, Y. J. Mol. Catal. A. 2000, 159, 115.doi: 10.1016/S1381-1169(00)00179-5
12. [12]
  (12) Zhang, J. L.;Wang, Y.; Ji, H.;Wei, Y. G.;Wu, N. Z.; Zuo, B. J.;Wang, Q. L. J. Catal. 2005, 229, 114. doi: 10.1016/j.jcat.2004.09.029
13. [13]
  (13) Li, X. N.; Xiang, Y. Z. Sci. China Ser. B 2007, 50, 746. doi: 10.1007/s11426-007-0040-x
14. [14]
  (14) Liu, L. Q.; Qiao, B. T.; Chen, Z. J.; Zhang, J.; Deng, Y. Q.Chem. Commun. 2009, 653.
15. [15]
  (15) Fatsikostas, A. N.; Kondarides, D. I.; Verykios, X. E. Catal.Today 2002, 75, 145. doi: 10.1016/S0920-5861(02)00057-3
16. [16]
  (16) Deluga, G. A.; Salge, J. R.; Schmidt, L. D.; Verykios, X. E.Science 2004, 303, 993. doi: 10.1126/science.1093045
17. [17]
  (17) Cortright, R. D.; Davda, R. R.; Dumesic, J. A. Nature 2002,418, 964. doi: 10.1038/nature01009
18. [18]
  (18) Li, T. Z.; Yang, Y.; Tao, Z. C.; Zhang, C. H.; Xiang, H.W.; Li, Y.W. Fuel Process Technol. 2009, 90, 1247. doi: 10.1016/j.fuproc.2009.06.006
19. [19]
  (19) Hao, Q. L.; Bai, L.; Xiang, H.W.; Li, Y.W. Chin. J. Catal.2008, 29, 969. [郝庆兰, 白亮, 相宏伟, 李永旺. 催化学报,2008, 29, 969.]
20. [20]
  (20) Wan, H. J.;Wu, B. S.; Li, T. Z.; Tao, Z. C. J. Fuel Chem.Technol. 2007, 35, 589. doi: 10.1016/S1872-5813(07)60036-X
21. [21]
  (21) Emiel, D. S.; Andrew, M. B.; Sergey, N.;Weckhuysen, B. M.J. Catal. 2009, 262, 244. doi: 10.1016/j.jcat.2008.12.021
22. [22]
  (22) Yan, X. H.; Sun, J. Q.;Wang, Y.W.; Yang, J. F. J. Mol. Catal.A-Chem. 2006, 252, 17. doi: 10.1016/j.molcata.2006.01.060
23. [23]
  (23) Zhao, S. L.; Liang, H. D.; Zhou, Y. F. Catal. Commun. 2007, 8,1305. doi: 10.1016/j.catcom.2006.11.033
24. [24]
  (24) Xu, H. Z.; Shi, J. H.;Wang, L. S.; Lü, L. X. Chin. J. Catal.1993, 14, 251. [徐慧珍, 施介华, 王利盛, 吕丽昕. 催化学报,1993, 14, 251.]
25. [25]
  (25) Chen, Y. F.; Xu, H. Z.; Xu,W. L. J. Zhejiang Agric. Univ. 1998,24, 255. [陈幼芳, 徐慧珍, 徐伟亮. 浙江农业大学学报,1998, 24, 255.]
26. [26]
  (26) Hilaire, S.;Wang, X.; Luo, T.; rte, R. J.;Wagner, J. Appl.Catal. A-Gen. 2001, 215, 271. doi: 10.1016/S0926-860X(01)00535-X
27. [27]
  (27) Farrauto, R. J.; Liu, Y.; Ruettinger,W.; llinich, O.; Shore, L.;Giroux, T. Catal. Rev. 2007, 49, 141. doi: 10.1080/01614940701220496
28. [28]
  (28) Trimm, D. L. Appl. Catal. A-Gen. 2005, 296, 1. doi: 10.1016/j.apcata.2005.07.011
29. [29]
  (29) Rosso, I.; Galletti, C.; Saracco, G.; Garrone, E.; Specchia, V.Appl. Catal. B 2004, 48, 195. doi: 10.1016/j.apcatb.2003.10.016
1. [1]
  Wenlong LI , Xinyu JIA , Jie LING , Mengdan MA , Anning ZHOU . Photothermal catalytic CO₂ hydrogenation over a Mg-doped In₂O_3-x catalyst. Chinese Journal of Inorganic Chemistry, doi: 10.11862/CJIC.20230421
2. [2]
  Hailian Tang , Siyuan Chen , Qiaoyun Liu , Guoyi Bai , Botao Qiao , Fei Liu . Stabilized Rh/hydroxyapatite Catalyst for Furfuryl Alcohol Hydrogenation: Application of Oxidative Strong Metal-Support Interactions in Reducing Conditions. Acta Physico-Chimica Sinica, doi: 10.3866/PKU.WHXB202408004
3. [3]
  Wen YANG , Didi WANG , Ziyi HUANG , Yaping ZHOU , Yanyan FENG . La promoted hydrotalcite derived Ni-based catalysts: In situ preparation and CO₂ methanation performance. Chinese Journal of Inorganic Chemistry, doi: 10.11862/CJIC.20230276
4. [4]
  Xiuyun Wang , Jiashuo Cheng , Yiming Wang , Haoyu Wu , Yan Su , Yuzhuo Gao , Xiaoyu Liu , Mingyu Zhao , Chunyan Wang , Miao Cui , Wenfeng Jiang . Improvement of Sodium Ferric Ethylenediaminetetraacetate (NaFeEDTA) Iron Supplement Preparation Experiment. University Chemistry, doi: 10.3866/PKU.DXHX202308067
5. [5]
  Lina Guo , Ruizhe Li , Chuang Sun , Xiaoli Luo , Yiqiu Shi , Hong Yuan , Shuxin Ouyang , Tierui Zhang . 层状双金属氢氧化物的层间阴离子对衍生的Ni-Al₂O₃催化剂光热催化CO₂甲烷化反应的影响. Acta Physico-Chimica Sinica, doi: 10.3866/PKU.WHXB202309002
6. [6]
  Ke QIAO , Yanlin LI , Shengli HUANG , Guoyu YANG . Advancements in asymmetric catalysis employing chiral iridium (ruthenium) complexes. Chinese Journal of Inorganic Chemistry, doi: 10.11862/CJIC.20240265
7. [7]
  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, doi: 10.3866/PKU.WHXB202406029
8. [8]
  Jiaxi Xu , Yuan Ma . Influence of Hyperconjugation on the Stability and Stable Conformation of Ethane, Hydrazine, and Hydrogen Peroxide. University Chemistry, doi: 10.3866/PKU.DXHX202402049
9. [9]
  Bing WEI , Jianfan ZHANG , Zhe CHEN . Research progress in fine tuning of bimetallic nanocatalysts for electrocatalytic carbon dioxide reduction. Chinese Journal of Inorganic Chemistry, doi: 10.11862/CJIC.20240201
10. [10]
  Jiahui YU , Jixian DONG , Yutong ZHAO , Fuping ZHAO , Bo GE , Xipeng PU , Dafeng ZHANG . The morphology control and full-spectrum photodegradation tetracycline performance of microwave-hydrothermal synthesized BiVO₄:Yb³⁺,Er³⁺ photocatalyst. Journal of Fuel Chemistry and Technology, doi: 10.1016/S1872-5813(24)60514-1
11. [11]
  Baitong Wei , Jinxin Guo , Xigong Liu , Rongxiu Zhu , Lei Liu . Theoretical Study on the Structure, Stability of Hydrocarbon Free Radicals and Selectivity of Alkane Chlorination Reaction. University Chemistry, doi: 10.12461/PKU.DXHX202406003
12. [12]
  Renqing Lü , Shutao Wang , Fang Wang , Guoping Shen . Computational Chemistry Aided Organic Chemistry Teaching: A Case of Comparison of Basicity and Stability of Diazine Isomers. University Chemistry, doi: 10.12461/PKU.DXHX202404119
13. [13]
  Xuewei BA , Cheng CHENG , Huaikang ZHANG , Deqing ZHANG , Shuhua LI . Preparation and luminescent performance of Sr_1-xZrSi₂O₇∶xDy³⁺ phosphor with high thermal stability. Chinese Journal of Inorganic Chemistry, doi: 10.11862/CJIC.20240096
14. [14]
  Hailang JIA , Hongcheng LI , Pengcheng JI , Yang TENG , Mingyun GUAN . Preparation and performance of N-doped carbon nanotubes composite Co₃O₄ as oxygen reduction reaction electrocatalysts. Chinese Journal of Inorganic Chemistry, doi: 10.11862/CJIC.20230402
15. [15]
  Kun WANG , Wenrui LIU , Peng JIANG , Yuhang SONG , Lihua CHEN , Zhao DENG . Hierarchical hollow structured BiOBr-Pt catalysts for photocatalytic CO₂ reduction. Chinese Journal of Inorganic Chemistry, doi: 10.11862/CJIC.20240037
16. [16]
  Zhanggui DUAN , Yi PEI , Shanshan ZHENG , Zhaoyang WANG , Yongguang WANG , Junjie WANG , Yang HU , Chunxin LÜ , Wei ZHONG . Preparation of UiO-66-NH₂ supported copper catalyst and its catalytic activity on alcohol oxidation. Chinese Journal of Inorganic Chemistry, doi: 10.11862/CJIC.20230317
17. [17]
  Juntao Yan , Liang Wei . 2D S-Scheme Heterojunction Photocatalyst. Acta Physico-Chimica Sinica, doi: 10.3866/PKU.WHXB202312024
18. [18]
  Shitao Fu , Jianming Zhang , Cancan Cao , Zhihui Wang , Chaoran Qin , Jian Zhang , Hui Xiong . Study on the Stability of Purple Cabbage Pigment. University Chemistry, doi: 10.3866/PKU.DXHX202401059
19. [19]
  Linjie ZHU , Xufeng LIU . Electrocatalytic hydrogen evolution performance of tetra-iron complexes with bridging diphosphine ligands. Chinese Journal of Inorganic Chemistry, doi: 10.11862/CJIC.20240207
20. [20]
  Qingqing SHEN , Xiangbowen DU , Kaicheng QIAN , Zhikang JIN , Zheng FANG , Tong WEI , Renhong LI . Self-supporting Cu/α-FeOOH/foam nickel composite catalyst for efficient hydrogen production by coupling methanol oxidation and water electrolysis. Chinese Journal of Inorganic Chemistry, doi: 10.11862/CJIC.20240028

Get Citation

PDF

XML

Metrics

PDF Downloads(919)
Abstract views(1368)
HTML views(9)

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