Citation: HONG Xin, TANG Ke. Preparation and adsorption denitrification of heteroatoms mesoporous molecular sieve Co-MCM-41[J]. Journal of Fuel Chemistry and Technology, ;2015, 43(6): 720-727. shu

Preparation and adsorption denitrification of heteroatoms mesoporous molecular sieve Co-MCM-41

HONG Xin ,
TANG Ke ^,

1.
School of Chemical and Environmental Engineering, Liaoning University of Technology, Jinzhou 121001, China

Corresponding author: TANG Ke,
Received Date: 28 November 2014
Available Online: 9 February 2015
Fund Project: 辽宁省自然科学基金(2014020113) (2014020113)辽宁省高等学校优秀人才支持计划(LJQ2012057) (LJQ2012057)辽宁工业大学教师启动资金(X201311)。 (X201311)

The MCM-41 and Co-MCM-41 molecular sieves, prepared by hydrothermal synthesis method, were characterized with X-ray diffraction (XRD), Fourier transform infrared spectrum (FT-IR), nitrogen adsorption and NH₃-TPD. The effects of aging time, crystallization temperature, crystallization time on the crystallization process of MCM-41 and Co-MCM-41 molecular sieves were investigated. The optimal conditions were as follows: 1 h of aging time, 110 ℃ of crystallization temperature and 2 d of crystallization time. XRD and FT-IR results indicated that Co was introduced into the framework of MCM-41. Brunauer-Emmett-Teller (BET) surface area and pore volume of MCM-41 and Co-MCM-41 were 986.42 m²/g, 637.69 m²/g, 0.762 1 m³/g and 0.537 2 m³/g respectively. The average pore diameter was 2.82 nm for both of MCM-41 and Co-MCM-41. The results of TPD showed that although MCM-41 and Co-MCM-41 possessed weak acidity, the acidity of Co-MCM-41 was stronger than MCM-41. Denitrification of model fuels containing about 1 737.35 μg(nitrogen)/g (16.03 mg(quinoline)/g) was studied over the synthesized MCM-41 and Co-MCM-41 with static adsorption at ambient conditions. The molecular size of quinoline, calculated by using density functional theory (DFT), was 0.711 6 nm×0.500 2 nm, implying that the quinoline easily access to the mesopores of MCM-41 and Co-MCM-41. The removal rate of basic nitrogen by Co-MCM-41 was clearly higher than MCM-41 due to its strong acidity and chemisorption between Co-MCM-41 and quinoline. Furthermore, Co-MCM-41 could be easily regenerated.
- Co-MCM-41,
- synthesis,
- chatacterization,
- denitrification
1. [1]
  [1] 王胜强, 梁燚, 杨磊, 于宏兵. 脱氮吸附剂深度脱除模拟含氮油中氮化物的研究[J]. 环境污染与防治, 2012, 34(9): 33-37. (WANG Sheng-qiang, LIANG Yi, YANG Lei, YU Hong-bing. Deep removal of nitrogen-containing compounds from vehicle fuels using denitrogenation adsorbent[J]. Environ Pollut Contr, 2012, 34(9): 33-37.)
2. [2]
  [2] 张伟东. 燃料油中硫、氮化合物组成对油品氧化安定性的影响的研究[D]. 天津: 天津大学, 2008. (ZHANG Wei-dong. Study on effects of common sulfide and nitride compounds on the oxidation stablity of fuel oil[D]. Tianjin: Tianjin University, 2008.)
3. [3]
  [3] TURAGA U T, MA X L, SONG C S. Influence of nitrogen compounds on deep hydrodesulfurization for 4, 6-dimethyldibenzothiophene over Al₂O₃- and MCM-41-supported Co-Mo sulfide catalysts[J]. Catal Today, 2003, 86(1/4): 265-275.
4. [4]
  [4] YANG H, CHEN J W, FAIRBRIDGE C, BRIKER Y, ZHU Y J, RING Z. Inhibition of nitrogen compounds on the hydrodesulfurization of substituted dibenzothiophenes in light cycle oil[J]. Fuel Process Technol, 2004, 85(12): 1415-1429.
5. [5]
  [5] LAREDO G C, ALTAMIRANO E, DE LOS REYES J A. Inhibition effects of nitrogen compounds on the hydrodesulfurization of dibenzothiophene: Part 2[J]. Appl Catal A: Gen, 2003, 243(2): 207-214.
6. [6]
  [6] KABE T, ISHIHARA A, QIAN W. Hydrodesulfurization and hydrodenitrogenation[M]. Tokyo, New York, Berlin: Kodansha Scientific, Wiley-VCH, 1999.
7. [7]
  [7] LAREDO G C, DE LOS REYES J A, CANO J L, CASTILLO J J. Inhibition effects of nitrogen compounds on the hydrodesulfurization of dibenzothiophene[J]. Appl Catal A: Gen, 2001, 207(1/2): 103-112.
8. [8]
  [8] 朱金柱, 沈健. SBA-15吸附脱除油品中的碱性氮化物[J]. 石油学报(石油加工), 2012, 40(11): 566-570. (ZHU Jin-zhu, SHEN Jian. Adsorption of basic nitrogen compounds from oil by SBA-15 zeolite[J]. Acta Pet Sin (Pet Process Sect), 2012, 40(11): 566-570.)
9. [9]
  [9] 朱金柱, 沈健, 韩英. Nb-SBA-15 的制备及吸附脱氮性能[J]. 硅酸盐学报, 2012, 40(11): 1666-1670. (ZHU Jin-zhu, SHEN Jian, HAN Ying. Preparation and adsoparation denitrication of Nb-SBA-15 zeolite[J]. J Chin Ceram Soc, 2012, 40(11): 1666-1670.)
10. [10]
  [10] 徐晓宇, 孙悦, 沈健, 翟玉龙. HY 和 USY 分子筛对模拟油品中碱性氮化物的吸附行为[J]. 化工进展, 2014, 33(4): 1035-1040. (XU Xiao-yu, SUN Yue, SHEN Jian, ZHAI Yu-long. Adsorption behavior of basic nitrides in model oil on HY and USY molecular sieves[J]. Chem Ind Eng Prog, 2014, 33(4): 1035-1040.)
11. [11]
  [11] 翟玉龙, 沈健. HY分子筛吸附脱除油品中碱性氮化物的研究[J]. 石油炼制与化工, 2011, 42(1): 41-44. (ZHAI Yu-long, SHEN Jian. Study on the adsorption of basic nitrogen compounds from oil with HY molecular sieve[J]. Pet Process Petrochem, 2011, 42(1): 41-44.)
12. [12]
  [12] 王福帅, 李会鹏, 赵华, 房斌斌. NaY/β复合分子筛改性及对模拟柴油中氮化物的吸附性能[J]. 石油炼制与化工, 2012, 43(11): 59-62. (WANG Fu-shuai, LI Hui-peng, ZHAO Hua, FANG Bin-bin. Modification of NaY/β composite molecular sieve and its adsorption performance of removing nitrogen containing compounds in model oil[J]. Pet Process Petrochem, 2012, 43(11): 59-62.)
13. [13]
  [13] 李少凯, 阮本玺, 沈健, 赵明飞. 硅胶吸附脱除模拟油品中的碱性氮化物[J]. 石油炼制与化工, 2013, 44(6): 22-25. (LI Shao-kai, RUAN Ben-xi, SHEN Jian, ZHAO Ming-fei. Study on nitrogen compounds adsorption performance of silica gel[J]. Pet Process Petrochem, 2013, 44(6): 22-25.)
14. [14]
  [14] 蒋超. 改性硅胶用于柴油吸附脱氮的基础研究[D]. 北京: 中国石油大学, 2010. (JIANG Chao. The basic research in denitrogenation of diesel oil by modified silica gel[D]. Beijing: China University of Petroleum, 2010.)
15. [15]
  [15] 王云芳, 迟志明. 介孔分子筛Al-MCM-41的吸附脱氮性能研究[J]. 石化技术与应用, 2014, 32(2): 113-117. (WANG Yun-fang, CHI Zhi-ming. Research on nitrogen adsorption removal performance of mesoporous molecular sieve Al-MCM-41[J]. Petrochem Technol Appl, 2014, 32(2): 113-117.)
16. [16]
  [16] 迟志明. 介孔分子筛用于柴油吸附脱氮的基础研究[D]. 北京: 中国石油大学, 2010. (CHI Zhi-ming. Basic research of Al-MCM-41 molecular sieve for denitrogenation of diese oil[D]. Beijing: China University of Petroleum, 2010.)
17. [17]
  [17] 张晗. 燃料中含氮化合物的吸附脱除[D]. 大连: 大连理工大学, 2009. (ZHANG Han. Adsorptive removal of nitrogen-containing compounds from fuel[D]. Dalian: Dalian University of Technology, 2009.)
18. [18]
  [18] 张燕, 李湘祁, 陈琼霞, 汤德平. 微波法合成有序Co-MCM-41介孔分子筛[J]. 化工时刊, 2008, 22(2): 12-15. (ZHANG Yan, LI Xiang-qi, CHEN Qiong-xia, TANG De-ping. Microwave synthesis of ordered mesoporous Co-MCM-41[J]. Chem Ind Times, 2008, 22(2): 12-15.)
19. [19]
  [19] ARAUJO A S, JARONIEC M. Synthesis and properties of Lanthanide incorporated mesoporous molecular sieves[J]. J Colloid Interface Sci, 1999, 218(2): 462-467.
20. [20]
  [20] 于健强, 李灿, 许磊, 李美俊, 辛勤, 刘中民. 以硅溶胶和三氯化钛为原料合成Ti-MCM-41分子筛I. Ti-MCM-41分子筛的合成[J]. 催化学报, 2001, 22(3): 267-270. (YU Jian-qiang, LI Can, XU Lei, LI Mei-jun, XIN Qin, LIU Zhong-min. Synthesis of Ti-MCM-41 using colloidal silica and titanium trichloride I. Synthesis of Ti-MCM-41 molecular sieve[J]. Chin J Catal, 2001, 22(3): 267-270.)
21. [21]
  [21] 史芸. Ti-MCM-41 分子筛的合成、改性及其催化酯交换反应性能的研究[D]. 天津: 天津大学, 2011. (SHI Yun. Synthesis, modification and catalytic performance of Ti-MCM-41 for transesterification[D]. Tianjin: Tianjin University, 2011.)
22. [22]
  [22] 于健强, 李灿, 许磊, 李美俊, 辛勤, 刘中民. 以硅溶胶和三氯化钛为原料合成 Ti-MCM-41分子筛. Ti-MCM-41分子筛的表征[J]. 催化学报, 2001, 22(4): 331-334. (YU Jian-qiang, LI Can, XU Lei, LI Mei-jun, XIN Qin, LIU Zhong-min. Synthesis of Ti-MCM-41 using colloidal silica and titanium trichloride II. Characterization of Ti-MCM-41 molecular sieve[J]. Chin J Catal, 2001, 22(4): 331-334.)
23. [23]
  [23] 赵杉林, 张扬健, 孙桂大, 翟玉春. 钒硅 MCM-41 沸石分子筛微波合成与表征[J]. 燃料化学学报, 1999, 27(2): 130-133. (ZHAO Shan-lin, ZHANG Yang-jian, SUN Gui-da, ZHAI Yu-chun. Synthesis of mesoporous molecular sieve VMCM-41 by microwave radiation and its characterization[J]. J Fuel Chem Technol, 1999, 27(2): 130-133.)
24. [24]
  [24] SUVANTO S, HUKKAMÄKIJ, PAKKANEN T T, PAKKANEN T A. High-cobalt-loaded MCM-41 via the gas-phase method[J]. Langmuir, 2000, 16(9): 4109-4115.
25. [25]
  [25] KARTHIK M, TRIPATHI A K, GUPTA N M, VINU A, HARTMANN M, PALANICHAMY M, MURUGESAN V. Characterization of Co, Al-MCM-41 and its activity in the t-butylation of phenol using isobutanol[J]. Appl Catal A: Gen, 2004, 268(1/2): 139-149.
26. [26]
  [26] 洪新, 唐克. NaY分子筛的改性及吸附脱氮性能[J]. 燃料化学学报, 2015, 43(2): 1-7. (HONG Xin, TANG Ke. Modification and adsorptive denitrification of NaY molecular sieve[J]. J Fuel Chem Technol, 2015, 43(2): 1-7.)
27. [27]
  [27] 邵为谠, 任靖, 曹光伟, 王安杰, 胡永康. 喹啉对Ni-Mo催化剂HDS性能的影响[J]. 石油学报(石油加工), 2011, 27(3): 348-354. (SHAO Wei-dang, REN Jing, CAO Guang-wei, WANG An-jie, HU Yong-kang. Effect of quinoline on the HDS performance of Ni-Mo catalysts[J]. Acta Pet Sin (Pet Process Sect), 2011, 27(3): 348-554.)
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