载铜球形活性炭的制备及其吸附脱硫性能的研究

李文秀; 崔安磊; 范俊刚; 孙向乐; 张志刚

载铜球形活性炭的制备及其吸附脱硫性能的研究

沈阳化工大学化学工程学院, 辽宁沈阳 110142

基金项目: 辽宁省高等学校优秀人才支持计划(LR2012013)。

详细信息

通讯作者:
张志刚, E-mail: zhzhgang@126.com; Tel: 024-89383736。

中图分类号: TQ424.1⁺9
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出版历程
- 收稿日期: 2012-10-19
- 修回日期: 2012-12-13
- 刊出日期: 2013-05-30

Synthesis of spherical activated carbon supported copper catalyst and its performance for adsorptive desulfurization

College of Chemical Engineering, Shenyang University of Chemical Technology, Shenyang 110142, China

摘要

摘要: 以122型弱酸性酚醛系阳离子交换树脂为炭前驱体,经过Cu²⁺交换、炭化和CO₂活化等过程制备得到负载金属铜的球形活性炭,对其进行了SEM、XRD、AAS和BET表征,采用动态吸附实验研究了其对模拟汽油中噻吩类硫化物的吸附性能,并且考察了甲苯和环己烯对其吸附性能的影响,对吸附脱硫机理进行了初步研究。结果表明,载铜球形活性炭上Cu以单质形态存在,并主要与硫原子产生配位作用,提高了对噻吩类硫化物的吸附性能,对噻吩(T)、3-甲基噻吩(MT)、2,5-二甲基噻吩(DMT)和苯并噻吩(BT)的饱和硫容依次为0.938、1.230、1.581和3.744 mg/g,吸附选择性依次为T < MT < DMT < BT。模拟汽油中加入甲苯和环己烯后,饱和硫容分别下降了77%和56%,这是甲苯和环己烯通过π电子与Cu发生作用,从而与硫化物产生竞争吸附导致的。
- 载铜球形活性炭 /
- 吸附性能 /
- 吸附选择性
Abstract: Phenolic weak acid cation exchange resin was used as carbon precursor to prepare spherical activated carbon supported copper catalyst by ion exchange, carbonization and activation with CO₂. The catalyst was characterized by SEM, XRD, AAS and BET. The adsorptive capacities for different sulfur-containing compounds were evaluated by dynamic adsorption experiments and the competitive effects of toluene and cyclohexene were investigated. The mechanism of adsorptive desulfurization was primarily studied as well. The results showed that metals in the spherical activated carbon existed in elemental form and improved the adsorption performance through direct coordination with sulfur atoms. The saturation capacities for thiophene(T), 3-methylthiophene(MT), 2,5-dimethylthiophene(DMT) and benzothiophene(BT) were 0.938, 1.230, 1.581 and 3.744 mg/g, respectively. The adsorptive selectivity increased in the order of T
- spherical activated carbon supported with copper /
- adsorption capacity /
- adsorptive selectivity

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参考文献(15)

查庆芳, 高南星, 李兆丰, 卓海波, 张玉贞. 石油焦系活性炭的吸附脱硫[J]. 燃料化学学报, 2007, 35(2): 192-197. (ZHA Qing-fang, GAO Nan-xing, LI Zhao-feng, ZHUO Hai-bo,ZHANG Yu-zhen.Adsorption desulfurization by activated carbon from petroleum coke[J]. Journal of Fuel Chemistry and Technology, 2007, 35(2): 192-197.)

赵地顺, 李发堂, 孙智敏. 核黄素光敏氧化噻吩脱硫研究[J]. 燃料化学学报, 2008, 36(2): 166-169. (ZHAO Di-shun, LI Fa-tang, SUN Zhi-min. Photosensitized oxidative desulfurization of thiophene by riboflavin[J].Journal of Fuel Chemistry and Technology, 2008, 36(2): 166-169.)

王建龙, 赵地顺, 周二鹏, 董芝. 吡啶类离子液体在汽油萃取脱硫中的应用研究[J]. 燃料化学学报, 2007, 35(3): 293-296. (WANG Jian-long, ZHAO Di-shun, ZHOU Er-peng, DONG Zhi. Desulfurization of gasoline by extraction with N-alkyl-pyridinium-based ionic liquids[J]. Journal of Fuel Chemistry and Technology, 2007, 35(3): 293-296.)

唐晓东, 李林. 汽油活性炭基脱硫吸附剂的制备与评价[J]. 燃料化学学报, 2009, 37(5): 629-634. (Tang Xiao-dong, Li Lin. Preparation and evaluation of gasoline activated carbon-based desulfurization adsorbent[J]. Journal of Fuel Chemistry and Technology, 2009, 37(5): 629-634.)

魏明, 王海彦, 马俊, 白英芝. 载体活化对PW₁₂/炭化树脂催化剂醚化活性的影响[J]. 辽宁石油化工大学学报, 2005, 25(1): 52-54. (WEI Min, WANG Hai-yan, MA Jun, BAI Ying-zhi. Effect of carrier activation on etherification activity of PW₁₂/carbonized resin catalyst[J]. Journal of Liaoning University of Petroleum & Chemical Technology, 2005, 25(1): 52-54.)

李秀灵, 李保山. Ni/D152树脂炭化催化剂的制备及其对异丙醇脱氢反应的催化性能[J]. 工业催化, 2008, 16(7): 16-20. (LI Xiu-ling, LI Bao-shan. Preparation of Ni/D152 carbonized resin catalyst and its catalytic behaviors for 2-propanol dehydrogenation reaction[J]. Industrial Catalysis, 2008, 16(7): 16-20.)

HUNTLEY D R, MULLINS D R, WINGEIER M P. Desulfurization of thiophenic compounds by Ni(Ⅲ): Adsorption andreactions of thiophene, 3-methylth-iophene, and 2,5-dimethylthiophene[J]. J Phys Chem, 1996, 100(50): 19620-19627.

BEZVERKHYY I, RQZHIKOV A, GADACZ G, BELLAT J P.Kinetics of thiophene reactive adsorption on Ni/SiO₂ and Ni/ZnO[J]. Catal Today, 2008, 130(1): 199-205.

BAEZA P, AGUILA G, GRACIA F, ARAYA P. Desulfurization by adsorption with copper supported on zirconia[J]. Catal Commun, 2008, 9(5): 751-755.

MA X, SUN L, SONG C. A new approach to deep desulfurization of gasoline, diesel fuel and jet fuel by selective adsorption for ultra-clean fuels and for fuel cell applications[J]. Catal Today, 2002, 77(1/2): 107-1l6.

KIM J H, MA X, ZHOU A, SONG C. Ultra-deep desulfurization and denitrogenation of diesel fuel by selective adsorption over three different adsorbents: A study on adsorptive selectivity and mechanism[J]. Catal Today, 2006, 111(1/2): 74-83.

唐克, 洪新, 宋丽娟, 孙兆林. 二次合成Y型杂原子分子筛的吸附脱硫研究[J]. 燃料化学学报, 2012, 40(4): 507-511. (TANG Ke, HONG Xin, SONG Li-juan, SUN Zhao-lin. Preparation of heteroatom Y zeolite by secondary synthesis and its performance in adsorptive desulfurization[J]. Journal of Fuel Chemistry and Technology, 2012, 40(4): 507-511.)

MA X, SPRAGUE M, SONG C. Deep desulfurization of gasoline by selective adsorption over nickel-based adsorbent for fuel cell applications[J]. Ind Eng Chem Res, 2005, 44(15): 5768-5775.

MA X, VELU S, KIM J H, SONG C. Deep desulfurization of gasoline by selective adsorption over solid adsorbents and impact of analytical methods on ppm-level sulfur quantification for fuel cell applications[J]. App Catal B, 2005, 56(2): 137-147.

VELU S, WATANAB S, MA X. Development of selective adsorbents for removing sulfur from gasoline for fuel cell applications[J]. Petr Chem Div Prepr, 2003, 48(2): 56-57.

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