改性SCR催化剂对Hg0催化氧化性能的研究

赵莉 何青松 李琳 陆强 董长青 杨勇平

引用本文: 赵莉, 何青松, 李琳, 陆强, 董长青, 杨勇平. 改性SCR催化剂对Hg0催化氧化性能的研究[J]. 燃料化学学报, 2015, 43(5): 628-634. shu
Citation:  ZHAO Li, HE Qing-song, LI Lin, LU Qiang, DONG Chang-qing, YANG Yong-ping. Research on the catalytic oxidation of Hg0 by modified SCR catalysts[J]. Journal of Fuel Chemistry and Technology, 2015, 43(5): 628-634. shu

改性SCR催化剂对Hg0催化氧化性能的研究

    通讯作者: 赵莉(1969-), 女, 博士, 副教授, 主要从事燃煤污染物控制技术研究, E-mail: zhaoli9533@163.com。
  • 基金项目:

    国家重点基础研究发展规划(973计划, 2015CB251501) (973计划, 2015CB251501)

    中央高校基本科研业务费(2014ZD17)。 (2014ZD17)

摘要: 采用一系列金属氧化物对商用SCR催化剂进行掺杂改性,筛选出最优Ce掺杂SCR催化剂,模拟实际烟气组分,考察了Ce改性催化剂对烟气中Hg0氧化的影响。实验结果表明,Ce掺杂比例适当可显著提高其催化活性,Ce最佳负载量为9%时,Hg0的催化氧化效率比未掺杂SCR催化剂提高近40%,BET和XRD也显示,CeO2在催化剂表面分散程度较好,未出现聚集现象。烟气工况对Hg0的催化氧化具有重要影响,其中,烟气组分HCl显著促进了Ce改性催化剂对Hg0的氧化,在一定温度范围内,Hg0的氧化效率随着温度升高而增加,在最佳空速、温度和烟气组分浓度时,Hg0的催化氧化效率可达95.11%。此外,掺杂CeO2之后SCR催化剂的脱硝性能并未受到影响。

English

  • 
    1. [1] ABICH I V, MOULIJN J A. Science and technology of novel processes for deep desulfurization of oil refinery streams: A review[J]. Fuel, 2003, 82(6): 607-631.[1] ABICH I V, MOULIJN J A. Science and technology of novel processes for deep desulfurization of oil refinery streams: A review[J]. Fuel, 2003, 82(6): 607-631.

    2. [2] EPA. Heavy-duty engine and vehicle standards and highway diesel fuel sulfur control requirements[R]. US Environmental Protection Agency, Air and Radiation, EPA420-F-00-057, 2000.[2] EPA. Heavy-duty engine and vehicle standards and highway diesel fuel sulfur control requirements[R]. US Environmental Protection Agency, Air and Radiation, EPA420-F-00-057, 2000.

    3. [3] MA X L, VELU S, KIM J H, SONG C S. 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]. Appl Catal B: Environ, 2005, 56(1): 137-147.[3] MA X L, VELU S, KIM J H, SONG C S. 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]. Appl Catal B: Environ, 2005, 56(1): 137-147.

    4. [4] 何爱珍, 刘红光, 王坤, 张玥, 袁莉. 轻质燃料油脱硫技术研究进展[J]. 工业催化, 2010, 18(7): 8-12.(HE Ai-zhen, LIU Hong-guang, WANG Kun, ZHANG Yue, YUAN Li. Studies on desulfurizaton technology of light fuel oil[J]. Ind Catal, 2010, 18(7): 8-12.)[4] 何爱珍, 刘红光, 王坤, 张玥, 袁莉. 轻质燃料油脱硫技术研究进展[J]. 工业催化, 2010, 18(7): 8-12.(HE Ai-zhen, LIU Hong-guang, WANG Kun, ZHANG Yue, YUAN Li. Studies on desulfurizaton technology of light fuel oil[J]. Ind Catal, 2010, 18(7): 8-12.)

    5. [5] 周继红, 罗一斌, 宗保宁. Y 型分子筛复合材料的成孔机理[J]. 石油炼制与化工, 2012, 43(1): 26-31.(ZHOU Ji-hong, LUO Yi-bin, ZONG Bao-ning. Formation mechanism of porous molecular sieve Y composite[J]. Petrol Process Petrochem, 2012, 43(1): 26-31.)[5] 周继红, 罗一斌, 宗保宁. Y 型分子筛复合材料的成孔机理[J]. 石油炼制与化工, 2012, 43(1): 26-31.(ZHOU Ji-hong, LUO Yi-bin, ZONG Bao-ning. Formation mechanism of porous molecular sieve Y composite[J]. Petrol Process Petrochem, 2012, 43(1): 26-31.)

    6. [6] TAKAHASHI A, YANG F H, YANG R T. New sorbents for desulfurization by π-complexation: Thiophene/benzene adsorption[J]. Ind Eng Chem Res, 2002, 41(10): 2487-2496.[6] TAKAHASHI A, YANG F H, YANG R T. New sorbents for desulfurization by π-complexation: Thiophene/benzene adsorption[J]. Ind Eng Chem Res, 2002, 41(10): 2487-2496.

    7. [7] VELU S, MA X L, SONG C S. Selective adsorption for removing sulfur from jet fuel over zeolite-based adsorbents[J]. Ind Eng Chem Res, 2003, 42(21): 5293-5304.[7] VELU S, MA X L, SONG C S. Selective adsorption for removing sulfur from jet fuel over zeolite-based adsorbents[J]. Ind Eng Chem Res, 2003, 42(21): 5293-5304.

    8. [8] ZHANG Z Y, SHI T B, JIA C Z, JI W J, CHEN Y, HE M Y. Adsorptive removal of aromatic organosulfur compounds over the modified Na-Y zeolites[J]. Appl Catal B: Environ, 2008, 82(1): 1-10.[8] ZHANG Z Y, SHI T B, JIA C Z, JI W J, CHEN Y, HE M Y. Adsorptive removal of aromatic organosulfur compounds over the modified Na-Y zeolites[J]. Appl Catal B: Environ, 2008, 82(1): 1-10.

    9. [9] 王娟, 张海波, 张秋卓, 曾辉, 蔡伟民. NiCeY改性沸石吸附燃料油中二苯并噻吩的研究[J]. 环境工程学报, 2008, 2(11): 1581-1584.(WANG Juan, ZHANG Hai-bo, ZHANG Qiu-zhuo, ZENG Hui, CAI Wei-min. Study on adsorption of dibenzothiophene in fuel using NiCeY zeolite[J]. Chin J Environ Eng, 2008, 2(11): 1581-1584.)[9] 王娟, 张海波, 张秋卓, 曾辉, 蔡伟民. NiCeY改性沸石吸附燃料油中二苯并噻吩的研究[J]. 环境工程学报, 2008, 2(11): 1581-1584.(WANG Juan, ZHANG Hai-bo, ZHANG Qiu-zhuo, ZENG Hui, CAI Wei-min. Study on adsorption of dibenzothiophene in fuel using NiCeY zeolite[J]. Chin J Environ Eng, 2008, 2(11): 1581-1584.)

    10. [10] SONG H, WAN X, DAI M, ZHANG J J, LI F, SONG H L. Deep desulfurization of model gasoline by selective adsorption over Cu-Ce bimetal ion-exchanged Y zeolite[J]. Fuel Process Technol, 2013, 116: 52-62.[10] SONG H, WAN X, DAI M, ZHANG J J, LI F, SONG H L. Deep desulfurization of model gasoline by selective adsorption over Cu-Ce bimetal ion-exchanged Y zeolite[J]. Fuel Process Technol, 2013, 116: 52-62.

    11. [11] 宋华, 高慧杰, 宋华林, 崔雪涵, 万霞, 苑丹丹. Cu(Ⅰ)-Ce(Ⅳ)-Y吸附剂的制备及其脱硫性能研究[J]. 燃料化学学报, 2014, 42(12): 1485-1492.(SONG Hua, GAO Hui-jie, SONG Hua-lin, CUI Xue-han, WAN Xia, YUAN Dan-dan. Preparation of Cu(Ⅰ)-Ce(Ⅳ)-Y adsorbent and its adsorptive desulfurization performance[J]. J Fuel Chem Technol, 2014, 42(12): 1485-1492.)[11] 宋华, 高慧杰, 宋华林, 崔雪涵, 万霞, 苑丹丹. Cu(Ⅰ)-Ce(Ⅳ)-Y吸附剂的制备及其脱硫性能研究[J]. 燃料化学学报, 2014, 42(12): 1485-1492.(SONG Hua, GAO Hui-jie, SONG Hua-lin, CUI Xue-han, WAN Xia, YUAN Dan-dan. Preparation of Cu(Ⅰ)-Ce(Ⅳ)-Y adsorbent and its adsorptive desulfurization performance[J]. J Fuel Chem Technol, 2014, 42(12): 1485-1492.)

    12. [12] SONG H, WAN X, SUN X. Preparation of AgY zeolites using microwave irradiation and study on their adsorptive desulphurisation performance[J]. Can J Chem Eng, 2013, 91(5): 915-923.[12] SONG H, WAN X, SUN X. Preparation of AgY zeolites using microwave irradiation and study on their adsorptive desulphurisation performance[J]. Can J Chem Eng, 2013, 91(5): 915-923.

    13. [13] 黎俊波, 刘习文, 曹灿灿, 郭嘉, 潘志权. CuY型分子筛制备及吸附脱硫影响因素研究[J]. 离子交换与吸附, 2012, 28(1): 18-25.(LI Jun-bo, LIU Xi-wen, CAO Can-can, GUO Jia, PAN Zhi-quan. Effect of different factors on adsorption of sulfur-containing compounds over CuY zeolites[J]. Ion Exch Adsorpt, 2012, 28(1): 18-25.)[13] 黎俊波, 刘习文, 曹灿灿, 郭嘉, 潘志权. CuY型分子筛制备及吸附脱硫影响因素研究[J]. 离子交换与吸附, 2012, 28(1): 18-25.(LI Jun-bo, LIU Xi-wen, CAO Can-can, GUO Jia, PAN Zhi-quan. Effect of different factors on adsorption of sulfur-containing compounds over CuY zeolites[J]. Ion Exch Adsorpt, 2012, 28(1): 18-25.)

    14. [14] BROWN D R, KEVAN L. Comparative electron spin resonance and optical absorption studies of silver-exchanged sodium Y zeolites: Silver centers formed on dehydration, oxidation, and subsequent. gamma.-irradiation[J]. J Phys Chem, 1986, 90(6): 1129-1133.[14] BROWN D R, KEVAN L. Comparative electron spin resonance and optical absorption studies of silver-exchanged sodium Y zeolites: Silver centers formed on dehydration, oxidation, and subsequent. gamma.-irradiation[J]. J Phys Chem, 1986, 90(6): 1129-1133.

    15. [15] 石川, 程谟杰, 曲振平, 杨学锋, 包信和. 银在甲烷选择性催化还原NO<em>x反应中的催化行为[J]. 催化学报, 2001, 22(6): 555-558.(SHI Chuan, CHENG Mo-Jie, QU Zhen-Ping, YANG Xue-feng, BAO Xin-he. Behavior of different silver species in the selective reduction of NOx by CH4 over Ag-HZSM-5 catalyst[J]. Chin J Catal, 2001, 22(6): 555-558.)[15] 石川, 程谟杰, 曲振平, 杨学锋, 包信和. 银在甲烷选择性催化还原NO<em>x反应中的催化行为[J]. 催化学报, 2001, 22(6): 555-558.(SHI Chuan, CHENG Mo-Jie, QU Zhen-Ping, YANG Xue-feng, BAO Xin-he. Behavior of different silver species in the selective reduction of NOx by CH4 over Ag-HZSM-5 catalyst[J]. Chin J Catal, 2001, 22(6): 555-558.)

    16. [16] 宋丽娟, 潘明雪, 秦玉才, 鞠秀芳, 段林海, 陈晓陆. NiY 分子筛选择性吸附脱硫性能及作用机理[J]. 高等学校化学学报, 2011, 32(3): 787-792.(SONG Li-juan, PAN Ming-xue, QIN Yu-cai, JU Xiu-fang, DUAN Lin-hai, CHEN Xiao-lu. Selective adsorption desulfurization performance and adsorptive mechanisms of NiY zeolites[J].Chem J Chin U, 2011, 32(3): 787-792.)[16] 宋丽娟, 潘明雪, 秦玉才, 鞠秀芳, 段林海, 陈晓陆. NiY 分子筛选择性吸附脱硫性能及作用机理[J]. 高等学校化学学报, 2011, 32(3): 787-792.(SONG Li-juan, PAN Ming-xue, QIN Yu-cai, JU Xiu-fang, DUAN Lin-hai, CHEN Xiao-lu. Selective adsorption desulfurization performance and adsorptive mechanisms of NiY zeolites[J].Chem J Chin U, 2011, 32(3): 787-792.)

    17. [17] ROMEO M, BAK K, EL FALLAH J, NORMAND F L, HILAIRE L. XPS study of the reduction of cerium dioxide[J]. Surf Interface Anal, 1993, 20(6): 508-512.[17] ROMEO M, BAK K, EL FALLAH J, NORMAND F L, HILAIRE L. XPS study of the reduction of cerium dioxide[J]. Surf Interface Anal, 1993, 20(6): 508-512.

    18. [18] SHI Y C, YANG X J, TIAN F P, JIA C Y, CHEN Y Y. Effects of toluene on thiophene adsorption over NaY and Ce(IV) Y zeolites[J]. J Nat Gas Chem, 2012, 21(4): 421-425.[18] SHI Y C, YANG X J, TIAN F P, JIA C Y, CHEN Y Y. Effects of toluene on thiophene adsorption over NaY and Ce(IV) Y zeolites[J]. J Nat Gas Chem, 2012, 21(4): 421-425.

    19. [19] WANG H G, SONG L J, JIANG H, XU J, JIN L L, ZHANG X T, SUN Z L. Effects of olefin on adsorptive desulfurization of gasoline over Ce(IV) Y zeolites[J]. Fuel Process Technol, 2009, 90(6): 835-838.[19] WANG H G, SONG L J, JIANG H, XU J, JIN L L, ZHANG X T, SUN Z L. Effects of olefin on adsorptive desulfurization of gasoline over Ce(IV) Y zeolites[J]. Fuel Process Technol, 2009, 90(6): 835-838.

    20. [20] HERNÁNDEZ-MALDONADO A J, YANGF H, QI G, YANG R T. Sulfur and nitrogen removal from transportation fuels by π-complexation[J]. J Chin Inst Chem Eng, 2006, 37(1): 9-16.[20] HERNÁNDEZ-MALDONADO A J, YANGF H, QI G, YANG R T. Sulfur and nitrogen removal from transportation fuels by π-complexation[J]. J Chin Inst Chem Eng, 2006, 37(1): 9-16.

  • 加载中
计量
  • PDF下载量:  0
  • 文章访问数:  577
  • HTML全文浏览量:  18
文章相关
  • 收稿日期:  2015-01-08
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

  1. 本站搜索
  2. 百度学术搜索
  3. 万方数据库搜索
  4. CNKI搜索

/

返回文章