仿生CuO-CeO2复合材料低温选择性催化还原脱硝性能
Selective Catalysis Reduction Denitrification Performance at Low Temperature of Biomimicking CuO-CeO2 Composite
摘 要
以擦镜纸纤维为模板, 经硝酸铈和硝酸铜溶液浸渍, 煅烧后制得CuO-CeO2复合材料, 分析了其微观形貌和物相组成, 研究了其表面性能以及催化脱硝性能, 并与商用纳米CeO2和块状CeO2的进行了对比。结果表明: CuO-CeO2复合材料为长管状, 管径约为7 μm, 其中的CuO和CeO2晶粒大小均匀, 粒径为5～8 nm, 自然堆积形成了纳米尺寸的孔隙; 该复合材料中存在立方萤石结构的CeO2, 与商用纳米CeO2相比, 粒径较小, 比表面积较大, 达到106.5 m2·g-1; 掺杂CuO的CuO-CeO2复合材料的催化活性较高, 在催化NH3还原NO时, 当温度为280 ℃ 时NO的转化率就超过了94%, 远高于商用块状CeO2和纳米CeO2的。
选择性催化还原
生物模板
氮氧化物
掺杂
CeO2
selective catalysis reduction
biotemplate
nitric oxide
doping
Abstract
The lens wiping paper fiber as a template was dipped in the solution of cerium nitrate and copper nitrate, and then was calcined to obtain the CuO-CeO2 composite. The micromorphology and phase composition of the composite were studied and the surface property and catalysis reduction denitrification performance were also analyzed and compared with those of commercial nano-CeO2 and bulk CeO2. The results show that the CuO-CeO2 composite was long-tube-like with a tube diameter of about 7 μm. The grains of CuO and CeO2 had a uniform size of 5-8 nm and naturally accumulated, forming the voids with nano-size. The CeO2 with a cubic fluorite structure in the composite had a smaller grain size and an increased specific surface area of 106.5 m2·g-1 comparing to those of commercial nano-CeO2. The catalytic activity of the CuO-CeO2 composite was relatively high on account of the doping of CuO. During catalytic reduction of NO by NH3, the conversation rate of NO by the composite achieved over 94% at 280 ℃, which was much higher than that of commercial bulk CeO2 and nano-CeO2.
中图分类号 TQ426.7 DOI 10.11973/jxgccl201612017
所属栏目 材料性能及应用
基金项目 国家自然科学基金资助项目(E080405; 21277094); 陕西省教育厅重点实验室项目(15JS082)
收稿日期 2015/4/28
修改稿日期 2016/9/13
网络出版日期
作者单位点击查看
备注陈志刚(1955-), 男, 江苏高邮人, 教授, 硕士。
引用该论文: CHEN Zhi-gang,LIU Can-bin,QIAN Jun-chao,ZHANG Kai. Selective Catalysis Reduction Denitrification Performance at Low Temperature of Biomimicking CuO-CeO2 Composite[J]. Materials for mechancial engineering, 2016, 40(12): 73～77
陈志刚,刘灿斌,钱君超,张凯. 仿生CuO-CeO2复合材料低温选择性催化还原脱硝性能[J]. 机械工程材料, 2016, 40(12): 73～77
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参考文献
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【11】YAO X, GAO F, YU Q, et al. NO reduction by CO over CuO-CeO2 catalysts: Effect of preparation methods［J］. Catalysis Science & Technology, 2013, 3(5): 1355-1366.
【12】王炜, 陈志刚, 陈丰. 以鱼鳞为模板合成仿生氧化铈及其性能［J］. 机械工程材料, 2012,36 (12):17-20.
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【14】RUMRUANGWONG M, WONGKASEMJIT S. Anionic surfactant-aided preparation of high surface area and high thermal stability ceria/zirconia-mixed oxide from cerium and zirconium glycolates via sol-gel process and its reduction property［J］. Applied Organometallic Chemistry, 2008, 22(3): 167-170.
【15】QIN J, LU J, CAO M, et al. Synthesis of porous CuO-CeO2 nanospheres with an enhanced low-temperature CO oxidation activity［J］. Nanoscale, 2010, 2(12): 2739-2743.
【2】ANDERSSON A, DENG J, DU K, et al. Regionally-varying combustion sources of the January 2013 severe haze events over eastern China［J］. Environmental Science & Technology, 2015, 49(4): 2038-2043.
【3】YAO S Y, XU W Q, JOHNSTON-PECK A C, et al. Morphological effects of the nanostructured ceria support on the activity and stability of CuO/CeO2 catalysts for the water-gas shift reaction［J］. Physical Chemistry Chemical Physics, 2014, 16(32): 17183-17195.
【4】FU M, LI C, LU P, et al. A review on selective catalytic reduction of NOx by supported catalysts at 100-300 ℃ — catalysts, mechanism, kinetics［J］. Catalysis Science & Technology, 2014, 4(1): 14-25.
【5】ZENG Z, LU P, LI C, et al. Removal of NO by carbonaceous materials at room temperature: A review［J］. Catalysis Science & Technology, 2012, 2(11): 2188-2199.
【6】SHEN Y, ZHU S.Deactivation mechanism of potassium additives on Ti0.8Zr0.2Ce0.2O2.4 for NH3-SCR of NO［J］. Catalysis Science & Technology, 2012, 2(9): 1806-1810.
【7】LIU Z, YI Y, LI J, et al. A superior catalyst with dual redox cycles for the selective reduction of NOx by ammonia［J］. Chemical Communications, 2013, 49(70): 7726-7728.
【8】陈丰, 陈志刚, 马娟宁. 水热法合成棒束状纳米CeO2粉体及其催化性能［J］. 机械工程材料, 2014,38 (6):89-90.
【9】CISTON J, SI R, RODRIGUEZ J A, et al. Morphological and structural changes during the reduction and reoxidation of CuO/CeO2 and Ce1-xCuxO2 nanocatalysts: In situ studies with environmental TEM, XRD, and XAS［J］. The Journal of Physical Chemistry C, 2011, 115(28): 13851-13859.
【10】DJINOVIC P, BATISTA J, CEHIC B, et al. Utilization of high specific surface area CuO-CeO2 catalysts for high temperature processes of hydrogen production: Steam re-forming of ethanol and methane dry re-forming［J］. The Journal of Physical Chemistry A, 2009, 114(11): 3939-3949.
【11】YAO X, GAO F, YU Q, et al. NO reduction by CO over CuO-CeO2 catalysts: Effect of preparation methods［J］. Catalysis Science & Technology, 2013, 3(5): 1355-1366.
【12】王炜, 陈志刚, 陈丰. 以鱼鳞为模板合成仿生氧化铈及其性能［J］. 机械工程材料, 2012,36 (12):17-20.
【13】QIAN J, CHEN Z, LIU C, et al. Biotemplated fabrication of hierarchical mesoporous CeO2 derived from diatom and its application for catalytic oxidation of CO［J］. Chinese Science Bulletin, 2014, 59(26): 3260-3265.
【14】RUMRUANGWONG M, WONGKASEMJIT S. Anionic surfactant-aided preparation of high surface area and high thermal stability ceria/zirconia-mixed oxide from cerium and zirconium glycolates via sol-gel process and its reduction property［J］. Applied Organometallic Chemistry, 2008, 22(3): 167-170.
【15】QIN J, LU J, CAO M, et al. Synthesis of porous CuO-CeO2 nanospheres with an enhanced low-temperature CO oxidation activity［J］. Nanoscale, 2010, 2(12): 2739-2743.
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