Influence of WO3 doping on properties of V2O5/TiO2-SnO2 catalysts for selective catalytic reduction of NOx by NH3

doi:10.16085/j.issn.1000-6613.2017.03.024

Abstract

Abstract:

TiO₂-SnO₂ solid solution was prepared by a co-precipitation method and V₂O₅-(x%)WO₃/TiO₂-SnO₂ catalysts were prepared by the impregnation method. The physicochemical properties were investigated by BET specific surface area,X-ray diffraction(XRD),in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS), NH₃ temperature-programmed desorption (NH₃-TPD) and high-resolution transmission electron microscopy(HRTEM). Their catalytic performance for the selective catalytic reduction of NO_x was also tested. The results indicate that the catalyst with 12% WO₃ exhibits 95% NO conversion within the wide temperature range of 250~400℃. The characterization results show that the specific surface area decreases with the load of WO₃ which is in a well-dispersed state. The strength of Brønsted acid sites are intensified after adding WO₃ which could account for the best catalytic performance of the catalyst V₂O₅-12%WO₃/TiO₂-SnO₂.

Key words: WO₃, V₂O₅, TiO₂-SnO₂ solid solution, support, selective catalytic reduction(SCR), catalyst

摘要：

采用共沉淀法制备TiO₂-SnO₂固溶体，浸渍法负载WO₃和V₂O₅得到一系列V₂O₅-（x%）WO₃/TiO₂-SnO₂脱硝催化剂。利用比表面积测定（BET）、X射线衍射（XRD）、原位漫反射傅里叶变换红外光谱（in situ DRIFTS）、程序升温脱附（NH₃-TPD）、高分辨率透射电子显微镜（HRTEM）等表征技术，结合脱硝性能测试，研究催化剂的表面特性、微观结构及脱硝活性。结果表明：V₂O₅-12% WO₃/TiO₂-SnO₂催化剂在250～400℃的温度窗口具有95%的NO_x转换率；随着WO₃负载量增加，催化剂比表面积有所减小；WO₃以无定形态存在于催化剂表面；催化剂表面Brønsted酸中心强度随WO₃负载量增加逐渐增大，这是V₂O₅-（12%）WO₃/TiO₂-SnO₂催化剂具有最佳脱硝活性的主要原因。

关键词: 三氧化钨, 五氧化二钒, TiO₂-SnO₂固溶体, 载体, 选择催化还原, 催化剂

CLC Number:

O643.36

LIAO Yongjin, ZHANG Yaping, ZHU Yiwen, YU Yuexi, WANG Longfei. Influence of WO₃ doping on properties of V₂O₅/TiO₂-SnO₂ catalysts for selective catalytic reduction of NO_x by NH₃[J]. Chemical Industry and Engineering Progress, 2017, 36(03): 951-956.

廖永进, 张亚平, 朱一闻, 余岳溪, 王龙飞. WO₃掺杂对V₂O₅/TiO₂-SnO₂催化剂NH₃选择性催化还原NO_x的影响[J]. 化工进展, 2017, 36(03): 951-956.

References

[1] 中国环境保护协会脱硫脱硝委员会. 脱硫脱硝行业2014年发展综述[J].中国环保产业,2015,12:4-23. Desulfurization and Denitration Committee of CAEPI. China development report on desulfurization and denitration industries in 2014[J]. China Environmental Protection Industry,2015,12:4-23.
[2] 中国环境保护产业协会脱硫脱硝委员会.我国脱硫脱硝行业2012年发展综述[J].中国环保产业,2013(7):8-20. Desulfurization and Denitration Committee of CAEPI. Development report on China desulfurization and denitration industries in 2012[J].China Environmental Protection Industry,2013(7):8-20.
[3] GB 13223-2011.火电厂大气污染物排放标准[S].北京:中国环境科学出版社,2011. GB 13223-2011.Emission standard of air pollutants for thermal power plants[S].Beijing:China Environmental Science Press,2011.
[4] 谭青,冯雅晨.我国烟气脱硝行业现状与前景及SCR脱硝催化剂的研究进展[J].化工进展,2011,30(s1):709-713. TAN Q,FENG Y C.Prensent status and perspective of China's flue gas denitration industry and research of SCR catalysts[J].Chemical Indusrty and Engineering Progress,2011,30(s1):709-713.
[5] LI K,WANG Y,WANG S,et al. A comparative study of CuO/TiO₂-SnO₂,CuO/TiO₂ and CuO/SnO₂ catalysts for low-temperature CO oxidation[J].Journal of Natural Gas Chemistry,2009,18(4):449-452.
[6] 贾彦荣,蒋晓原,郑小明. CuO/Sn_0.8Ti_0.2O₂催化剂的表征及对NO+CO反应活性研究[J].无机化学学报, 2006,22(3):525-532. JIA Y R,JIANG X Y,ZHENG X M.CuO/Sn_0.8Ti_0.2O₂ catalyst:characterization catalytic performance in NO + CO reaction[J]. Chinese Journal of Inorganic Chemistry,2006,22(3):525-532.
[7] 顾卫荣,周明吉,马薇,等.选择性催化还原脱硝催化剂的研究进展[J].化工进展,2012,31(7):1493-1500. GU W R,ZHOU M J,MA W,et al.Research progress on selective catalytic reduction de-NO_x catalysts[J]. Chemical Indusrty and Engineering Progress,2012,31(7):1493-1500.
[8] NOVA I,LIETTI L,TRONCONI E,et al. Dynamics of SCR reaction over a TiO₂ supported vanadia-tungsta commercial catalyst[J].Catalysis Today,2000,60(1):73-82.
[9] WU Z B,JIN R B,WANG H Q,et al. Effect of ceria doping on SO₂ resistance of Mn/TiO₂ for selective catalytic reduction of NO with NH₃ at low temperature[J].Catalysis Communications,2009,10(6):935-939
[10] 闫志勇,胡建飞,徐鸿.SCR烟气脱硝催化剂V₂O₅-WO₃/TiO₂性能研究[J].中国计量学院学报,2011,22(1):68-72. YAN Z Y,HU J F,XU H.Preparation of V₂O₅-WO₃/TiO₂ catalyst and properties of reduction NO_x[J].Journal of China University of Metrology,2011,22(1):68-72.
[11] DOS SANTOS V C,WILSON K,LEE A F,et al.Physicochemical properties of WOx/ZrO₂ catalysts for palmitic acid esterification[J]. Applied Catalysis B:Environmental,2015,162:75-84.
[12] FOO R,VAZHNOVA T,LUKYANOV D B,et al.Formation of reactive Lewis acid sites on Fe/WO₃-ZrO₂ catalysts for higher temperature SCR applications[J]. Aplied Catalysis B:Environmental, 2015,162:174-179.
[13] 李娟,张亚平,王文选,等.TiO₂-SnO₂基钨催化剂的表面性质和NH₃吸附特性及脱硝机理[J].东南大学学报(自然科学版),2016(1):92-99. JI J,ZHANG Y P,WANG W X,et al.Surface properties,NH₃ adsorption characteristic and NO_x removal mechanism of TiO₂-SnO₂ supported WO₃ catalysts[J].Journal of Southeast University(Natural Science Edition),2016(1):92-99.
[14] ZHANG L,LI L,CAO Y,et al.Promotional effect of doping SnO₂ into TiO₂ over a CeO₂/TiO₂ catalyst for selective catalytic reduction of NO by NH₃[J].Catalysis Science & Technology,2015,5(4):2188-2196.
[15] 朱崇兵,金保升,仲兆平,等.WO₃对于V₂O₅/TiO₂脱硝催化剂的抗中毒作用[J].锅炉技术,2009,40(1):63-67. ZHU C B,JIN B S,ZHONG Z P,et al.Anti-poisoning effect of WO₃ on V₂O₅/TiO₂ catalysts[J]. Boiler Technology,2009,40(1):63-67.
[16] ZHANG Y P,WANG X L,SHENG K,et al.WO₃ modification of MnO_x/TiO₂ catalysts for low temperature selective catalytic reduction of NO with ammonia[J].Chinese Journal of Catalysis,2012,33(9):1523-1531.
[17] 张亚平,汪小蕾,郑晓红,等.WO₃掺杂对MnO_x/TiO₂催化剂低温选择性催化还原NO_x的影响[J].中南大学学报:自然科学版, 2013,44(12):5165-5172. ZHANG Y P,WANG X L,ZHENG X H,et al.Influence of WO₃ doping on properties of MnO_x/TiO₂ catalyst for low-temperature selective catalytic reduction of NO_x by NH₃[J].Journal of Central South University(Science and Technology),2013,44(12):5165-5172.
[18] 余长林,杨凯,舒庆,等.WO₃/ZnO复合光催化剂的制备及其光催化性能[J].催化学报,2011,32(4):51-61. YU C L,YANG K,SHU Q,et al.Preparation of WO₃/ZnO composite photocatalyst and its photocatalytic performance[J].Chinese Journal of Catalysis,2011,32(4):51-61.
[19] 辛勤,罗孟飞.现代催化研究方法[M].北京:科学出版社,2009:83-88. XIN Q,LUO M F.Modern catalytic research methods[M].Beijing:Science Press,2009:83-88.
[20] RAMIS G,BUSCA G,BREGANI F,et al.Fourier transform-infrared study of the adsorption and coadsorption of nitric oxide,nitrogen dioxide and ammonia on vanadia-titania and mechanism of selective catalytic reduction[J].Applied Catalysis,1990,64:259-278.
[21] PINAEVA L G,SUKNEV A P,BUDNEVA A A,et al.On the role of oxygen in the reaction of NO reduction by NH₃ over monolayer V₂O₅/TiO₂ catalyst[J].Journal of Molecular Catalysis A:Chemical, 1996,112(1):115-124.
[22] SUN C Z,DONG L H,YU W J,et al.Promotion effect of tungsten oxide on SCR of NO with NH₃ for the V₂O₅-WO₃/Ti_0.5Sn_0.5O₂ catalyst:experiments combined with DFT calculations[J].Journal of Molecular Catalysis A,Chemical,2011,346(1):29-38.
[23] FAN Y,BAO X,WANG H,et al.A surfactant-assisted hydrothermal deposition method for preparing highly dispersed W/γ-Al₂O₃ hydrodenitrogenation catalyst[J].Journal of Catalysis,2007,245(2):477-481.
[24] 郭婉秋,张亚平,王文选,等.基于钛锡载体的SCR低温脱硝催化剂的表面性质研究[J].燃料化学学报,2015,11:1393-1401. GUO W Q,ZHANG Y P,WANG W X,et al.Study on the surface properties of TiO₂-SnO₂ supported catalysts for low temperature selective catalytic reduction of NO_x[J].Journal of Fuel Chemistry and Technology,2015,11:1393-1401.

Influence of WO₃ doping on properties of V₂O₅/TiO₂-SnO₂ catalysts for selective catalytic reduction of NO_x by NH₃

WO₃掺杂对V₂O₅/TiO₂-SnO₂催化剂NH₃选择性催化还原NO_x的影响

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

References

Related Articles 15

Recommended Articles

Metrics

Comments

[1]	ZHANG Mingyan, LIU Yan, ZHANG Xueting, LIU Yake, LI Congju, ZHANG Xiuling. Research progress of non-noble metal bifunctional catalysts in zinc-air batteries [J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 276-286.
[2]	SHI Yongxing, LIN Gang, SUN Xiaohang, JIANG Weigeng, QIAO Dawei, YAN Binhang. Research progress on active sites in Cu-based catalysts for CO₂ hydrogenation to methanol [J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 287-298.
[3]	XIE Luyao, CHEN Songzhe, WANG Laijun, ZHANG Ping. Platinum-based catalysts for SO₂ depolarized electrolysis [J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 299-309.
[4]	YANG Xiazhen, PENG Yifan, LIU Huazhang, HUO Chao. Regulation of active phase of fused iron catalyst and its catalytic performance of Fischer-Tropsch synthesis [J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 310-318.
[5]	WANG Lele, YANG Wanrong, YAO Yan, LIU Tao, HE Chuan, LIU Xiao, SU Sheng, KONG Fanhai, ZHU Canghai, XIANG Jun. Influence of spent SCR catalyst blending on the characteristics and deNO _x performance for new SCR catalyst [J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 489-497.
[6]	DENG Liping, SHI Haoyu, LIU Xiaolong, CHEN Yaoji, YAN Jingying. Non-noble metal modified vanadium titanium-based catalyst for NH₃-SCR denitrification simultaneous control VOCs [J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 542-548.
[7]	CHENG Tao, CUI Ruili, SONG Junnan, ZHANG Tianqi, ZHANG Yunhe, LIANG Shijie, PU Shi. Analysis of impurity deposition and pressure drop increase mechanisms in residue hydrotreating unit [J]. Chemical Industry and Engineering Progress, 2023, 42(9): 4616-4627.
[8]	WANG Peng, SHI Huibing, ZHAO Deming, FENG Baolin, CHEN Qian, YANG Da. Recent advances on transition metal catalyzed carbonylation of chlorinated compounds [J]. Chemical Industry and Engineering Progress, 2023, 42(9): 4649-4666.
[9]	GAO Yanjing. Analysis of international research trend of single-atom catalysis technology [J]. Chemical Industry and Engineering Progress, 2023, 42(9): 4667-4676.
[10]	ZHANG Qi, ZHAO Hong, RONG Junfeng. Research progress of anti-toxicity electrocatalysts for oxygen reduction reaction in PEMFC [J]. Chemical Industry and Engineering Progress, 2023, 42(9): 4677-4691.
[11]	GE Quanqian, XU Mai, LIANG Xian, WANG Fengwu. Research progress on the application of MOFs in photoelectrocatalysis [J]. Chemical Industry and Engineering Progress, 2023, 42(9): 4692-4705.
[12]	WANG Weitao, BAO Tingyu, JIANG Xulu, HE Zhenhong, WANG Kuan, YANG Yang, LIU Zhaotie. Oxidation of benzene to phenol over aldehyde-ketone resin based metal-free catalyst [J]. Chemical Industry and Engineering Progress, 2023, 42(9): 4706-4715.
[13]	GE Yafen, SUN Yu, XIAO Peng, LIU Qi, LIU Bo, SUN Chengying, GONG Yanjun. Research progress of zeolite for VOCs removal [J]. Chemical Industry and Engineering Progress, 2023, 42(9): 4716-4730.
[14]	WU Haibo, WANG Xilun, FANG Yanxiong, JI Hongbing. Progress of the development and application of 3D printing catalyst [J]. Chemical Industry and Engineering Progress, 2023, 42(8): 3956-3964.
[15]	XIANG Yang, HUANG Xun, WEI Zidong. Recent progresses in the activity and selectivity improvement of electrocatalytic organic synthesis [J]. Chemical Industry and Engineering Progress, 2023, 42(8): 4005-4014.