WO3 enhanced surface acidity of RuO2/ZrO2 and its performance in selective catalytic oxidation of NH3

被引:0
|
作者
Li F.-J. [1 ]
Zhang Y.-K. [1 ]
Yang C.-X. [1 ]
Zhang K.-X. [1 ]
Xia F.-T. [1 ,2 ]
Zhang Q.-L. [3 ]
Pang P.-F. [1 ]
Wang H.-M. [3 ]
机构
[1] Key Laboratory of Resource Clean Conversion in Ethnic Regions of Yunan Provincial Universities, Yunnan Minzu University, Kunming
[2] State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization, Kunming University of Science and Technology, Kunming
[3] Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming
基金
中国国家自然科学基金;
关键词
N[!sub]2[!/sub] selectivity; Rapid reaction; Selective catalytic oxidation; Surface acid sites; WO[!sub]3[!/sub;
D O I
10.19906/j.cnki.JFCT.2021015
中图分类号
学科分类号
摘要
In this paper, RuO2/ZrO2 catalyst and WO3 doped RuO2/WO3-ZrO2 catalysts with different WO3 loadings were designed and prepared for selective catalytic oxidation of ammonia. Among the catalysts, RuO2/ZrO2 catalyst exhibits excellent catalytic activity but poor N2 selectivity. It is worth noting that the activity of RuO2/ZrO2 catalyst remains unchanged after 5% or 10% WO3 doping, while the N2 selectivity at high temperature is significantly improved, and NH3 is completely transformed at 225 ℃. However, when WO3 content rises to 15% and 20%, the catalytic activity of RuO2/ZrO2 catalyst decreases slightly, while N2 selectivity is not further improved at high temperature. Therefore, it can be judged that the optimal WO3 content is 10%. In addition, it is found that WO3 doping can change the microstructure of the catalyst and the corresponding specific surface area increases with the increase of WO3 content through BET analysis. XRD, H2-TPR and XPS show that WO3 doping can change the crystal structure of ZrO2, increase the stability of the catalyst. According to the DRIFT spectra results, as WO3 is doped into the catalyst, the amount of surface acid sites on the catalyst increase. More surface acid sites can facilitate the adsorption of ammonia species, inhibit the rapid reaction between ammonia and oxygen, and avoid formation of more by-products, which are the key factors to improve the N2 selectivity. Copyright ©2021 Editorial Dept. of Journal of Fuel Chemistry and Technology. All rights reserved.
引用
收藏
页码:228 / 237
页数:9
相关论文
共 54 条
  • [1] GUO J J, PENG Y, ZHANG Y N., Comparison of NH<sub>3</sub>-SCO performance over CuO<sub>x</sub>/H-SSZ-13 and CuO<sub>x</sub>/HSAPO-34 catalysts[J], Appl Catal A: Gen, 585, 5, pp. 117-119, (2019)
  • [2] LIU H, FU M L, JIN X X, SHANG Y, SHINDELL D, FALUVE G, SHINDELL C, HE K., Health and climate impacts of ocean-going vessels in East Asia[J], Nature Clim Change, 6, 7, pp. 1037-1041, (2016)
  • [3] LONG R., Selective catalytic oxidation of ammonia to nitrogen over Fe<sub>2</sub>O<sub>3</sub>-TiO<sub>2</sub> prepared with a sol-gel method, J Catal, 207, 2, pp. 158-165, (2002)
  • [4] LIU J, SUN M M, LIN Q J, LIU S, XU H D, CHEN Y Q., Promotional effects of ethylenediamine on the low-temperature catalytic activity of selective catalytic oxidation of ammonia over Pt/SiAlO<sub>x</sub>: States and particle sizes of Pt[J], Appl Surf Sci, 481, 1, pp. 1344-1351, (2019)
  • [5] CHMIELARZ L, JABONSKA MAGDALENA, Advances in selective catalytic oxidation of ammonia to dinitrogen: A review[J], Rsc Adv, 5, 54, pp. 43408-43431, (2015)
  • [6] SANG M L, HONG S C., Promotional effect of vanadium on the selective catalytic oxidation of NH<sub>3</sub> to N<sub>2</sub> over Ce/V/TiO<sub>2</sub> catalyst, Appl Catal B: Environ, 163, 2, pp. 30-39, (2015)
  • [7] TANG X L, LI J Y, YI H H, YU Q J, GAO F Y, ZHANG R C, LI C L, CHU C., An efficient two-step method for NH<sub>3</sub> removal at low temperature using CoO<sub>x</sub>-CuO<sub>x</sub>/TiO<sub>2</sub> as SCO catalyst followed by NiMn<sub>2</sub>O<sub>4</sub> as SCR catalyst[J], Energ Fuels, 31, 8, pp. 8580-8593, (2017)
  • [8] SHOJAEE K, HAYNES B S, MONTOYA A., The catalytic oxidation of NH<sub>3</sub> on Co<sub>3</sub>O<sub>4</sub>(110): A theoretical study, Proc Combust Inst, 36, 3, pp. 4365-4373, (2016)
  • [9] RUTKOWSKA M, PACIA I, BASAG S, KOWALCZYK A, PIWOWARSKA Z, DUDA M, TARACH K A, GORA-MAREK K, MICHALIK M, DIAZ U, CHMIELARZ L., Catalytic performance of commercial Cu-ZSM-5 zeolite modified by desilication in NH<sub>3</sub>-SCR and NH<sub>3</sub> -SCO processes[J], Microprous Mesoporous Mater, 246, pp. 193-206, (2017)
  • [10] LONG R Q, YANG R T., Selective catalytic oxidation (SCO) of ammonia to nitrogen over Fe-exchanged zeolites[J], J Catal, 201, 1, pp. 145-152, (2001)