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MnFeTiOx/attapulgite catalysts with excellent potassium resistance for SCR of NOx with NH3 at low temperatures

Published online by Cambridge University Press:  26 February 2019

Yiran Tang ,
Yiyang Tao ,
Jiayi Wu ,
Linjing Xu ,
Xiaoyan Huang ,
Xingmeng Zhou ,
Aijuan Xie ,
Shiping Luo ,
Chao Yao  and
Xiazhang Li
Yiran Tang
Affiliation:
School of Petrochemical Engineering, Changzhou University, Changzhou 213164, People’s Republic of China
Yiyang Tao
Affiliation:
School of Fine Arts, Nanjing Normal University, Nanjing 210046, People’s Republic of China
Jiayi Wu
Affiliation:
School of Petrochemical Engineering, Changzhou University, Changzhou 213164, People’s Republic of China
Linjing Xu
Affiliation:
School of Petrochemical Engineering, Changzhou University, Changzhou 213164, People’s Republic of China
Xiaoyan Huang
Affiliation:
School of Petrochemical Engineering, Changzhou University, Changzhou 213164, People’s Republic of China
Xingmeng Zhou
Affiliation:
School of Petrochemical Engineering, Changzhou University, Changzhou 213164, People’s Republic of China
Aijuan Xie*
Affiliation:
School of Petrochemical Engineering, Changzhou University, Changzhou 213164, People’s Republic of China
Shiping Luo*
Affiliation:
School of Petrochemical Engineering, Changzhou University, Changzhou 213164, People’s Republic of China
Chao Yao
Affiliation:
School of Petrochemical Engineering, Changzhou University, Changzhou 213164, People’s Republic of China
Xiazhang Li
Affiliation:
School of Petrochemical Engineering, Changzhou University, Changzhou 213164, People’s Republic of China
*
a)Address all correspondence to these authors. e-mail: aijuan_xie@126.com
b)e-mail: shiping_luo@163.com
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Abstract

A series of metal oxides (MnFeOx, MnCrOx, MnTiOx, and MnFeTiOx) supported on attapulgite (ATP) were synthesized by coprecipitation for the low-temperature selective catalytic reduction (SCR) of NOx with NH3. Then, they were subjected to appropriate characterizations for their properties (XRD, TEM, BET, XPS, etc.). The catalytic activity of MnFeTiOx/ATP catalyst was over 95% NOx conversion within a wide temperature window between of 175 and 300 °C, and 88% N2 selectivity. Moreover, MnFeTiOx/ATP presented excellent potassium resistance relative to the traditional V–W–Ti catalyst, and its denitration performance was significantly improved. The NOx conversion rate could be restored to nearly 90% at 210 °C after removing potassium via washing of K–MnFeTiOx/ATP. In addition, the MnFeTiOx/ATP showed better SO2 resistance and stability than the traditional V–W–Ti catalyst. Therefore, the MnFeTiOx/ATP catalyst has been proved to have broad prospects in NH3-SCR.

Keywords

MnFeTiOx/ATPlow temperatureselective catalytic reductionNOx conversionpotassium resistance
Type
Article
Information
Journal of Materials Research , Volume 34 , Issue 7: Focus Section: Interconnects and Interfaces in Energy Conversion Materials , 15 April 2019 , pp. 1188 - 1199
Copyright
Copyright © Materials Research Society 2019 

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Footnotes

c)

These authors contributed equally to this work.

References

Blanco, J., Avila, P., Suárez, S., Yates, M., Martin, J.A., Marzo, L., and Knapp, C.: CuO/NiO monolithic catalysts for NOx removal from nitric acid plant flue gas. Chem. Eng. J. 97, 1–9 (2004).CrossRefGoogle Scholar
Forzatti, P.: Present status and perspectives in de-NOx SCR catalysis. Appl. Catal., B 222, 221–236 (2001).CrossRefGoogle Scholar
Li, J., Chang, H., Ma, L., Hao, J., and Yang, R.T.: Low-temperature selective catalytic reduction of NOx with NH3 over metal oxide and zeolite catalysts—A review. Catal. Today 175, 147–156 (2011).CrossRefGoogle Scholar
Cai, S., Hu, H., Li, H., Shi, L., and Zhang, D.: Design of multi-shell Fe2O3@MnOx@CNTs for the selective catalytic reduction of NO with NH3: Improvement of catalytic activity and SO2 tolerance. Nanoscale 8, 3588–3598 (2016).CrossRefGoogle ScholarPubMed
O’Malley, A.J., Hitchcock, I., Sarwar, M., Silverwood, I.P., Hindocha, S., Catlow, C.R., York, A.E., and Collier, P.J.: Ammonia mobility in chabazite: Insight into the diffusion component of the NH3-SCR process. Phys. Chem. Chem. Phys. 18, 17159–17168 (2016).CrossRefGoogle ScholarPubMed
Guo, Z., Liang, Q.H., Yang, Z., Liu, S., Huang, Z.H., and Kang, F.: Modifying porous carbon nanofibers with MnOx–CeO2–Al2O3 mixed oxides for NO catalytic oxidation at room temperature. Catal. Sci. Technol. 6, 422–425 (2016).CrossRefGoogle Scholar
Jiang, H., Wang, Q., Wang, H., Chen, Y., and Zhang, M.: MOF-74 as an efficient catalyst for the low-temperature selective catalytic reduction of NOx with NH3. ACS Appl. Mater. Interfaces 8, 26817–26826 (2016).CrossRefGoogle ScholarPubMed
Yao, X., Kong, T., Yu, S., Li, L., Yang, F., and Dong, L.: Influence of different supports on the physicochemical properties and denitration performance of the supported Mn-based catalysts for NH3-SCR at low temperature. Appl. Surf. Sci. 402, 208–217 (2017).CrossRefGoogle Scholar
Ettireddy, P.R., Ettireddy, N., Mamedov, S., Boolchand, P., and Smirniotis, P.G.: Surface characterization studies of TiO2 supported manganese oxide catalysts for low temperature SCR of NO with NH3. Appl. Catal., B 76, 123–134 (2007).CrossRefGoogle Scholar
Tang, F., Xu, B., Shi, H., Qiu, J., and Fan, Y.: The poisoning effect of Na+ and Ca2+ ions doped on the V2O5/TiO2 catalysts for selective catalytic reduction of NO by NH3. Appl. Catal., B 94, 71–76 (2010).CrossRefGoogle Scholar
Kröcher, O. and Elsener, M.: Chemical deactivation of V2O5/WO3–TiO2 SCR catalysts by additives and impurities from fuels, lubrication oils, and urea solution: I. Catalytic studies. Appl. Catal., B 77, 215–227 (2008).CrossRefGoogle Scholar
Chen, L., Li, J.H., and Ge, M.: The poisoning effect of alkali metals doping over nano V2O5–WO3/TiO2 catalysts on selective catalytic reduction of NOx by NH3. Chem. Eng. J. 170, 531–537 (2011).CrossRefGoogle Scholar
Wan, Q., Duan, L., Li, J., Chen, L., He, K., and Hao, J.: Deactivation performance and mechanism of alkali (earth) metals on V2O5–WO3/TiO2 catalyst for oxidation of gaseous elemental mercury in simulated coal-fired flue gas. Catal. Today 175, 189–195 (2011).CrossRefGoogle Scholar
Castellino, F., Jensen, A.D., Johnsson, J.E., and Fehrmann, R.: Influence of reaction products of K-getter fuel additives on commercial vanadia-based SCR catalysts part I. Potassium phosphate. Appl. Catal., B 86, 196–205 (2009).CrossRefGoogle Scholar
Zheng, Y.J., Jensen, A.D., Johnsson, J.E., and Thogersen, J.R.: Deactivation of V2O5–WO3–TiO2 SCR catalyst at biomass fired power plants: Elucidation of mechanisms by lab and pilot-scale experiments. Appl. Catal., B 83, 186–194 (2008).CrossRefGoogle Scholar
Kong, M., Liu, Q., Zhou, J., Jiang, L., Tian, Y., Yang, J., Ren, S., and Li, J.: Effect of different potassium species on the deactivation of V2O5–WO3/TiO2 SCR catalyst: Comparison of K2SO4, KCl, and K2O. Chem. Eng. J. 348, 637–643 (2018).CrossRefGoogle Scholar
Gao, F., Tang, X., Yi, H., Zhao, S., Wang, J., Shi, Y., and Meng, X.: Novel Co-or Ni–Mn binary oxide catalysts with hydroxyl groups for NH3-SCR of NOx at low temperature. Appl. Surf. Sci. 443, 103–113 (2018).CrossRefGoogle Scholar
Zamudio, M.A., Russo, N., and Fino, D.: Low temperature NH3 selective catalytic reduction of NOx over substituted MnCr2O4 spinel-oxide catalysts. Ind. Eng. Chem. Res. 11, 6668–6672 (2011).CrossRefGoogle Scholar
Liu, Z., Zhu, J., Li, J., Ma, L., and Woo, S.I.: Novel Mn–Ce–Ti mixed-oxide catalyst for the selective catalytic reduction of NOx with NH3. ACS Appl. Mater. Interfaces 16, 14500–14508 (2014).CrossRefGoogle Scholar
Wei, Y., Liu, J., Su, W., Sun, Y., and Zhao, Y.: Controllable synthesis of Ce-doped α-MnO2 for low-temperature selective catalytic reduction of NO. Catal. Sci. Technol. 7, 1565–1572 (2017).CrossRefGoogle Scholar
Yang, S., Qi, F., Xiong, S., Dang, H., Liao, Y., Wong, P.K., and Li, J.: MnOx supported on Fe–Ti spinel: A novel Mn based low temperature SCR catalyst with a high N2 selectivity. Appl. Catal., B 181, 570–580 (2016).CrossRefGoogle Scholar
Ying, W., Hao, F., and Rui, W.: Transition metals (Co, Zr, Ti) modified iron-samarium oxide as efficient catalysts for selective catalytic reduction of NOx at low-temperature. Appl. Surf. Sci. 459, 63–73 (2018).Google Scholar
Liu, Y., Kang, Y., Mu, B., and Wang, A.: Attapulgite/bentonite interactions for methylene blue adsorption characteristics from aqueous solution. Chem. Eng. J. 237, 403–410 (2014).CrossRefGoogle Scholar
Zhou, X., Huang, X., Xie, A., Luo, S., Yao, C., Li, X., and Zuo, S.: V2O5-decorated Mn–Fe/attapulgite catalyst with high SO2 tolerance for SCR of NOx with NH3 at low temperature. Chem. Eng. J. 326, 1074–1085 (2017).CrossRefGoogle Scholar
Luo, S., Zhou, W., Xie, A., Wu, F., Yao, C., Li, X., Zuo, S., and Liu, T.: Effect of MnO2 polymorphs structure on the selective catalytic reduction of NOx with NH3 over TiO2–Palygorskite. Chem. Eng. J. 286, 291–299 (2016).CrossRefGoogle Scholar
Liu, F., Shan, W., Lian, Z., Xie, L., Yang, W., and He, H.: Novel MnWOx catalyst with remarkable performance for low temperature NH3-SCR of NOx. Catal. Sci. Technol. 10, 2699–2707 (2013).CrossRefGoogle Scholar
Shan, W., Liu, F., He, H., Shi, X., and Zhang, C.: A superior Ce–W–Ti mixed oxide catalyst for the selective catalytic reduction of NOx with NH3. Appl. Catal., B 115, 100–106 (2012).CrossRefGoogle Scholar
Qiu, L., Pang, D., Zhang, C., Meng, J., Zhu, R., and Ouyang, F.: In situ IR studies of Co and Ce doped Mn/TiO2 catalyst for low-temperature selective catalytic reduction of NO with NH3. Appl. Surf. Sci. 357, 189–196 (2015).CrossRefGoogle Scholar
Słoczyński, J., Janas, J., Machej, T., Rynkowski, J., and Stoch, J.: Catalytic activity of chromium spinels in SCR of NO with NH3. Appl. Catal., B 24, 45–60 (2000).CrossRefGoogle Scholar
Gao, C., Shi, J-W., Fan, Z., Yu, Y., Chen, J., Li, Z., and Niu, C.: Eu–Mn–Ti mixed oxides for the SCR of NOx with NH3: The effects of Eu-modification on catalytic performance and mechanism. Fuel Process. Technol. 167, 322–333 (2017).CrossRefGoogle Scholar
Putluru, S.R., Schill, L., Jensen, A.D., Siret, B., Tabaries, F., and Fehrmann, R.: Mn/TiO2 and Mn–Fe/TiO2 catalysts synthesized by deposition precipitation-promising for selective catalytic reduction of NO with NH3 at low temperatures. Appl. Catal., B 165, 628–635 (2015).CrossRefGoogle Scholar
Li, Y., Li, Y., Wang, P., Hua, W., Zhang, S., Shi, Q., and Zhan, S.: Low-temperature selective catalytic reduction of NOx with NH3 over MnFeOx nanorods. Chem. Eng. J. 330, 213–222 (2017).CrossRefGoogle Scholar
Chen, Q-L., Guo, R-T., Wang, Q-S., Pan, W-G., Wang, W-H., Yang, N-Z., Lu, C-Z., and Wang, S-X.: The catalytic performance of Mn/TiWOx catalyst for selective catalytic reduction of NOx with NH3. Fuel 181, 852–858 (2016).CrossRefGoogle Scholar
Liu, R., Jiang, Y-W., Fan, H., Lu, Q., and Gao, F.: Metal ions induce growth and magnetism alternation of α-Fe2O3 crystals bound by high-index facets. Chem.–Eur. J. 18, 8957–8963 (2012).CrossRefGoogle ScholarPubMed
Fang, D., Xie, J., Mei, D., Zhang, Y., He, F., Liu, X., and Li, Y.: Effect of CuMn2O4 spinel in Cu–Mn oxide catalysts on selective catalytic reduction of NOx with NH3 at low temperature. RSC Adv. 49, 25540–25551 (2014).CrossRefGoogle Scholar
Guo, R-T., Li, M-Y., Sun, P., Liu, S.M., Wang, S-X., Pan, W-G., Liu, S-W., Liu, J., and Sun, X.: The enhanced resistance to P species of an Mn–Ti catalyst for selective catalytic reduction of NOx with NH3 by the modification with Mo. RSC Adv. 32, 19912–19923 (2017).CrossRefGoogle Scholar
Cai, S-X., Liu, J., Zha, K-W., Li, H.R., Shi, L-Y., and Zhang, D-S.: A general strategy for the in situ decoration of porous Mn–Co bi-metal oxides on metal mesh/foam for high performance de-NOx monolith catalysts. Nanoscale 9, 5648–5657 (2017).CrossRefGoogle ScholarPubMed
Xu, Q., Su, R-G., Cao, L., Li, Y-Q., Yang, C-Y., Luo, Y., Street, J., Jiao, P-C., and Ca, L-L.: Facile preparation of high-performance Fe-doped Ce–Mn/TiO2 catalysts for the low-temperature selective catalytic reduction of NOx with NH3. RSC Adv. 7, 48785–48792 (2017).CrossRefGoogle Scholar
Chen, L-Q., Li, R., Li, Z-B., Yuan, F-L., Niu, X-Y., and Zhu, Y-J.: Effect of Ni doping in NixMn1−xTi10 (x = 0.1–0.5) on activity and SO2 resistance for NH3-SCR of NO studied with in situ DRIFTS. Catal. Sci. Technol. 7, 3243–3257 (2017).CrossRefGoogle Scholar
Shu, Y., Sun, H., Quan, X., and Chen, S.: Enhancement of catalytic activity over the iron-modified Ce/TiO2 catalyst for selective catalytic reduction of NOx with ammonia. J. Phys. Chem. C 116, 25319–25327 (2012).CrossRefGoogle Scholar
Huang, X-Y., Xie, A-J., Zhou, X-M., Xia, J-W., Luo, S-P., Yao, C., and Li, X-Z.: Fabrication of γ-MnO2–Ce pillared montmorillonite for low temperature NH3-SCR. Z. Phys. Chem. 232, 1755–1769 (2018).CrossRefGoogle Scholar
Huang, X-Y., Xie, A-J., Wu, J-Y., Xu, L-J., Luo, S-P., Xia, J-W., Yao, C., and Li, X-Z.: Cerium modified MnTiOx/attapulgite catalyst for low-temperature selective catalytic reduction of NOx with NH3. J. Mater. Res. 33, 3559–3569 (2018).CrossRefGoogle Scholar
Guo, R-T., Wang, Q-S., Pan, W-G., and Zhen, W-L.: The poisoning effect of Na and K on Mn/TiO2 catalyst for selective catalytic reduction of NO with NH3: A comparative study. Appl. Surf. Sci. 317, 111–116 (2014).CrossRefGoogle Scholar
Kamata, H., Takahashi, K., and Odenbrand, C.U.: The role of K2O in the selective reduction of NO with NH3 over a V2O5(WO3)/TiO2 commercial selective catalytic reduction catalyst. J. Mol. Catal. A: Chem. 139, 189–198 (1999).CrossRefGoogle Scholar
Jiang, B-Q., Deng, B-Y., Zhang, Z-Q., and Wu, Z-L.: Effect of Zr addition on the low-temperature SCR activity and SO2 tolerance of Fe–Mn/Ti catalysts. J. Phys. Chem. C 118, 14866–14875 (2014).CrossRefGoogle Scholar
Roy, S., Viswanath, B., Hegde, M.S., and Madras, G.: Low-temperature selective catalytic reduction of NO with NH3 over Ti0.9M0.1O2−δ (M = Cr, Mn, Fe, Co, Cu). J. Phys. Chem. C 112, 6002–6012 (2008).CrossRefGoogle Scholar
Zheng, Y., Jensen, A-D., and Johnsson, J.E.: Deactivation of V2O5–WO3–TiO2 SCR catalyst at a biomass-fired combined heat and power plant. Appl. Catal., B 60, 253–264 (2005).CrossRefGoogle Scholar
Kustov, A-L., Rasmussen, S-B., Fehrmann, R., and Simonsen, P.: Activity and deactivation of sulphated TiO2- and ZrO2-based V, Cu, and Fe oxide catalysts for NO abatement in alkali containing flue gases. Appl. Catal., B 76, 9–14 (2007).CrossRefGoogle Scholar
Wang, W., Wang, F., Kang, Y., and Wang, A-Q.: Enhanced adsorptive removal of methylene blue from aqueous solution by alkali-activated palygorskite. Water, Air, Soil Pollut. 226, 9–13 (2015).CrossRefGoogle Scholar
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