Browse > Article
http://dx.doi.org/10.7464/ksct.2013.19.1.065

Catalytic Nitrate Reduction in Water over Mesoporous Silica Supported Pd-Cu Catalysts  

Kim, Min-Sung (Department of Chemical and Biological Engineering, Korea University)
Chung, Sang-Ho (Department of Chemical and Biological Engineering, Korea University)
Lee, Myung Suk (Department of Chemical and Biological Engineering, Korea University)
Lee, Dae-Won (Department of Chemical and Biological Engineering, Korea University)
Lee, Kwan-Young (GREEN SCHOOL, Korea University)
Publication Information
Clean Technology / v.19, no.1, 2013 , pp. 65-72 More about this Journal
Abstract
In this study, we investigated the activity of Pd and Cu co-incorporated on mesoporous silica support such as MCM-41 and SBA-15 for catalytic nitrate reduction in water. In pure hydrogen flow, nitrate concentration was gradually decreased with the reaction time, but nitrogen selectivity was too low due to very high pH of reaction medium after the reaction. In order to acquire high nitrogen selectivity, we utilized carbon dioxide as a pH buffer, which resulted in higher nitrogen selectivity (about 40%). For the above reaction conditions, Pd-Cu/MCM-41 showed better performance than Pd-Cu/SBA-15. The physicochemical properties of both catalysts were investigated to figure out the relationship between the characteristics of the catalysts and the catalytic activity on the catalytic nitrate reduction by $N_2$ adsoprtion-desorption, X-ray diffraction (XRD), $H_2$-temperature programmed reduction, X-ray photoelectron spectroscopy (XPS) techniques.
Keywords
Catalytic nitrate reduction; Pd-Cu/MCM-41; Pd-Cu/SBA-15; Water;
Citations & Related Records
Times Cited By KSCI : 3  (Citation Analysis)
연도 인용수 순위
1 Gasparovicova, D., Kralik, M., Hronec, M., Vallusova, Z., Vinek, H., and Corain, B., "Supported Pd-Cu Catalysts in the Water Phase Reduction of Nitrates: Functional Resin versus Alumina," J. Mol. Catal. A-Chem., 264, 93-102 (2007).   DOI   ScienceOn
2 Neyertz, C., Marchesini, F.A., Boix, A., Miro, E., and Querini, C. A., "Catalytic Reduction of Nitrate in Water: Promoted Palladium Catalysts Supported in Resin," Appl. Catal., A, 372, 40-47 (2010).   DOI   ScienceOn
3 Maia, M. P., Rodrigues, M. A., and Passos, F. B., "Nitrate Catalytic Reduction in Water Using Niobia Supported Palladium-Copper Catalysts," Catal. Today, 123, 171-176 (2007).   DOI   ScienceOn
4 Constantinou, C. L., Costa, C. N., and Efstathiou, A. M., "The Remarkable Effect of Oxygen on the $N_2$ Selectivity of Water Catalytic Denitrification by Hydrogen," Environ. Sci. Technol., 41, 950-956 (2007).   DOI   ScienceOn
5 Garron, A., Lazar, K., and Epron, F., "Effect of the Support on Tin Distribution in Pd-Sn/$Al_2O_3$ and Pd-Sn/$SiO_2$ Catalysts for Application in Water Denitration," Appl. Catal., B, 59, 57-69 (2005).   DOI   ScienceOn
6 Lee, G.-H., and Lee, G., "Effects of Operating Parameters on the Removal Performance of Nitrate-Nitrogen by Electrodialysis," Clean Technol., 15(4), 280-286 (2009).   과학기술학회마을
7 Huang, C.-P., Wang, H.-W., and Chiu, P.-C., "Nitrate Reduction by Metallic Iron," Water Res., 32(8), 2257-2264 (1998).   DOI   ScienceOn
8 Gavagnin, R., Biasetto, L., Pinna, F., and Strukul, G., "Nitrate Removal in Drinking Waters: the Effect of Tin Oxide in the Catalytic Hydrogenation of Nitrate by Pd/$SnO_2$ Catalysts," Appl. Catal., B, 38, 91-99 (2002).   DOI   ScienceOn
9 Xu, Z., Chen, L., Shao, Y., Yin, D., and Zheng, S., "Catalytic Hydrogenation of Aqueous Nitrate over Pd-Cu/$ZrO_2$ Catalysts," Ind. Eng. Chem. Res., 48, 8356-8363 (2009).   DOI   ScienceOn
10 Ryoo, W., "Reduction of Nitrate-Nitrogen by Zero-Valent Iron Nanoparticles Deposited on Aluminum via Electrophoretic Method," Clean Technol., 15(3), 194-201 (2009).   과학기술학회마을
11 Horold, S., Vorlop, K.-D., Tacke, T., and Sell, M., "Development of Catalysts for a Selective Nirate and Nitrite Removal from Drinking Water," Catal. Today, 17, 21-30 (1993).   DOI   ScienceOn
12 Barrabes, N., Just, J., Dafinov, A., Medina, F., Fierro, J. L. G., Sueiras, J. E., Salagre, P., and Cesteros, Y., "Catalytic Reduction of Nitrate on Pt-Cu and Pd-Cu on Active Carbon using Continuous Reactor. The Effect of Copper Nanoparticles," Appl. Catal., B, 62, 77-85 (2006).   DOI   ScienceOn
13 Pintar, A. and Batista, J., "Catalytic Hydrogenation of Aqueous Nitrate Solutions in Fixed-bed Reactors," Catal. Today, 53, 35-50 (1999).   DOI   ScienceOn
14 Vorlop, K.-D. and Tacke, T. "Erste Schritte auf dem Weg zur Edelmetall-katalysierten Nitrat- and Nitrit-entfernung aus Trinkwasser," Chem.-Ing.-Tech., 61(10), 836-837 (1989).   DOI
15 Chen, Y.-X., Zhang, Y., and Chen, G.-H., "Approriate Conditions or Maximizing Catalytic Reduction Efficiency of Nitrate into Nitrogen Gas in Groundwater," Water Res., 37, 2489-2495 (2003).   DOI   ScienceOn
16 Prüsse, U., and Vorlop, K.-D., "Supported Bimetallic Palladium Catalysts for Water-Phase Nitrate Reduction," J. Mol. Catal. A: Chem., 173, 313-328 (2001).   DOI   ScienceOn
17 Mikami, I., Sakamoto, Y., Yoshinaga, Y., and Okuhara, T., "Kinetic and Adsorption Studies on the Hydrogenation of Nitrate and Nitrite in Water using Pd-Cu on Active Carbon Support," Appl. Catal., B, 44, 79-86 (2003).   DOI   ScienceOn
18 Yoshinagana, Y., Akita, T., Mikami, I., and Okuhara, T., "Hydrogenation of Nitrate in Water to Nitrogen over Pd-Cu Supported on Active Carbon," J. Catal., 207, 37-45 (2002).   DOI   ScienceOn
19 Dodouche, I., Barbosa, D. P., Rangel, M. D. C., and Epron, F., "Palladium-tin Catalysts on Conducting Polymers for Nitrate Removal," Appl. Catal., B, 93, 50-55 (2009).   DOI   ScienceOn
20 Marchesini, F.A., Irusta, S., Querini, C., and Miro, E., "Nitrate Hydrogenation over Pt,In/$Al_2O_3$ and Pt,In/$SiO_2$. Effect of Aqueous Media and Catalyst Surface Properties upon the Catalytic Activity," Catal. Commun., 9, 1021-1026 (2008).   DOI   ScienceOn
21 Prusse, U., Hahnlein, M., Daum, J., and Vorlop, K.-D., "Improving the Catalytic Nitrate Reduction," Catal. Today, 55, 79-90 (2000).   DOI   ScienceOn
22 Chaplin, B. P., Roundy, E., Guy, K. A., Shapley, J. R., and Werth, C. J., "Effects of Natural Water Ions and Humic Acid on Catalytic Nitrate Reduction Kinetics Using an Alumina Supported Pd-Cu Catalyst," Environ. Sci. Technol., 40, 3075-3081 (2006).   DOI   ScienceOn
23 Gasparovicova, D., Kralik, M., Hronec, M., Biffis, A., Zecca, M., and Corain, B., "Reduction of Nitrates Dissolve in Water over Palladium-Copper Catalysts Supported on a Strong Cationic Resin," J. Mol. Catal. A: Chem., 244, 285-266 (2006).
24 Zhao, D., Feng, J., Huo, Q., Melosh, N., Fredrickson, G. H., Chmelka, B .F., and Stucky, G. D., "Triblock Copolymer Syntheses of Mesoporous Silica with Periodic 50 to 300 Angstrom Pores," Sci., 279, 548-552 (1998).   DOI   ScienceOn
25 Rodriguez, R., Pfaff, C., Melo, L., and Betancourt, P., "Characterization and Catalytic Performance of a Bimetallic Pt-Sn/ HZSM-5 Catalyst used in Denitration of Drinking Water," Catal. Today, 107-108, 100-105 (2005).
26 Chung, S.-H., Park, Y.-M., Kim, M.-S, and Lee, K.-Y., "The Effect of Textural Properties on the Hydrogenation of Succinic Acid using Palladium Incorporated Mesoporous Supports," Catal. Today, 185, 205-210 (2012).   DOI   ScienceOn
27 Beck, J. S., Beck, VartUli, J. C., Roth, W. J., Leonowicz, M. E., Kresge, C. T., Schmitt, K. D., Chu, C. T-W., Olson, D. H., Sheppard, E. W., McCullen, S. B., Higgins, J. B., and Schlenkert, J. L., "A New Family of Mesoporous Molecular Sives Prepared with Liquid Cystal Templates," J. Am. Chem. Soc., 114, 10834-10843 (1992).   DOI   ScienceOn
28 Sing, K. S. W., Everett, D. H., Haul, R. A. W., Moscou, L., Pierotti, R. A., Rouquerol, J., and Siemieniewska, T., "Reporting Physisorption Data for Gas/Solid Systems with Special Reference to the Determination of Surface Area and Porosity," Pure & Appl. Chem., 57(4), 603-619 (1985).   DOI
29 Parida, K. M., and Rath, D., "Structural Properties and Catalytic Oxidation of Benzene to Phenol over CuO-Impregnated Mesoporous Silica," Appl. Catal., A, 321, 101-108 (2007).   DOI   ScienceOn
30 Soares, O. S. G. P., Orfao, J. J. M., and Pereira, M. F., "Nitrate Reduction in Water Catalyzed by Pd-Cu on Different Supports," Desalination, 279, 367-374 (2011).   DOI   ScienceOn
31 Xiaoyuan, J., Cuanglie, L., Renxian, Z., Jianxin, M., Yu, C., and Xiaoming, Z., "Studies of Pore Structure, Temperature-programmed Reduction Performance, and Micro-Structure of CuO/$CeO_2$ Catalysts," Appl. Surf. Sci., 173, 208-220 (2001).   DOI   ScienceOn
32 Garron, A., and Epron, F., "Use of Formic Acid as Reducing Agent for Application in Catalytic Reduction of Nitrate in Water," Water Res., 39, 3073-3081 (2005).   DOI   ScienceOn
33 Cho, K. H., Park, J.-H., and Shin, C.-H., "Low Temperature CO Oxidation over Cu-Mn Mixed Oxides," Clean Technol., 16(2), 132-139 (2010).   과학기술학회마을
34 Zhu, H., Dong, L., and Chen, Y., "Effect of Titania Structure on the Properties of Its Supported Copper Oxide Catalysts," J. Colloid Interface Sci., 357, 497-503 (2011).   DOI   ScienceOn
35 Wada, K., Hirata, T., Hosokawa, S., Iwamoto, S., and Inoue, M., "Effect of Supports on Pd-Cu Bimetallic Catalysts for Nitrate and Nitrite Reduction in Water," Catal. Today, 185, 81-87 (2012).   DOI   ScienceOn
36 D'Arino, M., Pinna, F., and Strukul, G., "Nitrate and Nitrite Hydrogenation with Pd and Pt/$SnO_2$ Catalysts: The Effect of the Support Porosity and the Role of Carbon Dioxide in the Control of Selectivity," Appl. Catal., B, 53, 161-168 (2004).   DOI   ScienceOn
37 Epron, F., Gauthard, F., and Barbier, J., "Catalytic Reduction of Nitrate in Water on a Monometallic Pd/$CeO_2$ Catalyst," J. Catal., 206, 363-367 (2002).   DOI   ScienceOn
38 Gao, W., Guan, N., Chen, J., Guan, X., Jin, R., Zeng, H., Liu, Z., and Zhang, F., "Titania Supported Pd-Cu Bimetallic Catalyst for the Reduction of Nitrate in Drinking Water," Appl. Catal., B, 46, 341-351 (2003).   DOI   ScienceOn
39 Sa, J., Barrabes, N., Kleymenov, E., Lin, C., Fottinger, K., Safonova, O. V., Szlachetko, J., Bokhoven,, J. A. v., Nachtegaal, M., Urakawa, A., Crespo, G. A., and Rupprechter, G., "The Oxidation State of Copper in Bimetallic (Pt-Cu, Pd-Cu) Catalysts During Water Denitration," Catal. Sci. Technol., 2, 794-799 (2012).   DOI