Effect of the modification of alumina supports with chloride on the structure and catalytic performance of Ag/Al2O3 catalysts for the selective catalytic reduction of NOx with propene and H2/propene

doi:10.1016/S1872-2067(21)63904-9

Abstract

Abstract:

The effect of the modification of an alumina support with chloride on the structure and the catalytic performance of Ag/Al₂O₃ catalysts (SA) was investigated for the selective catalytic reduction (SCR) of NO using C₃H₆ or H₂/C₃H₆ as reductants. The Ag/Al₂O₃ catalyst and Cl^--modified Ag/Al₂O₃ catalysts (SA-Cl) were prepared by a conventional impregnation method and characterized by X-ray diffraction, Brunauer-Emmett-Teller isotherm analysis, electron probe microanalysis, transmission electron microscopy, UV-Vis diffuse reflectance spectroscopy, X-ray photoelectron spectroscopy, and hydrogen temperature-programmed reduction. The catalytic activities in the C₃H₆-SCR and H₂/C₃H₆-SCR reactions were evaluated, and the reaction mechanism was studied using in situ diffuse reflectance infrared Fourier transform spectroscopy and synchrotron vacuum ultraviolet photoionization mass spectroscopy (SVUV-PIMS). We found that Cl^- modification of the alumina-supported Ag/Al₂O₃ catalysts facilitated the formation of oxidized silver species (Ag_n^ᵟ+) that catalyze the moderate-temperature oxidation of hydrocarbons into partial oxidation products (mainly acetate species) capable of participating in the SCR reaction. The low-temperature promoting effect of H₂ on the C₃H₆-SCR ("hydrogen effect") was found to originate from the enhanced decomposition of strongly adsorbed nitrates on the catalyst surface and the conversion of these adsorbed species to -NCO and -CN species. This "H₂ effect" occurs in the presence of Ag_n^ᵟ+ species rather than the metallic Ag⁰ species. A gaseous intermediate, acrylonitrile (CH₂CHCN), was also identified in the H₂/C₃H₆-SCR reaction using SVUV-PIMS. These findings provide novel insights in the structure-activity relationship and reaction mechanisms of the SA-catalyzed HC-SCR reaction of NO.

Key words: In situ characterization, Reaction mechanism, Structure-activity relation, DRIFTS, Photoionization mass spectroscopy

Jia Wang, Rui You, Kun Qian, Yang Pan, Jiuzhong Yang, Weixin Huang. Effect of the modification of alumina supports with chloride on the structure and catalytic performance of Ag/Al₂O₃ catalysts for the selective catalytic reduction of NO_x with propene and H₂/propene[J]. Chinese Journal of Catalysis, 2021, 42(12): 2242-2253.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63904-9

https://www.cjcatal.com/EN/Y2021/V42/I12/2242

Figures/Tables 13

Fig. 1. NOx (a) and C3H6 (b) conversion as a function of reaction temperature during the C3H6-SCR of NO catalyzed by SA and SA-Cl catalysts.

Fig. 2. XRD patterns of various catalysts after calcination at 600 °C for 3 h.

Fig. 3. STEM (left), particle size distributions (middle) and HRTEM images (right) of the 2SA, 4SA, 2SA-Cl, and 4SA-Cl catalysts. Scale bar in the STEM images is 100 nm.

Fig. 4. UV-Vis DRS spectra of the SA and SA-Cl catalysts.

Fig. 5. H2-TPR profiles of Al2O3 supports and SA and SA-Cl catalysts.

Fig. 6. Ag 3d XPS spectra (dashed lines) of 2SA (a), 4SA (b), 2SA-Cl (c), and 4SA-Cl (d) catalysts and fitted Ag 3d5/2 peaks consisting of Ag+ and Ag0 components. The ratio of Ag+ is indicated in each panel.

Fig. 7. In situ DRIFTS spectra of γ-Al2O3 (a), 2SA (b), (c) 4SA, and (d) 4SA-Cl catalysts at the steady-state during the NO + O2 reaction (1000 ppm NO, 10% O2, Ar in balance, total flow: 50 mL/min) at 200 °C (black line), 300 °C (red line), and 400 °C (blue line).

Table 1 Assignment of observed vibrational bands in the in situ DFIFTS spectra.

Wavenumber (cm^-1)	Surface species	Ref.
1303, 1540, 1558	Monodentate nitrates	[51-54,56-58]
1582-1590	Bidentate nitrates	[51,52,57,59]
1614	Bridge-bound nitrates	[53,58,59]
1298-1300, 1526-1535	Carbonates	[60,61]
1376, 1392, 1588-1592, 2906, 3000	Formate	[60,61]
1454, 1580-1585, 2942	Acetate	[5,6,61,77]
1458, 1575	Carboxylate	[63,64]
1454-1458, 1561-1575, 1630-1643	Acrylate	[60]
2152	Cyanide (CN^-)	[60,74]
2230	Isocyanate	[15,16,60,74]
2340	Gas-phase CO₂	[79]

Fig. 8. In situ DRIFTS spectra of γ-Al2O3 (a,b), 2SA (c,d), 4SA (e,f), and 4SA-Cl (g,h) catalysts obtained during the steady-state C3H6 + O2 reaction (1500 ppm C3H6, 10% O2, Ar in balance, total flow: 50 mL/min) at 200 °C (black line), 300 °C (red line), and 400 °C (blue line).

Fig. 9. Time-resolved in situ DRIFTS spectra of (a,b) 4SA and (c,d) 4SA-Cl catalysts with surface intermediates formed under steady-state C3H6 + O2 reaction exposed to NO + O2 flow at 500 °C.

Fig. 10. NOx conversion over γ-Al2O3 (a), 2SA (b), 4SA (c), and 4SA-Cl (d) catalysts in the SCR process with and without H2. (1000 ppm NO, 1500 ppm C3H6, 0 or 1000 ppm H2, 10% O2, Ar in balance, total flow: 50 mL/min).

Fig. 11. In situ DRIFTS spectra of 2SA (a,b), 4SA (c,d), and 4SA-Cl (e,f) catalysts in the SCR process with and without H2 at 300 °C (1000 ppm NO, 1500 ppm C3H6, 0 or 1000 ppm H2, 10% O2, Ar in balance, total flow: 50 mL/min).

Fig. 12. SVUV-PIMS spectra of the gas-phase components in the (a) C3H6-SCRS and (b) H2/C3H6-SCR reactions at 300 °C catalyzed by 4SA ionized at a photon energy of 11.8 eV and in the H2/C3H6-SCR reactions at 300 °C catalyzed by 4SA-Cl ionized at photon energies of (c) 11.8 and (d) 10.6 eV.

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Effect of the modification of alumina supports with chloride on the structure and catalytic performance of Ag/Al₂O₃ catalysts for the selective catalytic reduction of NO_x with propene and H₂/propene

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