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Catalysts 2017, 7, 367 Catalysts 2017, 7, 367 Catalysts 2017, 7, 367 23 of 31 22 of 29 22 of 29 Figure 19. NH3-TPD profiles (a); and GGR variation of n-dodecane cracking (b) over Figure 19. NH3-TPD profiles (a); and GGR variation of n-dodecane cracking (b) over Figure 19. NH3-TPD profiles (a); and GGR variation of n-dodecane cracking (b) over ◦ phosphorus-modified ZSM-5 zeolites for 30 min at 550 °C under the pressure of 4 MPa: (a) ZSM-5-0 phosphorus-modified ZSM-5 zeolites for 30 min at 550 C under the pressure of 4 MPa: (a) ZSM-5-0 P; phosphorus-modified ZSM-5 zeolites for 30 min at 550 °C under the pressure of 4 MPa: (a) ZSM-5-0 (bP);Z(SbM)-Z5S-0M.2-5-P0;.2(5c)PZ;SM(c)-5Z-0S.M5P-5;-(0d.)5ZPS;M(d-5)-1ZPS;M(e-5)-Z1SMP;-5(e-2)PZ;SaMnd-5(-f2)ZP;SMan-d5-3(fP)[Z11S8M].-5C-o3pPyri[g11h8t]. P; (b) ZSM-5-0.25 P; (c) ZSM-5-0.5 P; (d) ZSM-5-1 P; (e) ZSM-5-2 P; and (f) ZSM-5-3 P [118]. ElCseovpiyeri,g2h0t1E7.lsevier, 2017. Copyright Elsevier, 2017. 5.3. Surface Acid Sites 5.3. Surface Acid Sites 5.3. Surface Acid Sites Too many acid sites on the external surface of ZSM-5 zeolite could lead to large carbon Too many acid sites on the external surface of ZSM-5 zeolite could lead to large carbon deposition Too many acid sites on the external surface of ZSM-5 zeolite could lead to large carbon deposition on the external surface during the catalytic reactions, which would cover the surface or on the external surface during the catalytic reactions, which would cover the surface or block the pore deposition on the external surface during the catalytic reactions, which would cover the surface or block the pore mouth. Then, the acid sites in the micropores cannot catalyze the reactants effectively, mouth. Then, the acid sites in the micropores cannot catalyze the reactants effectively, resulting in block the pore mouth. Then, the acid sites in the micropores cannot catalyze the reactants effectively, resulting in quick deactivation. Thus, the catalytic activity can be enhanced by passivating the acid quick deactivation. Thus, the catalytic activity can be enhanced by passivating the acid sites on the resulting in quick deactivation. Thus, the catalytic activity can be enhanced by passivating the acid sites on the external surface. external surface. sites on the external surface. A post-synthetic HNO3 treatment method was developed to selectively remove the acid sites on Apost-syntheticHNO treatmentmethodwasdevelopedtoselectivelyremovetheacidsiteson 3 A post-synthetic HNO3 treatment method was developed to selectively remove the acid sites on the external surface [124]. As a result, the treated ZSM-5 zeolite maintained high catalytic activity the external surface [124]. As a result, the treated ZSM-5 zeolite maintained high catalytic activity the external surface [124]. As a result, the treated ZSM-5 zeolite maintained high catalytic activity −1 (about 96%) with little carbon deposition (49.7 mg·−g1 ) even after reaction for 455 min, while, for the (about 96%) with little carbon deposition (49.7 mg·g−1 ) even after reaction for 455 min, while, for the (about96%)withlittlecarbondeposition(49.7mg·g )evenafterreactionfor455min,while,forthe parent ZSM-5 zeolite, the conversion decreased to about 67% with large carbon deposition (−1120 parent ZSM-5 zeolite, the conversion decreased to about 67% with large carbon deposition (120 mg·g ) parent ZSM-5 zeolite, the conversion decreased to about 67% with large carbon deposition (120 mg·g−1) (Figure 20). However, this method is only effective to treat zeolite prepared in the absence of (Figu−r1e 20). However, this method is only effective to treat zeolite prepared in the absence of organic mg·g ) (Figure 20). However, this method is only effective to treat zeolite prepared in the absence of organic structure-directing agent (OSDA). For zeolite prepared with the assistance of OSDA, not structure-directing agent (OSDA). For zeolite prepared with the assistance of OSDA, not only the organic structure-directing agent (OSDA). For zeolite prepared with the assistance of OSDA, not only the external surface Al but also large framework Al would be dissolved by HNO3 treatment. externalsurfaceAlbutalsolargeframeworkAlwouldbedissolvedbyHNO treatment. 3 only the external surface Al but also large framework Al would be dissolved by HNO3 treatment. Figure 20. Hexane conversion and product yield (mol %) for hexane cracking over zeolite catalysts at Figure 20. Hexane conversion and product yield (mol %) for hexane cracking over zeolite catalysts at Figure 20. Hexane conversion and product yield (mol %) for hexane cracking over zeolite catalysts 650 °C. The catalysts are: (a) parent H+-ZSM-5 OSDAF (Si/Al = 16.4); and (b) deAl(6.0)-ZSM-5 (Si/Al = ◦++ 650 °C. The catalysts are: (a) parent H -ZSM-5 OSDAF (Si/Al = 16.4); and (b) deAl(6.0)-ZSM-5 (Si/Al = at 650 C. The catalysts are: (a) parent H -ZSM-5 OSDAF (Si/Al = 16.4); and (b) deAl(6.0)-ZSM-5 22.6). W/F = 19.8 g-cat. h mol−1, and partial pressure of hexane = 5 kPa. BTX means the mixture of −1 −1 2(S2i.6/)A. Wl =/F22=.61)9..8Wg/-Fca=t.1h9.m8ogl-ca,ta.nhdmpaorltia,lapnrdespsuaretiaolfphrexsasnuere=o5f hkePxaa.nBeT=X5mkePaan.sBthTeXmiexatunrsethofe benzene, toluene and xylenes [124]. Copyright American Chemical Society, 2013. bmenixzteunre,otfoblueennzenaen,dtoxlyulenesan[1d24x]y.lCenoepsy[r1ig24h]t.ACmopeyrirciganhtCAhmemeriiccaalnSoCchietmy,ic2a0l1S3o.ciety, 2013. Rimer et al. [38] designed ZSM-5 zeolite with passivated surface acidity by adding silicalite-1 Rimer et al. [38] designed ZSM-5 zeolite with passivated surface acidity by adding silicalite-1 shell on the external surface. Few acid sites exist on the external surface of ZSM-5 zeolite after shell on the external surface. Few acid sites exist on the external surface of ZSM-5 zeolite afterPDF Image | Strategies to Enhance the Catalytic Performance of ZSM-5
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