Controllable Synthesis and Catalytic Applications of Hydrophobic Hybrid Zeolites†

doi:10.7503/cjcu20180560

Abstract

Abstract:

Ethyl/methyl-functionalized hybrid zeolites were synthesized using methyltriethoxysilane and ethyltriethoxysilane as organic silicon sources through rotating and static dry-gel conversion methods and characterized. The hydrophobicity of hybrid zeolites can be adjusted by synthetic routes, carbon chain length and gel composition, and hybrid zeolite with water contact angle of 124° were obtained. The catalyst prepared using hydrophobic hybrid zeolite as support showed excellent catalytic performance in the hydrogenation of phenol. It is ascribed to the aggregation of phenol molecules on the hydrophobic/lipophilic surface of catalyst that promotes the reaction efficiently.

Key words: Organic-inorganic hybrid zeolite, Controllable synthesis, Dry-gel conversion, Hydrophobicity, Hydrogenation

CLC Number:

O614
O643

TrendMD:

LI Dan, WU Zhonghan, ZHOU Dan, JIANG Ding, LU Xinhuan, XIA Qinghua. Controllable Synthesis and Catalytic Applications of Hydrophobic Hybrid Zeolites^†[J]. Chem. J. Chinese Universities, 2019, 40(7): 1359.

Figures/Tables 6

Table 1 Synthetic conditions of organic-inorganic hybrid zeolites by different DGC routes

Organic Si source	DGC route	Sample	Dry gel composition n(Al₂O₃)：n(Na₂O)：n(Si_O)：n(Si_I)：n(H₂O)^*	Si_I/Si_O	Crystal phase
ETES	Rotating	E_R-1	1.0：6.0：1.2：22.0：92.6	18.3	MOR, GIS
		E_R-2	1.0：6.0：2.3：20.9：92.6	9.1	MOR, GIS
		E_R-3	1.0：6.0：3.4：19.8：92.6	5.8	GIS, ANA
		E_R-4	1.0：6.0：4.5：18.7：92.6	4.2	ANA
	Static	E_S-1	1.0：6.0：1.2：22.0：92.6	18.3	MOR, GIS
		E_S-2	1.0：6.0：2.3：20.9：92.6	9.1	MOR, GIS
		E_S-3	1.0：6.0：3.4：19.8：92.6	5.8	GIS, ANA
		E_S-4	1.0：6.0：4.5：18.7：92.6	4.2	GIS, ANA
MTES	Rotating	M_R-1	1.0：6.0：2.3：20.9：92.6	9.1	GIS
		M_R-2	1.0：6.0：4.5：18.7：92.6	4.2	GIS
		M_R-3	1.0：6.0：6.9：16.3：92.6	2.4	GIS, ANA
		M_R-4	1.0：6.0：9.2：14.0：92.6	1.5	ANA
	Static	M_S-1	1.0：6.0：2.3：20.9：92.6	9.1	GIS
		M_S-2	1.0：6.0：4.5：18.7：92.6	4.2	GIS
		M_S-3	1.0：6.0：6.9：16.3：92.6	2.4	GIS
		M_S-4	1.0：6.0：9.2：14.0：92.6	1.5	GIS

Fig.1 XRD patterns of organic-inorganic hybrid zeolites prepared under rotating(A,C) and static(B, D) conditions, respectively, and simulated XRD patterns of inorganic MOR, GIS, and ANA structures(E)

Fig.2 SEM images of organic-inorganic hybrid zeolite samples(A1) ER-1; (B1) ES-1; (C1) MR-1; (D1) MS-1; (A2) ER-2; (B2) ES-2; (C2) MR-2; (D2) MS-2; (A3) ER-3; (B3) ES-3; (C3) MR-3; (D3) MS-3; (A4) ER-4; (B4) ES-4; (C4) MR-4; (D4) MS-4.

Fig.3 WCA of organic-inorganic hybrid zeolites samples prepared under rotating and static conditions(A) ER-1; (B) ES-1; (C) ER-2; (D) ES-2; (E) ER-3; (F) ES-3; (G) ER-4; (H) ES-4; (I) MR-4; (J) MS-4.

Fig.4 FTIR spectra of organic-inorganic hybrid zeolite samples

Fig.5 Hydrogenation of phenol over different hybrid zeolite catalystsReaction conditions: catalyst, 20 mg; phenol, 1.6 mmol; H2O,5.0 g; temperature, 130 ℃; time, 8 h; H2 pressure, 2.0 MPa.

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