Preparation and Catalytic Performance of Bowl-shaped Amphiphilic ZSM-5 Zeolites Supported Gold Nanoparticles †

doi:10.7503/cjcu20190415

Abstract

Abstract:

Bowl-shaped amphiphilic ZSM-5 zeolites, which have a lipophilic outer surface and a modified hydrophilic inner surface, were prepared by asymmetric modification via a classical amino graft-in situ reduction process. The gold nanoparticles were selectively grown on the inner surface of the zeolites. The samples were characterized by means of XRD, SEM, TEM, IR and XPS, and their catalytic properties for hydrogenation of nitrobenzene to aniline were investigated. Under very mild conditions(room temperature, water as solvent, without nitrogen protection) and lower reactant concentration(0.03 mol/L, lower than the solubility of nitrobenzene in water at room temperature), the catalyst exhibited the same catalytic activity and selectivity as other catalysts using organic solvents, and was significantly higher than other catalysts using water as catalyst. The amphiphilic structure of the support was proved to be the main reason for improving the catalytic effect. After six cycles, the catalytic activity and selectivity of the catalyst remained at the same level.

Key words: Gold nanoparticles, ZSM-5 zeolite, Asymmetric modification, Selective catalysis, Nitrobenzene

CLC Number:

O613.72
O643

TrendMD:

Siqi SUN,Ying WANG,Chuanyin SUN,Runwei WANG,Zhendong ZHANG,Zongtao ZHANG,Shilun QIU. Preparation and Catalytic Performance of Bowl-shaped Amphiphilic ZSM-5 Zeolites Supported Gold Nanoparticles ^†[J]. Chem. J. Chinese Universities, 2019, 40(12): 2436.

Figures/Tables 10

Scheme 1 Synthetic process of the samples

Fig.1 Powder XRD patterns of ZSM-5(A), etched-ZSM-5(B), E-ZSM-5(C) and Au/E-ZSM-5(D)

Fig.2 IR spectra of ZSM-5(a), lipophilic-ZSM-5(b) and etched-ZSM-5(c)

Fig.3 Carbon content of lipophilic-ZSM-5 with different silane amounts

Fig.4 SEM images of ZSM-5(A) and etched-ZSM-5 with different etching time Etching time/min: (B) 10; (C) 20; (D) 30; (E) 45; (F) 60.

Fig.5 TEM images of Au/E-ZSM-5(A), L-Au/E-ZSM-5(B) and Au/LE-ZSM-5(C)

Fig.6 Au4f XPS spectra of Au/E-ZSM-5

Fig.7 Catalytic performance of the samples

Fig.8 Schematic illustration of reduction of nitrobenzene(NB) with Au/E-ZSM-5 as catalyst

Catalyst(mass)	Reaction condition	Yield(%)	Selectivity(%)	Ref.
Au/E-ZSM-5(10 mg)	1 mmol NB+3 mmol NaBH₄, 25 min, 35 mL H₂O	99	100	This work
L-Au/E-ZSM-5(10 mg)	1 mmol NB+3 mmol NaBH₄, 25 min, 35 mL H₂O	2		This work
Au/ZSM-5(10 mg)	1 mmol NB+3 mmol NaBH₄, 25 min, 35 mL H₂O	20		This work
Bimetallic Au-Ag/m-SBA-15(5 mg)	0.01 mmol NB+1 mmol NaBH₄, 120 min, 10 mL EtOH	99		[10]
Ag/γ-Fe₂O₃(not mentioned)	5 mmol NB+0.5 mL hydrated hydrazine, 180 min, 10 mL EtOH, 80 ℃	70	80	[24]
C@Fe₃O₄@Pd(20 mg)	1 mmol NB+3 mmol NaBH₄, 30 min, 6 mL EtOH	99	99	[25]
Co-Ag(1:1)@NC(not mentioned)	0.5 mmol NB+2 mmol hydrated hydrazine, 60 min, 5 mL EtOH	ca. 100	100	[33]

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