Roles of Hydroxyl Radicals in Zeolite Synthesis

doi:10.7503/cjcu20200476

Abstract

Abstract:

Zeolites have been widely utilized in chemical industry as the most important solid catalysts because of their tunable acidities and shape selective catalysis. Synthesis of zeolites is usually performed via hydrothermal crystallization in a strong basic medium. Hydroxide ions（OH^?） are considered to catalyze the depolymerization and polymerization of the silicate and aluminate species. Recently， it was found that the hydroxyl radicals（·OH） existed in the hydrothermal synthesis system. By using physical or chemical methods such as ultraviolet irradiation and Fenton’s reagent， ·OH radicals can be introduced into the zeolite synthesis system， which remarkably accelerated the zeolite crystallization and promoted the formation of zeolites with higher SiO₂/Al₂O₃ ratio. Density functional theory calculations demonstrated that ·OH radicals significantly facilitated the depolymerization of the aluminosilicate gel by breaking the Si—O—Si bonds and the polymerization of the aluminosilicate anions around the hydrated cation species by remaking the Si—O—Si bonds， thus speeding up the nucleation and favoring Si incorporation into the zeolite frameworks. This review summarizes the recent progress in the application of ·OH radicals in the synthesis of zeolites， with an emphasis on the role and advantage of ·OH radicals in zeolite crystallization. The future perspective of the ·OH radical route for the synthesis of zeolites is pointed out.

Key words: Zeolite, ·OH radical, Hydrothermal synthesis, Silica to alumina ratio

CLC Number:

O611.4

TrendMD:

WANG Jianyu, ZHANG Qiang, YAN Wenfu, YU Jihong. Roles of Hydroxyl Radicals in Zeolite Synthesis[J]. Chem. J. Chinese Universities, 2021, 42(1): 11.

Figures/Tables 8

Fig.1 EPR spectra of DMPO?·OH adduct and BMPO?·OH adduct

Fig.2 Crystallization curves of zeolite NaA under UV conditions with different irradiances(A); comparison of simulated and experimental EPR spectra of DMPO?·OH adduct(a), DMPO?·Si adduct(b), and oxidized DMPO radicals(c), EPR spectrum of initial synthesis gel containing BMPO after 10 h under dark condition(d)(B); reactions of OH-(C) and ·OH(D) with [SiO2(OH)―O―SiO3]Na5 system and Gibbs free energy profiles for the reaction of OH-(blue) and ·OH(red) with [SiO2(OH)―O―SiO3]Na5 system(E)[14]Copyright 2016, American Association for the Advancement of Science.

Fig.3 Accelerated synthesis of zeolites under Gamma rays(γ?rays) irradiation(A) and Gibbs free energy profiles for the depolymerization of silicate by ·OH radicals(blue) and OH-(red)(B)[15]Copyright 2020, Wiley?VCH.

Fig.4 Schematic illustration of ·OH radical?assisted route for the synthesis of silicalite?1 in the presence of sodium persulfate(A) and yield of products with different amounts of TPAOH and sodium persulfate(B)[16]Copyright 2018, the Royal Society of Chemistry.

Fig.6 Characterizations of zeolite Y synthesized via conventional route(Y?0) and ·OH radical?assisted route(Y?R)(A—F); optimized geometries of the structures(G, H) and Gibbs free energy profiles(I, J) for condensation of the radicals with Al(OH)4Na(orange) and Si(OH)3ONa(blue)[20](A) XRD patterns; (B) N2 adsorption?desorption isotherms; (C, D) SEM images; (E, F) 29Si MAS NMR spectra. These results indicated that zeolite Y synthesized via conventional and ·OH radical?assisted routes are similar in the crystallinities, textural properties and morphologies.Copyright 2020, Wiley?VCH.

Fig.8 Characterizations of SBA?15 samples synthesized under different conditions(A—P); hydrolysis reactions of TEOS catalyzed by ·OH radicals(Q) and Gibbs free energy profiles for the attack of ·OH to TEOS(R)[22](A)―(D) Under UV irradiation; (E)―(H) without addition of radicals or acid; (I)―(L) with addition of Na2S2O8; (M)―(P) with addition of Fenton’s reagents.Copyright 2018, American Chemical Society.

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