高等学校化学学报 ›› 2021, Vol. 42 ›› Issue (1): 11.doi: 10.7503/cjcu20200476
所属专题: 分子筛功能材料 2021年,42卷,第1期
王健羽1,张强1,闫文付1,于吉红1,2
收稿日期:
2020-07-21
出版日期:
2021-01-10
发布日期:
2021-01-12
基金资助:
WANG Jianyu1, ZHANG Qiang1, YAN Wenfu1, YU Jihong1,2()
Received:
2020-07-21
Online:
2021-01-10
Published:
2021-01-12
Contact:
YU Jihong
E-mail:jihong@jlu.edu.cn
Supported by:
摘要:
沸石分子筛由于具有独特的形选催化作用及可调的酸性, 已成为化学工业中最重要的固体催化材料. 沸石分子筛的合成主要基于碱性条件下的水热晶化, OH?被认为起到催化硅铝物种的解聚及聚合作用. 近年来, 研究者发现了羟基自由基加速分子筛的水热晶化机制. 通过利用紫外光照射或芬顿反应等物理或化学方法向分子筛合成体系引入羟基自由基, 可以实现沸石分子筛的加速晶化及高硅沸石分子筛的合成. 理论计算结果表明, 羟基自由基可以促进Si—O—Si 键的断裂和重新生成, 从而显著加快分子筛成核并促进硅原子进入骨架. 本综述介绍了羟基自由基在沸石分子筛晶化方面的最新研究进展, 探讨了羟基自由基的主要作用和优势, 并对沸石分子筛合成的羟基自由基路线发展前景进行了展望.
中图分类号:
TrendMD:
王健羽, 张强, 闫文付, 于吉红. 羟基自由基在沸石分子筛合成中的作用. 高等学校化学学报, 2021, 42(1): 11.
WANG Jianyu, ZHANG Qiang, YAN Wenfu, YU Jihong. Roles of Hydroxyl Radicals in Zeolite Synthesis. Chem. J. Chinese Universities, 2021, 42(1): 11.
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.7 Schematic illustration of the isomorphous substitution of Ge with Si under neutral conditions and room temperature[21]Copyright 2019, the Royal Society of Chemistry.
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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