Advances in Hydroxyl Free Radical Assisted Synthesis of Zeolite

doi:10.6023/A22100420

Acta Chimica Sinica ›› 2023, Vol. 81 ›› Issue (1): 100-110.DOI: 10.6023/A22100420 Previous Articles

Review

羟基自由基辅助沸石分子筛合成的研究进展

张红丹, 兰欣雨, 程鹏^*()

沈阳师范大学化学化工学院能源与环境催化研究所沈阳 110034

投稿日期:2022-10-10 发布日期:2022-11-02

作者简介:

张红丹, 博士, 沈阳师范大学化学化工学院讲师, 硕士研究生导师, 主持国家自然科学基金青年项目1项, 省部级项目2项. 主要从事微纳米材料的设计合成及光催化性能研究和多级孔沸石分子筛的制备及C4烃裂解性能的研究.

兰欣雨, 沈阳师范大学化学化工学院2020级本科生. 主要从事超大孔沸石分子筛的探索合成.

程鹏, 博士, 沈阳师范大学化学化工学院副教授, 硕士研究生导师, 主持在研及完成国家自然科学基金2项, 省自然基金1项, 省教育厅重点项目1项. 入选辽宁省“兴辽英才计划”青年拔尖人才, 辽宁省高等学校创新人才支持计划, 沈阳市科技创新人才支持计划. 主要从事沸石分子筛的绿色合成及低碳烷烃裂解性能的研究.

基金资助:
项目受国家自然科学基金(22172102); 项目受国家自然科学基金(21701117); 项目受国家自然科学基金(22202137); “兴辽英才计划”(XLYC2007190); 沈阳市中青年科技创新人才支持计划(RC210044)

Advances in Hydroxyl Free Radical Assisted Synthesis of Zeolite

Hongdan Zhang, Xinyu Lan, Peng Cheng()

Institute of Catalysis for Energy and Environment, College of Chemistry and Chemical Engineering, Shenyang Normal University, Shenyang 110034, China

Received:2022-10-10 Published:2022-11-02
Contact: ^*E-mail: chengp1987@126.com
Supported by:
National Natural Science Foundation of China(22172102); National Natural Science Foundation of China(21701117); National Natural Science Foundation of China(22202137); LiaoNing Revitalization Talents Program(XLYC2007190); Shenyang Young and Middle-aged Scientific and Technological Innovation Talents Support Plan(RC210044)

As one of the most important solid catalysts in chemical industry, zeolites are widely used in different fields. How to prepare zeolites greenly and efficiently has become a research hot issue with the increase of consumption year by year. Hydroxyl free radical is a highly active species, which can promote the depolymerization and repolymerization of aluminosilicates in the zeolite initial gel, and then accelerating the zeolite crystallization process. Besides accelerating the crystallization of zeolite, many studies have shown hydroxyl free radicals have other functions in zeolite synthesis. In this review, the role of hydroxyl free radicals in the synthesis of zeolites is systematically introduced via different generation methods. The challenges of the hydroxyl free radical assisted strategy are put forward, and its development directions are prospected.

Key words: zeolite, hydroxyl free radical, structure directing agent, synthesis, acceleration

Cite this article

Hongdan Zhang, Xinyu Lan, Peng Cheng. Advances in Hydroxyl Free Radical Assisted Synthesis of Zeolite[J]. Acta Chimica Sinica, 2023, 81(1): 100-110.

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Fig. & Tab. 11

Figure 1. Crystallization processes under UV irradiation and dark conditions at 298 K. (A~D) The experimental XRD patterns of NaX and NaZ-21 synthesized under the UV conditions (A and B, black, 4.0 mW/cm2) and dark conditions (C and D, black) for 24 h, respectively. The corresponding simulated XRD patterns are plotted for comparison (A and B, red). (E) Crystallization curves of zeolite NaA under dark conditions and under UV conditions with irradiance of 2.0, 4.0 and 8.0 mW/cm2, with a Na2O/SiO2 molar ratio of 4.4[19]

Figure 2. Schematic illustration of UV assisted synthesis of mesoporous materials[22]

Figure 3. The deoligomerization pathway of titanium oligomers with the assistance of hydroxyl free radicals[25]

Figure 4. (A) Yield of products with different crystallization times and different concentrations of sodium persulfate (SPS); (B) yield of products at different crystallization times under the conditions of different dosage of organic structure directing agent (TPAOH) and sodium persulfate concentration (0.02 mol/L)[32]

Figure 5. Schematic illustration of ?OH radical-assisted route for the synthesis of zeolite Y in the presence of Fenton’s reagent[42]

Figure 6. Schematic illustration of radicalized seed assisted synthesis of zeolite ECR-1[50]

Figure 7. Schematic illustration of ultrasonic radiation assisted synthesis of ZSM-5[55]

Figure 8. Accelerated synthesis of zeolite A under Gamma rays (γ-rays) irradiation[58]

Figure 9. Schematic illustration of H2O2 assisted synthesis of high-silica zeolite Y[59]

Figure 10. Schematic diagram of the photocatalytic reaction mechanism of the semiconductor photocatalyst accelerating zeolite synthesis[62]

产生方法	优势	局限性
紫外辐射 γ射线辐射高能电子束辐射可见光辐射	强度易于控制	制备装置要求高; 对人体有不可逆转的伤害
等离子体超声波辐射	操作简便, 强度可控	•OH产生量不可控
Fenton试剂过硫酸盐 (NH₄)₂Ce(NO₃)₆	通过控制化学试剂的加入量进而控制•OH的量(半定量)	引入杂原子, 对分子筛的制备有一定影响
H₂O₂分解	方法简单, 无杂原子干扰	分解过程受外界条件影响较大
自由基化的晶种	无外来条件的干扰, 制备过程更纯净	因分子筛结构及组成众多, 自由基化的特定条件(球磨、煅烧等)不具有普适性

Table 1. Advantages and disadvantages of different methods to produce hydroxyl free radicals in the zeolite synthesis process

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羟基自由基辅助沸石分子筛合成的研究进展

Advances in Hydroxyl Free Radical Assisted Synthesis of Zeolite

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[1]	Lingyue Yang, Yunting Li, Chao Shu. Research Progress on Sultine [J]. Acta Chimica Sinica, 2024, 82(2): 171-189.
[2]	Yi Wan, Jianghua He, Yuetao Zhang. Research Progress in Precision Polymerization of Polar Olefin Monomers by Lewis Pairs^★ [J]. Acta Chimica Sinica, 2023, 81(9): 1215-1230.
[3]	Xupan Xu, Kai Fan, Shengze Zhao, Jian Li, Shan Gao, Zhongbiao Wu, Xiangju Meng, Feng-Shou Xiao. Enhanced Performance for Mesoporous Beta Zeolites Supported Pd in the Methane Catalytic Combustion^★ [J]. Acta Chimica Sinica, 2023, 81(9): 1108-1112.
[4]	Mei Hong, Jinqiang Gao, Tong Li, Shihe Yang. In-situ Etching Strategy for Manipulation of Hierarchical Zeolite and Its Application^★ [J]. Acta Chimica Sinica, 2023, 81(8): 937-948.
[5]	Shaoyan Gan, Shengyu Zhong, Liting Wang, Lei Shi. Synthesis and Application of Organic Hypervalent Bromine Reagents [J]. Acta Chimica Sinica, 2023, 81(8): 1030-1042.
[6]	Wenshan Zheng, Guanbin Gao, Hao Deng, Taolei Sun. Room Temperature Synthesis and Near-infrared Fluorescence Performance Optimization of Ag₂Se@Ag₂S Core-shell Quantum Dots [J]. Acta Chimica Sinica, 2023, 81(7): 763-770.
[7]	Yandong Zhang, Shoufei Zhu. Perspective for Phosphine Ligands with Cyclopropane Backbone^★ [J]. Acta Chimica Sinica, 2023, 81(7): 777-783.
[8]	Li Liu, Gang Zheng, Guoqiang Fan, Hongguang Du, Jiajing Tan. Research Progress in Organic Reactions Involving 4-Acyl/Carbamoyl/Alkoxycarbonyl Substituted Hantzsch Esters [J]. Acta Chimica Sinica, 2023, 81(6): 657-668.
[9]	Kanbinuer Nuermaimaiti, Chao Wang, Shiwei Luo, Abudu Rexit Abulikemu. Research on Selective Dehalogenation of α,α,α-Trihalogen (Chloro, Bromo) methyl Ketones Under Electrochemical Conditions [J]. Acta Chimica Sinica, 2023, 81(6): 582-587.
[10]	Wang Jun, Xu Xiaomei, Zhou Jiaolong, Zhao Yanan, Sun Xiuli, Tang Yong, He Sufang, Yang Hongmei. Synthesis of New Sulfur-free and Phosphorus-free Ether-ester and Study on Its Properties As Ashless Friction Modifier [J]. Acta Chimica Sinica, 2023, 81(5): 461-468.
[11]	Junchang Chen, Mingxing Zhang, Shuao Wang. Research Progress of Synthesis Methods for Crystalline Porous Materials [J]. Acta Chimica Sinica, 2023, 81(2): 146-157.
[12]	Yang Gao, Xuexin Zhang, Jinsheng Yu, Jian Zhou. Recent Advances in Catalytic Enantioselective Synthesis of α-Chiral Tertiary Azides^★ [J]. Acta Chimica Sinica, 2023, 81(11): 1590-1608.
[13]	Xiaochen Wang, Zeyao Ji, Jian Liu, Bingfu Wang, Hui Jin, Lixin Zhang. Advances in Organocatalytic Asymmetric Reactions Involving Thioesters [J]. Acta Chimica Sinica, 2023, 81(1): 64-83.
[14]	Zhiping Chen, Yongle Meng, Jing Lu, Wenwu Zhou, Zhiyuan Yang, Anning Zhou. Preparation of Fe@Si/S-34 Catalysts and Its Catalytic Performance for Syngas to Olefins [J]. Acta Chimica Sinica, 2023, 81(1): 14-19.
[15]	Xia Liu, Chunxiang Kuang, Changhui Su. Transition-metal Catalyzed 1,2,3-Triazole-assisted C—H Functionalization Processes [J]. Acta Chimica Sinica, 2022, 80(8): 1135-1151.