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Progress in Chemistry >

2024 , Vol. 36 >Issue 4: 525 - 536

DOI: https://doi.org/10.7536/PC230802

Review

Coupling Different Synthesis Routes to Prepare Zeolite Molecular Sieves

  • Zhao Xinhong , 1, 2, * ,
  • Wang Hao 1 ,
  • Ding Mengqi 1 ,
  • Li Hongwei 1, 2 ,
  • Ji Dong 1, 2 ,
  • Li Guixian 1, 2
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  • 1 School of Petrochemical Engineering, Lanzhou University of Technology, Lanzhou 730050, China
  • 2 Key Laboratory of Low Carbon Energy and Chemical Engineering of Gansu Provice, Lanzhou 730050, China
*e-mail:

Received date: 2023-08-15

  Revised date: 2023-11-27

  Online published: 2024-02-26

Supported by

National Natural Science Foundation of China(22168022)

Basic Research Innovation Group Project of Gansu Province(22JR5RA219)

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Abstract

zeolites as one kind of important porous materials have a wide range of applications in the fields of adsorption,ion exchange,and catalysis due To their special pore structure,suitable acidity,and high hydrothermal stability.the classical hydrothermal route of synthesizing zeolites suffers from low zeolite yields,high synthesis costs,and serious pollution.coupling the classical synthesis routes of zeolites with those recently developed new non-conventional routes is an important way to solve the above problems and achieve technological innovation in zeolite synthesis.to this end,this review firstly introduces the principles and characteristics of those non-conventional synthesis routes of zeolites,then briefly introduces the concepts of coupling synthesis routes of zeolites,and then focuses on the latest progress in the preparation of zeolites by microwave synthesis,solvent-free synthesis,and seed-directed synthesis coupled with other routes.Finally,the main problems existing in these coupling routes are analyzed and viewed。

Contents

1 Introduction

2 Introduction to the non-conventional synthesis routes of zeolites

2.1 Hydroxyl radical assisted synthesis route

2.2 Continuous flow synthesis route

2.3 Interzeolite conversion synthesis route

2.4 Ultragravity synthesis route

2.5 Mechanochemical assisted synthesis route

3 Coupling of microwave synthesis with other synthesis routes

3.1 Microwave-hydrothermal synthesis route

3.2 Microwave-ionothermal synthesis route

3.3 Microwave-solvent-free synthesis route

4 Coupling of solvent-free synthesis with other synthesis routes

4.1 Solvent-free and hydroxyl radical assisted synthesis route

4.2 Solvent-free and seed directed synthesis route

4.3 Solvent-free and mechanochemical assisted synthesis route

5 Coupling of the seed directed synthesis with other synthesis routes

5.1 Seed directed and hydroxyl radical assisted synthesis route

5.2 Seed directed and continuous flow synthesis route

6 Other coupling routes

6.1 Hydrothermal-seed-ultragravity synthesis route

6.2 Ionothermal-interzeolite conversion synthesis route

7 Comparison of various coupling synthesis routes of zeolites

8 Conclusions and outlook

Key words： microwave synthesis; ionothermal synthesis; solvent-free synthesis; seed-directed synthesis; coupling

Cite this article

Zhao Xinhong , Wang Hao , Ding Mengqi , Li Hongwei , Ji Dong , Li Guixian . Coupling Different Synthesis Routes to Prepare Zeolite Molecular Sieves[J]. Progress in Chemistry, 2024 , 36(4) : 525 -536 . DOI: 10.7536/PC230802

1 Introduction

Zeolite is a kind of unique microporous crystal with adjustable properties.Because of its regular pore structure,large specific surface area,unique adsorption properties and other characteristics,it can be widely used in adsorption and separation,industrial catalysis,ion exchange and other fields[1⇓⇓~4]。 at present,the classical synthesis routes of zeolite molecular sieves mainly include hydrothermal(solvothermal)synthesis,ionothermal synthesis,microwave synthesis,solvent-free synthesis,template-free synthesis and so on,each of which has its unique advantages and disadvantages.zeolite molecular sieves are usually prepared by hydrothermal synthesis route in industry,and the crystallization process usually lasts for a long time At a high temperature,and some zeolites need expensive templates,which leads to high cost,high energy consumption and environmental pollution in the synthesis process of zeolite molecular sieves.Therefore,how to prepare zeolite molecular sieves efficiently,economically and green has gradually become the focus of researchers。
the continuous innovation of zeolite synthesis routes is an important driving force for the continuous development of zeolite basic research and application research.In recent years,unconventional zeolite synthesis methods(routes)such as hydroxyl radical route,continuous flow synthesis route,high gravity synthesis technology and zeolite internal conversion have been developed.These new routes can be organically combined with classical zeolite synthesis technology,thus promoting the zeolite synthesis process towards a greener and sustainable goal。
Considering that the classical synthesis routes such as hydrothermal(solvothermal)synthesis,ionothermal synthesis,microwave synthesis,solvent-free synthesis and template-free synthesis have been introduced in many monographs in detail,this paper first introduces the principles and characteristics of these unconventional zeolite synthesis routes.Secondly,the research progress in the preparation of zeolite by coupling between the classical synthesis route and the unconventional route of zeolite was introduced,and the existing problems were summarized.Finally,the prospect of the synthesis of zeolite molecular sieve by coupling route was prospected[5]。

2 Introduction of Unconventional Synthesis Routes of Zeolite Molecular Sieve

2.1 Hydroxyl radical promoted synthetic route

in 2016,Yu Jihong's research group found that there were hydroxyl radicals in the hydrothermal synthesis system,and that the addition of hydroxyl radicals in the synthesis system could significantly accelerate the crystallization process of zeolite[6,7]。 Hydroxyl radical is a highly active species,which can accelerate the depolymerization and repolymerization of aluminosilicate in the gel by promoting the cleavage and regeneration of Si-O-Si bonds during the crystallization process of zeolite.Hydroxyl radical can replace part of the OH-to accelerate the crystallization rate of zeolite.The advantage of hydroxyl radical-assisted synthesis route is that it can accelerate the crystallization rate of zeolite,reduce the alkalinity of the synthesis system,reduce the amount of organic template,improve the yield of molecular sieve,promote the formation of core-shell structure and accelerate the synthesis of hierarchical pore molecular sieve.The disadvantage of this route is the lack of advanced in situ characterization technology to detect the role of·OH and its intermediates in the crystallization process of molecular sieves,which makes it difficult to achieve quantitative detection of hydroxyl radicals,so it is impossible to achieve precise control of the concentration of hydroxyl radicals 。

2.2 Continuous mobile phase synthesis route

the continuous mobile phase synthesis route of zeolite is a new route for zeolite synthesis developed by zeolite scientists in recent years.Compared with the traditional autoclave hydrothermal batch synthesis method,the continuous mobile phase synthesis method has shorter crystallization time,can realize the synthesis of zeolite with high crystallinity in minutes or even seconds,and has higher space-time yield[8]。 the limitation of this method is that the gelation process in the reaction usually makes the system too viscous to flow,so that the gel and crystal adhere to the pipe wall,resulting in pipeline blockage and reducing the utilization rate of raw materials。

2.3 Zeolite internal conversion synthetic route

zeolite internal conversion refers to a zeolite synthesis route In which a zeolite molecular sieve with one topological structure is converted into another molecular sieve with a new structure.the conventional zeolite synthesis route uses amorphous silicon source and aluminum source as starting materials.in contrast,the zeolite internal conversion route using crystalline zeolite as starting material has the characteristics of shorter crystallization time,faster crystallization rate,and can form a specific zeolite structure.the molecular sieve prepared by the zeolite internal conversion route has better specific application performance than the zeolite obtained by the same type of hydrothermal method.However,the mechanism of zeolite internal conversion is not yet clear。

2.4 High Gravity Synthesis Route

high gravity zeolite synthesis technology is to use the strong centrifugal force generated in the rotating packed bed to achieve high gravity environment and enhance the transfer and mixing process between materials.in the high gravity environment,the reactants can be rapidly and uniformly mixed before crystallization,and nanoparticles with controllable grains can be obtained by crystallization in a uniform environment.the advantage of this technology is that the operating conditions are simple and easy to industrialize,but there are still many problems to be further understood about the high gravity technology and its related equipment。

2.5 Mechanochemical synthetic route

mechanochemical methods mainly rely on mechanical forces to destroy the crystalline structure of solid reagents.during milling,small amounts of solvent or water may be added or released from the hydrated form of the reagent.These solvent additives may facilitate the reaction between the starting materials and the formation of intermediates and target materials.Compared with the traditional hydrothermal(solvothermal)synthesis route,Mechanochemical synthesis has been widely used in the synthesis of zeolite molecular sieves because of its high yield,less waste,and milder reaction conditions.However,the wear of the container During the grinding process will produce some pollution,which may affect the catalytic process。
Zeolite synthesis is one of the most active research branches in the field of porous materials.From the solvent point of view,the synthesis routes of zeolites can be divided into four types:hydrothermal synthesis,solvothermal synthesis,ionothermal synthesis and solvent-free synthesis.According to the structure of the template(or structure-directing agent)used,the synthetic routes of zeolites can be divided into three types:organic structure-directing agent,synergistic structure-directing agent and template-free route(template-free route includes two subtypes of inorganic structure-directing agents and seed crystal directing).Professor Xiao Fengshou's research group has called crystal seeds the third type of structure-directing agent[9]。 On the basis of reasonable classification of zeolite synthesis routes and careful analysis of the advantages of various routes,we combine various routes organically,which is called zeolite coupling synthesis route。
in recent years,with the concept of"green chemistry"deeply rooted In the hearts of the people,the shortcomings of the traditional synthesis route of zeolite molecular sieves have also been exposed.For example,most of the classical hydrothermal synthesis is carried out under alkaline conditions,and the waste liquid produced after the reaction will cause environmental pollution.the ionothermal route usually requires the use of expensive ionic liquids,which is costly and difficult to achieve large-scale production.the microwave synthesis route has a certain limitation on the penetration depth of different solvents,which limits the large-scale microwave synthesis of molecular sieves.In order to overcome the above shortcomings of the traditional zeolite preparation process,researchers are committed to developing more green and efficient coupling synthesis routes.Due to the microwave synthesis,solvent-free synthesis and seed-directed route,the zeolite synthesis has the advantages of lower energy consumption,more environment-friendly and lower synthesis cost,and can be conveniently coupled with other routes.Therefore,the following will focus on the research progress in the preparation of zeolite molecular sieves by coupling these three routes with other routes。

3 Coupling of microwave synthesis with other synthetic routes

the precondition of zeolite synthesis under microwave irradiation is that the reaction system must have good microwave absorption ability.Commonly used water and polar organic solvents are good absorbers of microwave.Therefore,microwave synthesis can be perfectly combined with hydrothermal synthesis In the synthesis of zeolite.in addition,ionic liquid(eutectic mixture)solvents and even solid materials such as activated carbon can absorb microwave energy efficiently.According to this characteristic,scholars have developed new routes of zeolite synthesis,such as microwave-ionothermal and microwave-solvent-free。

3.1 Microwave-hydrothermal synthesis route

the introduction of microwave technology into the traditional hydrothermal synthesis process is the microwave-assisted hydrothermal synthesis route.Compared with the conventional hydrothermal synthesis in an oven,microwave heating is helpful to improve the crystallinity and surface area of zeolite,accelerate the crystallization rate,and reduce the energy consumption.This coupling route is expected to achieve the goal of rapid production of molecular sieves。
hydrothermal synthesis is the earliest developed zeolite synthesis route,so the study of microwave-Hydrothermal synthesis of zeolites has been reported for a long time.Julbe et al.Rapidly synthesized Silicalite-1 zeolite with relatively uniform crystal size by controlling the output power and action time of microwave to optimize the nucleation and crystallization time[10]。 Shalmani et al.Synthesized a series of SAPO-34 crystals under different synthesis conditions by using a microwave-assisted hydrothermal route,and the crystal size and morphology of SAPO-34 could be controlled by adjusting the microwave irradiation time[11]。 Sharma et al.Prepared four kinds of MFI,FAU,LTA and AFI nano-molecular sieves with different silica-alumina ratios by the same method[12]。 Muraza et al.Synthesized an aluminum-rich CHA zeolite(Fig.1)by microwave hydrothermal synthesis without the use of structure-directing agents,and its crystallization time was shortened from 24 H in conventional hydrothermal synthesis to 6 H.Catalytic performance studies showed that the zeolite had good activity in methanol to olefins reaction[13]。 Ma et al.rapidly synthesized high-silica Beta zeolite with a size of 25–180 nm using a microwave-assisted hydrothermal route without the addition of fluorinated medium and seeds,and proved that microwave irradiation could not only induce the generation of hydroxyl radicals to promote the formation of Si-O-Si bonds,but also Rapidly heat the precursor solution to reduce the crystal size[14]。 Compared with the pure silica Beta zeolite prepared by the traditional method,the Beta zeolite prepared by the method has higher specific surface area and pore volume and excellent hydrophobicity,and the synthesis strategy can provide a new way for the synthesis of nano-sized high-silica zeolite。
图1 微波水热路线合成沸石分子筛示意图[13]

Fig. 1 Synthesis of zeolite molecular sieves by microwave-hydrothermal route[13]

3.2 Microwave-ionothermal synthesis route

ionic liquids have the potential to replace water as an ideal solvent for zeolite synthesis due to their high chemical stability,extremely low vapor pressure,and good microwave absorption properties.the new route of zeolite synthesis formed by the combination of microwave radiation and Ionic liquid is called microwave-ionothermal synthesis route,which inherits the advantages of microwave technology,such as high efficiency,fast crystallization and uniform synthesis products.At the same time,the synthesis can be carried out under normal pressure,which eliminates the safety problems caused by high hydrothermal pressure,and is a relatively green and efficient coupling route。
Xu et al.Applied microwave technology to ionothermal synthesis system and synthesized AEL-type aluminophosphate molecular sieve by this technology[15]。 Zhao's research team successfully synthesized a series of zeolite molecular sieve materials by microwave-ionothermal route with eutectic mixture as solvent,such as FeAlPO-16 with AST topology,SAPO-5 with hexagonal petal-like nano-thin layer,FeAPO-5 with high iron content(three seeds synthesized by different methods were introduced into the precursor)and Fe-LEV aluminophosphate molecular sieve with multi-level pore structure[16⇓⇓⇓~20]。 In particular,the structure-directing species in both FeAlPO-16 and Fe-LEV molecular sieves are combinations of two organic species that have never been reported before.Wong et al.Used the microwave ionothermal route to synthesize nano-sized AlPO4-5 molecular sieves with uniform particle size,and the AlPO4-5 nanocrystals synthesized by microwave had higher water absorption capacity than those synthesized by hydrothermal method[21,22]。 These studies demonstrate the great potential of the microwave-ionothermal route for the synthesis of zeolite molecular sieves of specific structure,size,morphology,and composition。

3.3 Microwave-solvent-free synthesis route

solvent-free synthesis has attracted much attention in recent years.solvent-free route can reduce the generation of waste because no additional water Solvent is added to the system.Compared with the traditional hydrothermal synthesis,this is a very green synthesis route.If the advantages of Solvent-free and microwave methods are effectively combined,on the one hand,the energy consumption can be reduced,on the other hand,the pollutants can be significantly reduced and the synthesis efficiency can be improved,which is in line with the concept of"green chemistry"。
under solvent-free conditions,the solid raw materials used for zeolite synthesis,such as silicon source,aluminum source and phosphorus source,have very weak ability to absorb microwave,so the solid synthesis system can not be heated to the commonly used zeolite crystallization temperature range(100~200℃)by microwave radiation.After comprehensive consideration,Zhao et al.Proposed that activated carbon,a common carbon material with strong microwave absorption capacity,could be used as a microwave absorption medium to synthesize zeolite molecular sieves Under solvent-free conditions[23]。 AlPO4-5 aluminophosphate molecular sieves with AFI topology were successfully synthesized by microwave irradiation under solvent-free conditions after a series of optimization of synthesis conditions.Because the activated carbon plays the role of a hard template at the same time,the finally obtained molecular sieve is a hierarchical porous material with both micropores and mesopores 。
the above results show that microwave synthesis can be conveniently coupled with other zeolite synthesis routes as long as the system can absorb microwaves.microwave changes the nucleation and crystal growth rate of zeolite in conventional hydrothermal synthesis,and broadens the range of reaction mixture ratio,so that some zeolite materials with specific topological structures(such as LEV and AST)and types(nano-thin layer,nano-crystal and multi-level pore)can be obtained by microwave coupling synthesis technology.Table 1 briefly summarizes the characteristics of microwave synthesis coupled with other synthetic routes and lists the types of zeolite structures that have been obtained。
表1 Characteristics of Zeolite Synthesis by Coupling Microwave Synthesis with Other Synthetic Routes

Table 1 Characteristics of microwave synthesis coupled with other routes in preparing zeolites

Microwave coupling routes Advantage Disadvantage Framework Ref
Microwave-hydrothermal synthesis route Owing to the advantages of rapid and uniform heating of microwave compared to conventional heating, the crystallization process of zeolites with microwave heating is more rapid to enter the crystal growth period, and the crystallization time is evidently shortened, making the process more energy saving. The experimental process of microwave hydrothermal routes is sometimes not safe, and organic templating agents or volatile solvents can still cause problems such as excessive pressure generation. MFI, CHA, FAU, LTA, AFI, *BEA 10⇓⇓⇓~14
Microwave-ionothermal synthesis route The ionic liquid is a good microwave absorber. The combination of microwave heating and ionic liquid can make heating more uniform, provide a faster heating rate, and allow for a shorter aging time. The number of ionic liquids is limited in variety, the reaction mechanism of the microwave-ionothermal synthesis route still lacks understanding, and its industrial application requires further research. AEL, AST, Fe-LEV, AFI 15⇓⇓⇓⇓⇓⇓~22
Microwave-solvent-free synthesis route Microwave and solvent-free coupling has the advantages of being fast and safe, having low energy consumption, andreducing the generation of wastewater. Not any of the synthesis reactions can occur in a microwave solvent-free system, and the types of molecular sieve synthesis are limited. AFI 23

4 Coupling of solvent-free synthesis with other zeolite synthesis routes.

As mentioned in Section 3.3,solvent-free synthesis can reduce pollutant emissions and obtain high zeolite yield,which is a very green and efficient zeolite synthesis route,so it has attracted wide attention in recent years[24⇓⇓~27]。 However,compared with the conventional hydrothermal synthesis,the solvent-free synthesis route still needs to be improved.First of all,because of the poor mobility of solid materials,solvent-free synthesis usually needs to be carried out at higher crystallization temperature and longer crystallization time,which greatly increases the energy consumption of synthesis.Secondly,due to the narrow composition range of precursors,it is impossible to directly synthesize zeolite molecular sieve materials with different pore structure parameters and acidity,which can be applied to different types of catalytic reactions.One possible way to solve the above problems is to organically couple solvent-free synthesis with other synthetic routes.Uch as microwave-solvent-free synthesis route,solvent-free hydroxyl radical promoted synthesis route,solvent-free seed synthesis route and solvent-free mechanochemical assisted synthesis route。

4.1 Solvent-free hydroxyl radical promoted synthetic route

As mentioned in Section 2.1,the introduction of hydroxyl radicals by UV irradiation or the addition of Fenton reagent in hydrothermal synthesis can significantly accelerate the crystallization process of zeolite.If this synthetic route can be successfully coupled with solvent-free synthesis,it is expected to solve the problem of high energy consumption of the latter.Based on this,our research group designed a new solvent-free synthesis route of Fe-ZSM-5 zeolite promoted by Fenton reagent,and synthesized Fe-ZSM-5 zeolite with extremely high crystallinity in a relatively short crystallization time at high temperature[28]。 Compared with the reference catalyst synthesized by the conventional solvent-free method,the Fe-ZSM-5 catalyst synthesized by this route showed better catalytic performance in the hydroxylation of phenol[29⇓~31]。 However,when the authors tried to extend this route to the synthesis of Fe-Beta and Fe-MOR zeolites,no hydroxyl radical promotion effect was observed,and the reason for the failure of the coupling of the two synthetic routes remains to be further explored。

4.2 Solvent-free seed-directed synthesis route

the earliest reported solvent-free route for zeolite synthesis used a higher dosage of organic templating agent,which is obviously unfavorable for its application in industry.If the solvent-free synthesis is successfully combined with the seed-directed synthesis route,the production cost of zeolite can be reduced and the environmental pollution can be reduced,which will undoubtedly greatly promote the application of zeolite in related fields.the physical and chemical properties of zeolite crystals can also be effectively modulated by introducing specific seeds into the precursors of solvent-free synthesis.Compared with the solvent-free hydroxyl radical route,which can only be applied to the synthesis of some zeolites,the solvent-free seed route has better universality。
Wu et al.Demonstrated a new strategy for zeolite synthesis by combining solvent-free and seed crystals,and successfully prepared Beta and ZSM-5 zeolites by fully grinding in a mortar to mix solid silica-alumina raw materials with seeds[32]。 The coupling route not only solves the problems of environmental pollution,high cost and the like caused by the use of an organic template agent,but also solves the problems of high self-generated pressure,low space utilization rate of a reaction kettle,waste water pollution and the like in a synthesis system caused by taking water as a solvent,This green coupling route provides new opportunities for the preparation of other molecular sieves and is also of great significance for the large-scale production of zeolites in industry.Zhao et al.Induced the initial gel formed by grinding and mixing aluminum isopropoxide,morpholine and phosphoric acid to synthesize AlPO4-34 molecular sieves with CHA topology by adding a proper amount of seed crystals,and the use of seed crystals significantly reduced the amount of organic structure-directing agent[33]。 Luo et al.Used anhydrous silicon source,aluminum source and sodium carbonate as raw materials to synthesize ZSM-5 zeolite nanocrystal aggregates with crystal size of 10~40 nm by solvent-free seeding route,which showed good catalytic activity in low density polyethylene cracking reaction[34]。 Zhang Peiqing et al.Used low-cost kaolin as raw material to synthesize ZSM-5 molecular sieve green and efficiently through solvent-free seeding route[35]。 Compared with the ZSM-5 zeolite catalyst prepared by the in-situ hydrothermal method,the ZSM-5 zeolite catalyst prepared by the in-situ hydrothermal method has the characteristics of higher crystallinity and specific surface area,smaller crystal size,slightly higher acid strength and similar pore structure。

4.3 Solvent-free mechanochemical synthetic route

in recent years,the advantages of solid-state reaction have been gradually reflected In the synthesis of zeolite molecular sieves and other porous materials.the mechanochemical synthesis of porous materials can not only reduce the pollution caused by solvents,but also further reduce costs and simplify the production process and flow.Mechanical milling is usually used to activate solid reactant precursors,and then heat these precursors under solvent-free conditions to synthesize various porous materials such as zeolites and MOFs.Therefore,mechanochemistry as a pretreatment method can be conveniently combined with the solvent-free synthesis route of zeolites。
Majano et al.Summarized the benefits of using mechanical ball milling as a tool for the preparation and"activation"of precursor mixtures in the hydrothermal synthesis of molecular sieves:faster crystallization kinetics and easier access to molecular sieve purity[36]。 Pashkova et al.synthesized SSZ-13 molecular sieve efficiently in a solvent-free system by mechanochemical pretreatment of a mixture of silicon and aluminum sources using a planetary ball mill,and the physical parameters of the zeolite products prepared by the solvent-free mechanochemical pretreatment route were consistent with those of the hydrothermally Synthesized zeolite[37]。 SSZ-13 zeolites with different Si/al ratios and crystal sizes CAN be obtained when different silicon sources are used as raw materials.Mizuno et Al.Also used a planetary ball mill to mechanochemically pretreat the starting material to synthesize ANA,can,GIS,SOD,FAU,and LTA zeolites by changing the silica-alumina ratio and crystallization temperature(Fig.2)[38]。 Under mechanochemical assistance,Larsen et al.Synthesized ZSM-5 molecular sieve and mordenite molecular sieve by solvent-free mechanochemical assisted synthesis route[39]。 the method avoids the use of zeolite seeds,and the obtained zeolite has a high surface area and shows similar performance to commercial catalysts in the catalytic conversion of biomass to hydroxymethylfurfural.Zhou et al.Also used this route to synthesize b-axis oriented ZSM-5 zeolite,whose morphology and acidity can be adjusted by ammonia.After optimization,the synthesized zeolite material showed a long catalytic life of 28 H and a propylene selectivity of 41%in the methanol to olefins reaction[40]。
图2 机械化学-无溶剂路线合成沸石分子筛示意图[38]

Fig. 2 Synthesis of zeolites by solvent-free and mechanochemistry route[38]

the above results show that the solvent-free synthesis route,combined with other synthesis routes,not only solves the problems of safety and low efficiency in traditional hydrothermal synthesis,but also partially solves the problems of environmental pollution and high synthesis cost caused by expensive or toxic organic templates and excessive solvent use.the development of these coupling routes provides a new path for the preparation of other zeolite molecular sieves,and has important reference significance for improving the current production process of zeolite.It is believed that more other synthetic strategies will be developed in the near future,such as the sodium-free route and the fluorine-free route combined with solvent-free to synthesize zeolites.Table 2 lists the types of zeolite structures that can be prepared by coupling the solvent-free synthesis route with other synthesis techniques,and briefly analyzes their technical characteristics。
表2 Characteristics of Zeolite Molecular Sieve Preparation by Coupling Solvent-free Synthesis Route with Other Technologies

Table 2 Characteristics of solvent-free synthesis coupled with other techniques in preparing zeolites

Solvent-free coupling routes Advantage Disadvantage Framework ref
Solvent-free hydroxyl radical synthesis route The introduction of hydroxyl radicals can appropriately reduce the amount of alkali in the synthesis system as well as the amount of organic templating agent and reduce the energy consumption in the synthesis process by improving the zeolite crystallization rate. Only a small number of zeolite molecular sieves can be synthesized via this route, and the promotion mechanism of hydroxyl radicals in the solvent-free condition still lacks understanding. Fe-MFI 28
Seed-directed solvent-free route The raw materials can be fully mixed with seeds by grinding under solvent-free conditions, which is conducive to the effective collision and spontaneous diffusion of molecules and helps all the reactants to participate in the synthesis reaction. The addition of an appropriate amount of seeds can shorten the induction period and inhibit the generation of other hetero-crystalline phases, which significantly reduces the synthesis time. The reaction is usually carried out in an immobile solid-solid system, resulting in the poor efficiency of heat conduction, which severely limits large-scale industrial applications. *BEA, MFI, CHA 32⇓⇓~35
Solvent-free mechanochemical-assisted route The coupling of solvent-free and mechanochemical methods makes up for the shortcomings of manual grinding, which is prone to producing amorphous products, and the high-energy ball milling process makes the mixing of the initial raw materials more homogeneous, which helps to increase the reactivity, and the operation process is simple and low-cost. Ball milling media and rapid powder movement processes are difficult to monitor, and most studies have been conducted in planetary ball mills for material pre-preparation, which is not yet available for large-scale processing. CHA, ANA, CAN, GIS, SOD, FAU, LTA, MFI 37⇓⇓~40

5 Coupling of the seed-directed synthesis route with other routes

Seed-directed synthesis is the most widely used method for large-scale industrial synthesis of zeolite molecular sieves.in the traditional industrial production of zeolite,adding a small amount of zeolite seeds to the synthesis system can play a role In improving the crystallization rate,reducing the synthesis time,and inhibiting the formation of miscellaneous crystals[41⇓~43]。 It is worth mentioning that template-free synthesis of nearly 10 zeolites has been achieved by introducing seeds into the hydrothermal synthesis system based on the CBU structural unit hypothesis[44⇓⇓⇓⇓⇓⇓~51]。 the reader is referred to The review paper written by Okubo's research group for research progress in this area[52]。 Another outstanding advantage of seed-directed zeolite synthesis is its universality,which can be combined with a variety of unconventional zeolite synthesis routes listed in Section 2.Bruter et al.Made a comprehensive summary of the research progress of zeolite internal conversion,including the seed direction-zeolite internal conversion method[53][54⇓⇓~57]。 Due to the limitation of space,this section only briefly introduces and reviews the research results of zeolite synthesis by the seed-hydroxyl radical promotion route and the seed-continuous flow synthesis route。

5.1 Seed-hydroxyl radical promotion route

Cheng et al.Developed a strategy of combining hydroxyl radicals with seeds to accelerate the crystallization of zeolites,namely the seeded hydroxyl radical-promoted synthesis method,by which NaA and nano-Silicalite-1 molecular sieves(Fig.3)were prepared with higher yields and faster crystallization rates[58,59]。 the key to this strategy is to introduce radicals into the seed crystal by grinding or heating,and this coupling method is easily realized in the large-scale synthesis of zeolite molecular sieves。
图3 晶种辅助羟基自由基合成Silicalite-1分子筛示意图[59]

Fig. 3 Seed-assisted hydroxyl radical synthesis of Silicalite-1 molecular sieves[59]

5.2 Seed-continuous flow synthesis route

Continuous flow method has a strong potential for expansion And can be coupled with a variety of technologies,the most common multi-technology coupling is the combination of seed-directed synthesis route,which can not only greatly accelerate the synthesis speed,but also have a stronger control over the product.the coupling of the two can solve the following problems:(1)reducing the synthesis period required for zeolite nucleation;(2)preventing the formation of impurity crystal phase;and(3)that production energy consumption is greatly reduce。
Okubo's research group first developed a synthesis technology combining continuous flow synthesis and seed crystal.the main feature of continuous flow synthesis is to use a stainless steel tubular reactor with good heat transfer performance instead of the traditional tank reactor.the addition of the seed crystal eliminates the energy barrier of spontaneous nucleation,and the coupling of the two makes the zeolite synthesis complete in a few minutes[60]。 With this technique,the complete crystallization of AlPO4-5 and SSZ-13 zeolite can be achieved in only 1 and 10 min,respectively(Fig.4 )[61,62][63,64]。 in contrast,the synthesis of the above two zeolites In the traditional crystallization reactor takes at least 24 H.Table 3 lists the types of zeolite structures that can be prepared by coupling the seed-directed route with other synthesis techniques,and briefly analyzes their respective technical characteristics。
图4 晶种-连续流动合成AlPO4-5分子筛示意图[61]

Fig. 4 Seed-assisted continuous flow synthesis of AlPO4-5 molecular sieves[61]

表3 Characteristics of Zeolite Synthesis by Coupling Seed-Directed Route with Other Synthetic Routes

Table 3 Characteristics of seed-directed synthesis coupled with other routes in zeolite preparation

Seed-directed coupling routes Advantage Disadvantage Framework ref
Seed-directed template-free synthesis route On the one hand, the addition of seeds eliminates the use of organic templating agents, maximizing the savings in production costs; on the other hand, seeds can be used as templates to induce the formation of zeolite frameworks. The synthesis process is cumbersome, and the types of molecular sieves that are synthesized are limited. EON, *BEA, MFI, TON, MOR, BOG 44⇓⇓⇓⇓⇓⇓~51
Seed-directed interzeolite transformation synthesis route The introduction of seeds with common composite building units with the target zeolite not only induces the generation of the target zeolite, but also accelerates the dissolution of the starting zeolite, accelerates the nucleation rate of the crystal, and shortens the crystallization time to a certain extent. The reaction is usually carried out under hydrothermal conditions, with a large amount of waste liquid discharge and high reaction pressure, which poses certain safety risks. *BEA, MFI, CHA,,STF, MTW 54⇓⇓~57
Seed-directed hydroxyl radical synthesis route An effective combination of seeds with highly active hydroxyl radicals can not only shorten the induction period and improve the utilization of raw materials, but also induce product-directed synthesis. The role of •OH and seeds in zeolite crystallization is not well understood at the molecular level, and problems such as the precise quantification of •OH have not yet been solved. LTA, MFI 58~59
Seed-directed continuous flow synthesis route A continuous flow reactor has a good heat and mass transfer effect, and the induction of seeds can strengthen the above effect further, making up for the thermal delay effect of the high-pressure reactor and reducing the synthesis time. This route not only improves the crystallization rate, but also effectively regulate the particle size of the product. Reaction gel makes the system viscosity easy to cause clogging, making the utilization of raw materials slightly reduced. This coupling method is currently limited to the laboratory development stage, and has not yet achieved industrial production. AFI, MFI 61⇓⇓~64

6 Other coupling routes

In addition to the above coupling routes,researchers have also developed other green coupling routes of zeolite molecular sieves,such as hydrothermal-seed-high gravity synthesis technology and ionothermal zeolite-internal conversion method。

6.1 Hydrothermal-Seed-High Gravity Synthesis Route

high gravity technology has been widely concerned by researchers as a means of enhancing mass transfer.In order to solve the problems of low reaction efficiency,large amount of expensive organic template and long synthesis cycle in the industrial hydrothermal preparation of molecular silica-alumina zeolite,researchers have developed a variety of optimized hydrothermal preparation methods of molecular silica-alumina zeolite,but most of these methods can not be applied in industry.In recent years,a new technology for the preparation of porous materials such as zeolite molecular sieves by combining high gravity technology with hydrothermal method can partially solve the above problems,which lays a foundation for the preparation and industrial application of high-performance zeolite molecular sieves。
Hydrothermal-seed-high gravity zeolite synthesis technology is mainly characterized by the use of a new type of reactor suitable for the enhancement of liquid-liquid mixing contact process,that is,rotating packed bed reactor,to enhance the mixing process of initial materials.the huge shear force generated by the rotation of the rotating packed bed can tear the liquid into very thin droplets,liquid films or liquid filaments,thus greatly enhancing the micromixing process.Hierarchically porous ZSM-5 and ultrafine NaY zeolites have been successfully prepared using this technique(fig.5)[65⇓⇓⇓~69][70]。 Obviously,this technique can be easily extended to solvothermal-high gravity or ionothermal-high gravity synthesis systems by simply replacing the solvent water with an organic solvent or a room temperature ionic liquid。
图5 水热-超重力技术合成ZSM-5沸石的实验装置示意图[66]

Fig. 5 Experimental setup for synthesizing ZSM-5 zeolite by hydrothermal-ultragravity technique[66]

6.2 Ionothermal-zeolite internal conversion synthetic route

zeolite internal conversion is usually carried out under hydrothermal conditions.However,the hydrothermal conversion process inevitably produces a large amount of waste and high autogenous pressure.These shortcomings will not only pollute the environment,but also cause a series of safety problems due to the high pressure.Therefore,it is of great significance to develop a green and sustainable coupling route of Zeolite internal conversion to solve the above problems。
Our research group has recently coupled ionothermal with zeolite internal conversion technology to realize the crystal transformation process from HY zeolite to HZSM-5 zeolite at atmospheric pressure[71]。 The HZSM-5 zeolite catalyst shows excellent catalytic performance in the reaction of methanol to aromatics.Under the conditions of 400℃,0.1 MPa and space velocity 1.9 h−1,the methanol conversion was more than 95%,the aromatics selectivity was as high as 46.6%,and the catalyst was not deactivated after 170 H of reaction.Its excellent catalytic performance is presumed to be mainly related to the following three factors:(1)the intracrystalline mesopores formed naturally during crystal transformation are beneficial to the mass transfer process;(2)that introduction of fluorine specie eliminates the silanol defect in the zeolite,and the presence of the silanol defect site is beneficial to the capture of macromolecular hydrocarbons,resulting in rapid deactivation of the catalyst;(3)The use of tetrapropylammonium bromide as a structure-directing agent(rather than sodium ions)makes the acid sites mainly distributed at the pore channel intersections,which is conducive to the formation of aromatic products.The unique feature of the ionothermal-zeolite internal conversion route is that the unique ionic environment of the crystal transformation process affects the pore microenvironment of the product zeolite,and the diversity of the types and properties of ionic liquids makes it possible to obtain some zeolite materials with unique physical and chemical properties by using this route.Table 4 lists the zeolite structure types that can be prepared by other synthesis techniques,and briefly analyzes their respective technical characteristics 。
表4 Characteristics of Zeolite Molecular Sieve Prepared by Other Coupling Routes

Table 4 Characteristics of other coupling routes of synthesizing zeolites

Other coupling routes Advantage Disadvantage Framework Ref
Hydrothermal-seed- ultragravity synthesis route The ultragravity technology can improve the microscopic mixing efficiency, which in turn enhances the heat and mass transfer efficiency, facilitates the homogeneous dispersion of seeds in the initial gel, contributes to the homogeneous growth of the product, and shortens the crystallization time. Basic theoretical research on the ultragravity technique is seriously lagging behind, and industrial scale-up research is difficult. MFI、FAU 65⇓⇓⇓⇓~70
Ionothermal-interzeolite conversion synthesis route The internalzeolite conversion route partly compensates for the defects of the long synthesis cycle of the ionothermal method. The addition of ionic liquid can reduce the use of organic template agents to a certain extent. The reaction can be carried out at atmospheric pressure, avoiding the safety hazards brought about by high pressure. Most ionic liquids are relatively expensive, thus increasing the synthesis cost. The problem of recycling ionic liquids has not yet been solved, making large-scale production difficult. MFI 71
In the past 20 years,the route of zeolite internal conversion has been widely developed,although the underlying regularity(such as the relationship between the structure of parent zeolite and daughter zeolite)has not been fully revealed.However,the coupling of this synthetic route with other routes provides a new opportunity to develop new high-performance zeolite catalysts and improve existing microporous materials to reduce their production costs[72]。

7 Comparison of Zeolite Coupling Synthesis Routes

to sum up,the coupling strategies of microwave synthesis,solvent-free synthesis,seed-directed synthesis and other synthetic routes have made great progress.However,these coupled synthetic routes are different in the scope and purpose of synthesis.For example,the coupling of microwave synthesis with other routes is mainly aimed at systems that can absorb microwaves,which also limits its scope of application due To the limited penetration of microwaves.the microwave coupling method inherits some of the advantages of microwave synthesis,which can synthesize the target zeolite in a wide range of compositions,and the obtained zeolite has a small crystal size and a narrow distribution.in recent years,the microwave coupling method has shown great potential in the synthesis of zeolite membranes.A variety of zeolite membranes have been synthesized by microwave coupling method,including NaA zeolite membrane,SAPO zeolite membrane and CHA zeolite membrane[73⇓⇓~76]。
Although solvent-free synthesis has made some new progress In coupling with other technologies,solvent-free synthesis routes have been widely used in the synthesis of some commonly used zeolites in industry.It is still necessary to use expensive organic templates,which on the one hand increases the cost of zeolite synthesis,and on the other hand offsets the benefits of solvent-free synthesis due to the environmental pollution caused by calcination to remove the templates.from this point of view,solvent-free synthesis is still far from industrial production.in addition,zeolites can usually only be synthesized within a narrow range of precursor compositions due to the immobile solid-solid system unique to solvent-free synthesis,thus limiting the ability to synthesize property-tunable zeolite materials using this route.Whether from the perspective of theoretical research or industrial application,the coupling of solvent-free and template-free routes with other synthetic routes is worth further exploring。
Compared with the coupling route of microwave synthesis and solvent-free synthesis,the seed-directed method can be perfectly coupled with other zeolite synthesis routes,which has good universality.seed-directed method is also a widely used method in zeolite industrial production at present.seeds can be well directed to a variety of target molecular sieve frameworks,including all-silica zeolite,silica-alumina zeolite,aluminophosphate zeolite,silica-aluminophosphate molecular sieve and so on.the seed coupling method can also be used to prepare hierarchical pore molecular sieves.From the point of view of application,it is worth studying in this field to use Seeds,inorganic structure-directing agents,cheap organic compounds and their combinations to direct the synthesis of promising zeolite materials under solvent-free conditions。

8 Conclusion and prospect

It is an important research direction in the field of zeolite in recent years to optimize the combination of different zeolite synthesis routes,give full play to their respective advantages,and realize the sustainable,green,simple and efficient synthesis of zeolite,and this direction has made gratifying progress.in this paper,the coupling of microwave synthesis,solvent-free synthesis and seed-directed synthesis with other synthetic routes is emphatically introduced,and their technical characteristics are briefly analyzed.These coupled synthetic strategies have shown great potential for the synthesis of zeolite molecular sieves with specific structures,sizes,morphologies,and compositions compared with single synthetic routes.Although many achievements have been made in this direction,there are still many important scientific problems to be solved。
First,most of the coupled synthesis routes are only applicable to a limited number of zeolite topology types,such as microwave-ionothermal method and solvent-free template-free method.How to extend it to the synthesis of other promising zeolites requires people to use some in situ techniques,such as in situ solid-state nuclear magnetic resonance and in situ ultraviolet Raman spectroscopy,combined with other ex situ techniques,such as high-resolution transmission electron microscopy and physical adsorption.the synthesis process of zeolite was investigated comprehensively and deeply to clarify the relationship between the synthesis parameters(raw materials,crystallization conditions,templates,etc.)and the structure of zeolite,and to reveal the crystallization mechanism,so as to realize the control of the crystallization process。
Secondly,most of the current coupling strategies are the combination of two synthesis routes.If three(or more)zeolite synthesis methods can be effectively combined,it is expected that more precise control of zeolite structure and properties can be achieved.People should make full use of the diversity of zeolite synthesis routes to develop a set of zeolite synthesis toolbox to realize the controlled synthesis of zeolites with specific structural properties.However,in order to achieve this goal,we need not only to fully understand the characteristics of various zeolite synthesis methods,but also to have a deep understanding of the unique crystallization law of various zeolites in view of the diversity of zeolite structure,composition and synthesis routes。
Finally,and most importantly,the application of zeolite molecular sieves synthesized by coupling strategy is still very limited,basically limited to the catalytic field.the structural and physicochemical properties(such as symmetry,defect,orientation,crystal size,composition,heteroatom and guest species distribution)of zeolite molecular sieves synthesized by coupling methods and corresponding zeolite materials synthesized by single routes should be studied.Heat absorption and water absorption properties,etc.),and summarize the rules contained therein,laying the foundation for its application in traditional fields such as adsorption separation and ion exchange,as well as emerging fields such as energy conversion and storage,electronic and optical devices,and health care[77]。
in a word,the focus of future work is to continue to develop new green synthesis coupling routes of molecular sieves and to increase the in-depth study of the mechanism of zeolite molecular sieve coupling method.At the same time,considering the large-scale production and industrial application of zeolite,designing a sustainable and efficient coupling route of zeolite synthesis may bring more benefits to basic research and industrial production,so more efforts should be made in the theoretical design of zeolite synthesis。

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