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In this work, we show for the first time that high-silica zeolites (MFI, TON, MTT, and *MRE) could be synthesized from a combined strategy of both zeolite seeding and alcohol filling in the absence of organic structure-directing agents (OSDAs). High-silica ZSM-5 zeolites with Si/Al ratios ranging from 38 to 240 (TF-Al-ZSM-5) could be synthesized via this route. The key to the success of this technique was the employment of an aluminosilicate precursor with a fully 4-coordinated aluminum species as the initial source, wherein the rearrangement and condensation of the silicate species, rather than the aluminate species, occurred during zeolite crystallization. In addition, heteroatoms, such as Fe and B, could be incorporated into the zeolite frameworks. Catalytic tests for the methanol-to-propylene (MTP) reaction exhibited good catalytic performance for TF-Al-ZSM-5, which was comparable to that of the aluminosilicate ZSM-5 zeolite synthesized with OSDAs. Hence, this method offers viable opportunities for the industrial production and catalytic application of high-silica zeolites in the future.

Ionothermal synthesis has been widely used for the preparation of aluminophosphate-based molecular sieves, coordination polymers, metal-organic frameworks, and covalent organic frameworks. However, this method is still challenging for synthesis of silica-based zeolites. Herein, we show a generalized ionothermal route to synthesize silica-based zeolites with MTT, TON, ITW, and MFI structures in the presence of NH4F as a mineralizing agent and ionic liquid as a solvent and/or structure directing agent. The presence of a suitable amount of NH4F plays a key role for the successful synthesis of these silica-based zeolites. This methodology might open a pathway to ionthermally synthesize silica-based zeolites.

Currently, the synthesis of pure silica zeolites always requires the presence of organic structure-directing agents (OSDAs), which direct the assembly pathway and ultimately fill the pore space. A sustainable route is now reported for synthesizing pure silica zeolites in the absence of OSDAs from a combined strategy of zeolite seeding and alcohol filling, where the zeolite seeds direct crystallization of zeolite crystals from amorphous silica, while the alcohol is served as pore filling in the zeolites. Very importantly, the alcohol could be fully washed out from zeolite pores by water at room temperature, which completely avoids calcination at high temperature for removal of OSDAs in the synthesis of pure silica zeolites.

For the first time, SSZ-39 zeolite has been directly prepared using conventional colloidal silica and sodium aluminate instead of using FAU zeolite as the raw material in the alkaline media. The adjustment of the Si/Al ratios in the starting materials to the suitable values is a key factor to prepare the aluminosilicate SSZ-39 zeolite. Various characterizations (for instance, X-ray diffraction, scanning electron microscopy, nitrogen sorption, solid 27Al NMR, and NH3-temperature-programmed desorption) display that the aluminosilicate SSZ-39 zeolite owns high crystallinity, uniform cuboid morphology, large surface area, four-coordinated aluminum species, and strong acidic sites. Inductively coupled plasma analysis shows that the SiO2/Al2O3 ratios of the SSZ-39 products are ranged from 12.8 to 16.8. Considering the special framework of the SSZ-39 zeolite, the yield of this synthesis is not higher than 21.3%. Moreover, the catalytic performance of Cu-SSZ-39 catalyst synthesized from this route is excellent in the selective catalytic reduction of NO x with NH3 (NH3-SCR).

Photocatalytic synthesis of hydrogen peroxide (H2O2) from water and oxygen is an alternative route for clean energy storage and chemical synthesis, but still having problems with insufficient H2O2 productivity and solar-to-chemical energy conversion efficiency. Herein, we reported a hybrid catalyst of proton-form titania nanotube with carbon dot (HTNT-CD) that is highly efficient for the production of H2O2 under visible-light irradiation (λ > 420 nm, H2O2 productivity at 3.42 mmol gcat−1⋅h−1), outperforming the titania catalysts containing noble metals and the carbon nitride catalysts reported previously. Multiple studies demonstrate that the protons on the HTNT-CD are crucial for the production of H2O2 by efficiently accelerating the half reaction of molecular oxygen reduction to form H2O2, and effectively hindering H2O2 decomposition under the irradiation conditions. This HTNT-CD catalyst gives solar-to-H2O2 apparent energy conversion efficiency at 5.2%, which is even 4.9 times of that (1.06%) over the catalyst derived from commercial P25 and CDs. More importantly, the HTNT-CD is stable, giving high H2O2 productivity in the continuous recycle tests.

The incorporation of metal heteroatoms into zeolites is an effective modification strategy for enhancing their catalytic performance. Herein, for the first time we report a generalized methodology for inserting metal heteroatoms (such as Sn, Fe, Zn, and Co) into the layered zeolite precursor RUB-36 via interlayer expansion by using the corresponding metal acetylacetate salt. Through this generalized methodology, Sn-JHP-1, Fe-JHP-1, Zn-JHP-1 and Co-JHP-1 zeolites could be successfully prepared by the reaction of RUB-36 and corresponding metal acetylacetate salt at 180 °C for 24 h in the presence of HCl solution. As a typical example, Sn-JHP-1 and calcined Sn-JHP-1 (Sn-JHP-2) zeolite is well characterized by the X-ray diffraction (XRD), diffuse reflectance ultraviolet-visible (UV-Vis), inductively coupled plasma (ICP), N2 sorption, temperature-programmed-desorption of ammonia (NH3-TPD) and X-ray photoelectron spectroscopy (XPS) techniques, which confirm the expansion of adjacent interlayers and thus the incorporation of isolated Sn sites within the zeolite structure. Notably, the obtained Sn-JHP-2 zeolite sample shows enhanced catalytic performance in the conversion of glucose to levulinic acid (LA) reaction.

Ultrathin nanosheets (6–8 nm) of aluminosilicate FER zeolites have been successfully synthesized using a sole small organic ammonium (N,N-diethyl-cis-2,6-dimethyl piperidinium, DMP). Catalytic tests on the skeletal isomerization of 1-butene to isobutene show that the FER nanosheets exhibit much higher conversion and selectivity than conventional FER zeolites.

In this work, several efficient heterostructured nanocomposites with enhanced CO2 photoreduction activity were successfully constructed by anchoring carbon quantum dots onto TiO2 using a facile microwave assisted synthesis strategy. The carbon quantum dots obtained by microwave treatment of thiourea and citric acid acted as a sensitizer in the composites to enhance light absorption. The high-resolution transmission electron microscopy (HR-TEM) revealed that a closely integrated interface between carbon quantum dots and TiO2 nanosheets was formed in the heterostructured nanocomposites. Furthermore, the photogenerated charge transfer and separation in the heterogeneous nanocomposites were demonstrated to be significantly improved when compared with that in pristine TiO2. Consequently, a remarkable enhancement of photocatalytic activity evaluated for CO2 photoreduction under simulated solar light irradiation can be found in the nanocomposites. Maximum CH4 and CO yields of 0.769 and 1.153 μmol, respectively, have been obtained from the photoreduction after one hour irradiation without any noble metal loaded on photocatalyst. The amounts of CH4 and CO generated over nanocoposite are 7.79 and 7.61 times as high as those on pristine TiO2. This encouraging performance in CO2 photoreduction shows that these nanocomposites might be a prospective material in environmental protection and energy conversion.

2,6-methyl-N-methylpyridinium, as a novel organic template, is employed for the synthesis of RTH aluminosilicate zeolite with a SiO2/Al2O3 ratio of 17.6. The amount of 2,6-methyl-N-methylpyridinium template, the Na2O/SiO2 ratio, the SiO2/Al2O3 ratio, and the H2O/SiO2 ratio in the starting gel significantly influence the crystallization of RTH zeolite. Several analytical methods such as XRD, SEM, N2 sorption, TG-DTA, DRIFT and NMR were employed for the characterisation of the obtained RTH zeolites and to understand the crystallization process with the new template. Very interestingly, the crystallization of RTH zeolite with the new template takes a very short time (12 h at 130 °C and 50 min at 240 °C) compared with conventional RTH zeolite synthesis reported in the literature (72 h at 130 °C). Theoretical calculations show that this novel organic template has lower interaction energies for zeolite cage space filling than those of the organic templates previously reported in the literature, which lead to stronger structural directing. Kinetic results show that the activation energy of this novel organic template is much lower than that of the traditional one. Catalytic tests show that copper exchanged RTH zeolite (Cu-RTH) exhibits good catalytic properties in the NH3-SCR reaction and the H-RTH zeolite catalyst has excellent selectivities for ethylene and propylene in MTO reactions.

The nanocomposite preparation procedure plays an important role in achieving a well-established heterostructured junction, and hence, an optimized photocatalytic activity. In this study, a series of g-C3N4/ZnO nanocomposites were prepared through two distinct procedures of a low-cost, environmentally-friendly, in-situ fabrication process, with urea and zinc acetate being the only precursor materials. The physicochemical properties of synthesized g-C3N4/ZnO composites were mainly characterized by XRD, UV&ndash, VIS diffuse reflectance spectroscopy (DRS), N2 adsorption-desorption, FTIR, TEM, and SEM. These nanocomposites&rsquo, photocatalytic properties were evaluated in methylene blue (MB) dye photodecomposition under UV and sunlight irradiation. Interestingly, compared with ZnO nanorods, g-C3N4/ZnO nanocomposites (x:1, obtained from urea and ZnO nanorods) exhibited weak photocatalytic activity likely due to a &ldquo, shading effect&rdquo, while nanocomposites (x:1 CN, made from g-C3N4 and zinc acetate) showed enhanced photocatalytic activity that can be ascribed to the effective establishment of heterojunctions. A kinetics study showed that a maximum reaction rate constant of 0.1862 min-1 can be achieved under solar light illumination, which is three times higher than that of bare ZnO nanorods. The photocatalytic mechanism was revealed by determining reactive species through adding a series of scavengers. It suggested that reactive ∙O2&minus, and h+ radicals played a major role in promoting dye photodegradation.

The conversion of bioethanol into valuable products is an important area in the conversion of biomass. We demonstrate the successful synthesis of bimetallic gold-palladium (Au-Pd) nanoparticles encapsulated within S-1 zeolite crystals (AuPd@S-1) by a solvent-free strategy. This strategy allows highly efficient use of the noble metals, with more than 96 % of the gold and palladium being loaded into the final samples. Electron microscopy characterization and investigations with probe molecules confirm that the Au-Pd nanoparticles are encapsulated inside the S-1 crystals. The AuPd@S-1 catalyst is very active for the aerobic oxidation of bioethanol, giving 100 % conversion and 99 % selectivity to acetic acid. Even in the presence of 90 % water, the catalyst still gives a conversion higher than 80 % and a selectivity of 95 %. More importantly, the AuPd@S-1 catalyst exhibits excellent stability in the oxidation of bioethanol. These features are important for future practical applications of the AuPd@S-1 catalyst.

We report a solvent-free synthesis of all silica Beta zeolite using a cheap organic template of tetraethylammonium bromide (TEABr). The method includes mixing, grinding and heating solid raw material in the absence of water solvent but the presence of zeolite seeds. The absence of water solvent significantly improves the efficiency of synthesis, while the addition of seeds remarkably enhances the crystallization rate. In addition, the use of a cheap organic template of TEABr greatly decreases the synthesis cost. The effects of the reaction compositions, including the molar ratios of NH4F/SiO2, TEABr/SiO2, and mass ratios of seeds to the silica, on the synthesis of the pure product were investigated using different temperature. Physicochemical characterizations, including XRD, SEM, TG and N2 sorption, show that the zeolitic product has good crystallinity, uniform crystals, and high surface area.

The development of the sustainable synthesis of zeolites has become a very hot topic in recent years. Herein, we report a sustainable route for synthesizing all-silica SOD zeolite under solvent-free conditions. The method of solvent-free synthesis includes mixing, grinding, and heating raw solids. The all-silica SOD zeolite obtained was well characterized by multiple measurement techniques (XRD, SEM, IR, thermogravimetric-differential thermal analysis (TG-DTA), and magic angel spinning nuclear magnetic resonance (MAS NMR)). The crystallization process of all-silica SOD zeolite was also investigated in detail by XRD, SEM, UV-Raman, and MAS NMR techniques. In addition, the effects of the crystallization compositions, including the molar ratios of Na2O/SiO2 and ethylene glycol/SiO2, on the synthesis of the pure all-silica SOD zeolite were investigated at different temperatures.

Structurally interlocked multi-armed carbon with a highly extended surface may be conveniently prepared by the deterministic growth of ZIF-8 on ZnO multiarms and the subsequent pyrolysis, which exhibits excellent stability and methanol corrosion resistance for oxygen reduction application.

The development of highly-efficient catalysts for conversion of glucose and fructose to 5-hydroxymethylfurfural (HMF) is of great importance. In this work, theoretical simulations form the basis for rational design and synthesis of a superhydrophobic mesoporous acid, that can completely prevent HMF hydration, giving HMF as sole product from full conversion of fructose. Interestingly, the combined superhydrophobic solid acid and superhydrophilic solid base catalysts are very efficient for one-pot conversion of glucose to HMF, giving a yield as high as 95.4 %. The excellent catalytic data in the conversion of glucose to HMF is attributed to the unique wettabilities of the solid acid and base catalysts.

Homogeneous chiral catalysts usually show higher catalytic activities than corresponding heterogeneous chiral catalysts, because of their easy interaction between catalytically active sites with reactant molecules. We demonstrate here superhydrophobic, chiral, and mesoporous catalysts (TsDPEN-Ru) synthesized from copolymerization of N-p-styrenesulfonyl-1,2-diphenylethylenediamine (V-TsDPEN) with divinylbenzene and loading of Ru species exhibiting much higher activities in asymmetric transfer hydrogenation (ATH) of ketones in aqueous solution than corresponding homogeneous chiral catalyst. This phenomenon is strongly related to the unique features of high enrichment for the reactants in superhydrophobic TsDPEN-Ru catalysts due to their good wettability, as well as easy transfer of product from the catalyst into water phase. These features open a door for design and developing a wide variety of chiral catalysts for asymmetric catalysis.

Sulfated porous carbon (PC-SO 3 H) catalyst was successfully synthesized from one-pot treatment of porous polydivinylbenzene in H 2 SO 4 at 250 °C, which exhibited very good catalytic performances in the production of 5-hydroxymethylfurfural from fructose.

Co-salen functionalized on graphene with an average pore size of 27.7 nm as a heterogeneous catalyst exhibited good catalytic activity and recyclability in cyclohexene oxidation.

Magnetically active and SO3H-functionalized ordered mesoporous resin and carbon (MOMR-SO3H, MOMC-SO3H) were successfully prepared by high-temperature hydrothermal synthesis from resol, copolymer surfactant, and iron cations at 180 °C, followed by sulfonation from sulfuric acid fuming. X-ray diffraction patterns show that MOMR-SO3H and MOMC-SO3H have ordered hexagonal mesoporous symmetry. N2 isotherms indicate that these samples have uniform and opened mesopores, high surface areas (335–591 m2/g), and large pore volumes (0.34–0.35 cm3/g). Transmission electron microscopy shows that iron nanoparticles, which are superparamagnetic in nature, are highly dispersed in MOMC-SO3H sample. Catalytic tests show that MOMC-SO3H is highly active and excellently recyclable in esterification of acetic acid with butanol, esterification of acetic acid with cyclohexanol, and condensation of benzaldehyde with ethylene glycol. More interestingly, MOMC-SO3H catalyst is magnetically active, showing potential applications for separating catalysts by a magnetic field in the future.

Small-pore zeolite levyne has been successfully synthesized following an organotemplate-free route using RUB-50 zeolite as seeds with the aid of a small amount of alcohols. Physicochemical characterization with a combination of techniques including XRD, N 2 adsorption, FE-SEM, 27 Al and 29 Si NMR, and TPD-NH 3 shows that the zeolitic product from this seed-directed organotemplate-free synthesis approach (designated as LEV-SDS) has good crystallinity, high surface area, uniform crystals, tetrahedral Al 3+ species, and abundant acidic sites. It is also found that alcohols play an important role in preparation of LEV-SDS zeolite by inhibiting the formation of MOR zeolite. Catalytic tests for the conversion of methanol-to-olefins (MTO) show that H-form of LEV-SDS zeolite exhibits good conversion of methanol and high selectivities for ethylene and propylene, which could be potentially important for using LEV-SDS zeolite as a catalyst in MTO reaction.

Novel excellent hydrophobic- mesoporous- polymer-based solid acid catalysts have been successfully synthesized by copolymerization of divinylbenzene (DVB) with sodium p-styrene sulfonate (H-PDVB-x-SO3H's) under solvothermal conditions. N2 isotherms and TEM images showed that H-PDVB-x-SO3H's have high BET surface areas, large pore volumes, and abundant mesoporosity; CHNS element analysis and acid–base titration technology showed that H-PDVB-x-SO3H's have adjustable sulfur contents (0.31–2.36 mmol/g) and acidic concentrations (0.26–1.86 mmol/g); TG curves showed that H-PDVB-x-SO3H's exhibited much higher stability of the active site (372 °C) than that of the acidic resin of Amberlyst 15 (312 °C); contact angle and water adsorption tests showed that H-PDVB-x-SO3H's exhibited excellent hydrophobic properties. Catalytic tests in esterification of acetic acid with cyclohexanol, esterification of acetic acid with 1-butanol, and condensation of benzaldehyde with ethylene glycol showed that H-PDVB-x-SO3H's were mo...

A solvent-free route is developed for synthesizing titanosilicate zeolites with good crystallinity, uniform crystals, high surface area, and tetrahedral Ti species in the framework. Catalytic tests show that S-TS-1 exhibits almost the same catalytic activity in hexane oxidation with H2O2 as that of conventional TS-1 synthesized by a hydrothermal route.

We report on our systematic investigation of Au nanoparticles highly dispersed in the mesopores of (s)-(–)-2-pyrrolidinone-5-carboxylic acid (Py)-modified SBA-15 (Au/SBA-15-Py) by using a series of modern techniques. 13C NMR and IR spectroscopies indicate that Py species are successfully grafted on the surface of mesopores in SBA-15; XRD patterns and N2 adsorption isotherms show that the sample mesostructures are well preserved; TEM images clearly confirm the uniform Au nanoparticles in the mesopores; and XPS suggests an interaction between Au nanoparticles with Py species. Interestingly, Au/SBA-15-Py catalysts always exhibit superior catalytic properties in the oxidation of cyclohexene and styrene by molecular oxygen at atmospheric pressure, compared with the pyrrolidone-free SBA-15 supported Au catalyst (Au/SBA-15-N). This phenomenon is reasonably related to the interaction between Au nanoparticles with Py species, which is consistent with results analyzed from our density-functional theory (DFT) calculations.

Conventional quantum dots inherently carry the risk of cytotoxicity. Considering the biomedical limitations, an amino acid and vitamin were utilized to prepare highly luminescent carbon dots. Ascorbic acid and lysine were used to synthesize water soluble carbon dots which are highly biocompatible as both reactants and essential nutrients.

Development of sustainable routes for synthesis of zeolites is very important because of wide applications of zeolites at large scale in the fields of catalysis, adsorption, and separation. Here we report a novel and generalized route for synthesis of zeolites in the presence of NH4F from grinding the anhydrous starting solid materials and heating at 140-240 °C. Accordingly, zeolites of MFI, BEA*, EUO, and TON structures have been successfully synthesized. The presence of F(-) drives the crystallization of these zeolites from amorphous phase. Compared with conventional hydrothermal synthesis, the synthesis in this work not only simplifies the synthesis process but also significantly enhances the zeolite yields. These features should be potentially of great importance for industrial production of zeolites at large scale in the future.

A family of polymer-attached phenanthrolines was prepared from solvothermal copolymerization of divinylbenzene with N-(1,10-phenanthroline-5-yl)acrylamide in different ratios. The polymer-supported copper catalysts were obtained through typical impregnation with copper(II) salts. The polymers and supported copper catalysts have been characterized by N2 adsortion, scanning electron microscopy (SEM), transmission electron microscopy (TEM), and thermogravimetric analysis (TG); they exhibit a high surface area, hierarchical porosity, large pore volume, and high thermal and chemical stabilities. The copper catalyst has proved to be highly active for Glaser homocoupling of alkynes and Huisgen 1,3-diolar cycloaddition of alkynes with benzyl azide under mild conditions at low catalyst loading. The heterogeneous copper catalyst is more active than commonly used homogeneous and nonporous polystyrene-supported copper catalysts. In particular, the catalyst is easily recovered and can be recycled at least ten times without any obvious loss in catalytic activity. Metal leaching was prevented due to the strong binding ability of phenanthroline and products were not contaminated with copper, as determined by ICP analysis.

Homogeneous catalysts usually show higher catalytic activities than heterogeneous catalysts because of their high dispersion of catalytically active sites. We demonstrate here that heterogeneous catalysts of ionic liquids functionalized on superhydrophobic mesoporous polymers exhibit much higher activities in transesterification to form biodiesel than homogeneous catalysts of the ionic liquids themselves. This phenomenon is strongly related to the unique features of high enrichment and good miscibility of the superhydrophobic mesoporous polymers for the reactants. These features should allow the design and development of a wide variety of catalysts for the conversion of organic compounds.

We have demonstrated that an organotemplate-free and seed-directed route has been successfully applied for synthesizing Fe-Beta zeolite with good crystallinity, high surface area, uniform crystals, and tetrahedral Al3+ and Fe3+ species. Catalytic tests for the direct decomposition of nitrous oxide indicate that the Fe-Beta exhibits excellent catalytic performance.

Sulfonated hollow sphere carbon (HSC-SO3H) was synthesized from carbonization of a SiO2–polymer core–shell structure, followed by removal of the SiO2 core and sulfonation with chlorosulfonic acid. HSC-SO3H shows superior performances in acetalisation of glycerol, which is related to the hollow sphere carbon shell with rich microporosity for good mass transfer in the reaction.

Graphene with its two-dimensional sheet of sp2-hybridized carbon is a hot topic in the fields of materials and chemistry due to its unique features. Herein, we demonstrate that sulfated graphene is an efficient solid catalyst for acid-catalyzed liquid reactions. The sulfated graphene was synthesized from a facile hydrothermal sulfonation of reduced graphene oxide with fuming sulfuric acid at 180 °C. Combined characterizations of XRD, Raman, and AFM techniques show that G-SO3H has a sheet structure (1–4 layers). IR spectroscopy shows that G-SO3H has a SO bond, and the XPS technique confirms the presence of an S element in G-SO3H. Acid–base titration indicates that the acidic concentration of sulfonic groups in the sulfated graphene is 1.2 mmol g−1. TG curves shows that the decomposition temperature (268 °C) of the sulfonic groups on the sulfated graphene is much higher than that of conventional SO3H-functionalized ordered mesoporous carbon (237 °C). Catalytic tests of the esterification of acetic acid with cyclohexanol, the esterification of acetic acid with 1-butanol, the Peckmann reaction of resorcinol with ethyl acetoacetate, and the hydration of propylene oxide show that sulfated graphene is much more active than the conventional solid acid catalysts of Amberlyst 15, OMC-SO3H, SO3H-functionalized ordered mesoporous silica (SBA-15-SO3H), graphene oxide, and reduced graphene oxide, which is attributed to the fact that the sulfated graphene almost has no limitation of mass transfer due to its unique sheet structure. Very importantly, the sulfated graphene has extraordinary recyclability in these reactions, which is attributed to the stable sulfonic groups on the sulfated graphene. The advantages, including high activities and good recyclability as well as simple preparation, are potentially important for industrial applications of the sulfated graphene as an efficient heterogeneous solid acid catalyst in the future.

The methanol-to-olefins (MTO) reaction over zeolites is of great importance due to the shortage of crude oil, and we demonstrate here a fast, organotemplate-free, and seed-directed synthesis of ZSM-34 zeolite, designated as ZSM-34-S, having very high selectivity for propylene. When the temperature is at 140–180 °C, ZSM-34-S zeolite could be crystallized for 2–6 h in the presence of ZSM-34 crystals as seeds. For industry, a fast and organotemplate-free synthesis, a typically green route, means significant savings in energy and costs. Characterizations using XRD, SEM, 27Al and 29Si MAS NMR, and N2 sorption techniques show that the ZSM-34-S crystals grow from the seeds of ZSM-34 crystals in an amorphous aluminosilicate. Catalytic tests of the MTO reaction show that HZSM-34-S has a very high selectivity for propylene (55.2%), which is even higher than that (47.0%) of SAPO-34 under the same conditions. Moreover, the hydrothermal treatment of HZSM-34-S significantly improves the catalyst life for MTO due to decreasing acidic concentration and increasing anti-deactivation. The combination of a “green” synthesis and the good catalytic performance of ZSM-34-S would be potentially important for the highly effective conversion of methanol, which can be easily obtained from coal, natural gas, or biomass at a large scale.

Hierarchically porous aluminophosphates (SF-APOs) and metal substituted aluminophosphates (SF-MAPOs, M = Co, Fe, Cr) have been synthesized via simple grinding and heating in the absence of solvent. Characterization results show that these mesoporous aluminophosphates have a hierarchically microporous/mesoporous structure. In addition, metal atoms can be efficiently incorporated into the walls of mesoporous aluminophosphates, and the SF-CoAPO sample shows high catalytic activity in cyclohexene oxidation compared with microporous samples. Special features of the “solvent-free” synthesis route, such as increasing product yield, saving energy, elimination of pollution, and convenience for incorporation of heterogeneous atoms, ensure its great potential in the synthesis of porous materials.