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The metal-exchanged zeolites as catalysts have been widely applied in many catalytic reactions, but their syntheses are environmentally unfriendly due to the multiple steps such as ion-exchange for the formation of a large amount of wastes. Herein, we for the first time report a method for one-pot fabrication of metal-zeolite catalysts (M-SSZ-13, M-Beta, M-ZSM-5, and M-EU-1; M = Cu, Co, Ni) from a combination of solvent-free and sodium-free routes by mixing, grinding, and heating the raw materials of aluminosilicate gel, organic templates, and metal-amine complexes. As a typical example, Cu-SSZ-13 zeolite is successfully synthesized from heating the mixture of aluminosilicate gel, organic template, and Cu-amine complex. Catalytic tests in selective catalytic reduction of NOx with NH3 (NH3-SCR) show that the synthesized Cu-SSZ-13 zeolite before and after hydrothermal aging at 750 °C for 16 h are completely comparable with the commercial Cu-SSZ-13 zeolite from the conventional hydrothermal synthesis. Very interestingly, the method in this work has obvious advantages such as high yield, reduced pollutants, and simple process, which should be potentially important for practical applications of the metal-zeolites in the future.

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.

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.

Developing sustainable routes for the synthesis of zeolites is still a vital and challenging task in zeolite scientific community. One of the typical examples is sustainable synthesis of aluminosilicate EU-1 zeolite, which is not very efficient and environmental-unfriendly under hydrothermal condition due to the use of a large amount of water as solvent. Herein, we report a sustainable synthesis route for aluminosilicate EU-1 zeolite without the use of solvent for the first time. The physicochemical properties of the obtained EU-1 zeolite are characterized by powder X-ray diffraction (XRD), scanning electron microscopy (SEM), thermogravimetry-differential thermal analysis (TG-DTA), N2 sorption, inductively coupled plasma (ICP) analysis, and solid nuclear magnetic resonance (NMR), which show the product has high crystallinity, uniform morphology, large BET surface area, and four-coordinated aluminum species. Moreover, the impact of synthesis conditions is investigated in detail. The sustainable synthesis of aluminosilicate EU-1 zeolite under solvent-free

As one of the most important porous materials, zeolites with intricate micropores have been widely employed as catalysts for decades due to their large pore volume, high surface area, and good thermal and hydrothermal stabilities. Among them, ferrierite (FER) zeolite with a two-dimensional micropore structure is an excellent heterogeneous catalyst for isomerization, carbonylation, cracking, and so on. In the past years, considering the important industrial application of FER zeolite, great efforts have been made to improve the synthesis of FER zeolite and thus decrease the synthesis cost and enhance catalytic performance. In this review, we briefly summarize the advances in the synthesis of FER zeolite including the development of synthesis routes, the use of organic templates, organotemplate-free synthesis, the strategies of morphology control, and the creation of intra-crystalline mesopores. Furthermore, the synthesis of hetero-atomic FER zeolites such as Fe-FER and Ti-FER has been discussed.

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.

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.

We show that a nickel-amine complex (nickel-diethylenetriamine, Ni-DETA) is an efficient organic template for the one-pot synthesis of Ni-SSZ-13 zeolite. The effects of the reaction compositions, including the molar ratios of SiO2/Al2O3, H2O/Al2O3, Ni-DETA/Al2O3, and Na2O/Al2O3, on the synthesis of the pure product were investigated using different temperatures and synthesis times. Physicochemical characterizations, including XRD, SEM, and 27Al NMR, show that the zeolitic product has good crystallinity, uniform crystals, and contains a tetrahedral Al3+ species. The N2 sorption isotherms, TG–DTA curves, IR spectra, and UV–Vis spectra show that Ni-DETA acts as a template in the product obtained. Interestingly, Ni-SSZ-13 zeolite is obtained by the conversion of Ni-Y zeolite produced in the crystallization process.

Preparation of aluminosilicate ferrierite (FER) zeolite nanosheets with controllable thickness in the presence of a sole organic ammonium is attractive, but still challenging. In this report, with the employment of N,N-diethyl-cis-2,6-dimethylpiperidinium (DMP) as both a structure directing agent and crystal growth inhibitor, aluminosilicate FER zeolite nanosheets, with a variety of crystal thicknesses, ranging from 6 to 200 nm, are successfully synthesized under hydrothermal conditions. Very interestingly, the amount of DMP in the starting gel is the key factor for crystal thickness control of aluminosilicate FER zeolite nanosheets. The obtained FER products, with different thicknesses, are well characterized by X-ray powder diffraction (XRD), scanning electron microscopy (SEM), N2 sorption, thermogravimetric analysis (TG), inductively coupled plasma (ICP), and magic angle spinning nuclear magnetic resonance (MAS NMR) techniques. This simple strategy might provide a novel avenue for the synthesis of other zeolite nanosheets with controllable thickness.

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–VIS diffuse reflectance spectroscopy (DRS), N2 adsorption-desorption, FTIR, TEM, and SEM. These nanocomposites’ 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 “shading effect”, 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 two 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− and h+ radicals played a major role in promoting dye photodegradation.

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.

Reported in this paper is a solvothermal synthesis of highly porous polydivinylbenzene. The nanoporous structures of the resultant polymers could be modulated from macro/mesoporosity to meso/microporosity by simply changing the amount of acetone solvent in the synthesis. A micro-phase separation during the solvothermal process was found to be the key factor for this transition in porous structures. The hierarchically porous polymers prepared here were characterized by N 2 physi-sorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM), and contact angle testing. Experimental results show that these nanoporous polymers have large BET surface areas (up to 420 m 2 /g), large pore volumes (up to 1.73 cm 3 /g), and superhydrophobicity due to their highly porous structures, which make these nanoporous materials an excellent candidate for selective removal of toxic volatile organic compounds (VOCs). In the adsorption tests, the nanoporous polymers show outstanding adsorptive capacity and very high selectivity to organic compounds, giving a great potential for indoor VOCs removal.

Magnetically active, thermally stable, and ordered mesoporous resin (MOMR-200) and carbon (MOMC-200) monoliths were prepared by one-pot hydrothermal synthesis from resol, copolymer surfactant, and iron cations at high-temperature (200 ∘C), followed by calcination at 360 ∘C and carbonization at 600 ∘C. X-ray diffraction results show that both MOMR-200 and MOMC-200 have ordered hexagonal mesoporous symmetry, and N2 isotherms indicate that these samples have uniform mesopores (3.71, 3.45 nm), high surface area (328, 621 m2/g) and large pore volume (0.31, 0.43 cm3/g). Transmission electron microscopy shows that iron nanoparticles, which are superparamagnetic in nature, are dispersed in the network. More importantly, the high temperature (200 ∘C) products exhibit much better stability than the samples synthesized at low temperature (100 ∘C). Interestingly, MOMC-200 has higher adsorption capacity for organic dyes when compared with commercial adsorbents (activated carbon and macroporous resin: XAD-4). Combining the advantages such as magnetically active, thermally stable networks, ordered and open mesopores, high surface area, large pore volume, adsorption of pollutants in water and desorption in ethanol solvent, MOMC-200 is potentially important for water treatments.

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.

The modern synthesis of zeolites typically uses organic structure-directing agents. Therefore, the developing of new templates is part of zeolite research. The design and synthesis of Cu-SSZ-13 using a novel template of a low-cost copper amine complex (Cu2+ coordinated with tetraethylenepentamine) were reported, where the copper amine complex is both a template for synthesizing the SSZ-13 structure and a source of copper species in the zeolite. The calculated size of the complex (0.728 nm x 0.922 nm) matches well with the CHA cages (0.73 nm x 1.2 nm), which are the building units of the SSZ-13 zeolite. Various techniques were used to investigate the chemical and physical properties of the synthesized zeolite. The results showed that the sample has the SSZ-13 zeolite structure, high crystallinity, adjustable Si/Al ratios, and controllable copper loading. Catalytic tests using the selective catalytic reduction of NOx with NH3 showed that the Cu-SSZ-13 was a superior catalyst, and it can be important for the abatement of environmentally harmful NOx.

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.