Structure-directing Agent Research Articles

Synthetic Placement of Active Sites in MFI Zeolites for Selective Toluene Methylation to para-Xylene.

Brønsted acidic zeolites are ubiquitous catalysts in fuel and chemical production. Broadening the catalytic diversity of a given zeolite requires strategies to manipulate the acid site placement at framework positions within distinct microporous locations. Here, we combine experiment and theory to elucidate how intermolecular interactions between organic structure-directing agents (OSDAs) and framework Al centers influence the placement of H+ sites in distinct void environments of MFI zeolites and demonstrate the catalytic consequences of active site location on kinetically controlled (403 K) toluene methylation to xylene regioisomers. Kinetic measurements, interpreted using mechanism-derived rate expressions and transition state theory, alongside density functional theory (DFT) calculations show that larger intersection environments similarly stabilize all three xylene isomer transition states without altering well-established aromatic substitution patterns (ortho/para/meta ∼ 60%:30%:10%), while smaller channel environments preferentially destabilize transition states that form bulkier ortho- and meta-isomers, thereby resulting in high intrinsic para-xylene selectivity (∼80%). DFT calculations reveal that the flexibility of nonconventional OSDAs (e.g., 1,4-diazabicyclo[2.2.2]octane) to reorient within MFI intersections and their ability to hydrogen-bond to form protonated complexes favor the placement of Al in smaller channel environments compared to conventional quaternary OSDAs (e.g., tetra-n-propylammonium). These molecular-level insights establish a mechanistic link between OSDA structure, active site placement, and transition state stability in MFI zeolites and provide active site design strategies that are orthogonal to crystallite design approaches harnessing complex reaction-diffusion phenomena to enhance regioisomer selectivity in the industrial production of valuable polymer precursors.

GO based nanocomposite hydrogel enabled high performance wearable all-solid supercapacitor based on hierarchical structure electrodes derived from ZIF-67

The flexible and wearable supercapacitors have attracted wide interest because of their widespread application in smart electronic devices with rapid charging and discharging. As an important part of supercapacitor, the electrode materials with a hollow structure, especially those with hierarchical structures that provide an array of continuous hollow cages, are considered promising. Because of its porous shell which is rich in redox reaction sites for supercapacitors. In this work, we fabricated a ZIF-67 derived hollow Co3O4 growth on the surface of 1D NiCo2O4 to assemble into a beaded structure. In this case, NiCo precursor acted as a structure-directing agent to grow a ZIF-67, a promising electroactive material of electrochemical capacitors to provide capacitance after calcination. Combined with the grapheneoxide (GO) based high conductivity hydrogel as the solid electrolyte, the capacitance of the flexible supercapacitor exhibited a high specific capacitance of 90F g−1 at 0.5 A/g, and it was sturdy and durable. There was no significant loss of capacitance while suffering from bending and pressing. The outstanding electrochemical properties of the all-solid supercapacitor can be attributed to the unique nanostructure of the electrode that created more reactive active sites, increased the diffusion pathway for electrolyte ions, along with the high conductivity of the hydrogel electrolyte.

Synthesis of Two-Dimensional Zeolite Nanosheets Applied to the Catalytic Cracking of a Waste Cooking Oil Model Compound to Produce Light Olefins.

Hierarchical zeolites can provide multidimensional spatial networks and, therefore, have significant potential as catalysts for the cracking of biomass to generate light olefins. The present work synthesized the diquaternary ammonium-type surfactant [C18H37-N+(CH3)2-(CH2)6-N+(CH3)2-C6H13]Br2, incorporating hydrophobic 18-carbon alkyl groups for usage as a structure-directing agent. This compound was subsequently used to prepare nanosheets of a hierarchical ZSM-5 two-dimensional zeolite (HNZSM-5) through a one-pot hydrothermal method. The crystal phase, morphology, and hierarchical structure of the HNZSM-5 were analyzed using various techniques, including X-ray diffraction, electron microscopy, and N2 adsorption/desorption. When applied to the catalytic cracking of a waste cooking oil model compound, the HNZSM-5 exhibited superior activity and stability compared with a conventional ZSM-5. This performance was attributed to the more accessible acid sites and unique lamellar structure of the former material. The HNZSM-5 also outlasted the conventional zeolite, showing deactivation after 45 h of reaction compared with 20 h, indicating exceptional stability and excellent resistance to coking.

Synthesis, characterization, and evaluation of the CO2 adsorption capacities of beta, ZSM-12, ZSM-48, and silicalite-1 zeolites obtained in the presence of tetraethylammonium hydroxide and 1,6-diaminohexane as organic structure-directing agents

Synthesis, characterization, and evaluation of the CO2 adsorption capacities of beta, ZSM-12, ZSM-48, and silicalite-1 zeolites obtained in the presence of tetraethylammonium hydroxide and 1,6-diaminohexane as organic structure-directing agents

Large-scale synthesis of size-controlled amorphous and anatase TiO2 via a benzoic acid-assisted sol-gel-hydrothermal process

The ability to control the particle size of titanium dioxide nanoparticles (TNPs) is crucial for their practical use. This study presents a method for preparing monodisperse amorphous and anatase TNPs with high surface areas and tunable grain sizes. The method combines a sol-gel process with a hydrothermal process, using benzoic acid (BA) as a structure-directing agent. By adjusting the hydrolysis and condensation rates of the titanium alkoxide, we can synthesize monodisperse amorphous TNPs with a controllable size range of 200–800 nm. Additionally, the amorphous TNPs synthesized through this method serve as raw material, enabling the morphology of anatase TNPs to be inherited from amorphous TNPs with a hydrothermal reaction time of 1 h. When the hydrothermal reaction time is extended to 10 h, the closely linked primary titanium dioxide is fully separated and replaced by ultra-fine anatase TNPs. This optimal scheme show promise for self-assembly and large-scale synthesis of monodisperse amorphous and anatase TNPs.

Assembled pentasil nanosheet zeolites: Adjusting the sheet thickness through a simple and direct dual templating approach

A simple one-step synthesis method is demonstrated, enabling the thickness of assembled silicalite nanosheets to be tuned from 2 to 30 nm. The adjustement is achieved by mixing two common organic structure-directing agents (OSDAs): tetrapropylammonium (TPA) and tetrabutylammonium (TBA). During the hydrothermal synthesis, there is a preferential uptake of TPA, and the proportion of incorporated TBA can be deduced accordingly. The proportion of TBA, known to favour silicalite nanosheets, determines the nanosheets’ thickness and the morphological variations observed.

Efficient degradation of naproxen in wastewater using Ag-deposited ZnO nanoparticles anchored on a house-of-cards-like MFI-type zeolite: Preparation and physicochemical evaluations of the photocatalyst

We utilized Pr6-diquat-5 as an organic structure-directing agent (OSDA) to synthesize hierarchically intergrown ZSM-5 (HI-ZSM-5) as a catalytic support. ZnO particles were deposited onto HI-ZSM-5 via precipitation to remediate naproxen (NPX) in wastewater, while Ag was photo-deposited onto ZnO to prevent electron-hole pair recombination. XRD analysis revealed crystalline structures and particle sizes influenced by synthesis temperatures, and FT-IR confirmed ZnO and Ag deposition onto HI-ZSM-5 surfaces. Based on N2 adsorption-desorption isotherms, all samples exhibited Type I and IV isotherms with H4-type hysteresis loops, indicating the presence of both micro- and mesopores within HI-ZSM-5. XPS analysis confirmed the presence of peaks indicating Zn in ZnO and metallic Ag interacting with ZnO. TEM analysis identified aggregated Ag/ZnO nanoparticles in the photocatalysts, while EDX confirmed uniform element distribution. FE-SEM images revealed a uniform distribution of ZnO and Ag on HI-ZSM-5 with “house-of-cards” morphologies. PL analysis indicated reduced electron-hole recombination and an extended lifespan. NPX photodegradation experimental results showed that the reaction rate constant of the 3 %AZ composite was 2.8 times higher than that of ZnO/HI-ZSM-5 (0.0163 vs. 0.059 min−1, respectively). Evaluation of influential operating parameters demonstrated 90.8 % elimination of NPX under optimum conditions: a catalyst dosage of 1.5 g L−1 at pH 5 within 120 min. The impact of common anions on NPX decontamination and the catalyst's capability for COD and TOC removal (up to 62.6 and 53.4 %, respectively) was also discussed. The 3 %AZ optimum catalyst could be recycled for 5 cycles with remarkable reusability, maintaining 80.1 % removal efficiency after five regeneration cycles.

Insights into the Synthesis of Spiral Beta Zeolite with Enhanced Catalytic Performance in VOC Abatement.

The rational synthesis of zeolites with designed morphology is a highly challenging task. In this study, we propose 1,5-bis(methylpiperidine)pentylammonium hydroxide (BMPPAOH) as an organic structure-directing agent (OSDA) based on theoretical calculations. The morphology of zeolite samples is characterized by XRD, SEM, TEM, N2 sorption isotherms, and UV Raman spectroscopy. This simple bis-quaternary ammonium salt favored the formation of spiral morphology in Beta zeolite spheres (S-Beta). The crystallization of zeolite in the presence of BMMPAOH is a two-stage process, where nanoparticles agglomerate into spheres in the early stages followed by the emergence of S-Beta crystals with spiral morphology. The synthesized Pt-S-Beta catalysts show higher catalytic activity in VOC abatement compared with other Pt-Beta samples.

Rational design on hierarchically porous Cu/ZSM-5 zeolite for promoting low-temperature NH3-SCR performance based on protectively alkali-etching strategy

In this study, organic structure-directing agents (OSDA) of TPA+ are used as templating agents to synthesize zeolites with different topologies, and are also served as protectants for alkali treatment to inhibit the severe silicon extraction from zeolite skeleton. The TPA+ cations could be bound to the negatively charged Al sites in the framework, so we prepared a series of Cu-based ZSM-5 catalysts with mesoporous/microporous composite structure by using TPA+ cation as a protectant for alkali treatment and evaluated the pore structures by using the hierarchy factor (HF). The results show the hierarchically mesoporous/microporous structure of the alkali-etched catalyst with the maximal HF (0.115) effectively improved the low-temperature activity on selective catalytic reduction (SCR) of NO by ammonia, achieving a complete NOx to N2 conversion at 225–400 ºC. It was shown that the TPA+ cation played an important role on protecting the crystallinity, long-range order, and pore connectivity of zeolites, and substantially widened the mesopore volume with the loss of a small portion of micropores. In addition, the alkali treatment strategy involving protectant was systematically studied, including the corresponding effect on the pore structure, redox ability, acidity, and copper ion dispersion. The N2 adsorption-desorption experiments revealed that the maximization of the HF can be obtained by adjusting the ratio of protectant to etchant (TPA+/OH-). Among them, the Cu/ZSM-5 catalyst associated with the ratio of TPA+/OH-=0.4 and the best activity has a maximum surface area of 515 m2/g, which enhances the mesopore volume (0.325 cm3/g) by approximately three times simultaneously with only a 16.9% loss of the micropore volume (0.154 cm3/g). The hierarchically porous zeolites not only enhance the diffusion of mobile hydrated copper ions and ammonia-solvated copper complexes, but also facilitate the dispersion of copper ions. This work provides a feasible strategy to rapidly enhance the low-temperature deNOx efficiency on the zeolite catalysts.

Harvest pitch-based carbon nanosheets by oxidation and in-situ template strategy for all-solid-state supercapacitors

Transforming coal tar pitch (CTP) into porous carbon nanosheets (PCNS) offers a dual advantage: maximizing the value of CTP while pioneering novel carbon materials. A key challenge in synthesizing pitch-based PCNS lies in the hydrophobic nature and polycondensation of polycyclic aromatic hydrocarbons (PAHs) in CTP, limiting the integration of water-soluble additives and the formation of desired pore structures. In this study, oxidation process, commonly used in preparing pitch-based carbon fibers, was introduced into the synthesis pitch-based PCNS to address the aforementioned challenges. Through oxidization modification, hydrophilic functional groups rich in O, N and P were introduced to PAHs, while macromolecules were partially broken down into smaller aromatic compounds. Following oxidation, the carbon nanosheet structure was successfully achieved through co-carbonization of oxidized CTP and urea, during which the structure-directing agent C3N4 was generated in-situ. Moreover, the efficacy of oxidation modification in the formation of nanosheet structures was assessed by comparing the structures of porous carbon derived from CTP both pre- and post-oxidation. In final, pitch-based PCNS were used in supercapacitors. In three-electrode system, capacitance of PCNS attained 331.3 F/g at 0.5 A/g, and its response speed, capacitance retention rate and ion transfer speed were also excellent. For solid state supercapacitor, its energy density and cycle stability after 10,000 cycles were 8.3 Wh/kg and 92.4%, respectively.

A chiral zeolite material with improved enantioselective catalytic properties prepared from readily accessible ephedrine alkaloids

Substituted-benzyl-containing N-methyl-ephedrinium derivatives (BMEP), prepared from the highly-accessible (1R,2S)- or (1S,2R)-ephedrine alkaloids, have been found to act as efficient structure-directing agents for the synthesis of chiral zeolite GTM-4 with –ITV framework structure, promoting the enantio-enrichment in one of the chiral crystalline polymorphs as a function of the organic handedness. Results of a systematic variation of substituents in the benzyl ring attached to the ephedrine core (with methyl-, fluoro- or chloro-groups in the different positions of the aromatic ring) revealed that F-containing SDAs brought about an improvement in the structure-directing ability toward the –ITV framework, giving asymmetric zeolite acid-catalysts that yielded notable enantiomeric excesses in the range of 40–45 % for the trans-stilbene oxide ring-opening with 1-butanol. Interestingly, the incorporation of a methyl group in ortho-position (oMBMEP) had a double positive effect: on the one hand, this SDA prevented the crystallization of the competing BEC phase, allowing the crystallization of the -ITV structure at higher temperature and with higher crystallinity, and on the other, it drove to GTM-4 asymmetric catalysts that yielded enantiomeric excesses up to 60 %, resulting in the chiral GTM catalysts with the best enantioselective properties found so far. Remarkably, our catalytic results show the same chiral activity (in terms of zeolite handedness) for GTM-4 materials prepared from benzyl-containing (1S,2S)-N-methyl-pseudoephedrinium (BMPS) and (1S,2R)-N-methyl-ephedrinium (BMEP) derivatives, thus suggesting that the host-guest transfer of chirality during crystallization with these chiral organic aromatic agents is imposed by the absolute configuration of the C1 atom to which the OH group is attached. The relatively high enantiomeric excess of 60 % achieved, combined with the high accessibility of the ephedrine chiral precursors used for the synthesis that enables the production of both crystalline handedness of the –ITV framework, bring these materials closer to a potential application as heterogeneous asymmetric catalysts for the synthesis of chiral compounds of interest.

One-Pot Synthesis of CHA/ERI-Type Zeolite Intergrowth from a Single Multiselective Organic Structure-Directing Agent.

We report the one-pot synthesis of a chabazite (CHA)/erionite (ERI)-type zeolite intergrowth structure characterized by adjustable extents of intergrowth enrichment and Si/Al molar ratios. This method utilizes readily synthesizable 6-azaspiro[5.6]dodecan-6-ium as the exclusive organic structure-directing agent (OSDA) within a potassium-dominant environment. High-throughput simulations were used to accurately determine the templating energy and molecular shape, facilitating the selection of an optimally biselective OSDA from among thousands of prospective candidates. The coexistence of the crystal phases, forming a distinct structure comprising disk-like CHA regions bridged by ERI-rich pillars, was corroborated via rigorous powder X-ray diffraction and integrated differential-phase contrast scanning transmission electron microscopy (iDPC S/TEM) analyses. iDPC S/TEM imaging further revealed the presence of single offretite layers dispersed within the ERI phase. The ratio of crystal phases between CHA and ERI in this type of intergrowth could be varied systematically by changing both the OSDA/Si and K/Si ratios. Two intergrown zeolite samples with different Si/Al molar ratios were tested for the selective catalytic reduction (SCR) of NOx with NH3, showing competitive catalytic performance and hydrothermal stability compared to that of the industry-standard commercial NH3-SCR catalyst, Cu-SSZ-13, prevalent in automotive applications. Collectively, this work underscores the potential of our approach for the synthesis and optimization of adjustable intergrown zeolite structures, offering competitive alternatives for key industrial processes.

Green and stable synthesis of MCM-56 zeolite by using choline chloride as template

It is desirable to develop eco-friendly structure-directing agents as an alternative to the highly toxic templates during the synthesis process of many zeolites. In this work, a MWW type zeolite (denoted as CC-MCM-56) was stably synthesized with ITQ-1 seed assistance by using a green and nuisance-less choline chloride (CC) as organic structure-directing agents instead of the conventional toxic (HMI) template. The CC-MCM-56 zeolite exhibited similar physicochemical properties to the conventional MCM-56 (HMI), including acid properties, high specific surface area, especially high external specific surface area and mesoporous volume, which performed an excellent result in the liquid-phase alkylation reaction of benzene with long-chain olefins. Our findings reveal that the synergistic effect of ITQ-1 seed and CC molecule enable a longer and more stable crystallization period during the synthesis process of MCM-56 zeolite. The SAXS result coupled with other techniques indicate that ITQ-1 seed is firstly dissolved to form more structural units which could interact with CC molecules, making more CC molecules attached to the surface half cup of the MWW lamellae and promoting the stable synthesis of CC-MCM-56 zeolite with thinner-layer structure. Finally, the synthesized CC-MCM-56 zeolite showed high reactivity and the conversion of 1-hexane and 1-dodecene achieved 90.5% and 90.6% respectively.

The interaction of the structure-directing agent with the zeolite framework determines germanium distribution in SCM-15 germanosilicate

The interaction of the structure-directing agent with the zeolite framework determines germanium distribution in SCM-15 germanosilicate

Concentration and reaction duration effects on synthesizing ZIF67 derivatives with NH4BF4 and NH4HF2 as efficient active material of energy storage device

Zeolitic imidazolate framework-67 (ZIF67) with large surface area and tunable pore structure is intensively applied as a tailoring target for design active materials. An in-situ tailoring technique is proposed to design ZIF67 derivatives by using structure directing agents (SDA) to induce favorable morphology and composition. Ammonium fluoride is a common SDA for modifying surface properties of active materials. With the same ammonium and similar fluorine-based groups, NH4BF4 and NH4HF2 are priming to play as SDA for synthesizing ZIF67 derivatives. In this study, the synthetic process of ZIF67 derivatives is tailored by varying the precursor concentration and reaction time in systems with NH4BF4 and NH4HF2 as SDA. The precursor concentration plays significant roles in the composition of ZIF67 derivatives. The reaction duration has higher influences on the morphology. The highest specific capacitance (CF) of 1347.0 F/g at 20 mV/s is achieved for the ZIF67 derivative synthesized using low concentration and 18 h, owing to favorable cobalt and nickel hydroxide compositions and two-dimensional sheet-like structure. An energy storage device composed of the optimal ZIF67 derivative and carbon electrodes shows a maximum energy density of 11.96 Wh/kg at 650 W/kg. The excellent cycling stability with CF retention of 83.6% and Coulombic efficiency of 92.0% is obtained after 10000 cycles.

Controlling Crystal Morphology of Anisotropic Zeolites with Elemental Composition.

The morphology of zeolite crystals strongly affects their textural, catalytic, and mechanical attributes. However, controlling zeolite crystal morphology without using modifiers or structure-directing agents remains a challenging task because of our limited understanding of the relationships between zeolite crystal shape, crystallization mechanism, and composition of the starting synthesis mixture. In this study, we aimed at developing a general method for controlling the morphology of zeolites by assessing the impact of the Si/T molar ratio of the synthesis gel on the growth rate of zeolite crystals in various crystallographic directions and on the final crystal morphology of the UTL germanosilicate with a 2D system of intersecting 14- and 12-ring pores. Our results showed that flat UTL crystals progressively thicken with the Si/Ge molar ratio, demonstrating that Ge concentration controls the relative rate of crystal growth in the perpendicular direction to the pore system. The morphology of other zeolites and zeotypes with an anisotropic structure, including AFI (12R), IFR (12R), MWW (10-10R), and IWW (12-10-8R), can also be predicted based on their Si/T ratio, suggesting a systematic pattern across zeolite structures and in a wide range of zeolite framework elements. Combined, these findings introduce a facile and cost-efficient method for directly controlling crystal morphology of zeolites with anisotropic structures with a high potential for scale-up while providing further insights into the role of elemental composition in zeolite crystal growth.

ZeoSyn: A Comprehensive Zeolite Synthesis Dataset Enabling Machine-Learning Rationalization of Hydrothermal Parameters.

Zeolites, nanoporous aluminosilicates with well-defined porous structures, are versatile materials with applications in catalysis, gas separation, and ion exchange. Hydrothermal synthesis is widely used for zeolite production, offering control over composition, crystallinity, and pore size. However, the intricate interplay of synthesis parameters necessitates a comprehensive understanding of synthesis-structure relationships to optimize the synthesis process. Hitherto, public zeolite synthesis databases only contain a subset of parameters and are small in scale, comprising up to a few thousand synthesis routes. We present ZeoSyn, a dataset of 23,961 zeolite hydrothermal synthesis routes, encompassing 233 zeolite topologies and 921 organic structure-directing agents (OSDAs). Each synthesis route comprises comprehensive synthesis parameters: 1) gel composition, 2) reaction conditions, 3) OSDAs, and 4) zeolite products. Using ZeoSyn, we develop a machine learning classifier to predict the resultant zeolite given a synthesis route with >70% accuracy. We employ SHapley Additive exPlanations (SHAP) to uncover key synthesis parameters for >200 zeolite frameworks. We introduce an aggregation approach to extend SHAP to all building units. We demonstrate applications of this approach to phase-selective and intergrowth synthesis. This comprehensive analysis illuminates the synthesis parameters pivotal in driving zeolite crystallization, offering the potential to guide the synthesis of desired zeolites. The dataset is available at https://github.com/eltonpan/zeosyn_dataset.

Polyamine functionalized cage hollow mesoporous SiO2 microspheres for CO2 capture over a wide temperature range

Hollow SiO2 microspheres have become attractive materials for nanotechnology applications owing to their biological inertness and high functionality. In this study, hydrophobic spherical hollow cages were formed using the soft stencil method with Pluronic F127 and cetyltrimethylammonium bromide (CTAB) as the structure-directing agent, and hollow nanoporous SiO2 microspheres (FHMS) were prepared using the soft template method. Various of amine functionalization modes were further employed to demonstrate the complexity of the relationship between pore structure/amidation mode/amine content and adsorption capacity. The hollow morphology of the porous silica was revealed using field-emission scanning electron microscopy (SEM) and transmission electron microscopy (TEM), and its porous properties were revealed using nitrogen adsorption-desorption isotherm measurements. Experiments on the fixed-bed dynamic adsorption process at 15% CO2 showed that the high specific surface area, high pore volume and amine content of the carriers had a positive effect on the adsorption performance. However, the accessibility of the adsorption centre was affected at high loadings, and the amine efficiency and adsorption capacity were reduced. The dual amine functionalized FHMS-G-I60 maintained the integrity and order of the hollow mesoporous carrier structure, and overcame the dilemma of easy loss in the cycle process of the impregnation method and the low adsorption capacity of the grafting method. It possessed an adsorption capacity of 3.62 mmol/g, high adsorption cycling stability (more than 99.5% adsorption maintained after 10 cycles) and high amine efficiency (0.2852 mmol CO2/mmol N). CO2-TPD analysis (Thermal Programmed Desorption) further showed that FHMS-G-I60 had a faster desorption rate and lower regeneration energy consumption. In general, such structure-directed prepared matrices and functionalized with different amines are promising and low-cost adsorbents that can be used to capture CO2 from ambient air and flue gases under different demands.

Al-rich Cu-SSZ-13 zeolite synthesized by interconversion from Y: Crystallization process resolution and application in the selective catalytic reduction of NO with NH3

Cu-SSZ-13 zeolite is a promising catalyst in the selective catalytic reduction (SCR) of NOx with NH3 and the interzeolite conversion is considered as a convenient method with relatively low cost to get the Al-rich SSZ-13 zeolite with great hydrothermal stability. However, the crystallization process of interzeolite conversion and its relation to the catalytic performance of Cu-SSZ-13 in the NH3-SCR of NOx are still poorly understood. Herein, the interzeolite conversion process of Y to SSZ-13 was well resolved and the effect of major synthesis factors on the hydrothermal stability and catalytic performance of Cu-SSZ-13 in the NH3-SCR of NOx was investigated. The results indicate that highly crystalline SSZ-13 can be synthesized by the interzeolite conversion from Y, using N,N,N-trimethyl-1-adamantammonium hydroxide (TMAdaOH) as the structure-directing agent (SDA) and with a SDA/Si molar ratio of 0.06–0.2. The Y zeolite of FAU framework is first degraded and decomposed into the oligomeric aluminosilicate fragments quickly in the alkaline circumstance; thereafter, the oligomeric fragments develop into the crystal nuclei that arouse the rapid crystallization of the SSZ-13 zeolite of CHA framework with the help of SDA and solid Al(OH)3, during which the Al(OH)3 source is dissolved and restructured to tetrahedral Al species and incorporated into the CHA framework. The synthesized Cu-SSZ-13 zeolite exhibits excellent catalytic performance in the NH3-SCR of NO, achieving an NO conversion of nearly 90% at a rather low temperature of 150 °C and a gaseous hourly space velocity (GHSV) of 100,000 h−1. Moreover, the Cu-SSZ-13 catalyst displays great hydrothermal stability and remains highly active even after aging at 800 °C. These results help to clarify the mechanism of interzeolite conversion and provide an effective method to synthesize highly crystalline Al-rich SSZ-13 zeolite with great potential for application in the NH3-SCR of NOx.

Disclosing the enhanced NH3-SCR-DeNOx activity of Cu-containing zeolite Y prepared with 15-Crown-5

The phase-pure zeolite Y with a high n(Si)/n(Al) ratio is obtained with the cyclic polyether 15-Crown-5 as a structure-directing agent. In copper-exchanged for this new zeolite outperformed other Cu-containing zeolite Y counterparts during NH3-SCR-DeNOx with more than 80% NO conversion and more than 85% N2 selectivity in the temperature range of 100 – 500 °C. The presence of Cu+ species located in sodalite cages with elevated redox cyclability guarantees high activity and N2 selectivity up to 400 °C over CuY-Crown. Above 400 °C, a high activity and N2 selectivity are related to the accessibility of chemisorbed NH3 to the gaseous NO during the NH3-SCR-DeNOx.