Protective desilication of β zeolite: A mechanism study and its application in ethanol-acetaldehyde to 1,3-butadiene

Zhang, Minhua; Qin, Yunan; Jiang, Haoxi; Wang, Lingtao

doi:10.1016/j.micromeso.2021.111359

Cited by 24 publications

(17 citation statements)

References 40 publications

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“…The catalytic performance of the reported catalysts for EtOH/AcH conversion is shown in Table S6. Compared with the results of Zr-SBA-15 and Zr-β , reported by our group, the hierarchical Zr-β zeolite in this work achieved higher ethanol–acetaldehyde conversion and butadiene selectivity. This indicates that the catalytic performance of hierarchical Zr-β zeolite is better than that of catalysts containing only microporosity or mesoporosity.…”

Section: Resultscontrasting

confidence: 56%

“…However, in zeolite catalysts, some carbonyl intermediates would be overcondensed into heavier carbon species via aldol condensation, which would cover the active sites in microporous channels and ultimately lead to fast deactivation. , Introducing mesoporosity into the zeolite matrix can enhance mass transfer and diffusion of heavier components while improving the accessibility of the active sites, thereby enhancing the activity and stability. , …”

Section: Introductionmentioning

confidence: 99%

“…In view of this situation, considering surfactants as mesoporogens , and tetraethylammonium hydroxide (TEAOH) for protecting the framework, we proposed a “dual-template” strategy to develop mesoporosity on incorporated β zeolites, which is shown in Scheme .…”

Section: Introductionmentioning

confidence: 99%

“…10,11 Introducing mesoporosity into the zeolite matrix can enhance mass transfer and diffusion of heavier components while improving the accessibility of the active sites, thereby enhancing the activity and stability. 12,13 Developing mesoporosity in incorporated β zeolites usually depends on the parent aluminosilicate, which undergoes a procedure containing desilication on aluminosilicate β zeolite and the dealumination−metallization process on hierarchical β zeolite. 14,15 Direct desilication on incorporated zeolite would lead to framework collapse, as its framework becomes unstable due to the removal of framework Al, 16−18 which can protect the zeolite framework from etching.…”

Section: Introductionmentioning

confidence: 99%

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Uniform Mesoporosity Development in Incorporated β Zeolite: Dual-Template Strategy

Dong

Wang

Yang

et al. 2022

Ind. Eng. Chem. Res.

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The hierarchical porosity of zeolite is a key factor affecting its catalytic activity and stability for bulky molecules involved reactions. However, it is still challenging to introduce mesoporosity into heteroatom-incorporated zeolites in a facile manner while maintaining the catalytic activity. In this work, a strategy for mesoporosity development in incorporated zeolites based on two templates (TEAOH and surfactants) under hydrothermal conditions was proposed, and hierarchical Zr-incorporated β zeolite was successfully prepared and used to catalyze the ETB reaction. In this process, OH– etches the zeolite framework while TEA+ preserves the microporous structure and the surfactant as the mesoporogen. The mesopore size (2.1–3.2 nm) can be tailored by changing the alkyl chain length (C10–C16) of the surfactant. During the treatment, the chemical environment of Zr in Zr-β zeolite did not change and the amount of Lewis acid was increased, showing that the mesoporosity could improve the accessibility of active sites. The hierarchical Zr-β zeolite showed better catalytic performance than the parent Zr-β zeolite in the ethanol–acetaldehyde to butadiene reaction, the conversion of ethanol and acetaldehyde can reach 63.7%, and the selectivity of butadiene can reach 76.6%. The stability of hierarchical Zr-β zeolite is significantly higher than that of microporous Zr-β zeolite, whose conversion can be maintained at 35.0% and selectivity at 70.9% at TOS = 24 h. The mesoporosity can increase the capability of coke which mitigates the deactivation.

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Section: Resultscontrasting

confidence: 56%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Uniform Mesoporosity Development in Incorporated β Zeolite: Dual-Template Strategy

Dong

Wang

Yang

et al. 2022

Ind. Eng. Chem. Res.

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“…The deposition of coke could be due to the formation of ash. If the catalyst is exposed to a high temperature for a long time, the ash or coke deposition can affect the reactivity, decreasing the pore size or altering it, as suggested in previous literature [28,29]. Consequently, the newly created micro-pores may quarter the part of coke deposition, sinking the materialization of coke deposition in its inherent micro-pores to some extent.…”

Section: Bet Profiles Of the Catalystmentioning

confidence: 89%

Production of 1,3-Butadiene from Ethanol Using Treated Zr-Based Catalyst

Bojang¹,

Wu²

2022

Catalysts

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The conversion of ethanol to 1,3-butadiene was carried out using a treated Zr-based catalyst at a temperature of 350–400 °C with different weight hourly space velocities in a fixed bed reactor. The catalysts used are commercial, but they underwent pretreatment. The commercial catalysts used were ZrO2, Zr(OH)2, 2% CaO-ZrO2, 30% TiO2-ZrO2, 50% CeO2-ZrO2 and 10% SiO2-ZrO2 in their modified or treated form. The characterizations of the catalysts were carried out using XRD, XPS, and TGA. The results indicated that ethanol conversion, yield, and selectivity of 1,3-butadiene operated weight hourly space velocity of 2.5 h−1 using 10% SiO2-ZrO2 were 95%, 80%, and 85%, respectively, at 350 °C. Using 50% CeO2-ZrO2 converted 70% ethanol with a 1,3-butadiene yield of 65%. The best Zr-based catalyst was 10% SiO2-ZrO2 as it gives a steady 1,3-butadiene yield, the Si-composition with ZrO2 gives a good catalytic pour of the catalyst-bed structure; hence, the life span was good. Using 30% TiO2-ZrO2 has an ethanol conversion of 70% with a 1,3-butadiene yield of 43%.

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Synthesis and Catalytic Applications of Advanced Sn‐ and Zr‐Zeolites Materials

Liu,

Zhu

2023

Advanced Science

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The incorporation of isolated Sn (IV) and Zr (IV) ions into silica frameworks is attracting widespread attention, which exhibits remarkable catalytic performance (conversion, selectivity, and stability) in a broad range of reactions, especially in the field of biomass catalytic conversion. As a representative example, the conversion route of carbohydrates into valuable platform and commodity chemicals such as lactic acid and alkyl lactates, has already been established. The zeotype materials also possess water‐tolerant ability and are capable to be served as promising heterogeneous catalysts for aqueous reactions. Therefore, dozens of Sn‐ and Zr‐containing silica materials with various channel systems have been prepared successfully in the past decades, containing 8 membered rings (MR) small pore CHA zeolite, 10‐MR medium pore zeolites (FER, MCM‐56, MEL, MFI, MWW), 12‐MR large pore zeolites (Beta, BEC, FAU, MOR, MSE, MTW), and 14‐MR extra‐large pore UTL zeolite. This review about Sn‐ and Zr‐containing metallosilicate materials focuses on their synthesis strategy, catalytic applications for diverse reactions, and the effect of zeolite characteristics on their catalytic performances.

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Protective desilication of β zeolite: A mechanism study and its application in ethanol-acetaldehyde to 1,3-butadiene

Cited by 24 publications

References 40 publications

Uniform Mesoporosity Development in Incorporated β Zeolite: Dual-Template Strategy

Uniform Mesoporosity Development in Incorporated β Zeolite: Dual-Template Strategy

Production of 1,3-Butadiene from Ethanol Using Treated Zr-Based Catalyst

Synthesis and Catalytic Applications of Advanced Sn‐ and Zr‐Zeolites Materials

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