Solvent-Free Synthesis of Zeolites from Anhydrous Starting Raw Solids

Wu, Qinming; Liu, Xiaolong; Zhu, Longfeng; Ding, Lin‐Fen; Gao, Pan; Wang, Qianqian; Pan, Shuxiang; Bian, Chaoqun; Meng, Xiangju; Xu, Jun; Maurer, Stefan; Müller, Ulrich; Xiao, Feng‐Shou

doi:10.1021/ja5124013

Cited by 191 publications

(118 citation statements)

References 54 publications

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“…[18] These compounds are constructed from corner-sharing tetrahedral building blocks,such as SiO 4 ,AlO 4 ,and PO 4 . [19,20] The discovery of MPF-1 offers anew approach to create inorganic zeolitic frameworks by using pentagonal building unit (that is, Figure 1. a)-c) The three different coordination modes of sodium ions (Na1, Na2, Na3) with the cyclo-N 5 À anion;a nd d) the h 5 -coordination mode of the cyclo-N 5 À anion with sodium ions.…”

Section: Angewandte Chemiementioning

confidence: 99%

Stabilization of the Pentazolate Anion in a Zeolitic Architecture with Na₂₀N₆₀ and Na₂₄N₆₀ Nanocages

Zhang

Wang

et al. 2018

Angewandte Chemie

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The experimental detection and synthesis of pentazole (HN 5 )a nd its anion (cyclo-N 5 À )h ave been actively pursued for the past hundred years.T he synthesis of an aesthetic three-dimensional metal-pentazolate framework (denoted as MPF-1) is presented. It consists of sodium ions and cyclo-N 5 À anions in whicht he isolated cyclo-N 5 À anions are preternaturally stabilized in this inorganic open framework featuring two types of nanocages (Na 20 N 60 and Na 24 N 60 ) through strong metal coordination bonds.T he compound MPF-1 is indefinitely stable at room temperature and exhibits high thermal stability relative to the reported cyclo-N 5 À salts. This finding offers anew approach to create metal-pentazolate frameworks (MPFs) and enables the future exploration of interesting pentazole chemistry and also related functional materials.Pentazole (HN 5 )a st he last member in the azole series has been attracting worldwide interest over the past century because of its intriguing aesthetic structure and potential applications as high-performance explosives or propellants. [1, 2] As triking feature of pentazole is that five nitrogen atoms enter ahighly symmetric ring with aromatic character. However,t he inherent instability of the cyclopentazolate anion (cyclo-N 5 À ), arising from its high calculated electron affinity of 5.06 eV and five sterically active free-valence electron pairs in the equatorial plane, [3] has severely hampered pentazole chemistry.D espite arylpentazoles having existed for more than half ac entury, [4] the experimental synthesis of the isolated cyclo-N 5 À salts as well as its parent HN 5 molecule in condensed phases still remains ag reat challenge.Inthis regard, intensive studies have demonstrated that the stability of pentazole ring in the arylpentazoles largely depends on the conjugation of the attached aryl ring featuring as trong electron-detonating group. [5] Theoretical calculations also indicated that the CÀNb ond that links the aryl and pentazole group has arather high dissociation barrier than either the N À Nsingle bond or N = Ndouble bond in the pentazole ring. [6] As ar esult, the biggest challenge in synthesizing ab ulk material containing the isolated cyclo-N 5 À anion is how to selectively cleave the relatively strong CÀ Nbond in the arylpentazoles while keeping the considerably weaker N À Na nd N = Nb onds of the pentazole ring intact.In view of the great attraction and unprecedented challenges in the experimental synthesis of the isolated cyclo-N 5 À anion or its parent HN 5 molecule,significant efforts have been devoted to theoretical studies and experimental detection of the cyclo-N 5 À anion in the solution at the start of this study. [7,8] Several pioneering studies in the experimental detection of cyclo-N 5 À anion were achieved through the negative ion electrospray ionization mass spectrometry (ESI-MS) and collision-induced dissociation (CID) as the analytical tool. [9][10][11] Very recently,the direct formation of cyclo-N 5 À in THF solution was successful through the redu...

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Section: Angewandte Chemiementioning

confidence: 99%

Stabilization of the Pentazolate Anion in a Zeolitic Architecture with Na₂₀N₆₀ and Na₂₄N₆₀ Nanocages

Zhang

Wang

et al. 2018

Angewandte Chemie

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“…This is probably owing to the shorten of b ‐axis of ZSM‐5 crystals since ZSM‐5 zeolite is composed of zig‐zag channels of 0.55×0.51 nm in (100) parallel to the a ‐axis and straight channels of 0.56×0.53 nm in (010) parallel to the b ‐axis. The straight channels are favorable for mass transfer, while the zig‐zag channels are better for product selectivity …”

Section: Methanol To Gasoline Reaction (Mtg) Testmentioning

confidence: 99%

“…This is probably owing to the shorten of b-axis of ZSM-5 crystals since ZSM-5 zeolite is composed of zig- The straight channels are favorable for mass transfer, while the zig-zag channels are better for product selectivity. [26] The deposited coke species in the deactivated catalysts were analyzed by GC-MS. As is seen from Figure 9, a large proportion of methyl-substituted benzenes and naphthalenes appear among the confined organic species for the SHF-ZSM-5 catalyst after deactivation, but very small amount of polycyclic species such as phenanthrene and pyrene are observed, which may be originated from the improving diffusion of the macro-/ meso-/microporous hollow structure. While almost no polycyclic species are presented in the deposited coke species of SHF-ZSM-5-X, methyl-substituted benzenes and naphthalenes become predominant cokes species.…”

Section: Methanol To Gasoline Reaction (Mtg) Testmentioning

confidence: 99%

Facile Solvent‐free Synthesis of Hollow Fiber Catalyst Assembled by c–axis Oriented ZSM‐5 Crystals

Zhou

Chen

et al. 2018

ChemCatChem

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Well crystallized hollow fibers assembled by c‐axis oriented ZSM‐5 crystals were successfully synthesized via a facile one‐pot solvent‐free route, using quartz fiber as silicon substrate and NH4HCO3 as the growing inhibitor on the crystal faces. The immigration of silica inside the quartz fibers formed the hollow morphology and the shell of hollow fiber was composed by the ZSM‐5 crystals. In addition, the length of c‐axis of ZSM‐5 could be controlled by the amount of NH4HCO3, which selectively inhibited the growth on (010) surface. The obtained ZSM‐5 hollow fibers gave a hierarchical structures composed by micro‐, meso‐ and macropores. Catalytic tests for methanol to gasoline (MTG) revealed that the resultant ZSM‐5 hollow fiber exhibited excellent performance with higher C5+ selectivity and longer lifetime due to the improved mass transfer inside the unique hollow fiber structure.

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“…Notably, the hydrothermal route has obvious disadvantages such as reduction of synthesis efficiency owing to autoclave space occupied by the water solvent, and formation of polluted wastes [17][18][19][20]. The use of expensive organic templates increases the zeolite cost in the production [19,20].…”

Section: Introductionmentioning

confidence: 99%

“…Recently, we have reported a solvent-free methodology for synthesis of pure silica zeolites (mainly silicalite-1) from anhydrous starting materials in the presence of NH 4 F [17]. Synthesis parameters and crystallization mechanism on silicalite-1 have been fully investigated.…”

Section: Introductionmentioning

confidence: 99%

Solvent-Free Synthesis of All Silica Beta Zeolite in the Presence of Tetraethylammonium Bromide

Cui¹,

Yan²,

Li³

et al. 2018

Crystals

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Abstract: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 NH 4 F/SiO 2 , TEABr/SiO 2 , 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 N 2 sorption, show that the zeolitic product has good crystallinity, uniform crystals, and high surface area.

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Solvent-Free Synthesis of Zeolites from Anhydrous Starting Raw Solids

Cited by 191 publications

References 54 publications

Stabilization of the Pentazolate Anion in a Zeolitic Architecture with Na₂₀N₆₀ and Na₂₄N₆₀ Nanocages

Stabilization of the Pentazolate Anion in a Zeolitic Architecture with Na₂₀N₆₀ and Na₂₄N₆₀ Nanocages

Facile Solvent‐free Synthesis of Hollow Fiber Catalyst Assembled by c–axis Oriented ZSM‐5 Crystals

Solvent-Free Synthesis of All Silica Beta Zeolite in the Presence of Tetraethylammonium Bromide

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Solvent-Free Synthesis of Zeolites from Anhydrous Starting Raw Solids

Cited by 191 publications

References 54 publications

Stabilization of the Pentazolate Anion in a Zeolitic Architecture with Na20N60 and Na24N60 Nanocages

Stabilization of the Pentazolate Anion in a Zeolitic Architecture with Na20N60 and Na24N60 Nanocages

Facile Solvent‐free Synthesis of Hollow Fiber Catalyst Assembled by c–axis Oriented ZSM‐5 Crystals

Solvent-Free Synthesis of All Silica Beta Zeolite in the Presence of Tetraethylammonium Bromide

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Stabilization of the Pentazolate Anion in a Zeolitic Architecture with Na₂₀N₆₀ and Na₂₄N₆₀ Nanocages

Stabilization of the Pentazolate Anion in a Zeolitic Architecture with Na₂₀N₆₀ and Na₂₄N₆₀ Nanocages