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Dive into the research topics where J.B. Nagy is active.

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Featured researches published by J.B. Nagy.


Zeolites | 1988

Identification of different tetrapropylammonium cations occluded in ZSM-5 zeolite by combined thermal analysis (t.g.-d.t.a.) and 13C-n.m.r. spectroscopy

J. El Hage-Al Asswad; N. Dewaele; J.B. Nagy; R.A. Hubert; Z. Gabelica; E.G. Derouane; F. Crea; R. Aiello; A. Nastro

The combined use of thermal analysis (t.g.-d.t.a.) and 13 C-n.m.r. spectroscopy allows one to identify four different structural environments for TPA + ions occluded in the ZSM-5 channels. A first low-temperature (ca. 380°) d.t.a. peak is assigned to less strongly held or outer shell “strained” TPA + ions (type I), while a large intermediate temperature (ca. 425°C) peak C1 is attributed to inner-strained TPA + ions (type II). Both TPA + species neutralize the SiO − defect groups. The high-temperature (ca. 475°C) peak is attributed to two different TPA + ions: those neutralizing the framework (Si-O-Al) − negative centers (type III) (for high Al content samples), and those in the relaxed form that also neutralize SiO − defect groups (type IV) (for both high- and low-Al-content samples). Types I–III all show the same 13 C-n.m.r. spectra (splitting of the CH 3 -n.m.r. line), while type IV exhibits only one n.m.r. line for the CH 3 - groups.


Zeolites | 1988

Aluminium distribution and cation location in various M-ZSM-5-type zeolites (M Li, Na, K, Rb, Cs, NH4)

J.B. Nagy; P. Bodart; H. Collette; J. El Hage-Al Asswad; Z. Gabelica; R. Aiello; A. Nastro; C. Pellegrino

Combining PIGE, EDX, AA, and thermal analyses with solid-state 29Si-n.m.r spectroscopy allowed us to determine the amounts of SiOR and (SiOAI)−R+ groups (R H, M, TPA). The amount of SiOR increases with decreasing aluminium content. At the external surface of the crystallites, an Al-rich phase is deposited, which is revealed to be a zeolitic phase rather than a MAIO2 species. The d.t.a. peak at ca. 360°C is attributed to external shell TPA species. Finally, the partial solvation of the cations is shown by both 7Li- and 23Na-n.m.r. results.


Zeolites | 1987

Structure and stability of tetrapropyl-ammonium (TPA) ions in various alkali—aluminosilicate hydrogel precursors to crystalline (M)ZSM—5 zeolites

Z. Gabelica; J.B. Nagy; P. Bodart; N. Dewaele; A. Nastro

Abstract The stability of TPA species interacting with various (Al,Si) hydrogel environments in the presence of alkali cations has been evaluated by thermal analysis (combined t.g.-d.t.a.-d.t.g.). Three different TPA—gel associations have been characterized by d.t.a. endotherms : crystalline (TPAX) n clusters (X = OH − ,Br − ) which are also detected by XRD, monomeric (TPAX) species in direct association with the (Al,Si) gel, and labile entities, [TPA + …(H 2 O) x ] bulky water clathrates, that interact very weakly with the remaining negative charges available after neutralization of the gel by small (Li,Na,K) alkali cations. The formation, relative concentration and stability of these species essentially depend on the relative amounts of Al 2 O 3 and M 2 O present in the gel, as well as on the nature (structure forming/breaking) of the alkali cations. Monomeric as well as water clathrated species lead to crystalline (M)ZSM—5 upon heating.


Applied Catalysis | 1988

Parameters affecting the optimal synthesis of zeolite ZSM-20

N. Dewaele; Lutgarde Maistriau; J.B. Nagy; Z. Gabelica; E.G. Derouane

Abstract Careful control of various synthesis parameters such as the composition of the precursor hydrogel, temperature and time, allowed the preparation, in optimum yield, of zeolite ZSM-20 from a hydrogel that usually yielded the more stable zeolite Beta. From a detailed physio-chemical characterization of both zeolites, essential differences were found between their framework structures and compositions. From a kinetic study of the formation of zeolite ZSM-20 under optimal conditions, we propose a mechanism which involves a liquid phase ion transportation.


Studies in Surface Science and Catalysis | 1988

GEL Composition Versus Organic Directing Agent Effects in the Synthesis of ZSM-39, ZSM-48 and ZSM-50 Zeolites

N. Dewaele; Z. Gabelica; P. Bodart; J.B. Nagy; G. Giordano; E.G. Derouane

Abstract Zeolite ZSM-48 prepared from a hydrogel containing an alkylamine admixed with TMA + ions incorporates these organic species, so that the total filling of the porous volume is achieved. However, when zeolite ZSM-39 crystallizes from a similar hydrogel (also containing TMA + ions, and with or without alkylamine and aluminium ions), part of the TMA + ions are dequaternated to trimethylamine and trimethylammonium species, which are also occluded into the large cavities of the ZSM-39 crystals. Hydrogels including hexamethonium (HM ++ ) ions, with or without ammonium species, lead to the formation of zeolites ZSM-48 and ZSM-50, depending on the initial aluminium content. In all cases, the amount of organic species occluded (either only HM ++ ions, or HM ++ together with hexyltrimethylammonium and trimethylammonium ions which result from the decomposition of the HM ++ ions) is governed by the filling of the zeolitic free pore volume.


Studies in Surface Science and Catalysis | 1986

Role of Alkali and Tetrapropylammonium Cations in (M)ZSM-5 Hydrogel Precursors

J.B. Nagy; P. Bodart; E.G. Derouane; Z. Gabelica; A. Nastro

The influence of alkali and tetrapropylammonium (TPA + ) cations on the organization of hydrogel precursors to ZSM-5 zeolite is examined by multinuclear high power solid state nuclear magnetic resonance techniques. Emphasis is put on the different states of the TPA + ions and on the interaction between the alkali cations (M + ) and the negative charges in the gel.


Applied Catalysis | 1986

Physicochemical characterization of zeolite ZSM-20

E.G. Derouane; N. Dewaele; Z. Gabelica; J.B. Nagy

Abstract Zeolite ZSM-20 is a silica-rich zeolite, possessing a faujasite-like character but having a hexagonal symmetry unit cell. It is synthesized in the presence of tetraethylammonium (TEA) cations as organic directing agents. Those act as counterions, in addition to Na+ cations, and are eventually occluded in the zeolite large cages where the electric field gradient is small.


Zeolites | 1995

The effect of thermal treatment and of grinding on silicalite-1 synthesized in the presence of fluoride ions

A. Fonseca; J.B. Nagy; J. El Hage-Al Asswad; R. Mostowicz; F. Crea; F. Testa

Abstract Synthesis in fluoride-containing medium leads to large silicalite crystals without SiOX defect groups. The four occluded tetrapropylammonium (TPA + ) ions/unit cell are ion pairs with 2 F − and 2 OH − . Grinding the samples in the presence of water leads to SiOH groups that are eliminated during calcination. The two endothermic peaks at 420 and 560°C of the TPA + decomposition are identified as being due to the Hoffmann degradation of the TPA + ion (first peak) and to the decomposition of the products of TPA + ion (second peak).


Zeolites | 1995

13C and 29Si n.m.r. characterization of silicalite-1, silicalite-2, and highly siliceous ZSM-48 zeolites containing tetraalkylammonium bromide, hexamethonium bromide, and diaminododecane, in the presence of fluoride ions

A. Fonseca; J.B. Nagy; J. El Hage-Al Asswad; G. Demortier; R. Mostowicz; F. Crea

Abstract Silica gels containing tetraalkylammonium bromide (TAA), hexamethonium (HM) bromide, and 1,2-diaminododecane (DADD) have been prepared in fluoride medium: 10 NaF  ( x TAABr  y HMBr 2  z DADD)  10 SiO 2  330 H 2 O with x + y + z = 1.25. TAA = tetramethyl-, tetraethyl-, tetrapropyl-, and tetrabutylammonium. Silicalite-1 (with TPA), silicalite-2 (with TBA), and ZSM-48 (with DADD) are the crystalline zeolites. TPA is preferentially occluded in silicalite-1, TBA in silicalite-2, and DADD in ZSM-48. However, HM and DADD are also occluded in minor amounts in silicalite-2, and some HM is always present in the channels of ZSM-48.


Archive | 1990

A 13C - and 129Xe-NMR Study of the Role of Tetraalkylammonium Cations in the Synthesis of High-Silica Zeolites

Q. Chen; J.B. Nagy; J. Fraissard; J. El Hage-Al Asswad; Z. Gabelica; E.G. Derouane; R. Aiello; F. Crea; G. Giordano; A. Nastro

The high silica gel is well organized around the tetraalkylammonium (TAA) cations during prenucleation stage. By combined 13C- and 129Xe- NMR, two TAA+ states, either hydrated or dehydrated, and three different TAA-gel associations can clearly be distinguished: 1. dispersed monomelic or dimeric (either hydrated or dehydrated) TAA+ species (1–2 cations per cavity, cavity diameter ~11–16 A) 2. less dispersed TAA+ ions (4–8 ions per cavity, cavity diameter ~17–23 A) 3. large aggregates (TAAX)n (X=OH, Br) (n gt; 15 per cavity, cavity diameter ~30–40 A)

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