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Synthesis and characterisation of transition-metal-substituted gallium phosphates with the laumontite structure 具有湖沸石结构的过渡金属取代磷酸镓的合成与表征
Zeolites Pub Date : 1997-11-01 DOI: 10.1016/S0144-2449(97)00099-7
Andrew D. Bond, Ann M. Chippindale , Andrew R. Cowley, Jennifer E. Readman, Anthony V. Powell
{"title":"Synthesis and characterisation of transition-metal-substituted gallium phosphates with the laumontite structure","authors":"Andrew D. Bond,&nbsp;Ann M. Chippindale ,&nbsp;Andrew R. Cowley,&nbsp;Jennifer E. Readman,&nbsp;Anthony V. Powell","doi":"10.1016/S0144-2449(97)00099-7","DOIUrl":"10.1016/S0144-2449(97)00099-7","url":null,"abstract":"<div><p>Three novel metal-substituted gallium phosphates, (C<sub>3</sub>N<sub>2</sub>H<sub>5</sub>)<sub>8</sub>[Me<sub>8</sub>Ga<sub>16</sub>P<sub>24</sub>O<sub>96</sub>] (Me = Co, Fe, Mn), have been synthesised under solvothermal conditions and their structures determined using single-crystal X-ray diffraction. They are isostructural, with monoclinic symmetry, space group C 2/c and unit-cell dimensions ca. 15 × 13 × 15 Å, β ca. 111°. The materials all have frameworks with the laumontite topology (structure type code LAU), constructed from alternating PO<sub>4</sub> and MO<sub>4</sub> tetrahedra (M = Me and Ga) with imidazole cations occupying sites within the channels of the framework. Magnetic susceptibility measurements show that the materials exhibit Curie-Weiss behaviour over wide ranges of temperature and that the transition metals are present as divalent cations.</p></div>","PeriodicalId":23983,"journal":{"name":"Zeolites","volume":"19 5","pages":"Pages 326-333"},"PeriodicalIF":0.0,"publicationDate":"1997-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S0144-2449(97)00099-7","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"82986613","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 25
Location of Brønsted sites in mordenite 丝光沸石中Brønsted遗址的位置
Zeolites Pub Date : 1997-11-01 DOI: 10.1016/S0144-2449(97)00114-0
Alberto Alberti
{"title":"Location of Brønsted sites in mordenite","authors":"Alberto Alberti","doi":"10.1016/S0144-2449(97)00114-0","DOIUrl":"10.1016/S0144-2449(97)00114-0","url":null,"abstract":"<div><p>Crystal structure refinements of mordenites indicate that partial (Si,Al) order in the tetrahedral sites regularly recurs within the observed range (6–9) Al/unit cell. Consequently, for a given Si/Al ratio, it is possible to determine the maximum number of OH groups that can be allocated on each framework oxygen. Assuming that only one proton can be bonded at the same time to the oxygens of a tetrahedron, structural data indicate that it is highly probable that Brønsted sites are on framework oxygens 02 and 07, heading toward the center of the 12-ring, and on 09, heading toward the center of the 8-ring, each with about the same population. The intensities of the i.r. stretching bands (around 3,600 cm<sup>−1</sup> wavenumbers) of the hydroxyls Si(OH)Al agree well with this result.</p></div>","PeriodicalId":23983,"journal":{"name":"Zeolites","volume":"19 5","pages":"Pages 411-415"},"PeriodicalIF":0.0,"publicationDate":"1997-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S0144-2449(97)00114-0","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"78879521","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 79
Diffuse reflectance i.r. spectroscopic study on hydroxyl groups of H-ZSM-5s having different sizes and properties h - zsm -5不同尺寸和性质羟基的漫反射红外光谱研究
Zeolites Pub Date : 1997-11-01 DOI: 10.1016/S0144-2449(97)00112-7
Shu-Bin Pu, Tomoyuki Inui
{"title":"Diffuse reflectance i.r. spectroscopic study on hydroxyl groups of H-ZSM-5s having different sizes and properties","authors":"Shu-Bin Pu,&nbsp;Tomoyuki Inui","doi":"10.1016/S0144-2449(97)00112-7","DOIUrl":"10.1016/S0144-2449(97)00112-7","url":null,"abstract":"<div><p>The stretching vibration of hydroxyl groups on H-ZSM-5 samples with different crystallite size and Al content was investigated by diffuse reflectance i.r. spectroscopy. Good linear relations for the intensity of the 3,740-cm<sup>−1</sup> for the region versus the external surface area and the intensity of the 3,610-cm<sup>−1</sup> for the region versus Al content were obtained. It is proven that the absorbance at 3,740 cm<sup>−1</sup> is attributed to the terminal (Si-) O-H groups, which are located completely on the external surface, and an absorbance at 3,610 cm<sup>−1</sup> is ascribed to (Al-)O-H groups, which are distributed on both the external and internal surface of H-ZSM-5.</p></div>","PeriodicalId":23983,"journal":{"name":"Zeolites","volume":"19 5","pages":"Pages 452-454"},"PeriodicalIF":0.0,"publicationDate":"1997-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S0144-2449(97)00112-7","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"79011088","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 19
Solid-state ion exchange in zeolites: Part 8. Interaction of lanthanum(III) chloride with zeolites under anhydrous conditions 沸石中的固态离子交换:第8部分。无水条件下氯化镧与沸石的相互作用
Zeolites Pub Date : 1997-11-01 DOI: 10.1016/S0144-2449(97)00118-8
Bogdan Sulikowski , Josef Find, Hellmut G. Karge, Daniel Herein
{"title":"Solid-state ion exchange in zeolites: Part 8. Interaction of lanthanum(III) chloride with zeolites under anhydrous conditions","authors":"Bogdan Sulikowski ,&nbsp;Josef Find,&nbsp;Hellmut G. Karge,&nbsp;Daniel Herein","doi":"10.1016/S0144-2449(97)00118-8","DOIUrl":"10.1016/S0144-2449(97)00118-8","url":null,"abstract":"<div><p>Interaction of lanthanum(III) chloride with hydrogen forms of ferrierite, mordenite, zeolite L, and faujasite, under completely anhydrous conditions, is described. The course of the interaction has been studied by <em>in situ</em> i.r. and XRD techniques. No evidence of interaction between LaCl<sub>3</sub> and small-pore H-ferrierite was found. The other three structures investigated do interact with LaCl<sub>3</sub> even under the complete exclusion of water or water vapor from the surroundings. Plausible mechanisms of the solid-state ion exchange in zeolites are also discussed.</p></div>","PeriodicalId":23983,"journal":{"name":"Zeolites","volume":"19 5","pages":"Pages 395-403"},"PeriodicalIF":0.0,"publicationDate":"1997-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S0144-2449(97)00118-8","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"85768119","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 24
Synthesis, characterization, and catalytic properties of a novel Germano-aluminophosphate molecular sieve with AEL structure: GeAPO-11 具有AEL结构的新型锗-磷酸铝分子筛:GeAPO-11的合成、表征及催化性能
Zeolites Pub Date : 1997-11-01 DOI: 10.1016/S0144-2449(97)00082-1
P. Mériaudeau, Vu A. Tuan, Le N. Hung, G. Szabo
{"title":"Synthesis, characterization, and catalytic properties of a novel Germano-aluminophosphate molecular sieve with AEL structure: GeAPO-11","authors":"P. Mériaudeau,&nbsp;Vu A. Tuan,&nbsp;Le N. Hung,&nbsp;G. Szabo","doi":"10.1016/S0144-2449(97)00082-1","DOIUrl":"10.1016/S0144-2449(97)00082-1","url":null,"abstract":"<div><p>A novel GeAPO-11 material has been synthesized and characterized. It is observed that Ge is incorporated in the molecular sieve framework, creating a new Brønsted acid site [Ge(OH)Al]. This catalyst is effective for skeletal isomerization of <em>n</em>-butene.</p></div>","PeriodicalId":23983,"journal":{"name":"Zeolites","volume":"19 5","pages":"Pages 449-451"},"PeriodicalIF":0.0,"publicationDate":"1997-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S0144-2449(97)00082-1","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"83264659","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 3
States of aluminum in zeolite β and influence of acidic or basic medium 铝在β沸石中的状态及酸性或碱性介质的影响
Zeolites Pub Date : 1997-11-01 DOI: 10.1016/S0144-2449(97)00103-6
Chun Yang, Qinhua Xuaf
{"title":"States of aluminum in zeolite β and influence of acidic or basic medium","authors":"Chun Yang,&nbsp;Qinhua Xuaf","doi":"10.1016/S0144-2449(97)00103-6","DOIUrl":"10.1016/S0144-2449(97)00103-6","url":null,"abstract":"<div><p>The states of aluminum in zeolites β were investigated in detail with FTIR spectroscopy. Three kinds of aluminum—framework, nonframework, and transient-state aluminum—were detected in template-removed zeolite β. The states of aluminum in our samples intensely depends on the nature of compensating cation, consistent with the conclusion of Brougeat-Lami et al. But some new assignments of aluminum species and new opinions about the states of aluminum and their transformation are proposed. From the experimental results, we suggest that, because the framework of zeolite β is deformable, the distortion and the tension of zeolite lattice occur when protons, which possess high electron affinity, are located at cationic sites, leading to the breakage of Al-O bond and the removal of aluminum. Therefore, zeolite β is subjected to dealumination in acidic medium. On the other hand, the high deformability also results in the relaxation of zeolite structure when H<sup>+</sup> is replaced by other cations (e.g., Na<sup>+</sup>) so that transient-state aluminum and even nonframework aluminum can go back into the framework. Owing to ion-exchange, the cationic nonframework aluminum species enter the solution; moreover, it can also reinsert into the framework after hydroxylation in basic medium.</p></div>","PeriodicalId":23983,"journal":{"name":"Zeolites","volume":"19 5","pages":"Pages 404-410"},"PeriodicalIF":0.0,"publicationDate":"1997-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S0144-2449(97)00103-6","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"80331219","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 71
Mutinaite, a new zeolite from Antarctica: The natural counterpart of ZSM-5 Mutinaite,一种来自南极洲的新型沸石:ZSM-5的天然对应物
Zeolites Pub Date : 1997-11-01 DOI: 10.1016/S0144-2449(97)00100-0
Ermanno Galli, Giovanna Vezzalini, Simona Quartieri, Alberto Alberti, Marco Franzini
{"title":"Mutinaite, a new zeolite from Antarctica: The natural counterpart of ZSM-5","authors":"Ermanno Galli,&nbsp;Giovanna Vezzalini,&nbsp;Simona Quartieri,&nbsp;Alberto Alberti,&nbsp;Marco Franzini","doi":"10.1016/S0144-2449(97)00100-0","DOIUrl":"10.1016/S0144-2449(97)00100-0","url":null,"abstract":"<div><p>Mutinaite is the third new zeolite from Ferrar dolerites at Mt. Adamson (Northern Victoria Land, Antarctica). The mineral occurs as subspherical aggregates of tiny radiating lath-like fibres or as aggregates of transparent, colourless to pale-milky, tiny tabular crystals; it has vitreous luster, white streak and good 100 cleavage. Mutinaite is brittle with d<sub>meas</sub> = 2.14(3) and d<sub>calc</sub> = 2.17 g/cm<sup>3</sup>. Optically, it is biaxial negative with α = 1.485(2), β = 1.487(2) and γ = 1.488(2). The orientation is X = b, Y = a, Z = c. Mutinaite is orthorhombic with <em>a</em> = 20.223(7), <em>b</em> = 20.052(8), <em>c</em> = 13.491 (5)Å, space group Pnma. The strongest powder X-ray diffraction lines are (d(Å), I, hkl): 11.20, 84, 101, 011; 9.98, 35, 200,020; 3.85, 100, 501, 051; 3.75, 98, 303; 3.67, 27, 133; 3.00, 32, 503. The framework topology is that of the synthetic zeolite ZSM-5. The chemical formula is: (Na<sub>2.76</sub>K<sub>0.11</sub>Mg<sub>0.21</sub>Ca<sub>3.78</sub>)<sub>Σ = 6.86</sub>(Al<sub>11.20</sub>Si<sub>84.91</sub>)<sub>Σ=96.11</sub>O<sub>192</sub> · 60H<sub>2</sub>O. The Si/Al ratio, equal to 7.6, is the highest found in a natural zeolite. Thermal stability and rehydration capacity are very high. The name is from Mutina, the ancient Latin name of the city of Modena.</p></div>","PeriodicalId":23983,"journal":{"name":"Zeolites","volume":"19 5","pages":"Pages 318-322"},"PeriodicalIF":0.0,"publicationDate":"1997-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S0144-2449(97)00100-0","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"88403322","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 35
Alkylation of toluene on HSAPO-5 with various Si concentrations 甲苯在不同硅浓度的HSAPO-5上的烷基化反应
Zeolites Pub Date : 1997-11-01 DOI: 10.1016/S0144-2449(97)00116-4
T. Masukawa, T. Komatsu, T. Yashima
{"title":"Alkylation of toluene on HSAPO-5 with various Si concentrations","authors":"T. Masukawa,&nbsp;T. Komatsu,&nbsp;T. Yashima","doi":"10.1016/S0144-2449(97)00116-4","DOIUrl":"10.1016/S0144-2449(97)00116-4","url":null,"abstract":"<div><p>HSAPO-5 with various Si concentrations was used as a catalyst for the alkylation of toluene with methanol to investigate weak acid sites. On HSAPO-5 with Si/(Al + P + Si) ≦ 0.026, the conversion of toluene increased with time on stream for a certain period, whereas the conversion decreased monotonously on HSAPO-5 with higher Si concentrations. Pretreatment with methanol on HSAPO-5 with Si/(Al + P + Si) = 0.018 increased the initial conversion of toluene. From the measurement of the amount of coke deposited on HSAPO-5, it is suggested that during the initial stage of the reaction coke is mainly produced by the reaction of methanol by itself at the acid sites on the external surface of HSAPO-5 with low Si concentrations. A small amount of coke thus formed would gradually retard the further self-conversion of methanol into coke. Therefore, the fraction of methanol used for the alkylation could increase, resulting in the increase in toluene conversion. It is suggested that the acid sites on the external surface are stronger than those formed by the substitution of Si for P but are weaker than those formed in aluminosilicate regions existing in HSAPO-5 with high Si concentrations.</p></div>","PeriodicalId":23983,"journal":{"name":"Zeolites","volume":"19 5","pages":"Pages 429-433"},"PeriodicalIF":0.0,"publicationDate":"1997-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S0144-2449(97)00116-4","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"76089309","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 10
Coordination state of gallium in MFI structures prepared by direct synthesis and by postsynthetic modification of boralites 硼钛矿直接合成及合成后修饰制备的MFI结构中镓的配位态
Zeolites Pub Date : 1997-11-01 DOI: 10.1016/S0144-2449(97)00089-4
Richard Klik, Vladimír Bosáček, Ludmila Kubelková, Dieter Freude, Dieter Michel
{"title":"Coordination state of gallium in MFI structures prepared by direct synthesis and by postsynthetic modification of boralites","authors":"Richard Klik,&nbsp;Vladimír Bosáček,&nbsp;Ludmila Kubelková,&nbsp;Dieter Freude,&nbsp;Dieter Michel","doi":"10.1016/S0144-2449(97)00089-4","DOIUrl":"10.1016/S0144-2449(97)00089-4","url":null,"abstract":"<div><p>High-field <sup>71</sup>Ga <em>MAS</em> n.m.r. spectroscopy shows that gallium occupies preferentially the framework positions in Ga-MFI structures prepared by direct synthesis from a gel. However, modifications of boralite with Ga<sup>3+</sup> in autoclave experiments provide structures with extraframework gallium species and only partially occupied boron vacancies in framework positions. Evidence of gallium oxohydrates in the modified samples was given by X-ray analysis. Extraframework gallium species with a quadrupole coupling constant of 8.8 MHz could be detected, but part of the extraframework gallium remains n.m.r. invisible.</p></div>","PeriodicalId":23983,"journal":{"name":"Zeolites","volume":"19 5","pages":"Pages 343-348"},"PeriodicalIF":0.0,"publicationDate":"1997-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S0144-2449(97)00089-4","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"78130979","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 10
Zeolite cycle sequences 沸石循环序列
Zeolites Pub Date : 1997-11-01 DOI: 10.1016/S0144-2449(97)00122-X
G. Thimm, W.E. Klee
{"title":"Zeolite cycle sequences","authors":"G. Thimm,&nbsp;W.E. Klee","doi":"10.1016/S0144-2449(97)00122-X","DOIUrl":"10.1016/S0144-2449(97)00122-X","url":null,"abstract":"<div><p>Cycle sequences are presented as topological invariants of zeolites. The sequences are calculated for 374 topologically inequivalent atoms in 105 zeolite frameworks. All sequences are found to be different. The first nonzero terms of the sequence indicate the length of the smallest rings, which occur in the given framework and show which of the atoms belong to these rings.</p></div>","PeriodicalId":23983,"journal":{"name":"Zeolites","volume":"19 5","pages":"Pages 422-424"},"PeriodicalIF":0.0,"publicationDate":"1997-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S0144-2449(97)00122-X","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"74422999","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 9
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