- Synthesis of Nanosized ZSM-5 Zeolites by Different Methods and Their Catalytic Performance in the Alkylation of Naphthalene
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Abstract: Three nanosized ZSM-5 zeolites were successfully prepared from reactive gelswith the same Si/Al ratios by different synthetic procedures that included theuse of tetrapropylammonium hydroxide or n-butylamine as a template and a seedingmethod that did not use an organic additive. The effect of the synthetic methodon the physicochemical properties of the prepared samples was investigated byXRD, XRF, XPS, N2 physisorption, SEM, TEM,27Al MAS NMR, NH3-TPD, andPy-FTIR. The catalytic performance of thenanosized ZSM-5 zeolites in the alkylation of naphthalene with methanol wascompared. The prepared samples were phase-pure, highly crystalline ZSM-5zeolites, but they had different bulk and surface Si/Al ratios as well astextural and acidic properties. The study of the prepared catalysts innaphthalene methylation revealed that both the acid characteristics of the ZSM-5nanosized zeolites and their textural properties were responsible for theiractivity in the reaction. A difference in the composition ofmonomethylnaphthalenes and dimethylnaphthalenes was attributed to the ability ofthe catalyst to isomerize the primary reaction products on acid sites located onthe external surface of the zeolite crystals. 2,7-DMN was found to be thepreferred reaction product over 2,6-DMN when formed at pore entrances to ZSM-5channels due to the differences in their dimensions. In contrast,2,6-dimethylnaphthalene could be produced on weaker external Br?nsted acidsites, which are hydroxyls attached to octahedral Al atoms. The presentedresults show that the method used to synthesize nanoscale ZSM-5 zeolites is acritical factor that determines the physicochemical properties and catalyticperformance of the resulting crystals.
- Wang, Yongchao,Kikhtyanin,Li, Cheng,Su, Xiaofang,Bai, Xuefeng,Wu, Wei
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p. 394 - 406
(2021/02/26)
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- PYRIDAZINONE HERBICIDES AND PYRIDAZINONE INTERMEDIATES USED TO PREPARE A HERBICIDE
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Disclosed are compounds of Formula I and N-oxides or salts thereof, wherein R1 is C1-C4alkyl or C3-C6cycloalkyl; R2 is H, Cl, Br or I; R3 is Cl or OR4; R4 is H or C1-C4 alkyl; R5 is H, F, Cl or CH3; and R6 is H or Cl. Also disclosed is a composition containing a compound of Formula I, and methods for controlling undesired vegetation comprising contacting the undesired vegetation or its environment with an effective amount of a compound of Formula I or a composition thereof. Also dislosed are methods for preparing a compound of Formula I.
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Page/Page column 44-45
(2020/05/13)
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- Methylation of 2-methylnaphthalene over metal-impregnated mesoporous MCM-41 for the synthesis of 2,6-triad dimethylnaphthalene isomers
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2,6-Dimethylnaphthalene (2,6-DMN) is one of the key intermediates for the production of polyethylene naphthalate (PEN), which demonstrates superior properties compared with the polyethylene terephthalate. However, the complex synthesis procedure of 2,6-DMN increases the production cost and decreases the commercialisation of PEN. In this study, selective synthesis of 2,6-triad DMN isomers (1,5-DMN, 1,6-DMN and 2,6-DMN) has been investigated by the methylation of 2-methylnaphthalene (2-MN) over mesoporous Cu/MCM-41 and Zr/MCM-41 zeolite catalysts. On the contrary of other DMN isomers, 2.6-triad isomers can effectively be converted to be profitable 2,6-DMN with an additional isomerisation reaction, which is a new approach to reach higher 2,6-DMN yield. The methylation reactions of 2-MN were investigated in a fixed-bed reactor at 400?°C and weight hourly space velocity of 1–3?h?1. The results showed that the activity of MCM-41 on the methylation of 2-MN has been enhanced with the impregnation of Cu. The conversion increased from about 17% to 35 wt% with the impregnation of Cu. Similarly, the 2,6-triad DMN selectivity and 2,6-/2,7-DMN ratio reached the maximum level (48 wt% and 1.95, respectively) over Cu-impregnated MCM-41 zeolite catalyst.
- Niftaliyeva, Aysel,Güle?, Fatih,Karaduman, Ali
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p. 2403 - 2416
(2020/02/11)
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- MULTICYCLIC COMPOUND AND ORGANIC LIGHT EMITTING DEVICE COMPRISING THE SAME
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The present specification provides a compound of chemical formula 1 and an organic light emitting device comprising the same. The compound described in the present invention can be used as a material of an organic material layer of the organic light emitting device. When manufacturing the organic light emitting device comprising the compound according to at least one embodiment, it is possible to obtain the organic light emitting device having high efficiency and long lifespan.COPYRIGHT KIPO 2020
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Paragraph 0307-0314
(2020/01/31)
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- A compound two spiral alkylations, ZSM - 12 molecular sieve preparation method and the preparation of ZSM - 12 molecular sieve and alkylation method
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The invention discloses a di-spirane compound, a preparation method for a ZSM-12 molecular sieve, the prepared ZSM-12 molecular sieve and an alkylation method. The di-spirane compound has a structureshown in a formula (I), wherein n is 2-6, X is an anion selected from Cl, Br, I or OH. The ZSM-12 molecular sieve is prepared by using the di-spirane compound provided by the invention; when the prepared ZSM-12 molecular sieve is used for catalyzing the alkylation method, the conversion rate is high, and the selectivity is good.
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-
Paragraph 0090-0094; 0098
(2019/10/04)
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- Selective synthesis of 2,6-triad dimethylnaphthalene isomers by disproportionation of 2-methylnaphthalene over mesoporous MCM-41
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2,6-Dimethylnaphthalene (2,6-DMN) is one of the crucial intermediates for the synthesis of polybutylenenaphthalate and polyethylene naphthalate (PEN). The complex synthesis procedure and the high cost of 2,6-DMN production significantly reduce the commercialisation of PEN even though PEN demonstrates superior properties compared with polyethylene terephthalate. 2,6-DMN can be produced by methylation of 2-methylnaphthalene (2-MN) and/or naphthalene, disproportionation of 2-MN, and/or isomerisation of dimethylnaphthalenes (DMNs). In this study, synthesis of 2,6-triad DMN isomers consisting of 2,6-DMN, 1,6-DMN, and 1,5-DMN have been investigated with the disproportionation of 2-MN over unmodified and Zr-modified mesoporous MCM-41 zeolite catalysts. In contrast to other DMN isomers, both 1,5-DMN and 1,6-DMN can be effectively isomerised to be profitable 2,6-DMN. The disproportionation of 2-MN experiments were carried out in a catalytic fixed-bed reactor in the presence of 1?g of catalyst at a temperature range of 350–500?°C and weight hourly space velocity between 1 to 3?h?1. The results demonstrated that mesoporous MCM-41 zeolite catalyst has a selective pore shape for 2,6-triad DMN isomers, which may allow a decrease in the production cost of 2,6-DMN. Additionally, 2,6-DMN was successfully synthesised by the disproportionation of 2-MN over MCM-41 zeolite catalyst. Furthermore, both the conversion of 2-MN and the selectivity of 2,6-DMN were considerably enhanced by the Zr impregnation on MCM-41.
- Güle?, Fatih,Niftaliyeva, Aysel,Karaduman, Ali
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p. 7205 - 7218
(2018/08/22)
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- Shape-selective methylation of naphthalene with methanol over SAPO-11 molecular sieve modified with hydrochloric acid and citric acid
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Herein, a series of SAPO-11 molecular sieves were modified by citric acid and hydrochloric acid. They were characterized by ICP, XRD, SEM, N2 adsorption-desorption, NH3-TPD, 29Si MAS NMR, and Py-IR and evaluated by the methylation of naphthalene with methanol to 2,6-dimethylnaphthalene (2,6-DMN). According to the XRD results, hydrochloric acid at a high concentration not only removed extra-framework aluminum but also deleted framework silicon; this resulted in the formation of crystal defects. N2 adsorption-desorption results showed that all the samples possessed micropores and secondary mesopores. The SAPO-11 sample modified with 4 mol L-1 hydrochloric acid for 30 min exhibited the largest secondary mesopore size distributions. NH3-TPD and 29Si MAS NMR showed that hydrochloric acid at a high concentration could eliminate more acid sites. SAPO-11 modified with 4 mol L-1 hydrochloric acid for 30 min presented high catalytic performance for the methylation of naphthalene; this was mainly attributed to the amount of secondary mesopores in the SAPO-11 molecular sieves.
- Wang, Xiaoxiao,Liu, Zhenmin,Guo, Fang,Wang, Yingchun,Wei, Xianxian,Li, Peng,Xue, Yongbing,Wang, Yuanyang,Guo, Shaoqing,Yu, Yue
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p. 243 - 250
(2018/01/17)
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- Stack the Bowls: Tailoring the Electronic Structure of Corannulene-Integrated Crystalline Materials
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We report the first examples of purely organic donor–acceptor materials with integrated π-bowls (πBs) that combine not only crystallinity and high surface areas but also exhibit tunable electronic properties, resulting in a four-orders-of-magnitude conductivity enhancement in comparison with the parent framework. In addition to the first report of alkyne–azide cycloaddition utilized for corannulene immobilization in the solid state, we also probed the charge transfer rate within the Marcus theory as a function of mutual πB orientation for the first time, as well as shed light on the density of states near the Fermi edge. These studies could foreshadow new avenues for πB utilization for the development of optoelectronic devices or a route for highly efficient porous electrodes.
- Rice, Allison M.,Dolgopolova, Ekaterina A.,Yarbrough, Brandon J.,Leith, Gabrielle A.,Martin, Corey R.,Stephenson, Kenneth S.,Heugh, Rebecca A.,Brandt, Amy J.,Chen, Donna A.,Karakalos, Stavros G.,Smith, Mark D.,Hatzell, Kelsey B.,Pellechia, Perry J.,Garashchuk, Sophya,Shustova, Natalia B.
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supporting information
p. 11310 - 11315
(2018/08/11)
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- Helical Threads: Enantiomerically Pure Carbo[6]Helicene Oligomers
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We report the synthesis of enantiomerically pure carbo[6]helicene oligomers with buta-1,3-diyne-1,4-diyl bridges between the helicene nuclei. The synthesis of monomeric (±)-2,15-bis[(triisopropylsilyl)ethynyl]carbo[6]helicene was achieved in 25 % yield over six steps. Pure (+)-(P)- and (?)-(M)-enantiomers were obtained by HPLC on a chiral stationary phase. The dimeric (+)-(P)2- and (?)-(M)2-configured and the tetrameric (+)-(P)4- and (?)-(M)4-configured oligomers were obtained by sequential oxidative acetylenic coupling. The ECD spectra of the tetrameric oligomers displayed large Cotton effect intensities of Δ?=?851 m?1 cm?1 at λ=370 nm ((M)4-enantiomer). We transformed the buta-1,3-diyne-1,4-diyl bridge in the dimeric (P)2 and (M)2 oligomer by heteroaromatization into a thiene-2,5-diyl linker. Although the resulting chromophore showed reduced ECD intensities, it exhibited a remarkably strong fluorescence emission at 450–500 nm, with an absolute quantum yield of 25 %.
- Schaack, Cédric,Sidler, Eric,Trapp, Nils,Diederich, Fran?ois
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supporting information
p. 14153 - 14157
(2017/10/17)
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- Hierarchical Corannulene-Based Materials: Energy Transfer and Solid-State Photophysics
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We report the first example of a donor–acceptor corannulene-containing hybrid material with rapid ligand-to-ligand energy transfer (ET). Additionally, we provide the first time-resolved photoluminescence (PL) data for any corannulene-based compounds in the solid state. Comprehensive analysis of PL data in combination with theoretical calculations of donor–acceptor exciton coupling was employed to estimate ET rate and efficiency in the prepared material. The ligand-to-ligand ET rate calculated using two models is comparable with that observed in fullerene-containing materials, which are generally considered for molecular electronics development. Thus, the presented studies not only demonstrate the possibility of merging the intrinsic properties of π-bowls, specifically corannulene derivatives, with the versatility of crystalline hybrid scaffolds, but could also foreshadow the engineering of a novel class of hierarchical corannulene-based hybrid materials for optoelectronic devices.
- Rice, Allison M.,Fellows, W. Brett,Dolgopolova, Ekaterina A.,Greytak, Andrew B.,Vannucci, Aaron K.,Smith, Mark D.,Karakalos, Stavros G.,Krause, Jeanette A.,Avdoshenko, Stanislav M.,Popov, Alexey A.,Shustova, Natalia B.
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supporting information
p. 4525 - 4529
(2017/04/11)
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- Electrochemically active porous organic polymers based on corannulene
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For the first time, porous organic polymers (POPs) based on the smallest buckybowl, corannulene (BB-POPs) have been synthesized. Three POPs were synthesised via Sonogashira co-polymerization of 1,2,5,6-tetrabromocorannulene and alkyne linkers. BB-POP-3 exhibits the highest surface area (SABET = 560 m2 g-1) and CO2 adsorption of 11.7 wt%, while they retain the redox properties of corannulene.
- Karunathilake, Arosha A.K.,Thompson, Christina M.,Perananthan, Sahila,Ferraris, John P.,Smaldone, Ronald A.
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supporting information
p. 12881 - 12884
(2016/11/06)
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- Nickel-catalyzed cross-coupling of anisole derivatives with trimethylaluminum through the cleavage of carbonoxygen bonds
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Nickel-catalyzed cross-coupling of methoxyarenes with trimethylaluminum is described. The use of 1,3-dicyclohexylimidazol-2-ylidene as a ligand and NaO'Bu as a base promotes the methylation of anisole derivatives via the cleavage of normally unreactive aryl carbonoxygen bonds.
- Morioka, Toshifumi,Nishizawa, Akihiro,Nakamura, Keisuke,Tobisu, Mamoru,Chatani, Naoto
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supporting information
p. 1729 - 1731
(2016/02/19)
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- Construction of polyaromatics via photocyclization of 2-(fur-3-yl) ethenylarenes, using a 3-furyl group as an isopropenyl equivalent synthon
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The construction of different types of substituted arenes was demonstrated through the photocyclization of 2-(fur-3-yl)ethenylarenes using a 3-furyl group as an isopropenyl equivalent synthon in the photocyclization reaction. The furan portion of the photocyclization intermediate could be fragmented via a base-induced elimination reaction to yield a series of substituted polyaromatics, including naphthalene, benzofuran, benzothiophene, phenanthrene, phenalene, acenaphthene, and triphenylene. Using different reagents, this method made it possible to introduce methyl or 2-hydroxyethyl groups as substituents at specific positions in these arenes.
- Chen, Ying-Zhe,Ni, Ching-Wen,Teng, Fu-Lin,Ding, Yi-Shun,Lee, Tunng-Hsien,Ho, Jinn-Hsuan
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p. 1748 - 1762
(2014/03/21)
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- Cross-coupling reaction with lithium methyltriolborate
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We newly developed lithium methyltriolborate as an air-stable white solid that is convenient to handle. The good performance of this triolborate for metal-catalyzed bond-forming reactions was demonstrated in palladium-catalyzed cross-coupling reactions wi
- Yamamoto, Yasunori,Ikizakura, Kazuya,Ito, Hajime,Miyaura, Norio
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p. 430 - 439
(2013/03/13)
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- Kilogram-scale production of corannulene
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An efficient entry process for the synthesis of corannulene has been demonstrated on kilogram scale. Compared to the discovery and gram-scale syntheses, the amounts of solvents and reagents per gram of product were greatly reduced. Priority was given to implement the least toxic agents possible. Improvements in the purification of products obviated the need for column chromatography, alleviating four chromatographic operations. A new reduction method for the final step of the synthesis decreased reaction time from 6 to 0.5 days, and avoided the use of 100 equiv of zinc metal. The process now comprises nine steps, each of which runs smoothly at 100-L scale with a charging of 3-12 kg of educt. A total of 1.3 kg corannulene was isolated. This kilogram-scale process reduces material costs by over 2 orders of magnitude compared to that for the published gram-scale syntheses. Key opportunities in the process are identified for further improvements that should make synthesis on 100-kg scale feasible with a target price for 1 that is suitable for commercial production and engineering application.
- Butterfield, Anna M.,Gilomen, Bruno,Siegel, Jay S.
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experimental part
p. 664 - 676
(2012/08/07)
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- Base-induced photorearrangements from 3-styrylfurans to 2-methylnaphthalenes
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Irradiation of 3-(4-substituted styryl)furans in basic media yielded a series of 7-substituted-2-methylnaphthalenes, including methoxy, isopropyl, ethyl, methyl, fluoro, and cyano substituents. This base-induced photorearrangement involves cis-trans photoisomerization, 6e photocyclization, base-induced elimination, and a Norrish Type I photoreaction and is a novel method to synthesize unsymmetrical 2,7-disubstituted naphthalenes.
- Ho, Jinn-Hsuan,Lee, Tunng-Hsien,Lo, Chia-Kai,Chuang, Chao-Li
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supporting information; experimental part
p. 7199 - 7201
(2012/01/05)
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- Methylation of naphthalene on MTW-type zeolites. Influence of template origin and substitution of Al by Ga
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Two templates, methyltriethylammonium bromide (MTEA) and tetraethylammonium bromide (TEA) were used to synthesize aluminosilicate ZSM-12 zeolites. Additionally, zeolites isomorphously substituted (partially or totally) by gallium were prepared with MTEA.
- Wu, Wei,Wu, Weiguo,Kikhtyanin,Li, Lingfei,Toktarev,Ayupov,Khabibulin,Echevsky,Huang, Juan
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experimental part
p. 279 - 288
(2010/11/18)
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- METHOD OF PURIFYING 2,7-DIMETHYLNAPHTHALENE
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[PROBLEMS] To provide a process for industrially stably producing a highly purified 2,7-dimethylnaphthalene with high yield from a dimethylnaphthalene isomer mixture at low production cost through convenient means. [MEANS FOR SOLVING PROBLEMS] There is provided a method of purifying 2,7-dimethylnaphthalene, characterized by including the step of bringing a raw oil containing a mixture of 1,7-dimethylnaphthalene and 2,7-dimethylnaphthalene together with a developing solvent into contact with L-type zeolite to thereby effect adsorption of 1,7-dimethylnaphthalene.
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Page/Page column 7-8
(2008/06/13)
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- Selective methylation catalyst, method of catalyst manufacture and methylation process
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Novel catalysts and processes in accordance with the invention can accomplish high selectivity and conversion of naphthalenic compounds such as the conversion of methylnaphthalene (2-MN) or naphthalene to 2,6-dimethylnaphthalene (2,6-DMN). The catalysts are prepared by treating, for example, a ZSM-5-type material with iron in the presence of a halogen such as a fluoride. The resulting catalyst includes iron, as well as a significant portion of aluminum present in the ZSM-5-type starting material. Processes for using the catalysts also are disclosed.
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Page/Page column 5
(2008/06/13)
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- The first helical-chiral phosphane ligands: rac-[5]- and rac-[6]-heliphos
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The syntheses of two helical, chiral phosphanes in their racemic forms are described. Their helicene backbone was built up using an improved photocyclization approach. The phosphorus functionalities were introduced in the last step. Up to now, separation of the enantiomers of the helicene phosphanes could be achieved analytically but not on a preparative scale.
- Terfort, Andreas,Goerls, Helmar,Brunner, Henri
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- Regioselective synthesis of substituted 1-methyl- and 2-methylnaphthalenes
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Regiospecifically substituted 1-methyl- and 2-methylnaphthalenes, 5-methyl- and 6-methyl-1,2,3,4-tetrahydroanthracenes have been synthesized in good yields through 1,2-addition of the corresponding α-lithio- o- or m-xylenes onto α-oxoketene dithioacetals or their dihydro derivatives followed by cyclodehydration of the resulting carbinols in the presence of borontrifluoride etherate.
- Yadav, K. Mallik,Mohanta, Pramod K.,Ila, Hiriyakkanavar,Junjappa, Hiriyakkanavar
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p. 14049 - 14056
(2007/10/03)
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- SHAPE SELECTIVE DISPROPORTIONATION OF METHYLNAPHTHALENE ON ZSM-5 CATALYST
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The conversion of 2-methylnaphthalene (2-MN) was studied at atmospheric pressure in a flow-type fixed bed reactor using H-Y, H-beta, H-mordenite, H-ZSM-5, H-ZSM-11 and H-ZSM-48 as catalysts.H-Y and H-beta exhibited high activities for disproportionation and isomerization of 2-MN.H-Mordenite and zeolites having medium size pores were active for the conversion of 2-MN which was mainly isomerized to 1-MN.The low disproportionation activities of these zeolites resulted from their shape selective properties.Disproportionation of 2-MN on the zeolite catalysts gave 2,6- and 2,7-dimethylnaphthalenes (DMN) in higher proportions than the thermodynamically attainable level.H-ZSM-5 was the most selective catalyst to produce these DMN isomers among the zeolite catalysts tested, although 2,7-DMN was formed in a higher proportion than 2,6-DMN.On H-mordenite catalyst, 2,6-DMN was more selectively formed than 2,7-DMN.The selectivity for 2,6-DMN against 2,7-DMN increased with increasing SiO2/Al2O3 ratio of H-mordenite.It is suggested that the composition of DMN isomers produced by disproportionation of 2-MN depends on the acid strength as well as on the shape selective properties of zeolites used.
- Kikuchi, Eiichi,Mogi, Yasuhiro,Matsuda, Takeshi
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p. 909 - 919
(2007/10/02)
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- Clathrate formation and molecular recognition by novel chalcogen-cyano interactions in tetracyanoquinodimethanes fused with thiadiazole and selenadiazole rings
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The intermolecular contacts between chalcogen atoms and cyano lone pairs were found to stabilize the crystalline state by electrostatic interaction. This interaction is one of the sources of the directionality in crystal packing of organic molecules and causes the formation of various types of inclusion lattices in the charge-transfer (CT) crystals of 1-3. By using highly selective formation of CT crystals with substituted aromatic hydrocarbons, particular isomers such as p-xylene or 2,6-dimethylnaphthalene (2,6-DMN) could be separated from the corresponding isomer mixtures. Lattice-related interaction plays a more significant role than molecular orbital interaction in the observed selectivity for para-disubstituted benzenes. However, the latter interaction is important for the recognition of 2,6-DMN from the 2,7 isomer.
- Suzuki, Takanori,Fujii, Hiroshi,Yamashita, Yoshiro,Kabuto, Chizuko,Tanaka, Shoji,Harasawa, Masako,Mukai, Toshio,Miyashi, Tsutomu
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p. 3034 - 3043
(2007/10/02)
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- Shape Selective Catalysis by ZSM-5 in Disproportionation of 2-Methylnaphthalene
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Disproportionation of methylnaphthalene (MN) was carried out on ZSM-5 catalysts.The external acid sites were eliminated by dealumination with (NH4)2SiF6.The dealuminated ZSM-5 gave 2,6- and 2,7-dimethylnaphthalene (DMN) from disproportionation of 2-methylnaphthalene (MN), due to its shape selective property.
- Matsuda, Takeshi,Yogo, Katsunori,Mogi, Yashuhiro,Kikuchi, Eiichi
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p. 1085 - 1088
(2007/10/02)
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- Electrophilic Aromatic Substitution. Part 35. Deviations from Additivity of Methyl Substituent Effects in Detritiation of Dimethylnaphthalenes: the Effect of Electron Supply on Bond Fixation
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Rate coefficients have been measured for protiodetritiation in anhydrous trifluoroacetic acid at 70 deg C of all positions of 1,3-, 1,4-, 1,5-, 1,8-, 2,3-, 2,6-, and 2,7-dimethylnaphthalenes.The derived partial rate factors show up to 10-fold departure from those calculated on the basis of additivity of the individual methyl substituent effects.Of the seventeen positions examined, all but three show reactivity which is greater than that calculated.The results point to a decrease in bond fixation in dimethylnaphthalenes compared to monomethylnaphthalenes, probably arising either from the increased electron supply in the former or from a sterically facilitated change in the shape of the naphthalene nucleus.Detritiation of 1,8-dimethylnaphthalene is accompanied by isomerisation to 1,7-dimethylnaphthalene due almost certainly to a sterically accelerated 1,2-methyl shift; this shift (which is the first observed during hydrogen exchange studies) accounts for discrepancies between previous measurements of the exchange rate of the (relatively unreactive) 3-position of 1,8-dimethylnaphthalene.The kinetics show that surface-catalysed protiodemethylation accompanies detritiation of 1,4-dimethylnaphthalene and this is aided by the high stability of the intermediate for this ipso-substitution.
- Neary, Adrian P.,Taylor, Roger
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p. 1233 - 1238
(2007/10/02)
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