Journal of Molecular Catalysis A: Chemical最新文献

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Synthesis, crystal structures and catalytic activity of Cu(II) and Mn(III) Schiff base complexes: Influence of additives on the oxidation catalysis of cyclohexane and 1-phenylehanol Cu(II)和Mn(III)希夫碱配合物的合成、晶体结构和催化活性:添加剂对环己烷和1-苯乙醇氧化催化的影响
IF 5.062
Journal of Molecular Catalysis A: Chemical Pub Date : 2017-01-01 DOI: 10.1016/j.molcata.2016.09.005
Oksana V. Nesterova , Dmytro S. Nesterov , Agnieszka Krogul-Sobczak , M. Fátima C. Guedes da Silva , Armando J.L. Pombeiro
{"title":"Synthesis, crystal structures and catalytic activity of Cu(II) and Mn(III) Schiff base complexes: Influence of additives on the oxidation catalysis of cyclohexane and 1-phenylehanol","authors":"Oksana V. Nesterova ,&nbsp;Dmytro S. Nesterov ,&nbsp;Agnieszka Krogul-Sobczak ,&nbsp;M. Fátima C. Guedes da Silva ,&nbsp;Armando J.L. Pombeiro","doi":"10.1016/j.molcata.2016.09.005","DOIUrl":"https://doi.org/10.1016/j.molcata.2016.09.005","url":null,"abstract":"<div><p>The complexes of copper [Cu(κ<em>ONN</em>’-HL)(NO<sub>3</sub>)(DMF)](NO<sub>3</sub>)∙H<sub>2</sub>O (<strong>1</strong>) and [Cu(κ<em>ONN</em>’-HL)Cl<sub>2</sub>]∙½DMSO (<strong>2</strong>), and of manganese [Mn(κ<em>ON</em>-HL)<sub>2</sub>Cl<sub>2</sub>]Cl (<strong>3</strong>) and [Mn(κ<em>ON</em>-HL)<sub>2</sub>(NO<sub>3</sub>)<sub>2</sub>](NO<sub>3</sub>)∙H<sub>2</sub>O (<strong>4</strong>) were synthesized by reactions of the respective chloride or nitrate salt with a non-aqueous solutions of the Schiff base aminoalcohol HL (product of condensation of salicylic aldehyde and aminoethylpiperazine) and characterized by X-ray diffraction analysis. The catalytic investigations disclosed a prominent activity of the copper compounds <strong>1</strong> and <strong>2</strong> towards oxidation of cyclohexane with hydrogen peroxide in the presence of various promoters (nitric, hydrochloric, oxalic acids and pyridine), under mild conditions. The unusual promoting effect of pyridine on the catalytic activity of the copper catalysts allowed to achieve yields up to 21% based on cyclohexane. Chromatographic studies revealed that cyclohexyl hydroperoxide is a main reaction product and chlorocyclohexane (in the presence of HCl as promoter) was also detected, suggesting a free radical reaction pathway with hydroxyl radicals as attacking species. Complexes <strong>1</strong> and <strong>2</strong> act also as catalysts in the oxidation of 1-phenylethanol with <em>tert</em>-butylhydroperoxide, showing acetophenone yields up to 62% and TON (turnover numbers) up to 620 in the presence of the K<sub>2</sub>CO<sub>3</sub> promoter.</p></div>","PeriodicalId":370,"journal":{"name":"Journal of Molecular Catalysis A: Chemical","volume":"426 ","pages":"Pages 506-515"},"PeriodicalIF":5.062,"publicationDate":"2017-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.molcata.2016.09.005","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"2171632","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: 39
Study of Lewis acid accelerated palladium catalyzed CH activation 路易斯酸加速钯催化CH活化的研究
IF 5.062
Journal of Molecular Catalysis A: Chemical Pub Date : 2017-01-01 DOI: 10.1016/j.molcata.2016.09.018
Orsolya Tischler , Szabolcs Kovács , Gábor Érsek , Péter Králl , János Daru , András Stirling , Zoltán Novák
{"title":"Study of Lewis acid accelerated palladium catalyzed CH activation","authors":"Orsolya Tischler ,&nbsp;Szabolcs Kovács ,&nbsp;Gábor Érsek ,&nbsp;Péter Králl ,&nbsp;János Daru ,&nbsp;András Stirling ,&nbsp;Zoltán Novák","doi":"10.1016/j.molcata.2016.09.018","DOIUrl":"https://doi.org/10.1016/j.molcata.2016.09.018","url":null,"abstract":"<div><p>Acceleration of palladium catalyzed C<img>H activation by various Lewis Acids was demonstrated on the directed <em>ortho</em>-alkenylation and acylation of acetanilide and urea derivatives. The universality of this effect was investigated by the study of different palladium catalysts, directing groups in the aromatic substrates and versatile Lewis acids. Experiments were carried out to monitor the reactions and to compare the behavior and activity of different types of Lewis acids. Kinetic investigation revealed a rate determining C<img>H activation step, and DFT studies were performed for the explanation of Lewis acid effect on C<img>H activation.</p></div>","PeriodicalId":370,"journal":{"name":"Journal of Molecular Catalysis A: Chemical","volume":"426 ","pages":"Pages 444-450"},"PeriodicalIF":5.062,"publicationDate":"2017-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.molcata.2016.09.018","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"2391729","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: 11
Click-binol-phosphoric acid catalysts in intramolecular enantioselective oxidative CH-bond functionalization 分子内对映选择性氧化ch键功能化的click -binol-磷酸催化剂
IF 5.062
Journal of Molecular Catalysis A: Chemical Pub Date : 2017-01-01 DOI: 10.1016/j.molcata.2016.09.006
Sebastian Stockerl , Daniel Gutiérrez , Olga García Mancheño
{"title":"Click-binol-phosphoric acid catalysts in intramolecular enantioselective oxidative CH-bond functionalization","authors":"Sebastian Stockerl ,&nbsp;Daniel Gutiérrez ,&nbsp;Olga García Mancheño","doi":"10.1016/j.molcata.2016.09.006","DOIUrl":"https://doi.org/10.1016/j.molcata.2016.09.006","url":null,"abstract":"<div><p>Counteranion-catalysis represents an appealing but challenging approach for the development of enantioselective oxidative C<img>H bond functionalization reactions. In this work, a new family of 3,3′-triazolyl BINOL-derived phosphoric acids was synthesized and employed in the intramolecular asymmetric C<img>H bond functionalization of <em>N</em>-aryl substituted tetrahydroisoquinolines. As previously reported with related structures, the presence of the triazole groups on the catalysts was key to attain enantioselectivity. Our study also shows the importance of choosing the appropriate regioisomeric triazole groups at the BINOL backbone to achieve a more efficient chirality transfer. Moderate enantiomeric ratios were obtained with the <em>N</em>-benzamide substrates, whereas the change of the nature of the nucleophile fragment was translated to a dramatic loss of the enantioselectivity. Therefore, it can be foreseen that there is a need for designing further superior catalyst structures to develop future counter-anion organocatalyzed asymmetric C<img>H bond functionalization reactions.</p></div>","PeriodicalId":370,"journal":{"name":"Journal of Molecular Catalysis A: Chemical","volume":"426 ","pages":"Pages 572-585"},"PeriodicalIF":5.062,"publicationDate":"2017-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.molcata.2016.09.006","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"2595833","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: 7
E-Selective dimerization of phenylacetylene catalyzed by cationic tris(μ-hydroxo)diruthenium(II) complex and the mechanistic insight: The role of two ruthenium centers in catalysis 阳离子三(μ-羟基)二钌(II)配合物催化苯乙炔的e -选择性二聚化及其机理:两个钌中心在催化中的作用
IF 5.062
Journal of Molecular Catalysis A: Chemical Pub Date : 2017-01-01 DOI: 10.1016/j.molcata.2016.08.027
Sayori Kiyota, Hirofumi Soeta, Nobuyuki Komine, Sanshiro Komiya , Masafumi Hirano
{"title":"E-Selective dimerization of phenylacetylene catalyzed by cationic tris(μ-hydroxo)diruthenium(II) complex and the mechanistic insight: The role of two ruthenium centers in catalysis","authors":"Sayori Kiyota,&nbsp;Hirofumi Soeta,&nbsp;Nobuyuki Komine,&nbsp;Sanshiro Komiya ,&nbsp;Masafumi Hirano","doi":"10.1016/j.molcata.2016.08.027","DOIUrl":"https://doi.org/10.1016/j.molcata.2016.08.027","url":null,"abstract":"<div><p>A dinuclear complex [(Me<sub>3</sub>P)<sub>3</sub>Ru(μ-OH)<sub>3</sub>Ru(PMe<sub>3</sub>)<sub>3</sub>]<sup>+</sup>[OPh]<sup>−</sup> (<strong>1</strong>) (0.5 mol%) catalyzes <em>E</em>-selective dimerization of phenylacetylene, which involves the C–H bond cleavage of phenylacetylene and resulting stereospecific C–C bond forming reaction, at 100<!--> <!-->°C for 2<!--> <!-->h to give (<em>E</em>)-1,4-diphenylbut-3-en-1-yne in quantitative yield (<em>E</em>/<em>Z</em> <!-->=<!--> <!-->91/9). Similar reactions using 4-nitro-, 4-cyano-, 4-trifluoromethyl-, 4-acetyl-, and 4-methylphenylacetylene give the corresponding enynes. The kinetic study for dimerization of phenylacetylene shows the second-order and first-order reactions with regard to the phenylacetylene and <strong>1</strong> concentrations, respectively, suggesting this reaction to be catalyzed by a dinuclear ruthenium complex. Addition of PMe<sub>3</sub> to the catalytic system strongly discourages the dimerization. These features are consistent with the scenario, where dissociation of a PMe<sub>3</sub> ligand from <strong>1</strong> gives a coordinatively unsaturated diruthenium species and one of the ruthenium centers performs as a reaction site for the enyne formation and the other ruthenium center behaves as a spectator in the catalysis.</p></div>","PeriodicalId":370,"journal":{"name":"Journal of Molecular Catalysis A: Chemical","volume":"426 ","pages":"Pages 419-428"},"PeriodicalIF":5.062,"publicationDate":"2017-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.molcata.2016.08.027","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"2660117","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: 5
Direct activation of CH4 to oxygenates and unsaturated hydrocarbons using N2O on Fe-modified zeolites 用N2O在铁改性沸石上直接活化CH4生成氧合物和不饱和烃
IF 5.062
Journal of Molecular Catalysis A: Chemical Pub Date : 2017-01-01 DOI: 10.1016/j.molcata.2016.11.008
Kyung Soo Park , Jeong Hwa Kim , So Hyun Park , Dong Ju Moon , Hyun-Seog Roh , Chan-Hwa Chung , Soong Ho Um , Joon-Hwan Choi , Jong Wook Bae
{"title":"Direct activation of CH4 to oxygenates and unsaturated hydrocarbons using N2O on Fe-modified zeolites","authors":"Kyung Soo Park ,&nbsp;Jeong Hwa Kim ,&nbsp;So Hyun Park ,&nbsp;Dong Ju Moon ,&nbsp;Hyun-Seog Roh ,&nbsp;Chan-Hwa Chung ,&nbsp;Soong Ho Um ,&nbsp;Joon-Hwan Choi ,&nbsp;Jong Wook Bae","doi":"10.1016/j.molcata.2016.11.008","DOIUrl":"https://doi.org/10.1016/j.molcata.2016.11.008","url":null,"abstract":"<div><p>Direct activation of CH<sub>4</sub> to oxygenates and unsaturated light hydrocarbons was investigated using Fe-modified ZSM-5 and Ferrierite (FER) for a partial oxidation of CH<sub>4</sub> with N<sub>2</sub>O oxidant. The amount of active α-oxygen sites and number of Bronsted acid sites on the Fe-modified zeolites were well correlated with CH<sub>4</sub> conversion rate and product distributions. The amount of α-oxygen sites was largely changed according to preparation method such as wet impregnation or ion-exchange of iron precursor and types of zeolites. A large number of Bronsted acid sites and α-oxygen sites on the Fe-modified FER revealed a higher oxygenate formation such as methanol and dimethyl ether (DME) with COx, and a larger number of strong acid sites on Fe-modified ZSM-5 was also responsible for a higher selectivity to light hydrocarbons by a successive dehydration of oxygenates formed. The different catalytic performances were verified through proper measurements of the amount and type of acidic sites as well as the α-oxygen sites measured by N<sub>2</sub>O pulse chemisorption. The Fe-modified FER prepared by impregnation method possessed a larger amount of α-oxygen sites due to abundant Bronsted acid sites, which was responsible for a higher rate of CH<sub>4</sub> conversion to oxygenates with the help of N<sub>2</sub>O decomposition on the α-oxygen sites originated from iron oxide nanoparticles.</p></div>","PeriodicalId":370,"journal":{"name":"Journal of Molecular Catalysis A: Chemical","volume":"426 ","pages":"Pages 130-140"},"PeriodicalIF":5.062,"publicationDate":"2017-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.molcata.2016.11.008","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"2878506","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: 18
Improved catalytic performance of acid-activated sepiolite supported nickel and potassium bimetallic catalysts for liquid phase hydrogenation of 1,6-hexanedinitrile 改善酸活化海泡石负载镍钾双金属催化剂对1,6-己二腈液相加氢的催化性能
IF 5.062
Journal of Molecular Catalysis A: Chemical Pub Date : 2017-01-01 DOI: 10.1016/j.molcata.2016.10.029
Yang Lv , Fang Hao , Pingle Liu , Shaofeng Xiong , He’an Luo
{"title":"Improved catalytic performance of acid-activated sepiolite supported nickel and potassium bimetallic catalysts for liquid phase hydrogenation of 1,6-hexanedinitrile","authors":"Yang Lv ,&nbsp;Fang Hao ,&nbsp;Pingle Liu ,&nbsp;Shaofeng Xiong ,&nbsp;He’an Luo","doi":"10.1016/j.molcata.2016.10.029","DOIUrl":"https://doi.org/10.1016/j.molcata.2016.10.029","url":null,"abstract":"<div><p>Different inorganic acids were used to activate sepiolite, and the acid-activated sepiolites supported nickel and potassium bimetallic catalysts were prepared. Nitrogen adsorption-desorption, hydrogen chemisorption, ammonia temperature programmed desorption (NH<sub>3</sub>-TPD), temperature programmed reduction (TPR), powder X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), Fourier Transform Infrared Spectroscopy (FTIR) and energy dispersive X-ray (EDX) were used to characterize the catalysts. The catalytic performance of the acid-activated sepiolite supported K-Ni bimetallic catalysts were investigated in 1,6-hexanedinitrile (HDN) hydrogenation in liquid phase. It was revealed that the potassium could increase the alkalinity of the catalyst with the aim of inhibiting the formation of the 1-azacycloheptane (ACH). And the addition of potassium reduces the particle size of nickel and improves its dispersion. Compared with hydrochloric acid and sulfuric acid, nitric acid treatment increases more silanol groups (Si<img>OH) on the sepiolite surface, which is helpful to nickel particles adsorption and dispersion. Nitric acid activated sepiolite supported nickel and potassium bimetallic catalysts (K-Ni/NASEP) present the best catalytic performance, the conversion of HDN comes up to 92.0% under moderate conditions of lower temperature and pressure, the selectivity to 6-aminocapronitrile (ACN) and 1,6-hexanediamine (HDA) is up to 95.2%.</p></div>","PeriodicalId":370,"journal":{"name":"Journal of Molecular Catalysis A: Chemical","volume":"426 ","pages":"Pages 15-23"},"PeriodicalIF":5.062,"publicationDate":"2017-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.molcata.2016.10.029","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"2391732","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: 20
Pd catalyzed couplings of “superactive esters” and terminal alkynes: Application to flavones and γ-benzopyranones construction Pd催化“超活性酯”与末端炔的偶联:在黄酮和γ-苯并吡喃酮构建中的应用
IF 5.062
Journal of Molecular Catalysis A: Chemical Pub Date : 2017-01-01 DOI: 10.1016/j.molcata.2016.10.030
Dandan Yang, Zhenhua Wang, Xiu Wang, Huaming Sun, Zunyuan Xie, Juan Fan, Guofang Zhang, Weiqiang Zhang, Ziwei Gao
{"title":"Pd catalyzed couplings of “superactive esters” and terminal alkynes: Application to flavones and γ-benzopyranones construction","authors":"Dandan Yang,&nbsp;Zhenhua Wang,&nbsp;Xiu Wang,&nbsp;Huaming Sun,&nbsp;Zunyuan Xie,&nbsp;Juan Fan,&nbsp;Guofang Zhang,&nbsp;Weiqiang Zhang,&nbsp;Ziwei Gao","doi":"10.1016/j.molcata.2016.10.030","DOIUrl":"https://doi.org/10.1016/j.molcata.2016.10.030","url":null,"abstract":"<div><p>Lewis base, <em>N</em>-methylmorpholine (NMM) accelerated Pd-catalyzed Sonogashira coupling of steric hindered super active esters, 1a–1e, and terminal alkynes. This approach provided an efficient synthetic protocol for a broad array of acylated <em>o</em>-alkynoylphenols compounds, 3a–3e, under moderate conditions. The mechanistic study clearly demonstrated that NNM stabilized the catalytic palladium species, and accelerated the leaving of triazine moiety during the catalytic cycle of the cross-coupling reactions. In addition, piperazine was found to efficiently catalyze the 6-endo cyclization of acylated <em>o</em>-alkynoylphenols, which achieved the diversity oriented synthesis of <em>γ</em>-benzopyranones, 4aa–4eg, with 93–99% yields.</p></div>","PeriodicalId":370,"journal":{"name":"Journal of Molecular Catalysis A: Chemical","volume":"426 ","pages":"Pages 24-29"},"PeriodicalIF":5.062,"publicationDate":"2017-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.molcata.2016.10.030","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"2878503","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: 11
Suzuki-Miyaura coupling reactions using novel metal oxide supported ionic palladium catalysts 新型金属氧化物负载离子钯催化剂的Suzuki-Miyaura偶联反应
IF 5.062
Journal of Molecular Catalysis A: Chemical Pub Date : 2017-01-01 DOI: 10.1016/j.molcata.2016.10.033
G.J. Lichtenegger , M. Maier , M. Hackl , J.G. Khinast , W. Gössler , T. Griesser , V.S.Phani Kumar , H. Gruber-Woelfler , P.A. Deshpande
{"title":"Suzuki-Miyaura coupling reactions using novel metal oxide supported ionic palladium catalysts","authors":"G.J. Lichtenegger ,&nbsp;M. Maier ,&nbsp;M. Hackl ,&nbsp;J.G. Khinast ,&nbsp;W. Gössler ,&nbsp;T. Griesser ,&nbsp;V.S.Phani Kumar ,&nbsp;H. Gruber-Woelfler ,&nbsp;P.A. Deshpande","doi":"10.1016/j.molcata.2016.10.033","DOIUrl":"https://doi.org/10.1016/j.molcata.2016.10.033","url":null,"abstract":"<div><p>Palladium substituted CeO<sub>2</sub>, SnO<sub>2</sub> and their mixed oxides have been synthesized in quantitative yields out of non-toxic and inexpensive precursors using a simple and rapid single step solution combustion method. The resulting oxides, especially the mixed oxides Ce<sub>0.79</sub>Sn<sub>0.20</sub>Pd<sub>0.01</sub>O<sub>2-δ</sub>, Sn<sub>0.79</sub>Ce<sub>0.20</sub>Pd<sub>0.01</sub>O<sub>2-δ</sub> and Sn<sub>0.99</sub>Pd<sub>0.01</sub>O<sub>2-δ</sub> proved to be highly active (TOF<!--> <!-->&gt;<!--> <!-->12,000<!--> <!-->h<sup>−1</sup>) for Suzuki-Miyaura cross-couplings of phenylboronic acid with various bromoarenes. The reactions were carried out in ambient air at moderate temperatures using environmentally friendly aqueous ethanol solutions as reaction solvents. Minimal amounts of palladium in the product solution (<!--> <!-->&lt;<!--> <!-->0.14<!--> <!-->mg/L), the reaction kinetics as well as catalyst poisoning tests support the thesis that the reaction proceeds via dissolved palladium species in a homogeneous reaction mechanism. Nevertheless, the synthesized catalysts could be reused for at least five times with only minor changes in activity and no changes in the crystal structure, indicating the high potential of the investigated catalysts as quasi-heterogeneous C<img>C coupling catalysts.</p></div>","PeriodicalId":370,"journal":{"name":"Journal of Molecular Catalysis A: Chemical","volume":"426 ","pages":"Pages 39-51"},"PeriodicalIF":5.062,"publicationDate":"2017-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.molcata.2016.10.033","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"1737688","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: 17
Unprecedented salt-promoted direct arylation of acidic sp2 CH bonds under heterogeneous Ni-MOF-74 catalysis: Synthesis of bioactive azole derivatives 在非均相Ni-MOF-74催化下,史无前例的盐促进酸性sp2 CH键的直接芳基化:生物活性唑衍生物的合成
IF 5.062
Journal of Molecular Catalysis A: Chemical Pub Date : 2017-01-01 DOI: 10.1016/j.molcata.2016.11.009
Huong T.T. Nguyen, Duc N.A. Doan, Thanh Truong
{"title":"Unprecedented salt-promoted direct arylation of acidic sp2 CH bonds under heterogeneous Ni-MOF-74 catalysis: Synthesis of bioactive azole derivatives","authors":"Huong T.T. Nguyen,&nbsp;Duc N.A. Doan,&nbsp;Thanh Truong","doi":"10.1016/j.molcata.2016.11.009","DOIUrl":"https://doi.org/10.1016/j.molcata.2016.11.009","url":null,"abstract":"<div><p>Herein, nickel-based metal-organic framework, Ni-MOF-74, was synthesized by a solvothermal method and its properties was characterized by a host of techniques. Ni-MOF-74 exhibited exceptional catalytic activity toward the direct arylation of azoles via C<img>H activation while other Ni-MOFs, nickel-based heterogeneous systems, and homogeneous counter parts displayed lower activity. Optimal conditions involved the use of Li<sub>2</sub>CO<sub>3</sub> or KCl salts in diglyme solvent in 18<!--> <!-->h and no additional ligand is required. This is the first and unprecedented report using KCl salt as promoter for arylation of heterocycles. By avoiding the use of strong bases and oxidants, optimized conditions are compatible with wide range of functional groups and heterocycles. Furthermore, by taking advantage of large aperture size of Ni-MOF-74, we are able to utilize optimized conditions to successfully synthesize several bioactive arylated azole derivatives. Previous studies using heterogeneous catalysts to approach these bioactive compounds are not performed in the literature. Leaching tests indicated that homogeneous catalysis via leached active nickel species is unlikely. Thus, the catalyst was facilely separated from the reaction mixture and reused several times without significant degradation of the catalytic reactivity.</p></div>","PeriodicalId":370,"journal":{"name":"Journal of Molecular Catalysis A: Chemical","volume":"426 ","pages":"Pages 141-149"},"PeriodicalIF":5.062,"publicationDate":"2017-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.molcata.2016.11.009","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"2595835","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: 34
The influence of multiwalled carbon nanotubes and graphene oxide additives on the catalytic activity of 3d metal catalysts towards 1-phenylethanol oxidation 多壁碳纳米管和氧化石墨烯添加剂对三维金属催化剂对1-苯乙醇氧化活性的影响
IF 5.062
Journal of Molecular Catalysis A: Chemical Pub Date : 2017-01-01 DOI: 10.1016/j.molcata.2016.07.015
Ana Paula C. Ribeiro , Emmanuele Fontolan , Elisabete C.B.A. Alegria , Maximilian N. Kopylovich , Roberta Bertani , Armando J.L. Pombeiro
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引用次数: 13
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