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The interaction of carbon monoxide with nickel—iron alloys. A comparison between single crystal surfaces and supported catalysts 一氧化碳与镍铁合金的相互作用。单晶表面与负载型催化剂的比较
Journal of Molecular Catalysis Pub Date : 1994-09-13 DOI: 10.1016/0304-5102(94)00081-6
E. Boellaard , R.J. Vreeburg, O.L.J. Gijzeman, J.W. Geus
{"title":"The interaction of carbon monoxide with nickel—iron alloys. A comparison between single crystal surfaces and supported catalysts","authors":"E. Boellaard ,&nbsp;R.J. Vreeburg,&nbsp;O.L.J. Gijzeman,&nbsp;J.W. Geus","doi":"10.1016/0304-5102(94)00081-6","DOIUrl":"10.1016/0304-5102(94)00081-6","url":null,"abstract":"<div><p>The interaction of carbon monoxide with nickel—iron alloys is studied on Ni(111)-Fe surfaces by means of ellipsometry and Auger electron spectroscopy, and by means of infrared spectroscopy on γ-Al<sub>2</sub>O<sub>3</sub>-supported Ni<sub><em>x</em></sub>Fe catalysts. The nickel-to-iron ratio of the alloy strongly affects the interaction with CO. On alloys with an iron atom fraction of 0.3 or less the adsorption of CO is molecular, whereas at fractions higher than 0.4 it is initially dissociative. Surfaces contaminated with carbon and oxygen exhibit a lower heat of adsorption. The presence of pre-adsorbed hydrogen lowers the amount of CO which can be adsorbed on Ni(111)-Fe surfaces, whereas on supported catalysts it leads to the formation of formate species already at room temperature.</p></div>","PeriodicalId":16567,"journal":{"name":"Journal of Molecular Catalysis","volume":"92 3","pages":"Pages 299-310"},"PeriodicalIF":0.0,"publicationDate":"1994-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/0304-5102(94)00081-6","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"81267917","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: 16
NMR at elevated gas pressures and its application to homogeneous catalysis 高气压下的核磁共振及其在均相催化中的应用
Journal of Molecular Catalysis Pub Date : 1994-09-13 DOI: 10.1016/0304-5102(94)00084-0
C.J. Elsevier
{"title":"NMR at elevated gas pressures and its application to homogeneous catalysis","authors":"C.J. Elsevier","doi":"10.1016/0304-5102(94)00084-0","DOIUrl":"10.1016/0304-5102(94)00084-0","url":null,"abstract":"<div><p>A selection of topics dealing with instrumentation and applications of NMR under high pressure of gases is presented, with emphasis on some recent advances in mechanistic studies of homogeneous hydrogenation and carbonylation reactions carried out in the laboratory of the author.</p></div>","PeriodicalId":16567,"journal":{"name":"Journal of Molecular Catalysis","volume":"92 3","pages":"Pages 285-297"},"PeriodicalIF":0.0,"publicationDate":"1994-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/0304-5102(94)00084-0","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"85793220","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: 28
First report on highly efficient alkene hydrogenation catalysed by Ni(salen) complex encapsulated in zeolite 沸石包封镍(salen)配合物催化烯烃高效加氢研究首次报道
Journal of Molecular Catalysis Pub Date : 1994-09-13 DOI: 10.1016/0304-5102(94)00091-3
Debabrata Chatterjee, Hari C. Bajaj, Amitava Das, Ketan Bhatt
{"title":"First report on highly efficient alkene hydrogenation catalysed by Ni(salen) complex encapsulated in zeolite","authors":"Debabrata Chatterjee,&nbsp;Hari C. Bajaj,&nbsp;Amitava Das,&nbsp;Ketan Bhatt","doi":"10.1016/0304-5102(94)00091-3","DOIUrl":"https://doi.org/10.1016/0304-5102(94)00091-3","url":null,"abstract":"<div><p>Ni(salen) (salen = bis-(salicylidene)ethylenediamine) complex was encapsulated in zeolite Y and hydrogenations of cyclohexene, cyclooctene, 1-hexene and benzene were carried out with Ni(salen) encapsulated zeolite at moderately high temperature (40°C) and pressure (60 atm of H<sub>2</sub>).</p></div>","PeriodicalId":16567,"journal":{"name":"Journal of Molecular Catalysis","volume":"92 3","pages":"Pages L235-L238"},"PeriodicalIF":0.0,"publicationDate":"1994-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/0304-5102(94)00091-3","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136412530","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: 0
Surface organometallic chemistry on zeolites: control of the pore opening of mordenite by grafting of thermally stable GeBu3 fragments 沸石表面有机金属化学:通过接枝热稳定GeBu3片段控制丝光沸石的开孔
Journal of Molecular Catalysis Pub Date : 1994-09-13 DOI: 10.1016/0304-5102(94)00087-5
Christophe Nédez , Agnès Choplin , Judith Corker , Jean-Marie Basset , Jean-François Joly , Eric Benazzi
{"title":"Surface organometallic chemistry on zeolites: control of the pore opening of mordenite by grafting of thermally stable GeBu3 fragments","authors":"Christophe Nédez ,&nbsp;Agnès Choplin ,&nbsp;Judith Corker ,&nbsp;Jean-Marie Basset ,&nbsp;Jean-François Joly ,&nbsp;Eric Benazzi","doi":"10.1016/0304-5102(94)00087-5","DOIUrl":"https://doi.org/10.1016/0304-5102(94)00087-5","url":null,"abstract":"<div><p>GeBu<sub>4</sub> reacts at 250°C with the external silanols of two different mordenites (Si/Al = 11 or 40) to give the surface organometallic complex SiOGeBu<sub>3</sub> <strong>1</strong> which has been characterized by <sup>13</sup>C CP-MAS NMR; <strong>1</strong> is able to discriminate sterically different alkanes such as n-hexane, 2-methyl-pentane, 2,3-dimethyl butane, 2,2,4-trimethyl pentane. Such discrimination is parallel to that already observed for SiOSnBu<sub>3</sub> grafted on the same mordenites. Interestingly and in contrast to the behaviour of the grafted tin complex, <strong>1</strong> even after treatment at 400°C is still able to separate n-hexane from isooctane, a property ascribed to a steric molecular control of the Ge(Bu)<sub>3</sub> fragment which has an exceptional thermal stability.</p></div>","PeriodicalId":16567,"journal":{"name":"Journal of Molecular Catalysis","volume":"92 3","pages":"Pages L239-L244"},"PeriodicalIF":0.0,"publicationDate":"1994-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/0304-5102(94)00087-5","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"91703976","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: 4
51V NMR and EPR study of the mechanistic details of oxidation with VO(O2) (Pic) (H2O)2 VO(O2) (Pic) (H2O)2氧化机理的51V NMR和EPR研究
Journal of Molecular Catalysis Pub Date : 1994-09-13 DOI: 10.1016/0304-5102(94)00069-7
E.P. Talsi , K.V. Shalyaev
{"title":"51V NMR and EPR study of the mechanistic details of oxidation with VO(O2) (Pic) (H2O)2","authors":"E.P. Talsi ,&nbsp;K.V. Shalyaev","doi":"10.1016/0304-5102(94)00069-7","DOIUrl":"10.1016/0304-5102(94)00069-7","url":null,"abstract":"<div><p>Using <sup>51</sup>V NMR, it was shown that peroxo complex VO(O<sub>2</sub>) (Pic) (H<sub>2</sub>O)<sub>2</sub> (Pic = picolinic acid) exists in CH<sub>3</sub>CN, MeOH and H<sub>2</sub>O in the forms of VO(O<sub>2</sub>) (Pic) H<sub>2</sub>O·CH<sub>3</sub>CN, VO(O<sub>2</sub>) (Pic) H<sub>2</sub>O·MeOH and VO(O<sub>2</sub>) (Pic) (H<sub>2</sub>O)<sub>2</sub>, respectively. To elucidate the nature of reactivity of vanadium peroxo complexes Of VO(O<sub>2</sub>) (Pic) H<sub>2</sub>O·S family towards hydrocarbons their interactions with spin trap 3,3,5,5-tetramethyl-pyrroline-<em>N</em>-oxide (TMPO) were investigated by EPR. Only the peroxo complex VO(O<sub>2</sub>) (Pic) H<sub>2</sub>O·CH<sub>3</sub>CN was reactive towards the hydrocarbons and the spin trap. This complex can abstract the β-hydrogen atom from TMPO (V<sup>V</sup> reduces to V<sup>IV</sup> by this reaction). Such hydrogen atom abstraction was not observed for the other radical species studied (free radicals OH•(HO<sub>2</sub>•), RO•(RO<sub>2</sub>•) and superoxo complex Pd<sub>3</sub>(OAc)<sub>5</sub>O<sub>2</sub>•). The latter species form with TMPO a spin adduct by addition to the double bond. The data provide evidence, that the diradical species V<sup>IV</sup>OO• are active particles of oxidation by VO(O<sub>2</sub>) (Pic) H<sub>2</sub>O·CH<sub>3</sub>CN.</p><p>Deactivation of VO(O<sub>2</sub>) (Pic) H<sub>2</sub>O·CH<sub>3</sub>CN upon substitution of CH<sub>3</sub>CN by stronger σ-donor ligands (e.g., H<sub>2</sub>O, MeOH, DMF) may be caused by prevention of electron transfer from the peroxo group to the metal to give V<sup>IV</sup>OO•. Vanadium(V) superoxo complex V<sup>V</sup>(O<sub>2</sub><sup>.−</sup>) detected by EPR in a solution of VO(O<sub>2</sub>) (Pic) (H<sub>2</sub>O)<sub>2</sub> in 30% H<sub>2</sub>O<sub>2</sub>was inert towards alkenes and spin traps.</p></div>","PeriodicalId":16567,"journal":{"name":"Journal of Molecular Catalysis","volume":"92 3","pages":"Pages 245-255"},"PeriodicalIF":0.0,"publicationDate":"1994-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/0304-5102(94)00069-7","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"84245506","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
A kinetic model for the pectin hydrolysis using an endo-acting pectinase from Rhizopus 根霉内作用果胶酶水解果胶的动力学模型
Journal of Molecular Catalysis Pub Date : 1994-09-13 DOI: 10.1016/0304-5102(94)00076-X
S. Todisco, V. Calabrò, G. Iorio
{"title":"A kinetic model for the pectin hydrolysis using an endo-acting pectinase from Rhizopus","authors":"S. Todisco,&nbsp;V. Calabrò,&nbsp;G. Iorio","doi":"10.1016/0304-5102(94)00076-X","DOIUrl":"https://doi.org/10.1016/0304-5102(94)00076-X","url":null,"abstract":"<div><p>Enzyme kinetics of pectin hydrolysis reaction catalysed by an <em>endo</em>-polygalacturonase from <em>Rhizopus</em> have been analysed experimentally in a stirred batch reactor at pH=4.5 and <em>T</em>=34°C using a sodium salt of polygalacturonic acid as substrate. The reaction products, consisting of oligomers of galacturonic acid, were classified in four classes of oligomeric fractions employing three hollow fibre ultrafiltration units characterised by different molecular weight cut-off (<em>MW</em><sub>co</sub>). On the basis of the time-concentration data, a kinetic model of the reacting system has been proposed in terms of a series-side reaction pattern. Identification of kinetic parameters was carried out by a non-linear regression optimization procedure based on the Powell's algorithm of conjugated directions. Finally, the kinetic model was used to predict the best reactor configuration able to control the product distribution for a given enzyme/substrate concentration ratio.</p></div>","PeriodicalId":16567,"journal":{"name":"Journal of Molecular Catalysis","volume":"92 3","pages":"Pages 333-346"},"PeriodicalIF":0.0,"publicationDate":"1994-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/0304-5102(94)00076-X","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"91703978","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: 6
Highly efficient oxygen transfer from tert-butyl hydroperoxide to benzylic carbons catalyzed by chromium(VI) oxide under high substrate/ hydroperoxide ratios 在高底物/过氧化氢比下，氧化铬催化过氧化氢叔丁基向苯碳的高效氧转移
Journal of Molecular Catalysis Pub Date : 1994-09-13 DOI: 10.1016/0304-5102(94)00082-4
Jacques Muzart, Abdelaziz N'Ait Ajjou
{"title":"Highly efficient oxygen transfer from tert-butyl hydroperoxide to benzylic carbons catalyzed by chromium(VI) oxide under high substrate/ hydroperoxide ratios","authors":"Jacques Muzart,&nbsp;Abdelaziz N'Ait Ajjou","doi":"10.1016/0304-5102(94)00082-4","DOIUrl":"https://doi.org/10.1016/0304-5102(94)00082-4","url":null,"abstract":"<div><p>Chromium(VI) oxide induces a quasi-quantitative transfer of one oxygen atom from <em>t</em>-BuOOH to a benzylic methylene group when a high ratio of substrate/hydroperoxide is employed, the corresponding carbonyl compound being the major oxidation compound. Hydroxylation and <em>tert</em>-butyl-peroxidation are the main reactions observed for a tertiary benzylic carbon. The interference of free benzylic radicals under these conditions is a minor reactive pathway.</p></div>","PeriodicalId":16567,"journal":{"name":"Journal of Molecular Catalysis","volume":"92 3","pages":"Pages 277-283"},"PeriodicalIF":0.0,"publicationDate":"1994-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/0304-5102(94)00082-4","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"91703979","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: 12
Photocatalytic degradation of chlorophenols to CO2 and HCl with polyoxotungstates in aqueous solution 多氧钨酸盐光催化降解氯酚成CO2和HCl的研究
Journal of Molecular Catalysis Pub Date : 1994-09-13 DOI: 10.1016/0304-5102(94)00083-2
A. Mylonas, E. Papaconstantinou
{"title":"Photocatalytic degradation of chlorophenols to CO2 and HCl with polyoxotungstates in aqueous solution","authors":"A. Mylonas,&nbsp;E. Papaconstantinou","doi":"10.1016/0304-5102(94)00083-2","DOIUrl":"https://doi.org/10.1016/0304-5102(94)00083-2","url":null,"abstract":"<div><p>Homogeneous oxygenated aqueous solutions of chlorophenols, undergo photodegradation (λ &gt; 320 nm) to CO<sub>2</sub> and Cl<sup>−</sup> by polyoxometalates W<sub>10</sub>O<sup>4−</sup><sub>32</sub>, PW<sub>12</sub>O<sup>3−</sup><sub>40</sub>, and SiW<sub>12</sub>O<sup>4−</sup><sub>40</sub>. Mineralization takes place, also, in the absence of dioxygen but the process is more than an order of magnitude slower. In presence of dioxygen the effectiveness of these catalysts compares with TiO<sub>2</sub> suspension.</p></div>","PeriodicalId":16567,"journal":{"name":"Journal of Molecular Catalysis","volume":"92 3","pages":"Pages 261-267"},"PeriodicalIF":0.0,"publicationDate":"1994-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/0304-5102(94)00083-2","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"90022049","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: 61
FTIR studies of CO chemisorption and reactivity on Rh/SiO2 catalysts promoted by niobium oxide 氧化铌促进的Rh/SiO2催化剂上CO的化学吸附和反应性的FTIR研究
Journal of Molecular Catalysis Pub Date : 1994-08-30 DOI: 10.1016/0304-5102(94)00072-7
O.S. Alekseev , T. Beutel , E.A. Paukshtis , Yu.A. Ryndin , V.A. Likholobov , H. Knözinger
{"title":"FTIR studies of CO chemisorption and reactivity on Rh/SiO2 catalysts promoted by niobium oxide","authors":"O.S. Alekseev ,&nbsp;T. Beutel ,&nbsp;E.A. Paukshtis ,&nbsp;Yu.A. Ryndin ,&nbsp;V.A. Likholobov ,&nbsp;H. Knözinger","doi":"10.1016/0304-5102(94)00072-7","DOIUrl":"10.1016/0304-5102(94)00072-7","url":null,"abstract":"<div><p>(Rh + Nb)/SiO<sub>2</sub> catalysts were obtained by anchoring of nanometer size Rh particles on surface low-valent Nb<sup><em>n</em> +</sup> ions. These materials exhibit the following specific features compared to Rh/SiO<sub>2</sub>: a low Rh surface coverage by chemisorbed hydrogen and carbon oxide; a high-frequency shift of linear CO absorption band and appearance of two absorption bands of a C- and O-bonded CO at 1704 and 1652 cm<sup>−1</sup>. On exposure to H<sub>2</sub>, the stability of surface carbonyls increases in the sequence: Rh-CO-Nb<sup><em>n</em> +</sup> &lt; Rh-CO ≤ Rh<sub>2</sub>(CO) &lt; Rh<sup>+</sup>(CO)<sub>2</sub>. The possible role of C- and O-bonded CO complexes in the conversion of syngas on supported rhodium catalysts promoted by transition element oxides is discussed.</p></div>","PeriodicalId":16567,"journal":{"name":"Journal of Molecular Catalysis","volume":"92 2","pages":"Pages 217-233"},"PeriodicalIF":0.0,"publicationDate":"1994-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/0304-5102(94)00072-7","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"87343101","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
Alkylation of isobutane with 2-butene using 1-butyl-3-methylimidazolium chloride—aluminium chloride molten salts as catalysts 1-丁基-3-甲基咪唑氯化铝熔盐催化异丁烷与2-丁烯的烷基化反应
Journal of Molecular Catalysis Pub Date : 1994-08-30 DOI: 10.1016/0304-5102(94)00065-4
Yves Chauvin , André Hirschauer, Hélène Olivier
{"title":"Alkylation of isobutane with 2-butene using 1-butyl-3-methylimidazolium chloride—aluminium chloride molten salts as catalysts","authors":"Yves Chauvin ,&nbsp;André Hirschauer,&nbsp;Hélène Olivier","doi":"10.1016/0304-5102(94)00065-4","DOIUrl":"10.1016/0304-5102(94)00065-4","url":null,"abstract":"<div><p>Isobutane was alkylated with 2-butene, in batchwise conditions, using liquid 1-butyl-3-methylimidazolium chloride—aluminium chloride molten salts as the acidic catalyst. The effect of the operating variables on the product composition has been investigated. The control of the acidity of the catalyst has made possible the production of a high quality alkylate.</p></div>","PeriodicalId":16567,"journal":{"name":"Journal of Molecular Catalysis","volume":"92 2","pages":"Pages 155-165"},"PeriodicalIF":0.0,"publicationDate":"1994-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/0304-5102(94)00065-4","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"85566328","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: 121
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