{"title":"Synthesis of nanoporous copper terephthalate [MIL-53(Cu)] as a novel methane-storage adsorbent","authors":"Mansoor Anbia, Sara Sheykhi","doi":"10.1016/S1003-9953(11)60419-2","DOIUrl":"10.1016/S1003-9953(11)60419-2","url":null,"abstract":"<div><p>Copper (II) dicarboxylate, MIL-53, metal-organic framework synthesized hydrothermally has been used for the first time as an adsorbent for methane gas adsorption. Methane adsorption capacity of MIL-53(Cu) was increased to about 8.52 mmol·g<sup>−1</sup> at 298 K and 35 bar for methane storage. The adsorbent was characterized by X-ray diffraction (XRD), Brunauer-Emmet-Teller (BET) method, Fourier transform infrared (FT-IR), thermo gravimetric analysis (TGA) and scanning electron microscopy (SEM). The adsorption property of CH<sub>4</sub>, on MIL-53(Cu) was investigated by volumetric measurement. The enhancement of CH<sub>4</sub> adsorption capacity of MIL-53(Cu) is attributed to the increase of micropore volume of MIL-53(Cu).</p></div>","PeriodicalId":56116,"journal":{"name":"Journal of Natural Gas Chemistry","volume":"21 6","pages":"Pages 680-684"},"PeriodicalIF":0.0,"publicationDate":"2012-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S1003-9953(11)60419-2","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"56795332","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}
{"title":"Preparation of mesoporous activated carbons from coal liquefaction residue for methane decomposition","authors":"Jianbo Zhang, Lijun Jin, Shengwei Zhu, Haoquan Hu","doi":"10.1016/S1003-9953(11)60429-5","DOIUrl":"10.1016/S1003-9953(11)60429-5","url":null,"abstract":"<div><p>Mesoporous activated carbons were prepared from direct coal liquefaction residue (CLR) by KOH activation method, and the experiments were carried out to investigate the effects of KOH/CLR ratio, solvent for mixing the CLR and KOH, and carbonization procedure on the resultant carbon texture and catalytic activity for catalytic methane decomposition (CMD). The results showed that optimal KOH/CLR ratio of 2: 1; solvent with higher solubility to KOH or the CLR, and an appropriate carbonization procedure are conductive to improving the carbon pore structure and catalytic activity for CMD. The resultant mesoporous carbons show higher and more stable activity than microporous carbons. Additionally, the relationship between the carbon textural properties and the catalytic activity for CMD was also discussed.</p></div>","PeriodicalId":56116,"journal":{"name":"Journal of Natural Gas Chemistry","volume":"21 6","pages":"Pages 759-766"},"PeriodicalIF":0.0,"publicationDate":"2012-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S1003-9953(11)60429-5","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"56796314","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}
{"title":"Adsorptive desulfurization over hierarchical beta zeolite by alkaline treatment","authors":"Fuping Tian, Xiaojian Yang, Yanchun Shi, Cuiying Jia, Yongying Chen","doi":"10.1016/S1003-9953(11)60414-3","DOIUrl":"10.1016/S1003-9953(11)60414-3","url":null,"abstract":"<div><p>Hierarchical beta zeolites with SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> molar ratios of 16 to 25 were obtained by alkaline treatment in NaOH solution. The effects of treatment temperature on crystallinity, textural properties and chemical composites were studied by XRD, N<sub>2</sub> sorption, FT-IR and XRF techniques. The desulfurization performance of parent and alkaline-treated beta zeolites was investigated by static absorption in four model fuels, containing four sulfur compounds of different molecular sizes like thiophene (TP), 3-methylthiophene (3-MT), benzothiophene (BT) and dibenzothiophene (DBT), respectively. The crystallinity was observed to be successfully maintained when the treatment temperature was below 50 °C. Mesoporosity of beta zeolite was evidently developed with alkaline treatment. The formation of mesopore remarkably improved the desulfurization performance for TP, 3-MT, BT and DBT, especially for DBT with larger molecular diameter. Though the addition of toluene in the model fuels resulted in a significant drop of the desulfurization performance of mesoporous beta zeolite, the introduction of cerium ions to some extent mitigated the effect of toluene, which means that both the adsorbents porous structure and the adsorption mode are responsible for the desulfurization performance. The adsorbent of cerium ion-exchanged mesoporous beta showed about 80% recovery of desulfurization after the first regeneration.</p></div>","PeriodicalId":56116,"journal":{"name":"Journal of Natural Gas Chemistry","volume":"21 6","pages":"Pages 647-652"},"PeriodicalIF":0.0,"publicationDate":"2012-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S1003-9953(11)60414-3","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"56795029","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}
Jianguo Liu, Yizan Zuo, Minghan Han, Zhanwen Wang, Dezheng Wang
{"title":"Stability improvement of the Nieuwland catalyst in the dimerization of acetylene to monovinylacetylene","authors":"Jianguo Liu, Yizan Zuo, Minghan Han, Zhanwen Wang, Dezheng Wang","doi":"10.1016/S1003-9953(11)60396-4","DOIUrl":"10.1016/S1003-9953(11)60396-4","url":null,"abstract":"<div><p>In the process of dimerization of acetylene to produce monovinylacetylene (MVA), the loss of active component CuCl in the Nieuwland catalyst due to the formation of a dark red precipitate was investigated. The formula of the precipitate was CuCl·2C<sub>2</sub>H<sub>2</sub>·1/5NH<sub>3</sub>, and it was presumed to be formed by the combination of NH<sub>3</sub>, C<sub>2</sub>H<sub>2</sub> and [Cu]-acetylene <em>p</em>-complex, which was an intermediate in the dimerization reaction. The addition of hydrochloric acid into the catalyst can reduce the formation of precipitate, whereas excessive H<sup>+</sup> is unfavorable to the dimerization reaction of acetylene. To balance between high acetylene conversion and low loss rate of CuCl, the optimum mass percentage of HCl in the added hydrochloric acid was determined. The result showed the optimum mass percentage of HCl decreased from 5.0% to 3.2% when the space velocity of acetylene was from 140 h<sup>−1</sup> to 360 h<sup>−1</sup>. The result in this work also indicated the pH of the Nieuwland catalyst should be kept in the range of 5.80–5.97 during the reaction process, which was good for both catalyst life and acetylene conversion.</p></div>","PeriodicalId":56116,"journal":{"name":"Journal of Natural Gas Chemistry","volume":"21 5","pages":"Pages 495-500"},"PeriodicalIF":0.0,"publicationDate":"2012-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S1003-9953(11)60396-4","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"56794423","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}
Bo Zhang , Shengguo Hui , Suhua Zhang , Yang Ji , Wei Li , Dingye Fang
{"title":"Effect of copper loading on texture, structure and catalytic performance of Cu/SiO2 catalyst for hydrogenation of dimethyl oxalate to ethylene glycol","authors":"Bo Zhang , Shengguo Hui , Suhua Zhang , Yang Ji , Wei Li , Dingye Fang","doi":"10.1016/S1003-9953(11)60405-2","DOIUrl":"10.1016/S1003-9953(11)60405-2","url":null,"abstract":"<div><p>Cu/SiO<sub>2</sub> catalysts prepared by a convenient and efficient method using the urea hydrolysis deposition-precipitation (UHDP) technique have been proposed focusing on the effect of copper loading. The texture, structure and composition are systematically characterized by ICP, FT-IR, N<sub>2</sub>-physisorption, N<sub>2</sub>O chemisorption, TPR, XRD and XPS. The formation of copper phyllosilicate is observed in Cu/SiO<sub>2</sub> catalyst by adopting UHDP method, and the amount of copper phyllosilicate is related to copper loading. It is found the structure properties and catalytic performance is profoundly affected by the amount of copper phyllosilicate. The excellent catalytic activity is attributed to the synergetic effect between Cu<sup>0</sup> and Cu<sup>+</sup>. DMO conversion and EG selectivity are determined by the amount of Cu<sup>0</sup> and Cu<sup>+</sup>, respectively. The proper copper loading (30 wt%) provides with the highest ratio of Cu<sup>+</sup>/Cu<sup>0</sup>, giving rise to the highest EG yield of 95% under the reaction conditions of <em>p</em> = 2.0 MPa, <em>T</em> = 473 K, H<sub>2</sub>/DMO = 80 and LHSV = 1.0 h<sup>−1</sup>.</p></div>","PeriodicalId":56116,"journal":{"name":"Journal of Natural Gas Chemistry","volume":"21 5","pages":"Pages 563-570"},"PeriodicalIF":0.0,"publicationDate":"2012-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S1003-9953(11)60405-2","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"56794638","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}
Rafik Benrabaa , Hamza Boukhlouf , Axel Löfberg , Annick Rubbens , Rose-Nöelle Vannier , Elisabeth Bordes-Richard , Akila Barama
{"title":"Nickel ferrite spinel as catalyst precursor in the dry reforming of methane: Synthesis, characterization and catalytic properties","authors":"Rafik Benrabaa , Hamza Boukhlouf , Axel Löfberg , Annick Rubbens , Rose-Nöelle Vannier , Elisabeth Bordes-Richard , Akila Barama","doi":"10.1016/S1003-9953(11)60408-8","DOIUrl":"10.1016/S1003-9953(11)60408-8","url":null,"abstract":"<div><p>Dry reforming of methane by CO<sub>2</sub> using nickel ferrite as precursor of catalysts was investigated. Nickel ferrite crystalline particles were prepared by coprecipitation of nitrates with NaOH or ammonia followed by calcination, or by hydrothermal synthesis without calcination step. The textural and structural properties were determined by a number of analysis methods, including X-ray diffraction (XRD), Raman spectroscopy and X-ray photoelectron spectroscopy (XPS), among which X-ray diffraction (XRD) was at room and variable temperatures. All synthesized oxides showed the presence of micro or nanoparticles of NiFe<sub>2</sub>O<sub>4</sub> inverse spinel, but Fe<sub>2</sub>O<sub>3</sub> (hematite) was also present when ammonia was used for coprecipitation. The reducibility by hydrogen was studied by temperature-programmed reduction (TPR) and in situ XRD, which showed the influence of the preparation method. The surface area (BET), particle size (Rietveld refinement), as well as surface Ni/Fe atomic ratio (XPS) and the behavior upon reduction varied according to the synthesis method. The catalytic reactivity was investigated using isopropanol decomposition to determine the acid/base properties. The catalytic performance of methane reforming with CO<sub>2</sub> was measured with and without the pre-treatment of catalysts under H<sub>2</sub> in 650-800 °C range. The catalytic conversions of methane and CO<sub>2</sub> were quite low but they increased when the catalysts were pre-reduced. A significant contribution of reverse water gas shift reaction accounted for the low values of H<sub>2</sub>/CO ratio. No coking was observed as shown by the reoxidation step performed after the catalytic reactions. The possible formation of nickel-iron alloy observed during the study of reducibility by hydrogen was invoked to account for the catalytic behavior.</p></div>","PeriodicalId":56116,"journal":{"name":"Journal of Natural Gas Chemistry","volume":"21 5","pages":"Pages 595-604"},"PeriodicalIF":0.0,"publicationDate":"2012-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S1003-9953(11)60408-8","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"56794699","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}
{"title":"Hydrogen generation from methanolysis of sodium borohydride over Co/Al2O3 catalyst","authors":"Dongyan Xu , Lin Zhao , Ping Dai , Shengfu Ji","doi":"10.1016/S1003-9953(11)60395-2","DOIUrl":"10.1016/S1003-9953(11)60395-2","url":null,"abstract":"<div><p>Co/Al<sub>2</sub>O<sub>3</sub> catalyst is prepared with an impregnation-chemical reduction method and used to catalyze the methanolysis of sodium borohydride (NaBH<sub>4</sub>) for hydrogen generation. At solution temperature of 0 °C, the methanolysis reaction can be effectively accelerated using Co/Al<sub>2</sub>O<sub>3</sub> catalyst and provide a desirable hydrogen generation rate, which makes it suitable for applications under the circumstance of low environmental temperature. The byproduct of methanolysis reaction is analyzed by X-ray diffraction (XRD) and Fourier transform infrared spectroscopy (FTIR). The characterization results indicate that methanol can be easily recovered after methanolysis reaction by hydrolysis of the methanolysis byproduct, NaB(OCH<sub>3</sub>)<sub>4</sub>. The catalytic activity of Co/Al<sub>2</sub>O<sub>3</sub> towards NaBH<sub>4</sub> methanolysis can be further improved by appropriate calcination treatment. The catalytic methanolysis kinetics and catalyst reusability are also studied over the Co/Al<sub>2</sub>O<sub>3</sub> catalyst calcined at the optimized temperature.</p></div>","PeriodicalId":56116,"journal":{"name":"Journal of Natural Gas Chemistry","volume":"21 5","pages":"Pages 488-494"},"PeriodicalIF":0.0,"publicationDate":"2012-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S1003-9953(11)60395-2","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"56794285","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}
{"title":"Initial estimation of hydrate formation temperature of sweet natural gases based on new empirical correlation","authors":"Mohammad Mahdi Ghiasi","doi":"10.1016/S1003-9953(11)60398-8","DOIUrl":"10.1016/S1003-9953(11)60398-8","url":null,"abstract":"<div><p>Production, processing and transportation of natural gases can be significantly affected by clathrate hydrates. Knowing the gas analysis is crucial to predict the right conditions for hydrate formation. Nevertheless, Katz gas gravity method can be used for initial estimation of hydrate formation temperature (HFT) under the circumstances of indeterminate gas composition. So far several correlations have been proposed for gas gravity method, in which the most accurate and reliable one has belonged to Bahadori and Vuthaluru. The main objective of this study is to present a simple and yet accurate correlation for fast prediction of sweet natural gases HFT based on the fit to Katz gravity chart. By reviewing the error analysis results, one can discover that the new proposed correlation has the best estimation capability among the widely accepted existing correlations within the investigated range.</p></div>","PeriodicalId":56116,"journal":{"name":"Journal of Natural Gas Chemistry","volume":"21 5","pages":"Pages 508-512"},"PeriodicalIF":0.0,"publicationDate":"2012-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S1003-9953(11)60398-8","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"56794760","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}
{"title":"Preparation and characterization of vanadium(IV) oxide supported on SBA-15 and its catalytic performance in benzene hydroxylation to phenol using molecular oxygen","authors":"Xing Chen , Wenguang Zhao , Feng Wang , Jie Xu","doi":"10.1016/S1003-9953(11)60394-0","DOIUrl":"10.1016/S1003-9953(11)60394-0","url":null,"abstract":"<div><p>Preparation of dispersed transition metal oxides catalyst with low oxidation state still remains a challenging task in heterogeneous catalysis. In this study, vanadium oxides supported on zeolite SBA-15 have been prepared under hydrothermal condition using V<sub>2</sub>O<sub>5</sub> and oxalic acid as sources of vanadium and reductant, respectively. The structures of samples, especially the oxidation state of vanadium, and the surface distribution of vanadium oxide species, have been thoroughly characterized using various techniques, including N<sub>2</sub>-physisorption, X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), UV-visible spectra (UV-Vis) and UV-visible-near infrared spectra (UV-Vis-NIR). It is found that the majority of supported vanadium was in the form of vanadium(IV) oxide species with the low valence of vanadium. By adjusting hydrothermal treatment time, the surface distribution of vanadium(IV) oxide species can be tuned from vanadium(IV) oxide cluster to crystallites. These materials have been tested in the hydroxylation of benzene to phenol in liquid-phase with molecular oxygen in the absence of reductant. The catalyst exhibits high selectivity for phenol (61%) at benzene conversion of 4.6%, which is a relatively good result in comparison with other studies employing molecular oxygen as the oxidant.</p></div>","PeriodicalId":56116,"journal":{"name":"Journal of Natural Gas Chemistry","volume":"21 5","pages":"Pages 481-487"},"PeriodicalIF":0.0,"publicationDate":"2012-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S1003-9953(11)60394-0","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"56794113","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}
{"title":"Oxidative reforming of methane for hydrogen and synthesis gas production: Thermodynamic equilibrium analysis","authors":"Antonio C.D. Freitas, Reginaldo Guirardello","doi":"10.1016/S1003-9953(11)60406-4","DOIUrl":"10.1016/S1003-9953(11)60406-4","url":null,"abstract":"<div><p>A thermodynamic analysis of methane oxidative reforming was carried out by Gibbs energy minimization (at constant pressure and temperature) and entropy maximization (at constant pressure and enthalpy) methods, to determine the equilibrium compositions and equilibrium temperatures, respectively. Both cases were treated as optimization problems (non-linear programming formulation). The GAMS® 23.1 software and the CONOPT2 solver were used in the resolution of the proposed problems. The hydrogen and syngas production were favored at high temperatures and low pressures, and thus the oxygen to methane molar ratio (O<sub>2</sub>/CH<sub>4</sub>) was the dominant factor to control the composition of the product formed. For O<sub>2</sub>/CH<sub>4</sub> molar ratios higher than 0.5, the oxidative reforming of methane presented autothermal behavior in the case of either utilizing O<sub>2</sub> or air as oxidant agent, but oxidation reaction with air possessed the advantage of avoiding peak temperatures in the system, due to change in the heat capacity of the system caused by the addition of nitrogen. The calculated results were compared with previously published experimental and simulated data with a good agreement between them.</p></div>","PeriodicalId":56116,"journal":{"name":"Journal of Natural Gas Chemistry","volume":"21 5","pages":"Pages 571-580"},"PeriodicalIF":0.0,"publicationDate":"2012-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S1003-9953(11)60406-4","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"93383391","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}