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1.
Chunfei Wu 《Fuel》2010,89(10):3022-11821
Polypropylene, polystyrene, high density polyethylene and their mixtures and real-world plastic waste were investigated for the production of hydrogen in a two-stage pyrolysis-gasification reactor. The experiments were carried out at gasification temperatures of 800 or 850 °C with or without a Ni-Mg-Al catalyst. The influence of plastic type on the product distribution and hydrogen production in relation to process conditions were investigated. The reacted Ni-Mg-Al catalysts were analyzed by temperature-programmed oxidation and scanning electron microscopy. The results showed that lower gas yield (11.2 wt.% related to the mass of plastic) was obtained for the non-catalytic non-steam pyrolysis-gasification of polystyrene at the gasification temperature of 800 °C, compared with the polypropylene (59.6 wt.%) and high density polyethylene (53.5 wt.%) and waste plastic (45.5 wt.%). In addition, the largest oil product was observed for the non-catalytic pyrolysis-gasification of polystyrene. The presence of the Ni-Mg-Al catalyst greatly improved the steam pyrolysis-gasification of plastics for hydrogen production. The steam catalytic pyrolysis-gasification of polystyrene presented the lowest hydrogen production of 0.155 and 0.196 (g H2/g polystyrene) at the gasification temperatures of 800 and 850 °C, respectively. More coke was deposited on the catalyst for the pyrolysis-gasification of polypropylene and waste plastic compared with steam catalytic pyrolysis-gasification of polystyrene and high density polyethylene. Filamentous carbons were observed for the used Ni-Mg-Al catalysts from the pyrolysis-gasification of polypropylene, high density polyethylene, waste plastic and mixed plastics. However, the formation of filamentous carbons on the coked catalyst from the pyrolysis-gasification of polystyrene was low.  相似文献   

2.
Chunfei Wu 《Fuel》2010,89(7):1435-1441
A novel Ni-Mg-Al-CaO catalyst/sorbent has been prepared by integration of the catalytic and CO2 absorbing properties of the material to maximise the production of hydrogen. The prepared catalyst was tested for hydrogen production from the pyrolysis-gasification of polypropylene by using a two-stage fixed-bed reaction system. X-ray diffraction (XRD), thermogravimetric analysis (TGA) and scanning electron microscopy (SEM)-energy dispersive X-ray spectrometry (EDXS) were used to characterize the prepared Ni-Mg-Al-CaO catalyst/sorbent. Ni-Mg-Al-CaO and calcined dolomite showed a stable carbonation conversion after several cycles of carbonation/calcination, while CaO showed a certain degree of decay. The calcined dolomite showed low efficiency for hydrogen production from pyrolysis-gasification of polypropylene. Increasing the gasification temperature resulted in a decrease of H2/CO ratio for the Ni-Mg-Al catalyst mixed with sand; however, a stable H2/CO ratio (around 3.0) was obtained for the Ni-Mg-Al-CaO catalyst. An increased Ni-Mg-Al-CaO catalyst/polypropylene ratio promoted the production of hydrogen from the pyrolysis-gasification of polypropylene. Approximately 70 wt.% of the potential H2 production was obtained, when the Ni-Mg-Al-CaO catalyst/polypropylene ratio and gasification temperature were 5 and 800 °C, respectively.  相似文献   

3.
The gasification of organics in supercritical water is a promising method for the direct production of hydrogen at high pressures, and in order to improve the hydrogen yield or selectivity, activities of various catalysts are evaluated. In this study, hydrogen production from 2-propanol over Ni/Al2O3 and Fe–Cr catalysts was investigated in supercritical water. The experiments were carried out in the temperature range of 400–600 °C and in the reaction time range of 10–30 s, under a pressure of 25 MPa. The hydrogen yields and selectivities of Ni/Al2O3 and Fe–Cr used in this study, and those of Pt/Al2O3 and Ru/Al2O3 used in our previous work were compared. The hydrogen contents of the gaseous products obtained by using Ni/Al2O3 and Fe–Cr were measured as 62 mol% and 70 mol%, respectively, at low temperatures and reaction times. However, the hydrogen yields remained in low levels when compared with that of Pt/Al2O3 used in previous study. Pt/Al2O3 was established to be the most effective and selective catalyst for hydrogen production. During the catalytic gasification of a 0.5 M solution of 2-propanol, hydrogen content up to 96 mol% and hydrogen yield of 1.05 mol/mol 2-propanol were obtained.  相似文献   

4.
A bubbling fluidized‐bed gasification system was selected for catalytic steam gasification of rice straw with four Ni‐based catalysts, i.e., Ni/Al2O3, Ni/CeO2, Ni/MnO2, and Ni/MgO. The effect of temperature, steam/biomass ratio (S/B), and catalyst/biomass ratio (C/B) on the gas composition, char conversion, and hydrogen yield was evaluated. It was found that higher temperature and S/B promote hydrogen production and char conversion. The results also demonstrated that the catalytic activity of Ni/Al2O3 under different S/B values is better than those of the other catalysts. Regarding the catalyst activity, all four catalysts exhibited good performance in terms of tar removal and carbon conversion. However, the performance of Ni/Al2O3 was superior to that of the other three catalysts.  相似文献   

5.
Catalytic gasification of waste motor oil (MO) for the generation of high purity of hydrogen and then integrated to a proton exchange membrane fuel cell (PEMFC) is economically and environmentally attractive. Thus, the objective of the present work was to investigate a MO catalytic gasification for generating high-purity hydrogen with 15 wt.% NiO/Al2O3 catalysts. In a lab-scale fixed-bed downdraft experimental approach, catalytic gasification of MO was accompanied by a substantial production of syngas at 760–900 K. From the XANES spectra, most of the Ni(II) reduced to Ni(0) was found in the MO catalytic gasification process. The EXAFS data also showed that the central Ni atoms have a Ni–O and a Ni–Ni with bond distances of 2.04 ± 0.05 Å and 2.48 ± 0.05 Å, respectively. In addition to over 85% of syngas generation, approximately 8.35 × 105 kcal h−1 of thermal energy was recovered and cold gas efficiency (CGE) was 77–84% when the catalytic gasifier was operated at O/C atomic ratios between 1.1 and 1.3. The proposed syngas production unit can be integrated in a fuel processor (e.g. PEMFC), in order to separate and purify the syngas to yield a 99.99% hydrogen stream. Moreover, cost or benefit analyses of MO catalytic gasifiers of 10- and 20-TPD (tons per day) were also performed.  相似文献   

6.
Hydrogen production by partial oxidation and steam reforming (POSR) of n‐octane was investigated over alumina‐supported Ni and Ni‐Pd catalysts. It showed that Ni‐Pd/Al2O3 had higher activity and hydrogen selectivity than the nickel catalyst under the experimental conditions, which indicated Ni‐Pd/Al2O3 could be an effective catalyst for the production of hydrogen from hydrocarbons.  相似文献   

7.
The reforming process of gasoline is an attractive technique for fuel processor or hydrogen station applications. We investigated catalytic autothermal reforming (ATR) of iso-octane and toluene over transition metal supported catalysts. The catalysts were prepared by an incipient wetness impregnation method and characterized by N2 physisorption, XRD, and TEM techniques before and after the reaction. Many of the tested catalysts displayed reasonably good activity towards the reforming reactions of iso-octane. Especially, Ni/Fe/MgO/Al2O3 catalyst showed more activity than the other catalysts tested in this study including commercial HT catalyst. Ni/Fe/MgO/Al2O3 catalyst showed good stability for 700 h in the ATR of iso-octane. No major change was observed in catalytic activity in ATR of iso-octane or in the structure of catalyst. Since iso-octane, toluene are surrogates of gasoline, Ni/Fe/MgO/Al2O3 catalyst can be considered as ATR catalyst for gasoline fuel processor and hydrogen station systems.  相似文献   

8.
Catalytic steam reforming of bio-oil was investigated in a fixed bed tubular reactor for production of hydrogen. Two series of nickel/alumina (Ni/Al2O3) supported catalysts promoted with ruthenium (Ru) and magnesium (Mg) were prepared. Each catalyst of the first series (Ru–Ni/Al2O3) was prepared by co-impregnation of nickel and ruthenium on alumina. They were examined to investigate the effect of adding ruthenium on the performance of the catalysts for hydrogen production. The effect of the temperature, the most effective parameter in the steam reforming of bio-oil, on the activity of the catalysts was also investigated. Each catalyst of the second series (Ni–MgO/Al2O3) was prepared by consecutive impregnation using various preparation procedures. They were tested to determine the effect of adding magnesium as well as the effect of the preparation procedure on the outlet gas concentrations. It was shown that in both series, the catalysts were more efficient in hydrogen production as well as carbon conversion than Ni/Al2O3 catalysts. The highest hydrogen yield was 85% which was achieved over Ru–Ni/Al2O3 at 950 °C. It was also found that the effect of adding a small amount of ruthenium was superior to that of nickel on the yield of hydrogen when the nickel content was equal to or greater than 10.7%.  相似文献   

9.

Abstract  

PtNi bimetallic and Ni monometallic catalysts supported on HY–Al2O3, HX–Al2O3, ZSM-5–Al2O3, USY–Al2O3, Beta–Al2O3 and Al2O3 were prepared and evaluated for the hydrogenation of maleic anhydride in the temperature range of 40–150 °C. Results from flow reactor studies showed that supports strongly affected the catalytic properties of different bimetallic and monometallic catalysts. The results showed that the HY–Al2O3 support exhibited the highest activity and selectivity. Using NiPt/Al2O3–HY catalyst and performing the reaction, it was possible to carry out the lowest reaction temperature ever carried at 100% conversion. Adding a small amount of Pt (0.5) to the Ni (5%)/Al2O3–HY catalyst that is effective for increasing the selectivity and activity. We also found that PtNi is an efficient catalyst for the one-pot conversion of maleic acid into succinic acid with 100% conversion at 40 °C.  相似文献   

10.
More than 130 Pt and Pd bimetallic catalysts were screened for hydrogen production by aqueous-phase reforming (APR) of ethylene glycol solutions using a high-throughput reactor. Promising catalysts were characterized by CO chemisorption and tested further in a fixed bed reactor. Bimetallic PtNi, PtCo, PtFe and PdFe catalysts were significantly more active per gram of catalyst and had higher turnover frequencies for hydrogen production (TOFH2) than monometallic Pt and Pd catalysts. The PtNi/Al2O3 and PtCo/Al2O3 catalysts, with Pt to Co or Ni atomic ratios ranging from 1:1 to 1:9, had TOFH2 values (based on CO chemisorption uptake) equal to 2.8–5.2 min−1 at 483 K for APR of ethylene glycol solutions, compared to 1.9 min−1 for Pt/Al2O3 under similar reaction conditions. A Pt1Fe9/Al2O3 catalyst showed TOFH2 values of 0.3–4.3 min−1 at 453–483 K, about three times higher than Pt/Al2O3 under identical reaction conditions. A Pd1Fe9/Al2O3 catalyst had values of TOFH2 equal to 1.4 and 4.3 min−1 at temperatures of 453 and 483 K, respectively, and these values are 39–46 times higher than Pd/Al2O3 at the same reaction conditions. Catalysts consisting of Pd supported on high surface area Fe2O3 (Nanocat) showed the highest turnover frequencies for H2 production among those catalysts tested, with values of TOFH2 equal to 14.6, 39.1 and 60.1 min−1 at temperatures of 453, 483 and 498 K, respectively. These results suggest that the activity of Pt-based catalysts for APR can be increased by alloying Pt with a metal (Ni or Co) that decreases the strengths with which CO and hydrogen interact with the surface (because these species inhibit the reaction), thereby increasing the fraction of catalytic sites available for reaction with ethylene glycol. The activity of Pd-based catalysts for APR can be increased by adding a water-gas shift promoter (e.g. Fe2O3).  相似文献   

11.
Catalytic performance of Ni/CeO2/Al2O3 catalysts prepared by a co-impregnation and a sequential impregnation method in steam gasification of real biomass (cedar wood) was investigated. Especially, Ni/CeO2/Al2O3 catalysts prepared by the co-impregnation method exhibited higher performance than Ni/Al2O3 and Ni/CeO2/Al2O3 prepared by the sequential impregnation method, and the catalysts gave lower yields of coke and tar, and higher yields of gaseous products. The Ni/CeO2/Al2O3 catalysts were characterized by thermogravimetric analysis, temperature-programmed reduction with H2, transmission electron microscopy and extended X-ray absorption fine structure, and the results suggested that the interaction between Ni and CeO2 became stronger by the co-impregnation method than that by sequential method. Judging from both results of catalytic performance and catalyst characterization, it is found that the intimate interaction between Ni and CeO2 can play very important role on the steam gasification of biomass.  相似文献   

12.
The microstructured Pt/ZSM-5/SSMF catalysts, for hydrocracking of paraffin wax, have been developed by impregnation method to place Pt onto thin-sheet ZSM-5/SSMF composites obtained by direct growth of ZSM-5 on the sinter-locked stainless steel microfibers (SSMF). The best catalyst is the one with ZSM-5 having a SiO2/Al2O3 weight ratio of 200, delivering ~ 95% conversion with 77.5% selectivity to liquid products or 64.4% selectivity to naphtha at 280 °C. This new approach is capable of increasing the naphtha selectivity with high activity maintenance in comparison with the literature catalysts.  相似文献   

13.
A composition of Cu/ZnO/Al2O3 catalysts prepared by the impregnation method was optimized for water gas shift reaction (WGSR) coupled with CO oxidation in the reformed gas. The optimum composition of the impregnated catalyst for high WGSR activity was 5 wt.% Cu/5 wt.% ZnO/Al2O3. The optimum loading amounts of Cu and ZnO in the impregnated catalyst were smaller than those in the coprecipitated catalyst. Its catalytic activity above 200 °C was comparable to that of the conventional coprecipitated Cu/ZnO/Al2O3 catalyst. However, the activity of the impregnated Cu/ZnO/Al2O3 catalysts was significantly lowered at 150 °C, whereas no deactivation was observed for the coprecipitated catalyst at the same temperature. It was found that deactivation occurred over impregnated catalysts with H2O and/or O2 in the reaction gas; it prevented CO adsorption on the surface.  相似文献   

14.

Abstract  

To develop an efficient catalyst for steam reforming of propane, Ni/LaAlO3 catalysts were prepared by deposition precipitation, impregnation, and solvo-thermal methods, and characterized by XRD, BET, H2-TPR, elemental analyses, and TEM. Ni/Al2O3 and Ni/CeO2 catalysts were also synthesized by the solvo-thermal method for comparison. The Ni/LaAlO3 catalysts exhibited better catalytic performance than both Ni/Al2O3 and Ni/CeO2 catalysts, and activities with Ni/LaAlO3 were found to be dependent upon the preparation methods. In particular, the Ni/LaAlO3 catalyst synthesized by the solvo-thermal method exhibited the highest activity presumably because tetrahydrofuran helps distribute generated Ni nanoparticles onto the catalyst surface in a uniform fashion. In addition, the solvo-thermally prepared Ni/LaAlO3 catalyst was found to be highly stable, with its activity being maintained at least during 100 h. The observed high stability is attributed to the excellent oxygen storage capacity of LaAlO3, which was first determined by thermogravimetric methods as well as by soot oxidations in the presence of Al2O3, CeO2, and LaAlO3. Compared to the Ni/Al2O3 and Ni/CeO2 catalysts, Ni/LaAlO3 exhibited suppressed carbon formation even at lower S/C ratios due to the superior oxygen transport ability of the LaAlO3 support.  相似文献   

15.
Previous results on different catalysts revealed that methylcyclohexane underwent selective dehydrogenation to form toluene and hydrogen. This reaction system is a useful prototype model for similar systems in the chemical process and petroleum refining industries, such as hydrotreating for aromatics reduction, desulfurization, denitrogenation, reforming for aromatics reduction, dehydrocyclization, and fuel processing of liquid hydrocarbons in the generation of hydrogen feed for fuel cells. Dehydrogenation of methylcyclohexane to toluene is a method for hydrogen storage in the form of liquid organic hydrides. The efficiency of the dehydrogenation reactions and the quantity of products depend on the catalyst used. In the case of the dehydrogenation of methylcyclohexane to toluene, a metallic function, usually platinum is required as the catalyst. Although, there were some different catalysts used by former researchers, there was almost no investigation about the use of the nickel catalysts for this reaction. From the economical point of view, more efficient catalysts and reaction engineering methods should be developed for these reactions.In this work dehydrogenation of methylcyclohexane was performed in a fixed-bed catalytic reactor in the temperature range of 653–713 K on prepared Ni/Al2O3 catalysts having 5, 10, 15 and 20 wt.% Ni content. The inlet flowrates of methylcyclohexane and hydrogen to the reactor were changed by keeping one of them constant in order to investigate their effects on this reaction.  相似文献   

16.
Supported-NiO catalysts were tested in the synthesis of carbon nanotubes and carbon nanofibers by catalytic decomposition of methane at 550 °C and 700 °C. Catalytic activity was characterized by the conversion levels of methane and the amount of carbons accumulated on the catalysts. Selectivity of carbon nanotubes and carbon nanofiber formation were determined using transmission electron microscopy (TEM). The catalytic performance of the supported-NiO catalysts and the types of filamentous carbons produced were discussed based on the X-ray diffraction (XRD) results and the TEM images of the used catalysts. The experimental results show that the catalytic performance of supported-NiO catalysts decreased in the order of NiO/SiO2 > NiO/HZSM-5 > NiO/CeO2 > NiO/Al2O3 at both reaction temperatures. The structures of the carbons formed by decomposition of methane were dependent on the types of catalyst supports used and the reaction temperatures conducted. It was found that Al2O3 was crucial to the dispersion of smaller NiO crystallites, which gave rise to the formation of multi-walled carbon nanotubes at the reaction temperature of 550 °C and a mixture of multi-walled carbon nanotubes and single-walled carbon nanotubes at 700 °C. Other than NiO/Al2O3 catalyst, all the tested supported-NiO catalysts formed carbon nanofibers at 550 °C and multi-walled carbon nanotubes at 700 °C except for NiO/HZSM-5 catalyst, which grew carbon nanofibers at both 550 °C and 700 °C.  相似文献   

17.
The catalytic performance of a series of Pt/Al2O3 catalysts, modified with Cr, Mn, Fe, Co, Ni, Cu and Sn, has been tested for the preferential oxidation of CO in hydrogen. The promoters were deposited onto the surface of a 5 wt.% monometallic Pt/Al2O3 catalyst using a controlled surface approach, to give a nominal promoter:Pt surface atomic ratio of 1:2 (corresponding to typically 0.15–0.25 wt.% of the promoting metal). The aim of this approach was to selectively create the Pt-promoter oxide interfacial sites considered to be important for the non-competitive dual-site mechanism proposed for such promoted catalysts. In this mechanism the promoting oxide is believed to act as an active oxygen provider, providing oxygen for the oxidation of the CO on the Pt. The catalysts were characterised using TEM, EDX, ICP-AES and CO chemisorption and results suggest that the promoter was successfully deposited on to the Pt surface. Even at the low loadings of promoter used, significant enhancement was observed in the catalytic performance of the PROX reaction in a simulated reformate mixture, for the Fe- and Co-promoted catalysts in particular (and to a lesser extent the Mn, Sn, Cu- and Ni-promoted catalysts), highlighting the successful preparation of the Pt-promoting metal oxide interfacial sites. The Mn-promoted catalyst, however showed no enhancement in the absence of water suggesting that the form of the promoting metal oxide may be particularly important for promotion of Pt for the PROX reaction.  相似文献   

18.
Lignin has been gasified with a Ni/Al2O3–SiO2 catalyst in sub/supercritical water (SCW) to produce gaseous fuels. XRD pattern at 6θ angle shows characteristic peaks of crystalline NiO, NiSi, and AlNi3, suggesting that Al2O3–SiO2 not only offers high surface area (122 m2 g) for Ni, but also changes the crystal morphology of the metal. 9 mmol/g of H2 and 3.5 mmol/g of CH4 were produced at the conditions that 5.0 wt% alkaline lignin plus 1 g/g Ni/Al2O3–SiO2 operating for 30 min at 550 °C. A kinetic model was also developed, and the activation energies of gas and char formation were calculated to be 36.68 ± 0.22 and 9.0 ± 2.4 kJ/mol, respectively. Although the loss of activity surface area during reuse caused slight activity reduction in Ni/Al2O3–SiO2, the catalyst system still possessed high catalytic activity in generating H2 and CH4. It is noted that sulfur linkage could be hydrolyzed to hydrogen sulfide in the gasification process of alkaline lignin. The stable chemical states of Ni/Al2O3–SiO2 grants its insensitivity to sulfur, suggesting that Ni/Al2O3–SiO2 should be economically promising for sub/supercritical water gasification of biomass in the presence of sulfur.  相似文献   

19.
The objective of the present study was to select the optimal catalyst and operating conditions for the manufacture of C9-alcohol, using C9-aldehyde and hydrogen, in a trickle bed reactor. When CaO, Ce2O3 or MgO was added as a promoter to the Ni/kieselguhr catalyst, the BET and Ni surface areas were increased. In the reaction for the manufacture of C9-alcohol, using C9-aldehyde and hydrogen in a batch reactor, a Ni–MgO/kieselguhr catalyst showed the highest activity. In addition, the catalyst using Na2CO3 as a precipitant showed the highest activity. According to the result of an experiment to find the optimal reaction conditions for C9-alcohol synthesis, using C9-aldehyde and hydrogen in a trickle bed reactor loaded with Ni–MgO/kieselguhr catalyst, the highest yield of C9-alcohol was 91.5 wt% at 130 °C, 400 psi and WHSV = 3. The C9-aldehyde hydrogenation performance of the Ni–MgO/kieselguhr catalyst was similar to that of a Cu/ZnO/Al2O3 catalyst, but superior to that of Cu–Ni–Cr–Na/Al2O3 and Ni–Mo/Al2O3 catalysts. In a long-term catalysis test, the Ni–MgO/kieselguhr catalyst showed higher stability than the Cu/ZnO/Al2O3 catalyst.  相似文献   

20.
Iron catalysts doped with Al2O3, CaO were obtained by melting iron oxide with 2.2 wt.% of Al2O3, 2.1 wt.% of CaO. The reduced catalyst was impregnated with lithium hydroxide water solution. Activity measurements were carried out in the laboratory installation in the temperature range 623–773 K under the pressure of 10 MPa. The activity of catalyst containing 0.79 wt.% of Li2O and reduced at 773 K was similar to the activity of an industrial iron catalyst doped with potassium oxide. After reduction at 923 K the catalyst containing 0.48 wt.% of Li2O was about 15% more active than the industrial catalyst. Increasing Li2O concentration results in the decrease of the surface area of a catalyst reduced at 923 K. The most active catalysts doped with lithium oxide were more active than the industrial catalyst when their activity was calculated and scaled down to surface area units.  相似文献   

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