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1.
This work presents the study of the catalytic activity of aluminum oxide supported Co-Schiff Base complex derived from 4,4′-Methylenebis(2,6-diethylaniline)-3,5-ditertbutylsalicylaldimine-Co-Schiff Base complex in sodium borohydride hydrolysis. This catalyst is characterized with XRD, FT-IR, SEM, TEM, and BET. The respective reaction kinetics have been calculated. With the catalyst condition, maximum reaction (initial) rate is 106540 and 147193,3 mL H2/gcat..min. at 30 °C and 50 °C. For this reaction apparent activation energy is 44,7792 kJ.mol−1 with 20–50 °C. The reaction order value (n) for this catalytic system is 0,31. Additionally when Al2O3 supported Co-Schiff Base complex compared with pure Co-Schiff Base complex, the experimental results show that the aluminum oxide support exhibits enhancing effect with 106540 and 64147 mL H2/gcat. min respectively in sodium borohydride hydrolysis to Hydrogen production.  相似文献   

2.
Herein, we report an efficient, environmentally friendly and stable catalyst development to hydrogen evolution from sodium borohydride hydrolysis. For this purpose, Ruthenium complex catalyst successfully fabricated via 5-Amino-2,4-dichlorophenol-3,5-ditertbutylsalisylaldimine ligand and RuCl3·H2O salt. Ru complex catalyst was identified with X-Ray Diffraction Analysis, Infrared Spectroscopy, Elemental Analysis, Transmission electron microscopy, Scanning Electron Microscope and Brunauer-Emmett-Teller Surface Area Analysis. According to the analysis results, it was confirmed that Ru complex catalyst was successfully synthesized. Ru complex was used as a catalyst in NaBH4 hydrolysis. The kinetic performance of Ru complex catalyst was evaluated at various reaction temperatures, various sodium borohydride concentration, catalyst concentration and sodium hydroxide concentration in hydrogen evolution. The apparent activation energy for the hydrolysis of sodium borohydride was determined as 25.8 kJ mol?1. With fully conversion, the promised well durability of Ru complex was achieved by the five consecutive cycles for hydrogen evolution in sodium borohydride hydrolysis The hydrogen evolution rates were 299,220 and 160,832 mL H2 gcat?1 min?1 in order of at 50 °C and 30 °C. Furthermore, the proposed mechanism of Ru complex catalyzed sodium borohydride hydrolysis was defined step by step. This study provides different insight into the rational design and utilization and catalytic effects of ruthenium complex in hydrogen evolution performance.  相似文献   

3.
The present study focused on the increasing of hydrogen evolution through hydrolysis of potassium borohydride in the presence of Ruthenium complex catalyst. It is the first time to use the Ru-Imine complex catalyst in KBH4 hydrolysis reaction to hydrogen evolution. The new Ru complex was synthesized from the tetradentate Imine ligand namely 4,4′-methylenebis (2,6-diethyl)aniline-3,5-di-tert-butylsalisylaldimine and Ru salt under the inert atmosphere. Ru-Imine complex was fully characterized by Elemental Analysis, Infrared Spectroscopy, Scanning Electron Microscope, X-Ray Diffraction Analysis, Brunauer-Emmett-Teller Surface Area Analysis and Transmission Electron Microscopy. By the synthesized Ru-Imine complex catalyst, the potassium borohydride hydrolysis reaction resulted in a lower energy barrier with 20,826 kJ/mol activation energy (Ea) for nth order kinetic model and 18,045 kJ/mol for Langmuir-Hinshelwood (L-H) kinetic model. According to the results Ru-complex was highly active and stable catalyst in KBH4 hydrolysis reaction to hydrogen evolution with 45,466 mL H2/gcat.min and 76,815 mL H2/gcat.min hydrogen generation rates at 30 °C and 50 °C respectively. Moreover Ru-Imine complex catalyst displayed 100% stability even at fifth recycle.  相似文献   

4.
Cerium oxide supported 5-Amino-2,4-dichlorophenol-3,5-ditertbutylsalisylaldimine-Nickel complex for the first time was used to produce H2 from hydrolysis of sodium borohydride. Cerium oxide supported Nickel complex catalyzed hydrolysis system was studied depend on temperature, concentration of sodium hydroxide, amount of Cerium oxide supported Ni complex catalyst, concentration of Ni complex and concentration of sodium borohydride. Cerium oxide supported Ni(II) complex display highly effective catalytic activity in sodium borohydride hydrolysis reaction. The obtained Cerium oxide supported Ni(II) complex catalyst was characterized by using Fourier Transform Infrared Spectroscopy, Scanning Electron Microscope, Transmission Electron Microscope, Brunauer-Emmett-Teller Surface Area Analysis, X-Ray Diffraction Analysis techniques. The catalyst stability was tested, even the fifth recycle the catalytic activity was maintained at 100%. Additionally the proposed Cerium oxide supported-Ni (II) complex catalyzed sodium borohydride hydrolysis mechanism was determined carefully. The experimental results showed that Cerium oxide supported Ni (II) complex catalyst accelerate sodium borohydride hydrolysis with 43,392 and 19,630 mL H2 gcat?1 min?1 hydrogen production rates at 50 °C and 30 °C respectively and 20,587 kJ mol?1 activation energy.  相似文献   

5.
In this study, the metallurgic sludge which contained oil and was obtained as waste of grinding, sharpening and milling parts was used in the production of hydrogen (H2) from sodium borohydride (NaBH4). The hydrolysis of NaBH4 with the metallurgic sludge catalyst was investigated depending on several parameters such as sodium hydroxide (NaOH) concentration, catalyst amount, NaBH4 concentration and temperature. The obtained metallurgic sludge catalyst was characterized by the XRD, FT-IR and SEM techniques and was evaluated for its activity in the H2 generation from NaBH4 hydrolysis. The maximum H2 production rate from the hydrolysis of NaBH4 with the metallurgic sludge catalyst was calculated as 9366 ml min−1.gcat−1. The value of activation energy was found as 48.05 kJ mol−1.  相似文献   

6.
This paper reports the experimental results on using TiO2 based Cu(II)-Schiff Base complex catalyst for hydrolysis of NaBH4. In the presence of Cu-Schiff Base complex which we reported in advance [1] and with titanium dioxide supports a novel catalyst named TiO2 supported 4-4′-Methylenbis (2,6-diethyl)aniline-3,5-di-tert-buthylsalisylaldimine-Cu complex is prepared, successfully. The synthesized catalyst was characterized by means of X-Ray Diffraction (XRD), Scanning Electron Microscope (SEM), Brunauer-Emmett-Teller Surface Area Analysis (BET) and Fourier Transform Infrared Spectroscopy (FT-IR). The as prepared catalyst was employed to generate hydrogen through hydrolysis reaction of NaBH4. Effects of different parameters (e.g. amount of Cu-Schiff Base complex in all catalyst, percentage of NaBH4, percentage of NaOH, amount of TiO2 supported Cu-Schiff Base complex catalyst and different temperatures) are also investigated. A high apparent activation energy (Ea), 25,196 kJ.mol-1 is calculated for hydrolysis of NaBH4 at 20–50 °C. Hydrogen generation rate was 14,020 mL H2/gcat.min and 22,071 mL H2/gcat.min in order of 30 °C and 50 °C.  相似文献   

7.
In the present study, a cobalt-doped catalyst was prepared from chicken eggshell powder (CEP) biowaste to be used in the hydrolysis of sodium borohydride (NaBH4). In the presence of the prepared catalyst (CEPcat), possible effects of the parameters of NaOH concentration (%), catalyst amount (g), NaBH4 concentration (%), process temperature (oC) and reusability affecting the hydrolysis of sodium borohydride were examined. The CEPcat obtained was characterized with FT-IR, TGA, XRD, SEM and EDX analyses. The hydrogen generation rate (HGR) was determined as 432 mL gCo−1 min−1 in the presence of 1 g CEPcat, a CoO/CaO ratio of 10/90 and 1% NaBH4 concentration. The activation energy of the NaBH4 hydrolysis reaction was calculated as 16.78 kJ mol−1. After 16 reuses of the CEPcat there was no significant decrease in the hydrogen volume. Compared to the first use while there was an increase in the HGR. These results showed that the CEPcat prepared has a significant advantage over other catalysts for use in NaBH4 hydrolysis.  相似文献   

8.
In present paper, the preparation and catalytic activity of Eupergit C polymer (EC) modified Co complex was reported. Scanning Electron Microscope (SEM), X-Ray Diffraction (XRD), Brunauer-Emmett-Teller Surface Area Analysis (BET), Fourier Transform Infrared Spectroscopy (FT-IR), Transmission Electron Microscopy (TEM) coupled with energy dispersive X-ray (EDX) and X-ray photoelectron spectroscopy (XPS) were used to characterization of catalyst. EC modified-Co complex was the first time examined as a catalyst in NaBH4 hydrolysis to H2 evolution. The kinetic calculations were determined by using two different kinetic methods. The low activation energy barriers were achieved as 21.673 kJ mol?1 for nth order model and as 21.061kJmol?1 for Langmuir-Hinshelwood (L-H) model at low temperatures. EC modified-Co complex catalyst exhibited high performance with H2 evolution rates of 3914 mL H2gcat?1min?1 and 9183 mLH2gcat?1min?1 at 30 °C–50 °C. Additionally, Langmuir–Hinshelwood mechanism was explained for EC modified Co complex catalyzed sodium borohydride hydrolysis reaction. The reusability experiments showed that EC modified-Co complex catalyst maintained excellent stability with 100% conversion and without significant lost after the 6th run.  相似文献   

9.
In this study, grinded apricot kernel shell (GAKS) biobased waste was used for the first time as a cost-effective, efficient, green and metal-free catalyst for hydrogen generation from the hydrolysis reaction of sodium borohydride (NaBH4). For the hydrogen production by NaBH4 hydrolysis reaction, GAKS was treated with various acids (HCl, HNO3, CH3COOH, H3PO4), salt (ZnCl2) and base (KOH). As a result, the phosphoric acid (H3PO4) demonstrated better catalytic activity than other chemical agents. The hydrolysis of NaBH4 with the GAKS-catalyst (GAKScat) was studied depending on different parameters such as acid concentration, furnace burning temperature and time, catalyst amount, NaBH4 concentration and hydrolysis reaction temperature. The obtained GAKScat was characterized by ICP-MS, elemental analysis, TGA, XRD, FT-IR, Boehm, TEM and SEM analyses and was evaluated for its catalytic activity in the hydrogen production from the hydrolysis reaction of NaBH4. According to the results, the optimal H3PO4 percentage was found as 15%. The maximum hydrogen generation rate from the hydrolysis of NaBH4 with the GAKScat was calculated as 20,199 mL min−1 gcat−1. As a result, it can be said that GAKS treated with 15% H3PO4 as a catalyst for hydrogen production is an effective alternative due to its high hydrogen production rate.  相似文献   

10.
The aim of this work is to prepare CoB catalysts supported on raw bentonite (CoB/bentonite) and Na-exchanged bentonite (CoB/Na-bentonite) by the impregnation and chemical reduction method. The prepared catalysts were characterized using X-ray diffractometry (XRD), X-ray fluorescence spectroscopy (XRF), scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS) and Fourier transform infrared spectroscopy (FTIR) techniques. The activities of the catalysts were tested in the hydrolysis reaction of sodium borohydride (NaBH4) in a semi-batch system. The volume of the evolved hydrogen gas was determined by a water displacement method. The effects of catalyst amount, NaOH (a base stabilizer) concentration, NaBH4 concentration and solution temperature on the hydrogen generation rate were investigated. The maximum hydrogen generation rates were determined as 921.94 mL/min.gcat for CoB/bentonite and 1601.45 mL/min.gcat for CoB/Na-bentonite when the 5 wt % NaBH4 and 10 wt % NaOH solutions were used at 50 °C. The activation energies (Ea) of the hydrolysis reaction over CoB/bentonite and CoB/Na-bentonite were determined as 55.76 and 56.61 kJ/mol, respectively.  相似文献   

11.
It is the first study to synthesize Co(II)-Schiff Base complex and to use it like a catalyst for potassium borohydride hydrolysis reaction to hydrogen production. Co(II)-complex is synthesized with CoCl2·6H2O and 5-Amino-2,4-dichlorophenol-3,5-di-tert-butylsalisylaldimine ligand. KBH4 hydrolysis reaction is studied according as percentage of KBH4, percentage of KOH, amount of Co-Schiff Base complex catalyst and temperature effects. Co-Schiff Base complex is highly effective catalyst and initial rates (Ro) of KBH4 hydrolysis reaction were 61220.00 and 99746.67 mL H2. g−1 cat. min−1 at 30 °C and 50 °C. Furthermore this study includes the kinetic calculations and for this reaction calculated activation energy is 17.56 kJ mol−1.  相似文献   

12.
Hydrogen is a sustainable, renewable and clean energy carrier that meets the increasing energy demand. Pure hydrogen is produced by the hydrolysis of sodium borohydride (NaBH4) using a catalyst. In this study, Ni/TiO2 catalysts were synthesized by the sol-gel technique and characterized by X-ray diffraction (XRD), X-ray fluorescence spectroscopy (XRF), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM) and Brunauer-Emmett-Teller (BET) methods. The effects of Ni loading ratio (20–40%), catalyst amount (75–200 mg), the concentration of sodium hydroxide (NaOH, 0.25–1 M), initial amount of NaBH4 (75–125 mg) and the reaction temperature (20–60 °C) on hydrogen production performance were examined. The hydrogen yield (100%) and hydrogen production rate (110.87 mL/gcat.min) were determined at the reaction conditions of 5 mL of 0.25 M NaOH, 100 mg NaBH4, 100 mg Ni/TiO2, 60 °C. Reaction order and activation energy were calculated as 0.08 and 25.11 kJ/mol, respectively.  相似文献   

13.
Due to the high volumetric density and environmentally friendly hydrolysis products, sodium borohydride as a promising candidate for chemical hydrogen storage has been intensively employed, but it needed expensive noble metals or complicated materials or processes. In this work, a new type of catalyst with very simple synthetic route form available and low-cost precursors has been introduced for hydrolysis of sodium borohydride with high efficiency. Fe2O3 nanosheets were synthesized with a straightforward route using glucose, urea and ferric nitrate and then the core sheets were coated by nitrogen doped carbon material using citric acid and urea as carbon and nitrogen sources. The core-shell nanosheets have been well confirmed by TEM images. Moreover, the elemental compositions were fully addressed by XPS analysis. Because of the acidic and basic groups on the presented material, the catalyst showed excellent catalytic activity with hydrogen production rate of 637 mL (H2) min−1·gcat −1. It is notable that the rate was calculated based on the whole amount of the catalyst, while in other reports the metal active sites have been employed for calculations. To find the most promising nanostructure of α-Fe2O3, influence of Fe2O3 morphology on the catalytic activity was also investigated.  相似文献   

14.
In this study, activated carbon is produced from defatted hazelnut bagasse at different activation conditions. The catalytic activities of activated carbons are evaluated for NaBH4 methanolysis and electrooxidation. These materials are characterized by N2 adsorption-desorption, FTIR, SEM-EDS and XPS and results show that these materials are prepared successfully. N2 adsorption-desorption results reveal that activated carbon (FH3-500) has the highest BET surface area as 548 m2/g, total pore volume as 0.367 cm3/g and micropore volume as 0.205 cm3/g. On the orher hand, as a result of hydrogen production studies, FH3-500 activated carbon catalyst has the highest initial hydrogen production rate compared to other materials. At 50 °C, this metal-free activated carbon catalyst has a high initial hydrogen production rate of 13591.20 mL/min.gcat, which is higher than literature values. Sodium borohydride electrooxidation measurements reveal that FH2-500 also has the highest electrocatalytic activity and stability. Hazelnut pulp-based activated carbons are firstly used as a metal-free catalyst in the methanolysis and electrooxidation of sodium borohydride, and its catalytic activity is good as a metal-free catalyst. The results show that the hazelnut pulp-based activated carbon catalyst is promising as a metal-free catalyst for the methanolysis and electrooxidation of sodium borohydride.  相似文献   

15.
Development of efficient catalysts for hydrogen evolution reaction is of key importance for the safe storage and utilization of hydrogen from the hydrolysis of NaBH4. In this study, a series of nanocatalysts containing iron- and nickel-based metal borides were developed through a mechanochemical route followed by a wet milling step. The use of the mole ratio of metal chlorides to NaBH4 as 1:2 enabled the simultaneous formation of Ni3B and FeB phases, while the room-temperature synthesis method caused a uniform morphology with an average particle size and surface are of 70 nm and 41.8 m2/g, respectively. This powder showed the best catalytic performance compared to other samples with a hydrogen generation rate value of 758 ml H2 min?1 gcat?1 at room temperature and an activation energy of 40.8 kJ/mol. The catalyst performed good durability for each cycle and retained about 70% of its initial catalytic activity after 5 cycles. The availability of active iron, nickel, and boron species on the surface contributed to the enhancement of catalytic activity. As-prepared catalysts can be considered as low-cost and reusable materials for the efficient hydrolysis of sodium borohydride.  相似文献   

16.
The fast release of hydrogen from borohydride is highly desired for a fuel cell system. However, the generation of hydrogen from borohydride is limited by the low activity and low stability of the catalyst. Herein, a highly active catalyst is synthesized through a simple one-step chemical reduction using bacterial cellulose (BC) derived carbon as a support for the active Co–B alloy. The morphology and microstructure of the BC/Co–B nanocomposite are characterized by SEM, TEM, XRD, and BET adsorption analysis. The BC/Co–B possesses high surface area (125.31 m2 g?1) high stability and excellent catalytic activity for the hydrolysis of NaBH4. Compared with unsupported Co–B nanocomposite or commercial carbon supported Co–B, the BC/Co–B nanocomposite shows greatly improved catalytic activity for the hydrolysis of NaBH4 with a high hydrogen generation rate of 3887.1 mL min?1 g?1 at 30 °C. An activation energy of 56.37 kJ mol?1 was achieved for the hydrolysis reaction. Furthermore, the BC/Co–B demonstrated excellent stability. These results indicate that the BC/Co–B nanocomposite is a promising candidate for the hydrolysis of borohydrides.  相似文献   

17.
At present, a novel and active catalyst, RuW/MWCNT catalyst, was successfully synthesized to complete the hydrolysis reaction of sodium borohydride (NaBH4). The activity of Ru catalyst was increased by adding tungsten (W) to ruthenium (Ru) on multi-walled carbon nanotube (MWCNT) support. Surface characterization of the catalyst was performed with scanning electron microscope (SEM-EDX), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and transmissing electron microscope (TEM) analysis methods. SEM-EDX revealed that RuW (95:5) catalyst metal ratio was obtained at desired nominal ratio. XRD characterization revealed that W addittion to the Ru structure increased its activity by forming an alloy. W addition Ru altered the electronic structure of the Ru. Parameters affecting the hydrolysis performance of RuW/MWCNT catalyst such as temperature, amount of catalyst, NaBH4 concentration and sodium hydroxide (NaOH) concentration were investigated. Adding NaOH to the reaction vessel reduced the activity of the RuW/MWCNT catalyst. From the hydrolysis measurements, the activation energy of RuW(95–5)/MWCNT catalyst was found to be 16.327 kjmol?1, the reaction order as 0.61 and the initial rate as 95,841,4 mL H2gcatmin?1. The stability of the RuW/MWCNT catalyst was tested using 5 times and it was observed that this novel RuW/MWCNT catalyst could complete the hydrolysis reaction despite repeated use.  相似文献   

18.
Achieving high catalytic performance with the lowest possible amount of noble metal is critical for any catalytic applications. Herein, we report a controllable method of preparing low Ru loaded, N-doped porous carbon embedded with cobalt oxide species (Ru/CoOx@NPC) using core-shell metal-organic framework (MOF) as a template. The optimized catalyst exhibits a highly powerful yet stable performance of H2 production through sodium borohydride (NaBH4) hydrolysis. The Ru/CoOx@NPC catalyst shows a fast H2 generation rate (8019.5 mL min?1 gcat?1), high turnover frequency (1118.6 mol min?1 molRu?1), and reusability. The carbonized ZIF-8 core and the ZIF-67 outer shell supplies a porous carbon moiety that not only improves the conductivity and but also provides uniform distribution of the active sites. The XPS analysis indicates that there is a strong electronic interaction between Co species and Ru species. The superior catalytic performance can be attributable to the large specific surface area as well as the synergy between Co-oxide and Ru clusters.  相似文献   

19.
In this study, nickel, nickel-chromium alloy, and nickel-vanadium alloy were coated to form a thin film on the slides prepared by magnetron sputtering process, which were used as a catalyst for the hydrolysis of alkaline sodium borohydride. Factors, such as the temperature of the solution, amount of the catalyst, initial pH of the solution and the performance of these catalysts on hydrogen generation rate were investigated using response surface methodology. Moreover, the catalysts were characterized using XRD and FE-SEM/EDS analyses. Utilizing the obtained optimum conditions of the response surface methodology estimation, the maximum hydrogen generation rate was 35,071 mL min−1 gNiV−1 from NiV catalyst at 60 °C, pH 6, and 1.75 g catalyst conditions. Under the same experiment conditions, the maximum hydrogen generation rates of Ni and NiCr catalyst systems are 28,362 mL min−1 gNi−1, and 30,608 mL min−1 gNiCr−1, respectively.  相似文献   

20.
In this study, 5-amino-2, 4-dichlorophenol-3, 5-ditertbutylsalisylaldimine-Ni complex catalyst is synthesised and used as an alternative to previous studies to produce hydrogen from hydrolysis of sodium borohydride. The resulting complex catalyst is characterised by XRD, XPS, SEM, FT-IR and BET surface area analyses. Experimental works are carried out at 30 °C with 2% NaBH4, 7% NaOH and 5 mg of catalyst. The maximum hydrogen production rate from hydrolysis of sodium borohydride with nickel-based complex catalyst compared to the pure nickel catalyst is increased from 772 ml min?1g?1 to 2240 ml min?1g?1 by an increase of 190%. At the same time, the hydrolysis reaction with pure nickel catalyst is completed in 145 min while the hydrolysis reaction with nickel-based complex catalyst is completed in 50 min. The activation energy of this hydrolysis reaction was calculated as 18.16 kJ mol?1. This work also includes kinetic information for the hydrolysis of NaBH4.The reusability of the nickel-based complex catalyst used in this study has also been studied. The nickel-based complex catalyst is maintained the activity of 72% after the sixth use, compared to the first catalytic use.  相似文献   

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