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1.
The use of hydrogen as an energy carrier is an attractive solution toward addressing global energy issues and reducing the effects of climate change. Design of new materials with high hydrogen sorption capacity and high stability is critical for hydrogen purification and storage. In this study, titanium dioxide nanotubes (TiO2NTs) were modified with palladium nanoparticles (PdNPs) utilizing a facile photo-assisted chemical deposition approach. Electrochemical anodization was employed for the direct growth of TiO2NTs. The PdNP functionalized TiO2NTs (TiO2NT/Pd) were characterized by scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS) and X-ray diffraction (XRD). The hydrogen sorption behaviours and stability of the TiO2NT/Pd nanocomposites were investigated and compared with nanoporous Pd networks that were deposited on a bulk titanium substrate (Ti/Pd) using cyclic voltammetry (CV) and chronoamperometry (CA). Our studies show that the TiO2NT/Pd nanocomposites possess a much higher hydrogen storage capacity, faster kinetics for hydrogen sorption and desorption, and higher stability than the nanoporous Pd.  相似文献   

2.
Hydrogen is envisaged to become an alternative clean energy source to fossil fuels that eventually lead to gradually increasing demand to design an efficient adsorbent for high storage capacity. Being inspired from the metal-doped adsorbents, mesoporous KIT-6 was functionalized with different metals namely Ce, Co, Cr, Cu, Ni, Pd, Pt, Sn and Ti with constant loading by wet impregnation method. Hydrogen adsorption performance showed that the metal doping improves the hydrogen storage capacity of KIT-6 except for KCu. Adsorbents KPd and KPt showed small hysteresis during adsorption/desorption analysis. Among all the metals, Pd-doped KIT-6 (KPd) showed the maximum uptake capacity (0.31 wt%) at atmospheric conditions. However, Sn-doped KIT-6 (KSn) showed the maximum uptake of 4.74 wt% at 77 K and 40 bar. This study provides a thorough insight in to the hydrogen adsorption/desorption behavior of the various metal–doped KIT-6 studied, which could be important first-hand information before designing the hydrogen storage material for the practical application.  相似文献   

3.
In this study, transition metals (TM) such as palladium (Pd) have been introduced on co-doped graphene and defect graphene sheets with nitrogen and boron ad-atoms to investigate the potentials of new adsorbents for hydrogen storage. The first principle studies using density functional theory (DFT) and DFT-D3 correction dispersion were undertaken to calculate the adsorption energy of hydrogen molecule on the graphene sheet. The results showed that applying Pd transition metal could enhance adsorption energy of hydrogen molecules towards pristine sheet. The main problem in applying transition metal on graphene sheets was concerned with clustering. However, the current defects in graphene sheets prevent clustering event. Our simulation results suggested that these defects reduced hydrogen adsorption and substitute dopants such as nitrogen and boron together on graphene sheets could improve the adsorption energy. Thus, two various forms of Pd decorated NB co-doped as hexagonal and double carbon vacancy (DCV) were introduced as new structures for hydrogen storage. A physical adsorption, which is appropriate for reversible hydrogen storage, was implemented for both novel adsorbents. In the two various forms of NB co-doped structures, DCV had the optimum adsorption behavior as adsorption energy level and density of state (DOS) phenomena. Moreover, the results of adsorption energy using DFT method were consistent with that of DFT-D3 correction dispersion and higher amounts of adsorption energy in DFT-D3 method were obtained. Finally, results introduced Pd decorated NB co-doped graphene sheets as a novel material for hydrogen storage.  相似文献   

4.
Hydrogen adsorption on porous materials is one of the possible methods proposed for hydrogen storage for transport applications. One way for increasing adsorption at room temperature is the inclusion of metal nanoparticles to increase hydrogen–surface interactions. In this study, ordered mesoporous carbon materials were synthesized by replication of nanostructured mesoporous SBA-15 silica. The combination of different carbon precursors allowed to tailor the textural, structural and chemical properties of the materials. These carbons were used for the synthesis of hybrid nanostructured carbon/palladium materials with different sizes of metal nanoparticles. The hydrogen sorption isotherms were measured at 77 K and 298 K between 0.1 and 8 MPa. Hydrogen storage capacities strongly correlate with the textural properties of the carbon at 77 K. At room temperature, Pd nanoparticles enhance hydrogen storage capacity by reversible formation of hydride PdHx and through the spillover mechanism. The hydrogen uptake depends on the combined influences of metal particle size and of carbon chemical properties. Carbons obtained from sucrose precursors lead to the hybrid materials with the highest storage capacities since they exhibits a large microporous volume and a high density of oxygenated surface groups.  相似文献   

5.
The effects of different amounts palladium loading on the hydrogen sorption characteristics of double-walled carbon nanotubes (DWCNTs) have been investigated. The physical properties of the pristine DWCNTs and Pd/DWCNTs were systematically characterized by X-ray diffraction, transmission electron microscopy, and Brunauer–Emmett–Teller surface area measurements. Pd nanoparticles were loaded on DWCNT surfaces for the dissociation of H2 into atomic hydrogen, which spills over to the defect sites on the DWCNTs. When we use different Pd content, the particle size and dispersion will be different, which affects the hydrogen storage capacity of the DWCNTs. In this work, the hydrogen storage capacities were measured at ambient temperature and found to be 1.7, 1.85, 3.0, and 2.0 wt% for pristine DWCNTS, 1.0 wt%Pd/DWCNTs, 2.0 wt%Pd/DWCNTs, and 3.0 wt%Pd/DWCNTs, respectively. We found that the hydrogen storage capacity can be enhanced by loading with Pd nanoparticles and selecting a suitable content. Furthermore, the sorption can be attributed to the chemical reaction between the atomic hydrogen and the dangling bonds of the DWCNTs.  相似文献   

6.
The effects of different reductants for palladium loading on the hydrogen sorption characteristics of double-walled carbon nanotubes (DWCNTs) have been investigated. Pd nanoparticles were loaded on DWCNT surfaces for dissociation of H2 into atomic hydrogen, which spills over to the defect sites on the DWCNTs. When we use different reductants, the reduction capabilities and other effects of the different reductants are different, which affects the hydrogen storage capacity of the DWCNTs. In this work, the amount of hydrogen storage capacity was determined (by AMC Gas Reactor Controller) to be 1.7, 2.0, 2.55, and 3.0 wt% for pristine DWCNTS and for 2.0%Pd/DWCNTs using H2, l-ascorbic acid, and NaBH4 as reductants, respectively. We found that the hydrogen storage capacity can be enhanced by loading with 2% Pd nanoparticles and selecting a suitable reductant. Furthermore, the sorption can be attributed to the chemical reaction between atomic hydrogen and the dangling bonds of the DWCNTs.  相似文献   

7.
Ordered mesoporous carbons were synthesized with a soft-template approach and modified with a water and tetrahydrofuran mixture having a H2O/THF molar ratio of 17:1 as potential adsorbent media for hydrogen storage. Hydrogen adsorption equilibrium on the carbon adsorbents was measured gravimetrically at 270 K and hydrogen pressures up to 163 bar. Enhanced hydrogen adsorption was observed on the carbon adsorbents doped with 0.5 wt.% and 0.75 wt.% of H2O/THF due to the combined effects of hydrogen adsorption on the carbon surface and formation of a binary H2–H2O–THF clathrate. Hydrogen adsorption capacities on the carbon adsorbents doped with 0.5 wt.%, 0.75 wt.% of H2O/THF, and the pure carbon at 270 K and 163 bar are 0.747 wt.%, 0.646 wt.% and 0.585 wt.%, respectively. The hydrogen adsorption isotherms on all the doped carbon adsorbents are of typical Type III and can be well correlated by the Freundlich equation. A desorption hysteresis loop was observed on the carbon adsorbents doped with 0.5 wt.% and 0.75 wt.% of H2O/THF, which was probably caused by the pore size difference during the adsorption and desorption steps.  相似文献   

8.
Hydrogen fuel is becoming a hot topic among the scientific community as an alternative energy source. Hydrogen is eco-friendly, renewable, and green. The synthesis and development of materials with great potential for hydrogen storage is still a challenge in research and needs to be addressed to store hydrogen economically and efficiently. Various solid-state materials have been fabricated for hydrogen energy storage; however, carbon-based nanocomposites have gained more attention because of its high surface area, low processing cost, and light weight nature. Carbon materials are easy to modify with various metals, metal oxides (MOs), and other organometallic frameworks because of the functional groups available on the surface and edges that increase the storage capacity of hydrogen. In addition, chemisorption is another way to enhance the hydrogen storage capacity of carbon-based nanocomposites. In this review, we discuss the success achieved thus far and the challenges that remain for the physical and chemical storage of hydrogen in various carbon-based nanocomposites. Various compositions of catalysts (eg, metal, MOs, alloy, metal organic frameworks) and carbon materials are designed for hydrogen storage. Superior energy storage in hybrids and composites as compared with pristine materials (catalysts or carbon nanotubes) is governed by the interaction, activation, and hydrogen adsorption/absorption mechanism of materials in the reaction profile. (Nano)composites comprising carbon material with metals, MOs, or alloys are important in this field, not only because of their potential for hydrogen sorption but also their significant cyclic stability and high efficiency upon successive adsorption-desorption cycles.  相似文献   

9.
Hydrogen is a good alternative to replace fossil fuels in automobiles. Storage of hydrogen for vehicular applications with high gravimetric density is a challenging task. The hydrogen sorption capacity of [1,1]paracyclophane functionalized with Li is investigated using density functional theory. Li functionalized [1,1]paracyclophane physisorbs 8 H2 achieving the maximum hydrogen weight percentage up to 13.42 %. All positive vibrational frequencies and a significant difference in the energy of frontier molecular orbitals confirm the stability and high absolute hardness of the host. Molecular dynamics simulations prove the thermal stability and reversibility of hydrogen adsorption over Li functionalized [1,1]paracyclophane implying the ease of on-board reversible hydrogen storage. Our findings confirm that Li decorated [1,1]paracylophane is a good hydrogen storage material meeting the 2020 targets of DOE.  相似文献   

10.
A hybrid molecular simulation, as a combination of molecular dynamics and Grand Canonical Monte Carlo simulation, is performed to investigate the storage capacity of hydrogen in carbon nanostructure adsorbents. Pure graphene sheet, nitrogen-doped graphene sheet, palladium-decorated graphene sheet and nitrogen-doped graphene sheet decorated with palladium atoms are selected for this purpose. Palladium is added to the structure in atomic and nanoparticle forms. Initially, all selected systems are optimized using density functional theory (DFT). The atomic charges of various structures are incorporated in the hybrid simulation. Then, hybrid simulations of hydrogen adsorption in different structures are performed at a temperature of 300 K in the pressure range of 1–40 bar. Simulation results show that among various structures, the simultaneous doping of graphene sheet with nitrogen atom and decoration of sheets by palladium atoms could increase the storage capacity by about 437% in comparison to pure graphene. In addition, the atomic form of palladium is more efficient than its nanoparticle form. Finally, comparing the adsorption capacity of the proposed structure with the target set by the US Department of Energy for 2020 indicates that proposed nanostructure can improve this target for hydrogen storage in comparison with previous carbon structure materials.  相似文献   

11.
Due to the advantage of catalytic activity on the process of hydrogen sorption/desorption and high affiliation with hydrogen, iron nanoparticles are a hybrid within an ordered mesoporous carbon with nitrogen functional groups on the surface and are used as a host for improving the electrochemical hydrogen storage. This iron and nitrogen dual-doped ordered mesoporous carbon material is synthesized through a nano-casting method which uses SBA-15 as a hard template and iron phthalocyanine as the iron, nitrogen and carbon source. After characterization of the synthesized material by SEM, TEM, XRD, Raman, XPS and Nitrogen sorption/desorption measurements, this hybrid material demonstrated a hydrogen storage capacity of 120 mAh g−1. This is associated with the fast kinetics of electrochemical hydrogen insertion, low self-discharge and the good cycling capability. Furthermore, the hydrogen stored inside the synthesized composited carbon material shows excellent rate performance under various states of discharge current densities. Results suggest that the enhanced electrochemical hydrogen storage performances may due to the electro-catalytic activity of iron nanoparticle, basicity nature of nitrogen functionality on the surface, mesoporous carbon with large surface area, large porosity and interconnected pore structure.  相似文献   

12.
In the emerging front of research, much attention is focused on the usage of hydrogen as a promising alternative energy carrier that can potentially replace fossil fuels. Conversely, the realization of hydrogen as an energy carrier becomes impounded since the light weight and compact hydrogen storage materials are still prerequisites for hydrogen fuel cell technology. In the present study, the performance of nanoclay composites composed of acid treated halloysite clay nanotubes (A-HNTs) and hexagonal boron nitride nanoparticles (h-BN) are investigated towards hydrogen storage. where facile ultrasonic approach was adopted. The prepared A-HNT–h-BN nanoclay composites subjected to various characterization techniques such as X-ray Diffraction (XRD), micro–Raman Spectroscopy, Fourier Transform Infrared Spectroscopy (FTIR), UV–Visible Diffuse Reflectance Spectroscopy (DRS), Scanning Electron Microscopy (SEM) with Energy Dispersive X-Ray Spectroscopy (EDX) and High Resolution Transmission Electron Microscopy (HRTEM) with Selected Area Transmission Electron Diffraction (SAED). The presence of h-BN nanoparticles at the surface of A-HNTs can be seen from HRTEM images and these findings are supported by XRD, FTIR and Raman results. Hydrogen adsorption studies are performed using Sieverts-like hydrogenation setup. A 2.88 wt% of hydrogen storage capacity and 100% desorption were achieved for the A-HNT–5wt% h-BN nanoclay composite at 50 °C. The adsorbed hydrogen possess the average binding energy of 0.33 eV, which lies in the recommended range (0.2–0.4 eV) for fuel cell applications. So it is expected that A-HNT–h-BN nanoclay composites will serve as a better hydrogen storage material for fuel cell applications in the near future.  相似文献   

13.
Pd doped Multi-Walled Carbon Nanotubes were prepared via supercritical carbon dioxide deposition method in order to enhance the hydrogen uptake capacity of carbon nanotubes at ambient conditions. A new bipyridyl precursor that enables reduction at moderate conditions was used during preparation of the sample. Both XRD analyses and TEM images confirmed that average Pd nanoparticle size distribution was around 10 nm. Hydrogen adsorption and desorption experiments at room temperature with very low pressures (0–0.133 bar) were conducted together with temperature programmed desorption (TPD) and reduction (TPR) experiments on undoped and doped materials to understand the complete hydrogen uptake profile of the materials. TPD experiments showed that Pd nanoparticles increased the hydrogen desorption activity at moderate temperatures around at 38 °C while for undoped materials it was determined around at 600 °C. Moreover, a drastic enhancement of hydrogen storage was recorded from 44 μmol/g sample for undoped material to 737 μmol/g sample for doped material through adsorption/desorption isotherms at room temperature. This enhancement, also verified by TPR, was attributed to spillover effect.  相似文献   

14.
One of the most famous porous adsorbents used for separation and storage of several gases is metal organic framework (MOF). In this study, the experimental data related to hydrogen adsorption on and desorption from five adsorbents including MOF-5, MOF-177, MOF-200, MOF-205 and MOF-210 is adopted. Then, the hydrogen sorption is modeled by applying Perturbed Hard Sphere Chain Equation of State (PHSC EoS). PHSC equation of state has three molecular-based parameters, namely, the number of segments per molecule, the hard-sphere diameter and the non-bonded interaction energy, respectively. The amount of hydrogen uptake in the adsorbents is obtained through gas-adsorbents phase equilibrium calculations at temperature 77 K and various pressures up to 80 × 105 Pa. Finally, the result is compared with the experimental data to show the precision of PHSC equation of state in predicting the hydrogen sorption trend.  相似文献   

15.
This work presents the synthesis and characterization of multi-walled carbon nanotubes (multi-walled CNTs) deposited with Pd or V and their hydrogen storage capacity measured by Sievert's volumetric apparatus. The CNTs were grown by the CVD method using LPG and LaNi5 as the carbon source and catalyst, respectively. Pd was impregnated on the CNTs by the reflux method with hydrogen gas as a reducing agent, while V was embedded on the CNTs by the vapor deposition method. The average metal particle size deposited on the CNTs was around 5.8 nm for Pd and 3.6 nm for V. Hydrogen adsorption experiments were performed at room temperature and at −196 °C under a hydrogen pressure of 65 bar. At −196 °C, the treated CNTs had a maximum hydrogen uptake of 1.21 wt%, while the CNTs deposited with Pd (Pd-CNTs) and CNTs deposited with V (V-CNTs) possessed lower surface areas, inducing lower hydrogen adsorption capacities of 0.37 and 0.4 wt%, respectively. For hydrogen sorption at room temperature, the CNTs decorated with the metal nanoparticles had a higher hydrogen uptake compared to the treated CNTs. Hydrogen adsorption capacity was 0.125 and 0.1 wt% for the Pd-CNTs and V-CNTs, respectively, while the hydrogen uptake of the treated CNTs was <0.01 wt%. For the second cycle, only half of the first hydrogen uptake was obtained, and this was attributed to the re-crystallization of the defect sites on the carbon substrate after the first hydrogen desorption.  相似文献   

16.
Multi-walled carbon nanotubes (MWCNTs) with diameter of about 50 nm were synthesized using thermal chemical vapor deposition. We have investigated the influence of Mg doping to the MWCNTs on its hydrogen storage property. TEM micrographs showed that Mg was attached to the MWCNTs and discontinuous arrangement of the carbon walls was recognized in the MWCNTs. According to XPS and BET analyses, the surface functional groups and pore size of the Mg-MWCNTs are increased by interactions between the Mg and the MWCNT’s outer walls. The electrochemical discharging curves of the MWCNTs and Mg-doped MWCNTs revealed that the hydrogen storage capacity was 363 and 450 mAhg−1, respectively. Volumetric technique determined that the hydrogen storage capacity of the MWCNTs and Mg-MWCNTs was 0.7 and 1.5 wt%, respectively. There are likely a couple of mechanism for Mg metal that used as dopant to pure MWCNTs, one involves increasing of adsorption binding energy and desorption temperature due to increasing defect sites (oxygen functional groups), while the second explains by electron transfer from metal atoms to carbon atoms resulting in a considerable increase in both the adsorption binding energy and desorption temperature.  相似文献   

17.
In this work a series of carbons with different structural and textural properties were characterised and evaluated for their application in hydrogen storage. The materials used were different types of commercial carbons: carbon fibers, carbon cloths, nanotubes, superactivated carbons, and synthetic carbons (carbon nanospheres and carbon xerogels). Their textural properties (i.e., surface area, pore size distribution, etc.) were related to their hydrogen adsorption capacities. These H2 storage capacities were evaluated by various methods (i.e., volumetric and gravimetric) at different temperatures and pressures. The differences between both methods at various operating conditions were evaluated and related to the textural properties of the carbon-based adsorbents. The results showed that temperature has a greater influence on the storage capacity of carbons than pressure. Furthermore, hydrogen storage capacity seems to be proportional to surface area, especially at 77 K. The micropore size distribution and the presence of narrow micropores also notably influence the H2 storage capacity of carbons. In contrast, morphological or structural characteristics have no influence on gravimetric storage capacity. If synthetic materials are used, the textural properties of carbon materials can be tailored for hydrogen storage. However, a larger pore volume would be needed in order to increase storage capacity. It seems very difficult approach to attain the DOE and EU targets only by physical adsorption on carbon materials. Chemical modification of carbons would seem to be a promising alternative approach in order to increase the capacities.  相似文献   

18.
The anticipated energy crisis due to the extensive use of limited stock fossil fuels forces the scientific society for find prompt solution for commercialization of hydrogen as a clean source of energy. Hence, convenient and efficient solid-state hydrogen storage adsorbents are required. Additionally, the safe commercialization of huge reservoir natural gas (CH4) as an on-board vehicle fuel and alternative to gasoline due to its environmentally friendly combustion is also a vital issue. To this end, in this study we report facile synthesis of polymer-based composites for H2 and CH4 uptake. The cross-linked polymer and its porous composites with activated carbon were developed through in-situ synthesis method. The mass loadings of activated carbon were varied from 7 to 20 wt%. The developed hybrid porous composites achieved high specific surface area (SSA) of 1420 m2/g and total pore volume (TPV) of 0.932 cm3/g as compared to 695 m2/g and 0.857 cm3/g for pristine porous polymer. Additionally, the porous composite was activated converted to a highly porous carbon material achieving SSA and TPV of 2679 m2/g and 1.335 cm3/g, respectively. The H2 adsorption for all developed porous materials was studied at 77 and 298 K and 20 bar achieving excess uptake of 4.4 wt% and 0.17 wt% respectively, which is comparable to the highest reported value for porous carbon. Furthermore, the developed porous materials achieved CH4 uptake of 8.15 mmol/g at 298 K and 20 bar which is also among the top reported values for porous carbon.  相似文献   

19.
The water vapor sorption capacity and corresponding generated heat amount are the most important properties for adsorbents in thermochemical heat storage systems. In order to understand the adsorption/desorption behavior of three nanoporous molecular sieves such as 5A, mordenite and natural clinoptilolite (with different structures, Si/Al ratios and balancing cations), the pure zeolites and their composites (obtained by depositing NaOH onto the molecular sieves) were characterized in their structural and surface properties by using appropriate techniques (N2 adsorption isotherms at ?196 °C, XRD and (MAS) NMR). The adsorption of water was performed using a Setaram TG‐DSC 111 apparatus. Three successive cycles of hydration (at 20 °C)/dehydration (at 150 °C) were carried out to check the stability of the system in conditions close to those used in adsorption heat pumps. The measured heats of dehydration vary in the 183–614 kJ kg?1sample range for the various samples that present also different water vapor sorption capacities (from ≈ 0.08 to ≈ 0.14 kgH2O kg?1sample). The water adsorption/desorption behavior of the zeolites was mainly related to the porous structure and to the Si/Al ratio, that drive the affinity of zeolite to water. The experimental results showed that the impregnation of the three kinds of nanoporous zeolites with different amounts of sodium hydroxide negatively affects the sorption characteristics of the composites. The blockage of zeolite pores (that limits the access to water molecules), the slight amorphization of the zeolite structure and the formation of carbonates are some of the phenomena identified to influence the water sorption onto NaOH‐containing composites. Copyright © 2016 John Wiley & Sons, Ltd.  相似文献   

20.
Hydrogen storage nanocomposites prepared by high energy reactive ball milling of magnesium and vanadium alloys in hydrogen (HRBM) are characterised by exceptionally fast hydrogenation rates and a significantly decreased hydride decomposition temperature. Replacement of vanadium in these materials with vanadium-rich Ferrovanadium (FeV, V80Fe20) is very cost efficient and is suggested as a durable way towards large scale applications of Mg-based hydrogen storage materials. The current work presents the results of the experimental study of Mg–(FeV) hydrogen storage nanocomposites prepared by HRBM of Mg powder and FeV (0–50 mol.%). The additives of FeV were shown to improve hydrogen sorption performance of Mg including facilitation of the hydrogenation during the HRBM and improvements of the dehydrogenation/re-hydrogenation kinetics. The improvements resemble the behaviour of pure vanadium metal, and the Mg–(FeV) nanocomposites exhibited a good stability of the hydrogen sorption performance during hydrogen absorption – desorption cycling at T = 350 °C caused by a stability of the cycling performance of the nanostructured FeV acting as a catalyst. Further improvement of the cycle stability including the increase of the reversible hydrogen storage capacity and acceleration of H2 absorption kinetics during the cycling was observed for the composites containing carbon additives (activated carbon, graphite or multi-walled carbon nanotubes; 5 wt%), with the best performance achieved for activated carbon.  相似文献   

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