Enhanced electrochemical hydrogen storage capacity of multi-walled carbon nanotubes by TiO2 decoration

Electrochemical hydrogen storage of multi-walled carbon nanotubes (MWCNTs) decorated by TiO₂ nanoparticles (NPs) has been studied by the galvanostatic charge and discharge method. The TiO₂ NPs are deposited on the surface of MWCNTs by sol-gel method. Structural and morphological characterizations have been carried out using XRD, SEM and TEM, respectively. TiO₂ NPs can significantly enhance the discharge capacity of MWCNTs. The cyclic voltammograms analysis indicates that the electrical double layer contributes little to the discharge capacity of TiO₂-decorated MWCNTs. The MWCNTs modified with a certain amount of TiO₂ NPs have a discharge capacity of 540 mAh/g, corresponding to an electrochemical hydrogen storage capacity of about 2.02 wt%, which is quite interesting for the battery applications. The enhancement effect of TiO₂ NPs on the discharge capacity of MWCNTs could be related to the increased effective area for the adsorption of hydrogen atoms in the presence of TiO₂ NPs on MWCNTs and the preferable redox ability of TiO₂ NPs.     

The effect of various acids treatment on the purification and electrochemical hydrogen storage of multi-walled carbon nanotubes

The effects of HCl, HNO₃, H₂SO₄ and HF acids on the purification and the electrochemical hydrogen storage of multi-walled carbon nanotubes (MWCNTs) were studied. The MWCNTs were synthesized on Fe–Ni catalyst by thermal chemical vapor deposition method. The X-ray diffraction and thermal gravimetric analysis results indicated that the MWCNTs purified by HF acid had the highest impurities as compared with the other acids. The N₂ adsorption results at 77 K indicated that all the samples were mainly mesoporous and the purified MWCNTs by HF acid had the highest surface area as compared with the other acids. The hydrogen storage capacities of the purified MWCNTs by the following acids were in ascending order as: H₂SO₄, HCl, HNO₃ and HF. It was found that the 1–2 nm micropores in the MWCNTs are very important for hydrogen storage. Further, the presences of catalyst and defective sites in MWCNTs influence the hydrogen storage capacity.     

Enhanced hydrogen storage capacity of Pt-loaded CNT@MOF-5 hybrid composites

We report on an easy synthesis method for the preparation of a hybrid composite of Pt-loaded MWCNTs@MOF-5 [Zn₄O(benzene-1,4-dicarboxylate)₃] that greatly enhanced hydrogen storage capacity at room temperature. To prepare the composite, we first prepared Pt-loaded MWCNTs, which were then incorporated in-situ into the MOF-5 crystals. The obtained composite was characterized by various techniques such as powder X-ray diffractometry, optical microscopy, porosimetry by nitrogen adsorption, and hydrogen adsorption. The analyses confirmed that the product has a highly crystalline structure with a Langmuir specific surface area of over 2000 m²/g. The hybrid composite was shown to have a hydrogen storage capacity of 1.25 wt% at room temperature and 100 bar, and 1.89 wt% at cryogenic temperature and 1 bar. These H₂ storage capacities represent significant increases over those of virgin MOF-5s and Pt-loaded MWCNTs.     

Effect of multi-wall carbon nanotubes supported palladium addition on hydrogen storage properties of magnesium hydride

To improve the hydrogen storage performance of magnesium hydride, multi-wall carbon nanotubes supported palladium (Pd/MWCNTs) was introduced to the magnesium-based materials. Pd/MWCNTs catalysts with different amounts of Pd (20 wt.%, 40 wt.%, 60 wt.%, 80 wt.%) were synthesized by a solution chemical reduction method. Afterwards, Mg₉₅–Pd_m/MWCNTs_5−m (m = 0, 1, 2, 3, 4, 5) were prepared for the first time by hydriding combustion synthesis (HCS) and mechanical milling (MM). It is determined by X-ray diffraction (XRD) analysis that Pd/MWCNTs can significantly increase the hydrogenation degree of magnesium during the HCS process. The microstructures of the composites obtained by transmission electron microscope (TEM) and field emission scanning electronic microscopy (FESEM) analyses show that Pd nanoparticles are well supported on the surface of carbon nanotubes and the Pd/MWCNTs are dispersed uniformly on the surface of MgH₂ particles. Moreover, it is revealed that there is a synergistic effect of MWCNTs and Pd on the hydrogen storage properties of the composites. The Mg₉₅–Pd₃/MWCNTs₂ shows the optimal hydriding/dehydriding properties, requiring only 100 s to reach its saturated hydrogen absorption capacity of 6.67 wt.% at 473 K, and desorbing 6.66 wt.% hydrogen within 1200 s at 573 K. Additionally, the dehydrogenation activation energy of MgH₂ in this system is decreased to 78.6 kJ/mol H₂, much lower than that of as-received MgH₂.     

Hydrogenation behavior of high-energy ball milled amorphous Mg2Ni catalyzed by multi-walled carbon nanotubes

Amorphous Mg₂Ni alloy was successfully synthesized by means of mechanical alloying. Then, the multi-walled carbon nanotubes (MWCNTs) were added by high-energy ball milling to catalyze the amorphous alloy. The X-ray diffraction (XRD) spectroscopy reveal that the as-cast Mg₂Ni alloy has presented a completely amorphous state under specific conditions of high-energy ball milling process. Different process parameters of ball-to-powder ratio (10:1, 20:1, 40:1) and milling time have been attempted for the preparation of amorphous Mg₂Ni alloy. The results show that the milling time and ball-to-powder weight ratio have significantly influence on the amorphization process of crystalline Mg₂Ni alloy. Before and after the milling, phase compositions and microstructures of the prepared materials were characterized by XRD, scanning electron microscope (SEM), electron energy dispersion spectrum (EDS) and transition electron microscope (TEM) approaches. The morphology of composite Mg₂Ni/MWCNTs was investigated, the TEM images show that the MWCNTs imbed on the surface of the particles after milling for 1 h, and the MWCNTs with and without tubular structure have been observed. The hydrogen storage properties of amorphous Mg₂Ni alloys were improved by the catalytic effect of MWCNTs. The catalytic effect and mechanism of MWCNTs on the hydrogen storage properties of amorphous Mg₂Ni alloy are discussed and investigated.     

A reversible hydrogen storage material of Li-decorated two-dimensional (2D) C4N monolayer: First principles calculations

Two-dimensional (2D) materials can be regarded as potential hydrogen storage candidates because of their splendid chemical stability and high specific surface area. Recently, a new dumbbell-like carbon nitride (C₄N) monolayer with orbital hybridization of sp³ is reported. Motivated from the above exploration, the hydrogen adsorption properties of Li-decorated C₄N monolayer are comprehensively investigated via first principles calculations based on the density functional theory (DFT). It is found that the Dirac points and Dirac cones exists in the Brillouin zone (BZ) from the calculated electronic structure and indicates the C₄N can be used as an excellent topological material. Also, the calculated phonon spectra demonstrate that the C₄N monolayer owns a strong stability. Moreover, the calculated binding energy of decorated Li atom is bigger than its cohesive energy and results in Li atoms disperse over the surface of C₄N monolayer uniformly without clustering. In addition, the Li₈C₄N complex can capture up to 24H₂ molecules with an optimal hydrogen adsorption energy of −0.281 eV/H₂ and achieves the hydrogen storage density of 8.0 wt%. The ab initio molecular dynamics (AIMD) simulations suggest that the H₂ molecules can be desorbed quickly at 300 K. This study reveals that Li-decorated C₄N monolayer can be served as a promising hydrogen storage material.     

The mechanism and sorption kinetic analysis of hydrogen storage at room temperature using acid functionalized carbon nanotubes

The present work investigates the effect of acid functionalization of multiwalled carbon nanotubes (MWCNTs) on the physisorption based mechanism of hydrogen storage at room temperature. For this purpose, a suite of functionalized CNT samples is synthesized and subjected to a comprehensive range of material characterization techniques and hydrogen storage measurements. Nitric acid (HNO₃) and the mixture of sulphuric acid and nitric acid (H₂SO₄:HNO₃) are used for the synthesis at oxidation temperatures of 80 °C and 100 °C. Electron microscopy and X-ray photoelectron spectroscopy results reveal that acid functionalization causes major alternation in the physicochemical properties of the CNTs due to the varied concentration of oxygen functional groups. Particularly, the H₂SO₄:HNO₃ functionalized sample at 100 °C is found to have the highest interlayer spacing, oxygen to carbon ratio (26.09 at. %), defect content, and specific surface area (215.3 m²/g). These features collectively contribute to substantially improved hydrogen storage properties, including a ～150% increase in the hydrogen storage capacity at 298 K and 50 bar. Furthermore, kinetic analysis shows that the desorption follows a multiple diffusion process which is sensitive to the oxygen functional groups and structural defects, hence reducing the rate of desorption; whereas the adsorption is controlled by a more rapid, three-dimensional diffusion process.     

Progress of graphene and loaded transition metals on Mg-based hydrogen storage alloys

Mg-based hydrogen storage alloys have become a research hotspot in recent years owing to their high hydrogen storage capacity, good reversibility of hydrogen absorption/desorption, low cost, and abundant resources. However, its high thermodynamic stability and slow kinetics limit its application, so the modification of Mg-based hydrogen storage alloys has become the development direction of Mg-based alloys. Transition metals can be used as catalysts for the dehydrogenation of hydrogen storage alloys due to their excellent structural, electrical, and magnetic properties. Graphene, because of its unique sp² hybrid structure, excellent chemical stability, and a specific surface area of up to 2600 m²/g, can be used as a support for transition metal catalysts. In this paper, the internal mechanism of graphene as a catalyst for the catalysis of Mg-based hydrogen storage alloys was analyzed, and the hydrogen storage properties of graphene-catalyzed Mg-based hydrogen storage alloys were reviewed. The effects of graphene-supported different catalysts (transition metal, transition metal oxides, and transition metal compounds) on the hydrogen storage properties of Mg-based hydrogen storage alloys were also reviewed. The results showed that graphene played the roles of catalysis, co-catalysis, and inhibition of grain aggregation and growth in Mg-based hydrogen storage materials.     

Effect of MWCNTs and lithium modified MWCNTs on electrochemical hydrogen storage properties of Co0.9Cu0.1Si alloy

Mechanical alloying technique was used to prepare the Co_0.9Cu_0.1Si alloy. Composite materials of Co_0.9Cu_0.1Si doping with different amounts of multi-walled carbon nanotubes (MWCNTs) or lithium modified MWCNTs (Li-MWCNTs) were obtained via ball-milling to improve the hydrogen storage performance of Co_0.9Cu_0.1Si. XRD, SEM and TEM were used to analysis the structural properties of the samples. A three-electrode battery system was carried out to test the electrochemical properties. After the addition of MWCNTs, the composites showed higher discharge capacity, stronger HRD, better cyclic stability and lower charge-transfer resistance than the original Co_0.9Cu_0.1Si alloy. The electro-catalytic function of MWCNTs, the reduction of particle size and the raise of specific surface area for Co_0.9Cu_0.1Si alloy may provide larger electrochemically accessible area and rapid channel for hydrogen transportation, which are important to enhance the electrochemical performance of the alloy. Moreover, a further improvement was achieved after the addition of Li-MWCNTs, illustrating that the MWCNTs and lithium species had synergistic effects in improving the discharge capacity and reaction kinetics of the Co_0.9Cu_0.1Si alloy electrode. As the weight ratio of the alloy and Li-MWCNTs was 15:1, the optimal discharge capacity of 624.4 mAh/g and the highest capacity retention of 67.5% were achieved.     

Diatom frustule-graphene based nanomaterial for room temperature hydrogen storage

Development of a room temperature hydrogen storage material is vital for the realization of a hydrogen economy. Towards achieving this goal, we present the use of naturally occurring diatom frustule for the synthesis of a novel nanomaterial that can achieve a hydrogen storage capacity of ~4.83 wt% at 25 ^°C and ~20 bar H₂ equilibrium pressure. We have effectively combined the large surface area of few layer graphene(G), the unique physical and chemical properties of diatom frustules(D) such as chemical inertness and good porosity and the ability of transition metals and their alloys (Pd₃Co) to adsorb large amounts of hydrogen. The resulting nanomaterial (Pd₃Co-D(100)-G) has a surface area of 163.25 m²/g and pore volume of 0.84 cm³/g. The observations in the present study suggest that increased surface area and porosity play a key role in achieving high hydrogen storage capacity at relatively low H₂ equilibrium pressures and room temperature conditions.     

The synthesized nickel-doped multi-walled carbon nanotubes for hydrogen storage under moderate pressures

Hydrogen adsorption capacity of Multiwalled carbon nanotubes (MWCNTs) decorated with Nickel (Ni) nanoparticles has been presented at room temperature and under moderate pressures of 4–20 bar. The functionalization of carbon nanotubes was carried by H₂SO₄-HNO₃ reducing agents and the Ni supported MWCNTs (Ni-MWCNTs) were prepared by wet chemical method. The structure and morphology characterization of samples were performed by XRD, TEM, EDX and SEM analyses. These nanotubes then subjected to hydrogenation step by using Sievert's-like apparatus. The hydrogenation of the Ni-MWCNTs was performed at 298 K and moderate hydrogen pressures of 4–20 bar. The obtained results show that there is a correlation between hydrogen storage capacity and hydrogen pressure that; as the pressure was increased, hydrogen uptake capacity enhanced due to physisorption. In addition, maximum hydrogen storage capacity of Ni-MWCNTs was found to be 0.298 wt % at room temperature and under pressure of 20 bar.     

H2 adsorption mechanism in Mg modified multi-walled carbon nanotubes for hydrogen storage

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.     

A study on the effects of Fex/Niy/MgO(1−x−y) catalysts on the volumetric and electrochemical hydrogen storage of multi-walled carbon nanotubes

The effects of various ratios of Fe/Ni/MgO and growth temperatures on yield, diameter and quality of multi-walled carbon nanotubes (MWCNTs) were studied. Thermal gravimetric analysis (TGA) confirmed that the MWCNT yield depends on Fe/Ni ratio with the following order; Fe_0.5 Ni_0.5 > Fe > Fe_0.75 Ni_0.25 > Fe_0.25 Ni_0.75 > Ni. The results indicated that there is an optimum temperature (940 °C) for the MWCNT growth both from quality and quantity (yield) aspects as compared to other temperatures. Moreover, the changes on Fe/Ni to MgO ratio for the MWCNT growth revealed that Fe/Ni/MgO with the ratio of 17.5/17.5/65 had the highest quality and surface area as compared to the other ratios. The hydrogen storage capacities of MWCNTs grown on Fe/Ni/MgO with various ratios obtained by using volumetric technique were in ascending order as 17.5/17.5/65, 15/15/70, 12.5/12.5/75, 10/10/80, 20/20/60, 22.5/22.5/55 and 25/25/50. In addition, the defective sites and mean diameter of the MWCNTs influenced the desorption temperature of stored hydrogen. Hydrogen storage by using electrochemical technique showed that Fe/Ni/MgO with the ratio of 17.5/17.5/65 had the highest hydrogen storage capacity compared with the other ratios. Based on electrochemical analysis, there are two regimes for hydrogen adsorption on the MWCNTs, one at about 0.8 V and the other at 0.15 V. The study on two kinds of adsorption region showed that the ratio of hydrogen storage capacity at 0.8 V to hydrogen storage capacity at 0.15 V increased with the increasing of the mean diameter of MWCNTs. The ratio reached to maximum value for the MWCNTs grown on Fe/Ni/MgO with the ratio of 20/20/60 as compared to the other ratios.     

Calcium-decorated graphdiyne as a high hydrogen storage medium: Evaluation of the structural and electronic properties

Graphdiyne (GDY) is a new member of carbon allotropes consisting of sp and sp² hybridized carbon atoms. In this work, the hydrogen adsorption on Calcium (Ca) decorated GDY and the influence of adatom on structural properties of GDY are investigated, using first principles plane wave calculations with Van der Waals corrections. The results show that similar to graphyne (GY) and unlike carbon nanotube (CNT), fullerene and graphene, clustering of Ca on GDY hinders due to the higher binding energy of the adatom to the carbon frame than the Ca cohesive energy. It can be seen that the Ca-decoration promotes hydrogen storage capacity of GDY, extremely (E_ads = ?0.266 and ?0.066 eV for Ca-decorated and pristine GDY, respectively). It is concluded that, the best site for the Ca trapping is 18-membered ring in which, Ca lies in-plane of GDY (E_ads = ?3.171 eV). Fourteen H₂ molecules (with the average adsorption energy of ～0.2 eV/H₂) can be adsorbed on the Ca atom from one side. The hydrogen storage capacity is estimated to be as high as 17.95 wt% for the both sides of GDY. So, the Ca-decorated GDY is offered as a promising candidate for hydrogen storage applications.     

Oxygen‐modified multiwalled carbon nanotubes: physicochemical properties and capacitor functionality

Multiwalled carbon nanotubes (MWCNTs) have found numerous applications in energy conversion systems. The current work focused on the introduction of oxygen moieties onto the walls of MWCNTs by five different reagents and investigating the associated physicochemical properties. Oxygen‐containing groups were introduced onto MWCNTs using an ultrasound water‐bath treatment with HNO₃, HCl, H₂O₂ or HCl/HNO₃ solution. Physicochemical properties were characterised by Fourier transform infrared spectroscopy, scanning electron microscopy, transmission electron microscopy, Raman, thermal gravimetric analysis, textural characteristics, cyclic voltammetry and electrochemical impedance spectroscopy. The study focus was mainly on linking the physicochemical properties of oxygen‐functionalised MWCNTs and suitability in electrochemical capacitors using group one sulfates. From the Fourier transform infrared spectroscopy KBr pellet protocol, peaks at 3400, 2370 and 1170 cm^?1 suggest oxygen‐containing functionalities on MWCNTs. HNO₃ treatment introduced highest oxygen‐containing moieties and achieved highest specific capacitance in Li₂SO₄ and Na₂SO₄ electrolytes of 36.200 F g^?1 (77 times better than pristine) and 45.100 F g^?1 (2.5 times enhancement), respectively. For K₂SO₄, it was 33.600 F g^?1 (4.9 times better) with HNO₃/HCl‐treated samples. Oxygen‐functionalised MWCNTs displayed both pseudo and electrochemical double‐layer mechanism of enhanced charge storage and cycle stability in group one sulfates electrolytes. The dominating charge storage mechanism was pseudo, and Na₂SO₄ was the best electrolyte amongst the three group one sulfates investigated. Copyright © 2017 John Wiley & Sons, Ltd.     

Effects of MWCNTs on improving the hydrogen storage performance of the Li3N system

In this paper, the influence of multi-walled carbon nanotube (MWCNT)-doping on the hydrogen storage properties of the Li₃N system was systematically investigated. Compared with the pure Li₃N sample, the MWCNT-doped Li₃N sample shows faster hydrogen absorption and desorption kinetics and a drastically improved cycling stability. Along with increasing MWCNT content, the hydrogen storage improvement becomes more apparent. When the MWCNT doping level reaches 10 mol%, the enhancement effect is significant. The improved hydrogen storage properties of the Li₃N system by MWCNT-doping can be reduced to the physical effect of ball milling, the increased specific surface area and large pores as well as the good thermal conductivity of MWCNTs.     

Efficient hydrogen storage in defective graphene and its mechanical stability: A combined density functional theory and molecular dynamics simulation study

A combined density functional theory and molecular dynamics approach is employed to study modifications of graphene at atomistic level for better H₂ storage. The study reveals H₂ desorption from hydrogenated defective graphene structure, V₂₂₂, to be exothermic. H₂ adsorption and desorption processes are found to be more reversible for V₂₂₂ as compared to pristine graphene. Our study shows that V₂₂₂ undergoes brittle fracture under tensile loading similar to the case of pristine graphene. The tensile strength of V₂₂₂ shows slight reduction with respect to their pristine counterpart, which is attributed to the transition of sp² to sp³-like hybridization. The study also shows that the V₂₂₂ structure is mechanically more stable than the defective graphene structure without chemically adsorbed hydrogen atoms. The current fundamental study, thus, reveals the efficient recovery mechanism of adsorbed hydrogen from V₂₂₂ and paves the way for the engineering of structural defects in graphene for H₂ storage.     

Interface effects in NaAlH4–carbon nanocomposites for hydrogen storage

For practical solid-state hydrogen storage, reversibility under mild conditions is crucial. Complex metal hydrides such as NaAlH₄ and LiBH₄ have attractive hydrogen contents. However, hydrogen release and especially uptake after desorption are sluggish and require high temperatures and pressures. Kinetics can be greatly enhanced by nanostructuring, for instance by confining metal hydrides in a porous carbon scaffold. We present for a detailed study of the impact of the nature of the carbon–metal hydride interface on the hydrogen storage properties. Nanostructures were prepared by melt infiltration of either NaAlH₄ or LiBH₄ into a carbon scaffold, of which the surface had been modified, varying from H-terminated to oxidized (up to 4.4 O/nm²). It has been suggested that the chemical and electronic properties of the carbon/metal hydride interface can have a large influence on hydrogen storage properties. However, no significant impact on the first H₂ release temperatures was found. In contrast, the surface properties of the carbon played a major role in determining the reversible hydrogen storage capacity. Only a part of the oxygen-containing groups reacted with hydrides during melt infiltration, but further reaction during cycling led to significant losses, with reversible hydrogen storage capacity loss up to 40% for surface oxidized carbon. However, if the carbon surface had been hydrogen terminated, ∼6 wt% with respect to the NaAlH₄ weight was released in the second cycle, corresponding to 95% reversibility. This clearly shows that control over the nature and amount of surface groups offers a strategy to achieve fully reversible hydrogen storage in complex metal hydride-carbon nanocomposites.     

Synergistic effects of multiwalled carbon nanotubes and Al on the electrochemical hydrogen storage properties of Mg2Ni-type alloy prepared by mechanical alloying

Mg_2−xAl_xNi (x = 0, 0.25) electrode alloys with and without multiwalled carbon nanotubes (MWCNTs) have been prepared by mechanical alloying (MA) under argon atmosphere at room temperature using a planetary high-energy ball mill. The microstructures of synthesized alloys are characterized by XRD, SEM and TEM. XRD analysis results indicate that Al substitution results in the formation of AlNi-type solid solution that can interstitially dissolve hydrogen atoms. In contrast, the addition of MWCNTs hardly affects the XRD patterns. SEM observations show that after co-milling with 5 wt. % MWCNTs, the particle sizes of both Mg₂Ni and Mg_1.75Al_0.25Ni milled alloys are decreased explicitly. The TEM images reveal that ball milling is a good method to cut long MWCNTs into short ones. These MWCNTs aggregate along the boundaries and surfaces of milled alloy particles and play a role of lubricant to weaken the adhesion of alloy particles. The majority of MWCNTs retain their tubular structure after ball milling except a few MWCNTs whose tubular structure is destroyed. Electrochemical measurements indicate that all milled alloys have excellent activation properties. The Mg_1.75Al_0.25Ni-MWCNTs composite shows the highest discharge capacity due to the synergistic effects of MWCNTs and Al on the electrochemical hydrogen storage properties of Mg₂Ni-type alloy. However, the improvement on the electrode cycle stability by adding MWCNTs is unsatisfactory.     

Compaction of LiBH4-MgH2 doped with MWCNTs-TiO2 for reversible hydrogen storage

According to catalytic effects of TiO₂ on kinetic properties of hydrides and thermal conductivity of multiwall carbon nanotubes (MWCNTs) favoring heat transfer during de/rehydrogenation, improvement of dehydrogenation kinetics of compacted 2LiBH₄-MgH₂ by doping with MWCNTs decorated with TiO₂ (MWCNTs-TiO₂) is proposed. Via solution impregnation of Ti-isopropoxide on MWCNTs and hydrothermal reaction to produce TiO₂, high surface area and good dispersion of TiO₂ on MWCNTs surface are obtained. Composite of 2LiBH₄-MgH₂ is doped with 5–15 wt. % MWCNTs-TiO₂ and compacted into the pellet shape (diameter and thickness of 8 and 1.00–1.22 mm, respectively). By doping with 15 wt. % MWCNTs-TiO₂, not only fast dehydrogenation kinetics is obtained, but also reduction of onset dehydrogenation temperature (ΔT = 25 °C). Besides, gravimetric and volumetric hydrogen storage capacities of compacted 2LiBH₄-MgH₂ increase to 6.8 wt. % and 68 gH₂/L, respectively, by doping with 15 wt. % MWCNTs-TiO₂ (～twice as high as undoped sample). The more the MWCNTs-TiO₂ contents, the higher the apparent density (up to ～1.0 g/cm³ by doping with 15 wt. % MWCNTs-TiO₂). The latter implies good compaction, resulting in the development of volumetric hydrogen capacity. In the case of mechanical stability during cycling, compacted 2LiBH₄-MgH₂ doped with at least 10 wt. % MWCNTs-TiO₂ maintains the pellet shape after rehydrogenation. Although increase of porosity (up to 30%), leading to the reduction of thermal conductivity, is detected after rehydrogenation of compacted 2LiBH₄-MgH₂ doped with 15 wt. % MWCNTs-TiO₂, comparable kinetics during cycling is obtained. This benefit can be achieved from thermal conductivity of MWCNTs.