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Keywords = hydrogen storage and spillover

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36 pages, 7620 KiB  
Review
Hydrogen Energy Storage via Carbon-Based Materials: From Traditional Sorbents to Emerging Architecture Engineering and AI-Driven Optimization
by Han Fu, Amin Mojiri, Junli Wang and Zhe Zhao
Energies 2025, 18(15), 3958; https://doi.org/10.3390/en18153958 - 24 Jul 2025
Viewed by 479
Abstract
Hydrogen is widely recognized as a key enabler of the clean energy transition, but the lack of safe, efficient, and scalable storage technologies continues to hinder its broad deployment. Conventional hydrogen storage approaches, such as compressed hydrogen storage, cryo-compressed hydrogen storage, and liquid [...] Read more.
Hydrogen is widely recognized as a key enabler of the clean energy transition, but the lack of safe, efficient, and scalable storage technologies continues to hinder its broad deployment. Conventional hydrogen storage approaches, such as compressed hydrogen storage, cryo-compressed hydrogen storage, and liquid hydrogen storage, face limitations, including high energy consumption, elevated cost, weight, and safety concerns. In contrast, solid-state hydrogen storage using carbon-based adsorbents has gained growing attention due to their chemical tunability, low cost, and potential for modular integration into energy systems. This review provides a comprehensive evaluation of hydrogen storage using carbon-based materials, covering fundamental adsorption mechanisms, classical materials, emerging architectures, and recent advances in computationally AI-guided material design. We first discuss the physicochemical principles driving hydrogen physisorption, chemisorption, Kubas interaction, and spillover effects on carbon surfaces. Classical adsorbents, such as activated carbon, carbon nanotubes, graphene, carbon dots, and biochar, are evaluated in terms of pore structure, dopant effects, and uptake capacity. The review then highlights recent progress in advanced carbon architectures, such as MXenes, three-dimensional architectures, and 3D-printed carbon platforms, with emphasis on their gravimetric and volumetric performance under practical conditions. Importantly, this review introduces a forward-looking perspective on the application of artificial intelligence and machine learning tools for data-driven sorbent design. These methods enable high-throughput screening of materials, prediction of performance metrics, and identification of structure–property relationships. By combining experimental insights with computational advances, carbon-based hydrogen storage platforms are expected to play a pivotal role in the next generation of energy storage systems. The paper concludes with a discussion on remaining challenges, utilization scenarios, and the need for interdisciplinary efforts to realize practical applications. Full article
(This article belongs to the Section A5: Hydrogen Energy)
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43 pages, 12779 KiB  
Review
Functionalization of Nanomaterials for Energy Storage and Hydrogen Production Applications
by Mohamed Salaheldeen, Ahmed M. Abu-Dief and Tarek El-Dabea
Materials 2025, 18(4), 768; https://doi.org/10.3390/ma18040768 - 10 Feb 2025
Cited by 7 | Viewed by 2144
Abstract
This review article provides a comprehensive overview of the pivotal role that nanomaterials, particularly graphene and its derivatives, play in advancing hydrogen energy technologies, with a focus on storage, production, and transport. As the quest for sustainable energy solutions intensifies, the use of [...] Read more.
This review article provides a comprehensive overview of the pivotal role that nanomaterials, particularly graphene and its derivatives, play in advancing hydrogen energy technologies, with a focus on storage, production, and transport. As the quest for sustainable energy solutions intensifies, the use of nanoscale materials to store hydrogen in solid form emerges as a promising strategy toward mitigate challenges related to traditional storage methods. We begin by summarizing standard methods for producing modified graphene derivatives at the nanoscale and their impact on structural characteristics and properties. The article highlights recent advancements in hydrogen storage capacities achieved through innovative nanocomposite architectures, for example, multi-level porous graphene structures containing embedded nickel particles at nanoscale dimensions. The discussion covers the distinctive characteristics of these nanomaterials, particularly their expansive surface area and the hydrogen spillover effect, which enhance their effectiveness in energy storage applications, including supercapacitors and batteries. In addition to storage capabilities, this review explores the role of nanomaterials as efficient catalysts in the hydrogen evolution reaction (HER), emphasizing the potential of metal oxides and other composites to boost hydrogen production. The integration of nanomaterials in hydrogen transport systems is also examined, showcasing innovations that enhance safety and efficiency. As we move toward a hydrogen economy, the review underscores the urgent need for continued research aimed at optimizing existing materials and developing novel nanostructured systems. Addressing the primary challenges and potential future directions, this article aims to serve as a roadmap to enable scientists and industry experts to maximize the capabilities of nanomaterials for transforming hydrogen-based energy systems, thus contributing significantly to global sustainability efforts. Full article
(This article belongs to the Special Issue Nanotechnology and Nanomaterials for Energy Applications)
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15 pages, 10460 KiB  
Article
Preparation of Nanoporous Carbon from Rice Husk with Improved Textural Characteristics for Hydrogen Sorption
by Bakhytzhan Lesbayev, Nurgali Rakhymzhan, Gaukhar Ustayeva, Yerkebulan Maral, Meiram Atamanov, Moldir Auyelkhankyzy and Ayazhan Zhamash
J. Compos. Sci. 2024, 8(2), 74; https://doi.org/10.3390/jcs8020074 - 11 Feb 2024
Cited by 8 | Viewed by 2113
Abstract
This study proposes a method to control the pore-forming process by performing preliminary mechanical activation of the initial rice husk before carbonization. Preliminary mechanical activation of the initial rice husk leads to the loosening of the intercellular substance and its partial depolymerization, thereby [...] Read more.
This study proposes a method to control the pore-forming process by performing preliminary mechanical activation of the initial rice husk before carbonization. Preliminary mechanical activation of the initial rice husk leads to the loosening of the intercellular substance and its partial depolymerization, thereby increasing the availability of its internal structure for pore formation during carbonization and chemical activation. Using the method described above, nanoporous carbon was obtained with a Brunauer–Emmett–Teller (BET)-calculated specific surface area of 2713 m2/g, a micropore specific surface area calculated by using the Dubinina–Radushkevich (D-R) method of 3099 m2/g, and a total pore volume calculated by using the Barett–Joyner–Halenda (BJH) method of 1.625 cm3/g. Due to these characteristics, the adsorption capacity in the obtained sample was for hydrogen 3.7 wt.% at a temperature of −190 °C and a pressure of 9 kgf/cm2, which is 29.7% higher than the adsorption capacity of nanoporous carbon obtained based on rice husk without mechanical activation. The composite “carbon–platinum” NC-2/Pt10%, at a temperature of 20 °C and a pressure of 9 kgf/cm2, showed an increase in sorption capacity of 27% compared to pure nanoporous carbon NC-2, which is explained by the emergence of the spillover effect. Full article
(This article belongs to the Section Composites Manufacturing and Processing)
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11 pages, 4029 KiB  
Article
Hydrogen Storage Properties of Economical Graphene Materials Modified by Non-Precious Metal Nickel and Low-Content Palladium
by Yiwen Chen, Habibullah, Guanghui Xia, Chaonan Jin, Yao Wang, Yigang Yan, Yungui Chen, Xiufang Gong, Yuqiu Lai and Chaoling Wu
Inorganics 2023, 11(6), 251; https://doi.org/10.3390/inorganics11060251 - 8 Jun 2023
Cited by 12 | Viewed by 3049
Abstract
Ni/Pd co-modified graphene hydrogen storage materials were successfully prepared by a solvothermal method using NiCl2·6H2O and Pd(OAc)2 and reduced graphene oxide (rGO). By adjusting the hydrothermal temperature, Pd–Ni is successfully alloyed, and the size of the obtained nanoparticles [...] Read more.
Ni/Pd co-modified graphene hydrogen storage materials were successfully prepared by a solvothermal method using NiCl2·6H2O and Pd(OAc)2 and reduced graphene oxide (rGO). By adjusting the hydrothermal temperature, Pd–Ni is successfully alloyed, and the size of the obtained nanoparticles is uniform. The electronic structure of Pd was changed by alloying, and the center of the D-band moved down, which promoted the adsorption of hydrogen. The NiPd-rGO-180 sample, in which 180 represents the solvothermal temperature in centigrade (°C), has the highest hydrogen storage capacity of 2.65 wt% at a moderate condition (RT/4MPa). The excellent hydrogen storage performance benefits from the synergistic hydrogen spillover effect of Pd–Ni bimetal. The calculated hydrogen adsorption energies of Ni2Pd2-rGO are within the ideal range (−0.20 to −0.60 eV) of hydrogen ads/desorption; however, the introduction of substrate defects and the cluster orientation alter the hydrogen adsorption energy. This work provides an effective reference for the design and optimization of carbon-based hydrogen storage materials. Full article
(This article belongs to the Special Issue 10th Anniversary of Inorganics: Inorganic Materials)
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13 pages, 6037 KiB  
Article
In Situ Ni-Doped Hierarchically Porous Carbon Nanofibers Derived from Polyacrylonitrile/Pitch for Hydrogen Storage at Ambient Temperature
by Fuquan Song, Lintao Huang, Heying Ding, Shiming Zhang and Jinbiao Yu
Sustainability 2023, 15(11), 8722; https://doi.org/10.3390/su15118722 - 29 May 2023
Cited by 12 | Viewed by 2103
Abstract
Porous carbon nanofibers doped with nickel (Ni) were successfully fabricated through electrospinning, carbonization, and CO2 activation techniques using polyacrylonitrile (PAN) and petroleum pitch as carbon sources and nickel acetate as the dopant. During the activation process, Ni was reduced and dispersed in [...] Read more.
Porous carbon nanofibers doped with nickel (Ni) were successfully fabricated through electrospinning, carbonization, and CO2 activation techniques using polyacrylonitrile (PAN) and petroleum pitch as carbon sources and nickel acetate as the dopant. During the activation process, Ni was reduced and dispersed in situ on the carbon matrix. The effects of Ni doping content on the morphology and structure of the carbon nanofibers were systematically investigated using SEM, TEM, XPS, XRD, Raman, and BET analyses. The experimental results revealed that the prepared materials had a hierarchically porous structure and that Ni nanoparticles played multiple roles in the preparation process, including catalyzing pore expansion and catalytic graphitization. However, particle agglomeration and fiber fracture occurred when the Ni content was high. In the adsorption/desorption experiments, the sample with 10 wt% Ni doping exhibited the highest specific surface area and micropore volume of 750.7 m2/g and 0.258 cm3/g, respectively, and had the maximum hydrogen storage capacity of 1.39 wt% at 298 K and 10 MPa. The analyses suggested that the hydrogen adsorption mechanism contributed to enhanced H2 adsorption by the spillover effect in addition to physisorption. Full article
(This article belongs to the Special Issue Advanced Energy Materials for Sustainability)
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13 pages, 2296 KiB  
Article
On the Problem of “Super” Storage of Hydrogen in Graphite Nanofibers
by Yury S. Nechaev, Evgeny A. Denisov, Alisa O. Cheretaeva, Nadezhda A. Shurygina, Ekaterina K. Kostikova, Andreas Öchsner and Sergei Yu. Davydov
C 2022, 8(2), 23; https://doi.org/10.3390/c8020023 - 29 Mar 2022
Cited by 6 | Viewed by 3500
Abstract
This article is devoted to some fundamental aspects of “super” storage in graphite nanofibers (GNF) of “reversible” (~20–30 wt.%) and “irreversible” hydrogen (~7–10 wt.%). Extraordinary results for hydrogen “super” storage were previously published by the group of Rodriguez and Baker at the turn [...] Read more.
This article is devoted to some fundamental aspects of “super” storage in graphite nanofibers (GNF) of “reversible” (~20–30 wt.%) and “irreversible” hydrogen (~7–10 wt.%). Extraordinary results for hydrogen “super” storage were previously published by the group of Rodriguez and Baker at the turn of the century, which been unable to be reproduced or explained in terms of physics by other researchers. For the first time, using an efficient method of processing and analysis of hydrogen thermal desorption spectra, the characteristics of the main desorption peak of “irreversible” hydrogen in GNF were determined: the temperature of the highest desorption rate (Tmax = 914–923 K), the activation energy of the desorption process (Q ≈ 40 kJ mol−1), the pre-exponential rate constant factor (K0 ≈ 2 × 10−1 s−1), and the amount of hydrogen released (~8 wt.%). The physics of hydrogen “super” sorption includes hydrogen diffusion, accompanied by the “reversible” capture of the diffusant by certain sorption “centers”; the hydrogen spillover effect, which provides local atomization of gaseous H2 during GNF hydrogenation; and the Kurdjumov phenomenon on thermoelastic phase equilibrium. It is shown that the above-mentioned extraordinary data on the hydrogen “super” storage in GNFs are neither a mistake nor a mystification, as most researchers believe. Full article
(This article belongs to the Special Issue Carbon Materials for Physical and Chemical Hydrogen Storage)
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19 pages, 6128 KiB  
Review
Recent Progress Using Solid-State Materials for Hydrogen Storage: A Short Review
by Seul-Yi Lee, Jong-Hoon Lee, Yeong-Hun Kim, Jong-Woo Kim, Kyu-Jae Lee and Soo-Jin Park
Processes 2022, 10(2), 304; https://doi.org/10.3390/pr10020304 - 3 Feb 2022
Cited by 154 | Viewed by 19121
Abstract
With the rapid growth in demand for effective and renewable energy, the hydrogen era has begun. To meet commercial requirements, efficient hydrogen storage techniques are required. So far, four techniques have been suggested for hydrogen storage: compressed storage, hydrogen liquefaction, chemical absorption, and [...] Read more.
With the rapid growth in demand for effective and renewable energy, the hydrogen era has begun. To meet commercial requirements, efficient hydrogen storage techniques are required. So far, four techniques have been suggested for hydrogen storage: compressed storage, hydrogen liquefaction, chemical absorption, and physical adsorption. Currently, high-pressure compressed tanks are used in the industry; however, certain limitations such as high costs, safety concerns, undesirable amounts of occupied space, and low storage capacities are still challenges. Physical hydrogen adsorption is one of the most promising techniques; it uses porous adsorbents, which have material benefits such as low costs, high storage densities, and fast charging–discharging kinetics. During adsorption on material surfaces, hydrogen molecules weakly adsorb at the surface of adsorbents via long-range dispersion forces. The largest challenge in the hydrogen era is the development of progressive materials for efficient hydrogen storage. In designing efficient adsorbents, understanding interfacial interactions between hydrogen molecules and porous material surfaces is important. In this review, we briefly summarize a hydrogen storage technique based on US DOE classifications and examine hydrogen storage targets for feasible commercialization. We also address recent trends in the development of hydrogen storage materials. Lastly, we propose spillover mechanisms for efficient hydrogen storage using solid-state adsorbents. Full article
(This article belongs to the Section Biological Processes and Systems)
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18 pages, 5824 KiB  
Article
Hydrogen Storage in Untreated/Ammonia-Treated and Transition Metal-Decorated (Pt, Pd, Ni, Rh, Ir and Ru) Activated Carbons
by Mohamed F. Aly Aboud, Zeid A. ALOthman and Abdulaziz A. Bagabas
Appl. Sci. 2021, 11(14), 6604; https://doi.org/10.3390/app11146604 - 18 Jul 2021
Cited by 15 | Viewed by 3426
Abstract
Hydrogen storage may be the bottle neck in hydrogen economy, where hydrogen spillover is in dispute as an effective mechanism. In this context, activated carbon (AC) was doped with nitrogen by using ammonia gas, and was further decorated with platinum, palladium, nickel, rhodium, [...] Read more.
Hydrogen storage may be the bottle neck in hydrogen economy, where hydrogen spillover is in dispute as an effective mechanism. In this context, activated carbon (AC) was doped with nitrogen by using ammonia gas, and was further decorated with platinum, palladium, nickel, rhodium, iridium and ruthenium, via an ultrasound-assisted impregnation method, with average particle sizes of around 74, 60, 78, 61, 67 and 38 nm, respectively. The hydrogen storage was compared, before and after modification at both ambient and cryogenic temperatures, for exploring the spillover effect, induced by the decorating transition metals. Ammonia treatment improved hydrogen storage at both 298 K and 77 K, for the samples, where this enhancement was more remarkable at 298 K. Nevertheless, metal decoration reduced the hydrogen uptake of AC for all of the decorated samples other than palladium at cryogenic temperature, but improved it remarkably, especially for iridium and palladium, at room temperature. This observation suggested that metal decoration’s counter effect overcomes hydrogen spillover at cryogenic temperatures, while the opposite takes place at ambient temperature. Full article
(This article belongs to the Special Issue Recent Advances of Hydrogen Storage in Carbon-Based Materials)
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10 pages, 1433 KiB  
Article
H2 Transformations on Graphene Supported Palladium Cluster: DFT-MD Simulations and NEB Calculations
by Francesco Ferrante, Antonio Prestianni, Marco Bertini and Dario Duca
Catalysts 2020, 10(11), 1306; https://doi.org/10.3390/catal10111306 - 12 Nov 2020
Cited by 15 | Viewed by 3464
Abstract
Molecular dynamics simulations based on density functional theory were employed to investigate the fate of a hydrogen molecule shot with different kinetic energy toward a hydrogenated palladium cluster anchored on the vacant site of a defective graphene sheet. Hits resulting in H2 [...] Read more.
Molecular dynamics simulations based on density functional theory were employed to investigate the fate of a hydrogen molecule shot with different kinetic energy toward a hydrogenated palladium cluster anchored on the vacant site of a defective graphene sheet. Hits resulting in H2 adsorption occur until the cluster is fully saturated. The influence of H content over Pd with respect to atomic hydrogen spillover onto graphene was investigated. Calculated energy barriers of ca. 1.6 eV for H-spillover suggest that the investigated Pd/graphene system is a good candidate for hydrogen storage. Full article
(This article belongs to the Special Issue Computational Chemistry and Catalysis: Prediction and Design)
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21 pages, 5769 KiB  
Review
Reversible Hydrogen Storage Using Nanocomposites
by Sesha Srinivasan, Dervis Emre Demirocak, Ajeet Kaushik, Meenu Sharma, Ganga Ram Chaudhary, Nicoleta Hickman and Elias Stefanakos
Appl. Sci. 2020, 10(13), 4618; https://doi.org/10.3390/app10134618 - 3 Jul 2020
Cited by 40 | Viewed by 6219
Abstract
In the field of energy storage, recently investigated nanocomposites show promise in terms of high hydrogen uptake and release with enhancement in the reaction kinetics. Among several, carbonaceous nanovariants like carbon nanotubes (CNTs), fullerenes, and graphitic nanofibers reveal reversible hydrogen sorption characteristics at [...] Read more.
In the field of energy storage, recently investigated nanocomposites show promise in terms of high hydrogen uptake and release with enhancement in the reaction kinetics. Among several, carbonaceous nanovariants like carbon nanotubes (CNTs), fullerenes, and graphitic nanofibers reveal reversible hydrogen sorption characteristics at 77 K, due to their van der Waals interaction. The spillover mechanism combining Pd nanoparticles on the host metal-organic framework (MOF) show room temperature uptake of hydrogen. Metal or complex hydrides either in the nanocomposite form and its subset, nanocatalyst dispersed alloy phases illustrate the concept of nanoengineering and nanoconfinement of particles with tailor-made properties for reversible hydrogen storage. Another class of materials comprising polymeric nanostructures such as conducting polyaniline and their functionalized nanocomposites are versatile hydrogen storage materials because of their unique size, high specific surface-area, pore-volume, and bulk properties. The salient features of nanocomposite materials for reversible hydrogen storage are reviewed and discussed. Full article
(This article belongs to the Special Issue Clean Energy and Fuel Storage 2020)
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13 pages, 4090 KiB  
Article
A Comparison of Hydrogen Storage in Pt, Pd and Pt/Pd Alloys Loaded Disordered Mesoporous Hollow Carbon Spheres
by Martyna Baca, Krzysztof Cendrowski, Wojciech Kukulka, Grzegorz Bazarko, Dariusz Moszyński, Beata Michalkiewicz, Ryszard J. Kalenczuk and Beata Zielinska
Nanomaterials 2018, 8(9), 639; https://doi.org/10.3390/nano8090639 - 21 Aug 2018
Cited by 35 | Viewed by 5371
Abstract
Comprehensive study to evaluate the ability of hydrogen uptake by disordered mesoporous hollow carbon spheres doped witch metal such as Pt, Pd or Pt/Pd was conducted. They were synthesized facilely using sonication and then calcination process under vacuum at the temperature of 550 [...] Read more.
Comprehensive study to evaluate the ability of hydrogen uptake by disordered mesoporous hollow carbon spheres doped witch metal such as Pt, Pd or Pt/Pd was conducted. They were synthesized facilely using sonication and then calcination process under vacuum at the temperature of 550 °C. The effect on hydrogen sorption at neat-ambient conditions (40 °C, up to 45 bar) was thoroughly analyzed. The results clearly revealed that metal functionalization has a significant impact on the hydrogen storage capacity as the mechanism of gas uptake depends on two factors: metal type and certain size of particles. Thus, functionalized spheres adsorb hydrogen by physisorption forming metal hydrides or metal hydrides combined with hydrogen spillover effect. As a result, a sample with narrower distribution of nanoparticles and smaller specific size exhibited enhanced hydrogen uptake. Full article
(This article belongs to the Special Issue Carbon nanostructure for energy storage and conversion)
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13 pages, 1997 KiB  
Article
Hydrogen Storage in Pristine and d10-Block Metal-Anchored Activated Carbon Made from Local Wastes
by Mohamed F. Aly Aboud, Zeid A. ALOthman, Mohamed A. Habila, Claudia Zlotea, Michel Latroche and Fermin Cuevas
Energies 2015, 8(5), 3578-3590; https://doi.org/10.3390/en8053578 - 28 Apr 2015
Cited by 23 | Viewed by 7443
Abstract
Activated carbon has been synthesized from local palm shell, cardboard and plastics municipal waste in the Kingdom of Saudi Arabia. It exhibits a surface area of 930 m2/g and total pore volume of 0.42 cm3/g. This pristine activated carbon [...] Read more.
Activated carbon has been synthesized from local palm shell, cardboard and plastics municipal waste in the Kingdom of Saudi Arabia. It exhibits a surface area of 930 m2/g and total pore volume of 0.42 cm3/g. This pristine activated carbon has been further anchored with nickel, palladium and platinum metal particles by ultrasound-assisted impregnation. Deposition of nanosized Pt particles as small as 3 nm has been achieved, while for Ni and Pd their size reaches 100 nm. The solid-gas hydrogenation properties of the pristine and metal-anchored activated carbon have been determined. The pristine material exhibits a reversible hydrogen storage capacity of 2.3 wt% at 77 K and 3 MPa which is higher than for the doped ones. In these materials, the spillover effect due to metal doping is of minor importance in enhancing the hydrogen uptake compared with the counter-effect of the additional mass of the metal particles and pore blocking on the carbon surface. Full article
(This article belongs to the Special Issue Hydrides: Fundamentals and Applications)
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