ACS Nano
·
2021
·
IF 15.881
Wen Zhu,Li Ren,Chong Lu,Hao Xu,Fengzhan Sun,Zhewen Ma,Jianxin Zou
MXenes are considered as potential support materials for nanoconfinement of MgH2/Mg to improve the hydrogen storage properties. However, it has never been realized so far due to the stacking and oxidation problems caused by unexpected surface terminations (−OH, −O, etc.) on MXenes. In this study, hexadecyl trimethylammonium bromide was used to build a 3D Ti3C2Tx architecture of folded nanosheets to reduce the stacking risk of flakes, and a bottom-up self-assembly strategy was successfully applied to synthesize ultradispersed MgH2 nanoparticles anchored on the surface of the annealed 3D Ti3C2Tx (Ti-MX). The composite with a 60 wt % loading of MgH2 NPs, 60MgH2@Ti-MX, starts to decompose at 140 °C and is capable of releasing 3.0 wt % H2 at 150 °C within 2.5 h. In addition, a reversible capacity up to 4.0 wt % H2 was still maintained after 60 cycles at 200 °C without obvious loss in kinetics. In situ high-resolution TEM observations of the decomposition process together with other analyses revealed that the nanosize effect caused by the nanoconfinement and the multiphasic interfaces between MgH2(Mg) and Ti-MX, especially the in situ formed catalytic TiH2, were main reasons accounting for the superior hydrogen sorption performances.
研究领域:
材料科学
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氢气储存
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纳米技术
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能量存储
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·Vol. 46
·期 55
·28134-28143
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IF 5.816
Jisheng Yang,Kemin Zhang,Zhewen Ma,Xu Zhang,Tianping Huang,Subrata Panda,Jianxin Zou
Herein, a new type of trimesic acid-Ni based metal organic framework (TMA-Ni MOF) was synthesized and then, its derivative Ni@C was introduced into MgH 2 as destabilizer through high energy ball milling to prepare a Mg–Ni@C–H composite. X-ray diffraction analyses indicate the formation of Mg 2 Ni/Mg 2 NiH 4 as major phases after dehydrogenation/rehydrogenation of the composite, respectively. Two hydrogen absorption plateaus are observed in the Mg–Ni@C–H composite, corresponding to the hydrogenation of Mg and Mg 2 Ni, with the enthalpy change values of −75.8 and −52.3 kJ mol −1 H 2 respectively. Thus, it can be concluded that a destabilization effect is brought by Ni@C on thermodynamic properties of MgH 2 . In addition, the hydriding/dehydriding kinetics of MgH 2 is notably accelerated with the addition of Ni-based MOF derivative. The activation energy values of both hydrogen absorption and desorption are significantly lowered down with the assistance of Ni@C. Moreover, stable hydrogen de/absorption capacity and kinetics are remained during 25 cycles of high-rate re/dehydrogenation, which can be ascribed to the carbon-wrapped structure of the composite, with which the aggregation of the nanosized particles can be evidently avioded.
研究领域:
材料科学
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氢能
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金属有机框架
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能量存储
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DOI
高影响因子
Journal of Magnesium and Alloys
·
2026
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IF 15.8
Yulin Huang,Fenghua Wei,Yang Zhang,Xinan Zhang,Yiming Wang,Chen Huang,Yuke Li,Jingcai Chang
Interactions between metals and heteroatom-coordinated sites on the carbon matrix are crucial for enhancing the kinetics and thermodynamics of Mg/MgH 2 . Herein, we reported a sustainable K 2 FeO 4 activation strategy that converts high-sulfur petroleum coke into a sulfur self-doped porous carbon hosting FeNi–S coordinated active sites. Tailoring the alloyed electronic structure and exposing more catalytically active sites substantially enhanced the hydrogenation and dehydrogenation kinetics of Mg/MgH 2 with (FeNi)S@PPC. Its peak dehydrogenation temperature was 95.39 °C lower than that of ball-milled MgH 2 . In addition, it enabled MgH 2 to release 4.89 wt.% H 2 within 20 min at 275 °C, exceeding its sulfur-free counterpart (FeNi)@PPC by 1.41 wt.%. Moreover, the (FeNi)S@PPC/MgH 2 showed 99.5% capacity retention after 30 cycles, indicating excellent reversibility. Mechanistic investigations revealed that intrinsic sulfur self-doping induced a stable FeNi–S coordination environment, which lowered the D-band center of FeNi to −1.349 eV. The electronic redistribution was found to weaken the FeNi–(H) intermediate, lowering the dissociation and diffusion energy barrier by 0.39 eV and facilitating hydrogenation. This also reduced the energy required for Mg–H dissociation into H 2 by 0.65 eV. Consequently, the dehydrogenation activation energy was decreased to 97.09 kJ·mol − 1 , with the rate-limiting step shifting to a low-energy barrier three-dimensional interfacial reaction (R3 model). Overall, this study establishes a green valorization route for high-sulfur petroleum coke and elucidates a fundamental metal–sulfur charge transfer mechanism that substantially enhances magnesium-based hydrogen storage.
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Fangyi Wu,Meijia Liu,Yuanhang Wang,Hansen Zou,Hanqing Xu,Chao Wu,Fangong Kong
The 2LiBH 4 -MgH 2 composite has garnered extensive attention for industrial-scale hydrogen storage due to its excellent hydrogen capacity which has potential in addressing the increasing requirements for elevated energy density and extended cycle life. However, its practical application is still restricted by sluggish dehydrogenation kinetics and unsatisfactory thermodynamic stability. In this study, these limitations are addressed by introducing aluminum fluoride (AlF 3 ) as a catalyst, and the catalytic effect and mechanism are further investigated. The 2LiBH 4 -MgH 2 doped with 10% AlF 3 presents an extremely low onset dehydrogenation temperature of 181.8 °C. Specially, the nucleation period of MgB 2 is further decreased to 137 min, which is 49.91% shorter than that of the unmodified sample. In the case of dehydrogenation, it can release 6.33 wt% H 2 in 15 min at 400 °C. Kinetic analysis shows that the dehydrogenation activation energy is reduced to 174.93 kJ/mol, which is 65.65 kJ/mol lower than that of the ball-milled 2LiBH 4 -MgH 2 . Notably, in terms of hydrogen absorption, 9.38 wt% H 2 is absorbed within 34.2 min at 400 °C. When temperature reaching up to 350 °C, the composite can absorb 4.57 wt% H 2 within 1 h. Mechanistic analysis reveals that AlF 3 reacts with LiH and MgB 2 to generate LiF, MgF 2 , Li 3 AlF 6 and MgAlB 4 , and these products could alter the reaction pathway and further reduce the reaction energy barrier. Additionally, the reversible phase transformations of Al/Mg/Mg 17 Al 12 offer sufficient active sites during the re/dehydrogenation. Finally, MgF 2 and LiF serve as electron-shuttling media, thereby enhancing the hydrogen diffusion kinetics. This study not only proposes a viable method for improving the hydrogen storage behavior of 2LiBH 4 -MgH 2 , but also broadens the understanding of fluoride-assisted catalytic mechanisms.
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DOI
高影响因子
Advanced Energy Materials
·
2026
·
IF 25.5
Xue Ke,Yuanyuan Zhang,Fulai Qi,Qian Zhang,Xinqiang Wang,Yanxia Liu,Ke Wang,Jindou Shi,Zichao Shen,Mingchang Zhang,Yuanchao Yang,Fan Gao,Wengang Cui,Zhenglong Li,Yaxiong Yang,Lixian Sun,Jian Chen,Hongge Pan
Magnesium hydride (MgH 2 ) is widely regarded as a highly promising solid-state hydrogen storage material. However, its practical application is severely constrained by high operating temperatures and sluggish hydrogen absorption/desorption kinetics arising from multistep reaction energy barriers. Here, we rationally tailor a quinary Ti-based rutile-type high-entropy oxide to overcome these intrinsic limitations for the first time. The onset dehydrogenation temperature of the hybrid reduces to 195°C, which is 163°C lower than that of pristine MgH 2 . The composite releases 5.88 wt.% H 2 within 10 min at 250°C, accompanied by a 58% reduction in the apparent dehydrogenation activation energy. Moreover, a 1.84 wt.% H 2 uptake can be achieved within only 20 s at room temperature. The coexistence of various multivalent metal cations, lattice distortions, abundant defects, and oxygen vacancies in (TiNbCrTaFe)O 2 substantially reduces the multi-step reaction energy barriers during MgH 2 de/hydrogenation, enabling the overall kinetics to surpass those of all previously reported high-entropy catalyst-modified MgH 2 systems. This work expands the compositional design space and application scope of high-entropy oxides and provides a viable strategy for advanced hydrogen storage and catalytic systems.
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产品关联
DOI
高影响因子
Journal of Magnesium and Alloys
·
2025
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IF 13.8
Xiaoying Yang,Xinqiang Wang,Ruijie Liu,Yanxia Liu,Zhenglong Li,Wengang Cui,Fulai Qi,Yaxiong Yang,Jian Chen,Hongge Pan
The role of catalysts in enhancing the hydrogen storage kinetics of the Mg/MgH 2 system is pivotal. However, the exploration of efficient catalysts and the underlying principles of their design remain both a prominent focus and a significant challenge in current research. In this study, we present a bimetallic oxide of Bi 2 Ti 2 O 7 hollow sphere as a highly effective catalyst for MgH 2 . As a result, the Bi 2 Ti 2 O 7 -catalyzed Mg/MgH 2 system lowers the hydrogen desorption initiation temperature to 194.3 °C, reduces the peak desorption temperature to 245.6 °C, decreases the dehydrogenation activation energy to 82.14 kJ·mol −1 , and can absorb 5.4 wt. % of hydrogen within 60 s at 200 °C, demonstrating outstanding hydrogen ab/desorption kinetics, compared to pure MgH 2 . Additionally, it can maintain a high hydrogen capacity of 5.2 wt. %, even after 50 dehydrogenation cycles, showing good cycle stability. The characterization results show that the high-valent Bi and Ti in Bi 2 Ti 2 O 7 are reduced to their low-valent or even zero-valent metallic states during the dehydrogenation and hydrogenation process, thus establishing an in-situ multivalent and multi-element catalytic environment. Density functional theory calculations further reveal that the synergistic effects between Bi and Ti in the Bi-Ti mixed oxide facilitate the cleavage of Mg-H bonds and lower the kinetic barrier for the dissociation of hydrogen molecules, thereby substantially enhancing the kinetics of the Mg/MgH 2 system. This study presents a strategic method for developing efficient catalysts for hydrogen storage materials by harnessing the synergistic effects of metal elements.
研究领域:
材料科学
·
能源存储
·
催化
·
纳米技术
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Magnesium and Alloys
·
2025
·
IF 13.8
Guorong Zhang,Taigen Liang,Fen Xu,Lixian Sun,Sheng Wei,Jiaxi Liu,Lina Qin,Xia Lin,Yongpeng Xia
Magnesium hydride (MgH 2 ) is a promising solid-state hydrogen storage material due to its high hydrogen content and cyclic stability. However, its practical applications are limited by slow desorption kinetics and a high dehydrogenation temperature. To address these challenges, Pt-loaded MAX fibers with oxygen vacancies (Pt@MFs) have been synthesized by using vortex and hydrothermal methods. And the effects of the Pt@MFs on the hydrogen storage properties of MgH 2 are investigated. The results display that the MgH 2 doped with 10wt% Pt@MFs begins dehydrogenation at 169.3 °C and absorbs 5.73 wt% hydrogen in just 30 s at 125 °C and 30 bar hydrogen pressure. After 30 cycles, the MgH 2 –10 wt% Pt@MFs retains 98.7% of its initial capacity, showcasing excellent cycling stability. The synergistic effect of the MAX fiber network's active sites, oxygen vacancies, anchored Pt nanoparticles and intermetallic compounds (PtTi, Pt 3 Ti) in the MgH 2 –10 wt% Pt@MFs composite significantly enhances hydrogen storage kinetics by facilitating diffusion, optimizing electron transfer, and weakening Mg-H bonds. The design concept of this material offers a novel strategy for improving the kinetics and stability of MgH 2 .
研究领域:
材料科学
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纳米科技
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能源化学
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固体化学
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催化化学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Wen Zhu,Subrata Panda,Chong Lu,Zhewen Ma,Darvaish Khan,Jinjian Dong,Fengzhan Sun,Hao Xu,Qiuyu Zhang,Jianxin Zou
In this work, we report the remarkable catalytic effects of a novel Ti3C2 MXene-based catalyst (Ni@Ti-MX), which was prepared via self-assembling of Ni nanoparticles onto the surface of exfoliated Ti3C2 nanosheets. The resultant Ni@Ti-MX catalyst, characterized by ultradispersed Ni nanoparticles being anchored on the monolayer Ti3C2 flakes, was introduced into MgH2 through ball milling. In situ transmission electron microscopy (TEM) analysis revealed that a synergetic catalytic effect of multiphase components (Mg2Ni, TiO2, metallic Ti, etc.) derived in the MgH2 + Ni@Ti-MX composite exhibits remarkable improvements in the hydrogen sorption kinetics of MgH2. In particular, the MgH2 + Ni@Ti-MX composite can absorb 5.4 wt % H2 in 25 s at 125 °C and release 5.2 wt % H2 in 15 min at 250 °C. Interestingly, it can uptake 4 wt % H2 in 5 h even at room temperature. Furthermore, the dehydrogenation peak temperature of the MgH2 + Ni@Ti-MX composite is about 221 °C, which is 50 and 122 °C lower than that of MgH2 + Ti-MX and MgH2, respectively. The excellent hydrogen sorption properties of the MgH2 + Ni@Ti-MX composite are primarily attributed to the peculiar core–shell nanostructured MgH2@Mg2NiH4 hybrid materials and the interfacial coupling effects from different catalyst–matrix interfaces. The results obtained in this study demonstrate that using self-assembling of transition-metal elements on two-dimensional (2D) materials as a catalyst is a promising approach to enhance the hydrogen storage properties of MgH2.
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2018
·
IF 4.229
Xin Zhang,Zhengyang Shen,Ni Jian,Jianjiang Hu,Fang Du,Jianhua Yao,Mingxia Gao,Yongfeng Liu,Hongge Pan
Herein, we demonstrate the successful preparation of a novel complex transition metal oxide (TiVO 3.5 ) by oxidizing a solid-solution MXene (Ti 0.5 V 0.5 ) 3 C 2 at 300 °C and its high activity as a catalyst precursor in the hydrogen storage reaction of MgH 2 . The prepared TiVO 3.5 inherits the layered morphology of its MXene precursor, but the layer surface becomes very coarse because of the presence of numerous nanoparticles . Adding a minor amount of TiVO 3.5 remarkably reduces the dehydrogenation and hydrogenation temperatures of MgH 2 and enhances the reaction kinetics. The 10 wt% TiVO 3.5 -containing sample exhibits optimal hydrogen storage properties, as it desorbs approximately 5.0 wt% H 2 in 10 min at 250 °C and re-absorbs 3.9 wt% H 2 in 5 s at 100 °C and under 50 bar of hydrogen pressure. The apparent activation energy is calculated to be approximately 62.4 kJ/mol for the MgH 2 -10 wt% TiVO 3.5 sample, representing a 59% reduction in comparison with pristine MgH 2 (153.8 kJ/mol), which reasonably explains the remarkably reduced dehydrogenation operating temperature. Metallic Ti and V are detected after ball milling with MgH 2 ; they are uniformly dispersed on the MgH 2 matrix and act as actual catalytic species for the improvement of the hydrogen storage properties of MgH 2 .
研究领域:
材料科学
·
能源存储
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.3
Quanhui Hou,Qianyang Wang,Xiao Xu,Zhihao Xu,Peng Jiang,Maziar Ashuri,Yunxuan Zhou,Zhao Ding
Developing efficient and scalable catalysts remains crucial for advancing practical MgH 2 -based solid-state hydrogen storage. In this work, an oxide-precatalyst strategy is proposed, where Fe 3 O 4 nanoparticles are uniformly anchored on leaf-derived porous carbon to form a Fe 3 O 4 /leaf-carbon catalyst that converts in situ into highly dispersed Fe/MgO interfaces during the initial dehydrogenation process. The resultant MgH 2 + 10 wt% Fe 3 O 4 /leaf-carbon composite exhibits a markedly improved hydrogen sorption performance, with an onset desorption temperature of 215 °C, releasing 6.41 wt% H 2 within 8 min at 350 °C, and reabsorbing 6.22 wt% H 2 at 175 °C (3 MPa) within 1 h. Notably, the activation energies for hydrogenation and dehydrogenation are drastically reduced to 53.27 kJ mol −1 and 91.45 kJ mol −1 , respectively. Furthermore, after undergoing 20 consecutive adsorption cycles, this composite material still maintained 96.3 % of its hydrogen storage capacity compared to the initial hydrogen absorption. Structural characterizations confirm that Fe 3 O 4 is reduced to Fe while forming a stable Fe/MgO heterointerface that provides abundant active sites and accelerates hydrogen diffusion. This study elucidates the oxide-to-metal interface transformation mechanism as an effective pathway to simultaneously lower thermodynamic barriers and enhance kinetic reversibility, offering a cost-effective and sustainable strategy for engineering next-generation MgH 2 -based hydrogen storage materials.
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产品关联
DOI
高影响因子
Progress in Natural Science-Materials International
·
2021
·Vol. 31
·期 1
·152-158
·
IF 3.607
Zhonghui Sun,Jia Zhou,Qingan Zhang
A new MgH 2 –PrF 3 –Al–Ni composite was prepared by ball milling under hydrogen atmosphere. After initial dehydrogenation and rehydrogenation, Pr 3 Al 11 , MgF 2 , PrH 3 and Mg 2 NiH 4 nanoparticles formed accompanying the main phase MgH 2 . The hydrogen absorption-desorption properties were measured by using a Sieverts-type apparatus. The results showed that the MgH 2 –PrF 3 –Al–Ni composite improved cycle stability and enhanced hydrogen desorption kinetics. The improvement of hydrogen absorption-desorption properties is ascribed to the synergetic effect of the in situ formed Pr 3 Al 11 , MgF 2 , PrH 3 and Mg 2 NiH 4 nanoparticles. This work provides an important inspiration for the improvement of hydrogen storage properties in Mg-based materials.
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Chia-Tse Lee,Haoyuan Zheng,Chen Jin,Hang Che,Li Wang,Yuyuan Zhao,Shixuan He,Xinhua Wang,Yifeng Yu,Mi Yan
Metal nitrogen hydride (Li-Mg-N-H) is regarded as an ideal hydrogen storage material for automotive applications due to its advantages of high hydrogen storage capacity (5.6 wt%), low operating temperature, and good cycling performance, but the comprehensive hydrogen storage performance of this material still could be improved. For this reason, this paper constructed a Li-Na-Mg-N-H composite system by synthesizing NaMgH 3 to replace MgH 2 in the Li-Mg-N-H system. The improvement of the hydrogen absorption and desorption properties of the composite system after the replacement of MgH 2 by NaMgH 3 was investigated. Various properties and test results showed that the composite system after the replacement of MgH 2 by NaMgH 3 showed better hydrogen absorption and desorption properties. The initial/peak hydrogen release temperatures of Li-Na-Mg-N-H decreased from 135 ˚C/245 ˚C to 105 ˚C/145 ˚C, and the apparent activation energy of hydrogen release was reduced from 114.90 to 104.05 kJ/mol which means the kinetics of hydrogen absorption and desorption was greatly improved. The mechanism study shows that NaMgH 3 will react with LiNH 2 and forms the intermediate product Li 3 Na(NH 2 ) 4 during the hydrogen release process, which changes the hydrogen desorption pathway of the composite system and thus the hydrogen absorption and desorption kinetics were improved.
研究领域:
材料科学
·
氢气储存
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能源材料
·
固态化学
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DOI
高影响因子
危险品化学品经营许可证（带存储）