International Journal of Minerals Metallurgy and Materials
·
2022
·Vol. 30
·期 1
·54-62
·
IF 3.85
Xu Nuo,Yuan Zirui,Ma Zhihong,Guo Xinli,Zhu Yunfeng,Zou Yongjin,Zhang Yao
MgH 2 with a large hydrogen capacity is regarded as a promising hydrogen storage material. However, it still suffers from high thermal stability and sluggish kinetics. In this paper, highly dispersed nano-Ni has been successfully prepared by using the polyol reduction method with an average size of 2.14 nm, which significantly improves the de/rehydrogenation properties of MgH 2 . The MgH 2 —10wt% nano-Ni sample starts releasing H 2 at 497 K, and roughly 6.2wt% H 2 has been liberated at 583 K. The rehydrogenation kinetics of the sample are also greatly improved, and the adsorption capacity reaches 5.3wt% H 2 in 1000 s at 482 K and under 3 MPa hydrogen pressure. Moreover, the activation energies of de/rehydrogenation of the MgH 2 —10wt% nano-Ni sample are reduced to (88 ± 2) and (87 ± 1) kJ·mol −1 , respectively. In addition, the thermal stability of the MgH 2 —10wt% nano-Ni system is reduced by 5.5 kJ per mol H 2 from that of pristine MgH 2 . This finding indicates that nano-Ni significantly improves both the thermodynamic and kinetic performances of the de/rehydrogenation of MgH 2 , serving as a bi-functional additive of both reagent and catalyst.
研究领域:
材料科学
·
化学工程
·
能源存储
✓ 已验证
DOI
高影响因子
CHEMISTRY OF MATERIALS
·
2024
·
IF 7.2
Yichen Qi,Zeyang Zhang,Qinke Tang,Jiangchuan Liu,Rui Shi,Jiguang Zhang,Yana Liu,Jun Wang,Jiankun Zhang,Shihao Chen,Yunfeng Zhu
Catalysis has been demonstrated to be effective in enhancing the kinetics of MgH2, which has been widely investigated as one of the most promising solid-state hydrogen storage materials. It is essential and challenging to design catalysts with high activity and to understand the corresponding interaction mechanisms between the catalysts and MgH2, especially for multiphase catalyst systems. In this study, an elaborated VS2/NiS2 catalyst based on well-combined components and heterostructure is exploited to substantially improve the hydrogen storage performance of MgH2. Impressively, rapid dehydrogenation (3.4 wt % H2 in 900 s at 498 K) and low-temperature hydrogenation (3.7 wt % H2 in 7200 s at 348 K) properties are achieved in the MgH2–VS2/NiS2 system. The activation energies for the hydrogen absorption/desorption are calculated to be 32.1/86.7 kJ mol–1, which represents a considerable reduction of 60.9% and 43.6% compared to the as-milled MgH2, respectively. Detailed investigations reveal that the enhanced hydrogen absorption/desorption kinetics are mainly attributed to the synergistic effect induced by the in situ-formed Mg2Ni/VH2 heterostructure and the “hydrogen pump” of Mg2Ni/Mg2NiH4. The Mg2Ni/VH2 heterostructure elongate Mg–H bonds, while the “hydrogen pump” of Mg2Ni/Mg2NiH4 facilitate H transfer. This work offers a fresh perspective for application of multicomponent catalysts in the field of metal hydrides.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
·
2020
·Vol. 45
·期 2
·3129-3141
·
IF 3.741
Xuelian Zhang,Ke Wang,Xin Zhang,Jianjiang Hu,Mingxia Gao,Hongge Pan,Yongfeng Liu
Summary High operation temperatures and slow reaction kinetics are major obstacles to use MgH 2 as a solid hydrogen store. We report here the synthesis of Nb 2 O 5 hollow spheres (o-Nb 2 O 5 ) with wall thickness of approximately 50 nm and mossy surfaces using a facile hydrothermal and calcination process, which showed high activity in catalysis of MgH 2 for hydrogen storage. The dehydrogenation onset temperature of MgH 2 was decreased to 195°C with 7 wt% of o-Nb 2 O 5 . More than 5.5 wt% H 2 can be desorbed at 300°C within 5 minutes. Hydrogen re-absorption starts even at 25°C and reaches 5.6 wt% within 5 minutes at 200°C. Practical hydrogen capacity stabilizes at 5.8 wt% after 10 cycles of hydrogen uptake/release. The o-Nb 2 O 5 was found to be reduced in situ by MgH 2 to low-valence Nb species during the initial dehydrogenation process, which functions as an active catalyst and leads to the enhanced dehydrogenation kinetics.
研究领域:
材料科学
·
催化
·
能源存储
✓ 已验证
DOI
高影响因子
Nanoscale
·
2024
·
IF 5.8
Lei Sun,Rong Sun,Jianjun Liu,Mengzhou Zhu,Xiaoqin Zhang,Dongliang Guo,Kangyong Yin,Zhiyun Zhuang,Xueqiong Zhu,Peng Xiao
MgH2 used in solid-state hydrogen storage still suffers from high thermal stability and slow hydrogen absorption–desorption kinetics. Here, we report a hybrid of MgH2–Ti3C2/graphene prepared through a facile wet chemical method followed by a ball-milling method. It was confirmed that the coupling of Ti3C2 and graphene possesses a synergistic effect on the hydrogen desorption and absorption reactions of MgH2/Mg. The initial temperature of MgH2–Ti3C2/graphene to desorb hydrogen was reduced to 169 °C significantly and it could desorb 6.8 wt% H2 within 6 min at a constant temperature of 300 °C. Moreover, the desorbed sample could start to absorb hydrogen at room temperature and achieve a capacity of 6.0 wt% when the temperature was gradually increased to 350 °C. These results are far superior to pristine MgH2, disclosing that the addition of two-dimensional Ti3C2/graphene is an efficient strategy to boost the hydrogen storage performance of MgH2.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2022
·
IF 6.76
Jiaqi Zhang,Quanhui Hou,Yanbing Liu,Xinglin Yang
The design of catalysts with excellent catalytic activity plays an important role in the field of solid-state hydrogen storage of new energy sources. Herein, a novel hydrangea-like NiO@NiMoO 4 composite catalyst was prepared through a facile hydrothermal reaction. Subsequently, NiO@NiMoO 4 was doped into MgH 2 by ball milling to solve the problems of high dehydrogenation temperature and slow desorption kinetics of MgH 2 . It can be seen from the experimental results that the MgH 2 + 10 wt% NiO@NiMoO 4 composite starts to dehydrogenate at about 190 °C, which is about 170 °C lower than that of pure MgH 2 . Meanwhile, after complete dehydrogenation, the composites can start to absorb hydrogen below 40 °C. Compared with pure MgH 2 , the activation energy of hydrogen absorption and dehydrogenation of the composite decreased by 47.6 kJ/mol and 46.5 kJ/mol, respectively. In 10th cycle tests, the MgH 2 + 10 wt% NiO@NiMoO 4 composite still has good cycle stability. After adding a small amount of biomass charcoal, the hydrogen storage capacity can even be maintained above 97%. Furthermore, the characterization results show that the in situ generated new species Mo and Mg 2 Ni/Mg 2 NiH 4 synergistically promote the adsorption and dissociation of hydrogen. This new synergistic mechanism provides new comprehensive insights for improving reversible hydrogen storage in MgH 2 .
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2022
·Vol. 9
·期 15
·3874-3884
·
IF 7.779
Mengchen Song,Liuting Zhang,Zhendong Yao,Jiaguang Zheng,Danhong Shang,Lixin Chen,Hong Li
Maintaining fast hydrogen storage kinetics is a key challenge for the practical application of MgH2. To address this challenge, understanding the mechanism of kinetics that declines during cycling is crucial but it has not been systematically investigated to date. In this paper, three different Fe nanocatalysts were synthesized and then doped into MgH2 to form new composites. The MgH2-Fe composite had significantly reduced operating temperatures and activation energy compared to that of undoped MgH2. During cycling, a capacity retention of 93.4% was obtained after the 20th cycle. For a better understanding of the declining performance, prolonged incubation was intentionally performed. Grain growth was found in MgH2 and the Fe nanocatalysts, which was directly responsible for capacity loss and kinetic degradation. These findings provide fundamental insights to facilitate designing and preparing catalytic hydrogen storage systems with superior cycling performance.
研究领域:
材料科学
·
能源工程
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Jianshe Zhang,Chunling Zheng,Yingjie Wang,Tingting Zhai,Yanghuan Zhang,Dianchen Feng
This research paper explores the influence of varying the quantity of La–Ni@3DG catalyst on the hydrogen storage capabilities of MgH 2 . La–Ni@3DG catalyst was prepared using lanthanum chloride heptahydrate and nickel chloride hexahydrate as raw materials combined with three-dimensional graphene, then mixed with MgH 2 via ball milling to prepare MgH 2 + x wt.% La–Ni@3DG ( x = 0, 3, 5, 7) composite alloy. X-ray diffraction analysis showed that the composite alloy was mainly composed of the MgH 2 phase, with the presence of Mg and (La, Ni) phases detected. With increased La–Ni@3DG addition, the broadening of the MgH 2 diffraction peak significantly improved, indicating the catalyst promoted alloy phase structure uniformity and crystallinity. The composite alloy forms new phases such as LaH 3 , LaNi 3 H 6 , and Mg 2 NiH 4 during hydrogen absorption. These phases cooperate with in-situ formed LaH 3 and Mg 2 Ni to significantly improve the reversible hydrogen absorption and desorption properties of MgH 2 . Adding La–Ni@3DG catalyst has a significant positive effect on the hydrogen absorption and desorption of MgH 2 , leading to a considerable improvement. At 553 K, the composite alloy reaches hydrogen absorption equilibrium faster than pure MgH 2 , and the temperature for hydrogen absorption is significantly reduced to 373 K. The dehydrogenation performance is also improved, with 5 wt.% La–Ni@3DG is showing the best dehydrogenation performance at 553 K. The initial dehydrogenation temperature commences at approximately 505 K, while the dehydrogenation activation energy attains its minimum value: a remarkably low 109.91 kJ/mol H 2 . Additionally, the addition of catalyst reduces the pressure of the hydrogen absorption and desorption platform, effectively reducing the hysteresis effect during hydrogen absorption and desorption when the catalyst content is 5 wt.%, the enthalpy change and entropy change of the composite alloy reach a minimum, −70.45 kJ/mol H 2 and 74.38 kJ/mol H 2 (hydrogen absorption), −101.93 J/K/mol H 2 and 103.68 J/K/mol H 2 (hydrogen desorption), respectively.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2020
·
IF 6.155
Chongyang Yuan,Wei Chen,Zunxian Yang,Zhenguo Huang,Xuebin Yu
MgH 2 is regarded as a potential hydrolysis material for the hydrogen generation due to its high theoretical hydrogen yield, abundant source on earth and environmentally friendly hydrolysates. However, the quickly formed passive magnesium hydroxide layer on the surface of MgH 2 will hinder its further hydrolysis reaction, leading to sluggish reaction kinetics and low H 2 yield. In this paper, we explore the improvement of different anions and cations in solutions for the hydrolysis of MgH 2 . It is found that the cations in the solution promote the reaction rate of MgH 2 hydrolysis through the hydrolysate-induced growth effect, among which the fastest hydrogen yield can get 1664 mL/g within a few minutes in the Fe 2 (SO 4 ) 3 solution. As for the anions, it enables different microstructures of the Mg(OH) 2 hydrolysate which give rise to enhanced water utilization. Specially, for the mixed 0.5 M MgCl 2 + 0.05 M MgSO 4 solution, the water utilization rate attains the optimum value of 51.3 %, much higher than that of the single MgCl 2 or MgSO 4 solutions. These findings are of great significance for the application of MgH 2 hydrolysis as hydrogen generation.
研究领域:
材料科学
·
化学工程
·
氢能
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2019
·Vol. 11
·期 15
·7465-7473
·
IF 6.97
Meng Zhang,Xuezhang Xiao,Xinwei Wang,Man Chen,Yunhao Lu,Meijia Liu,Lixin Chen
Transition metal compounds are one of the highly efficient types of catalyst for improving the reaction kinetics of hydrogen storage materials. Among all the transition metals, titanium and its compounds show great catalytic effects on magnesium hydride. In this study, for the first time, TiO2 nanosheets with exposed {001} facets were synthesized and doped into MgH2. The TiO2 nanosheet (NS)-doped MgH2 showed superior kinetic performance and the lowest desorption temperature. The onset temperature of MgH2 + 5 wt% TiO2 NS for the release of hydrogen was 180.5 °C and the corresponding peak temperature was 220.4 °C, which are much lower than those of pure MgH2 and also distinctly lower than those of MgH2 + 5 wt% TiO2 nanoparticles (NP). For the isothermal dehydrogenation analysis, the MgH2 + 5 wt% TiO2 NS could release 6.0 wt% hydrogen within 3.2 min at 260 °C and desorb 5.8 wt% hydrogen within 6 min at 240 °C. It is worth noting that the MgH2 + 5 wt% TiO2 NS can even release 1.2 wt% hydrogen at a temperature as low as 180 °C within 300 min. The hydrogenation kinetics of MgH2 + 5 wt% TiO2 NS is also greatly improved, which could absorb hydrogen within only a few seconds at mild temperature. It can take up 3.3 wt% hydrogen at 50 °C and 5.4 wt% at 100 °C within 10 s. It is demonstrated that the tremendous enhancement in reaction kinetics of MgH2 can be ascribed to the nanometer size and highly active {001} facets of anatase TiO2. The higher average surface energy can significantly reduce the hydrogen desorption activation energy of MgH2 to 67.6 kJ mol−1, thus easily improving the hydrogen desorption properties.
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Tian Tian,Fang Liu,Xiaoying Zhang,Jiali Wang,Shengting Li,Wei Chen,Yufei Song,Jinping Li,Guang Liu
In the field of solid hydrogen storage , Magnesium hydride (MgH 2 ) is the promising material. However, the practical application was hindered due to slow kinetics performance and unfavorable thermodynamic property. In this study, porous nanosheet NiO was prepared by the calcination of Ni(OH) 2 synthesized using the hydrothermal way and subsequently introduced in MgH 2 by ball milling . The resulting MgH 2 -5 wt% NiO material conveyed significantly enhanced hydrogen storage property. The initial dehydrogenation temperature was decreased to 210 °C, which is 114 °C lower than that of Ball-milling MgH 2 . The MgH 2 -5 wt% NiO released 6.4 wt% H 2 within 10 min at 300 °C.And at room temperature it begins to uptake hydrogen. The MgH 2 -5 wt% NiO composite also displayed excellent cyclic stability, retaining the 96.2 % of capacity retention rate after 40 cycles. Furthermore, added NiO catalyst reduced the hydrogen desorption activation energy of MgH 2 from 133.69 ± 12.55 kJ/mol to 81.47 ± 7.48 kJ/mol. The superior performance owed to the in-situ generation of Mg 2 Ni/Mg 2 NiH 4 during the reaction between NiO and MgH 2 . These intermediates act as the “hydrogen pump,” weakening the Mg–H bond strength to improving the hydrogen storage properties of MgH 2 . This study displays that the catalyst of porous nanosheet NiO can obviously better the hydrogen storage property of MgH 2 , making it a more viable candidate for practical applications.
研究领域:
材料科学
·
能源化学
·
纳米材料
·
固态储氢
·
催化化学
·
热力学与动力学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Shiteng Long,Yang Qin,Huafeng Fu,Jia Hu,Hansong Xue,Yu'an Chen,Fusheng Pan
Developing medium temperature hydrogen storage materials is important for the practical application of the Studies have demonstrated that V-based catalysts exhibit exceptional catalytic activity in the dehydrogenation of MgH 2 at medium levels. However, the V-base catalysts primarily concentrates on hydrogen desorption, and there is a necessity for further enhancement of hydrogen absorption properties. To solve this problem, herein we prepared a bimetallic oxide. Co can enhance the hydrogen absorption and desorption properties of MgH 2 as the catalyst and it influences the performance of hydrogen absorption more obviously than the hydrogen desorption performance. It is found that MgH 2 catalyzed by Co 3 V 2 O 8 can absorb 1.31 wt% hydrogen within 30 min even under room temperature and can release 3.41 wt% hydrogen within 120 min at temperatures as low as 225 °C. The activation energy of MgH 2 -6 wt.%Co 3 V 2 O 8 is determined to 68.5 kJ/mol, which is 50.2 % lower than that of Ball-MgH 2 . XRD combined with TEM measurements revealed that the in-situ formed Co and V 2 O 3 can weaken the H H and Mg H bonds respectively to improve the hydrogen storage properties of MgH 2 . These discoveries provide guideline of the further design of high efficiency catalysts for Mg-based hydrogen storage materials.
研究领域:
材料科学
·
化学工程
·
催化
·
能源存储
✓ 已验证
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2023
·
IF 10.9
Yuxiao Jia,Xuancheng Wang,Leijie Hu,Xuezhang Xiao,Shuoqing Zhang,Jiahuan He,Jiacheng Qi,Ling Lv,Fen Xu,Lixian Sun,Lixin Chen
Ultrafine carbon-based transition metal compounds have been widely investigated as efficient catalysts for enhancing the hydrogen storage performance of magnesium hydride. In this work, the carbon thermal shock method is applied to synthesize the ultrafine carbon-encapsulated NbC nanoparticles with an average grain size of 17.3 nm. The MgH 2 –10 wt% NbC/C composites show excellent low-temperature hydrogen storage performance with the onset dehydrogenation temperature of 196.1 °C, which is 92.2 °C and 98 °C lower than that of MgH 2 –10 wt% NbC and undoped MgH 2 , respectively. Specifically, MgH 2 –10 wt% NbC/C can absorb 6.71 wt% H 2 at 100 °C within 30 min around and retain almost 100% reversible hydrogen desorption capacity after 10 cycles. For the catalytic mechanism, the electron transfer process between multi-valence Nb cations of in-situ formed NbH x and Mg, H atoms can greatly improve the cyclic de/rehydrogenation kinetics of MgH 2 -NbC/C. Besides, the enhancement of dehydrogenation kinetics can also be ascribed to MgH 2 particle refinement by NbC nanoparticles, and destabilization of the Mg-H bond caused by carbon substrate. This investigation not only proves that carbon-encapsulated NbC nanoparticles can greatly enhance the hydrogen storage performance of MgH 2 but provides an idea of preparing carbon-based transition metal carbides as effective catalysts for magnesium-based hydrogen storage materials.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）