Sustainable Energy & Fuels
·
2020
·Vol. 4
·期 5
·2192-2200
·
IF 5.503
Zhewen Ma,Qiuyu Zhang,Wen Zhu,Darvaish Khan,Chuanzhu Hu,Tianping Huang,Wenjiang Ding,Jianxin Zou
TMA-TM (TM = Fe, Ni) MOFs were synthesized successfully by a facile method. A MgH2-TM MOF (TM = Fe, Ni) composite was obtained via ball milling and the corresponding hydrogen storage performance was investigated. Particularly, high-resolution transmission electron microscopy was performed to in situ characterize the dehydrogenation behavior of the MgH2-TM MOF composite. The results reveal that nano α-Fe and Mg2NiH4/Mg2Ni derived from the TMA-TM MOFs display a synergetic improving effect on the de/hydrogenation of MgH2. During the hydrogen desorption process, Mg2NiH4/Mg2Ni works as a “hydrogen pump” to quickly deliver hydrogen and facilitates hydrogen diffusion. Meanwhile, α-Fe accelerates the nucleation and growth of Mg by reducing the nucleation energy of Mg from MgH2. The hydriding activation energy of the MgH2-TM MOF declines to 45.3 kJ mol−1 H2. Meanwhile, the peak dehydriding temperature of the MgH2-TM MOF is 530.9 K, which is much lower compared with the MgH2–Fe MOF composite (541.7 K) and as-milled MgH2 (685.2 K). Therefore, nano Mg2Ni and α-Fe derived from the TMA-TM MOFs can remarkably improve the hydrogen storage properties of the MgH2/Mg system due to their synergetic catalytic effects.
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Linglong Yao,Xuanyu Lyu,Jiguang Zhang,Yana Liu,Yunfeng Zhu,Huaijun Lin,Yao Zhang,Liquan Li
Nanostructuring and catalyzing are effective methods for improving the hydrogen storage properties of MgH 2 . In this work, transition-metal-carbides (TiC, ZrC and WC) are introduced into Mg–Ni alloy to enhance its hydrogen storage performance. 5 wt% transition-metal-carbide containing Mg 95 Ni 5 (atomic ratio) nanocomposites are prepared by mechanical milling pretreatment followed by hydriding combustion synthesis and mechanical milling process, and the synergetic enhancement effects of Mg 2 NiH 4 and transition-metal-carbides are investigated systematically. Due to the inductive effect of Mg 2 NiH 4 and charge transfer effect between Mg/MgH 2 and transition-metal-carbides, Mg 95 Ni 5 -5 wt.% transition-metal-carbide samples all exhibit excellent hydrogen storage kinetic at moderate temperature and start to release hydrogen around 216 °C. Among them, 2.5 wt% H 2 (220 °C) and 4.7 wt% H 2 (250 °C) can be released from the Mg 95 Ni 5 -5 wt.% TiC sample within 1800 s. The unique mosaic structure endows the Mg 95 Ni 5 -5 wt.% TiC with excellent structural stability, thus can reach 95% of saturated hydrogen capacity within 120 s even after 10 cycles of de-/hydrogenation at 275 °C. And the probable synergistic enhancement mechanism for hydrogenation and dehydrogenation is proposed.
研究领域:
材料科学
·
能源工程
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2021
·
IF 3.171
Liuting Zhang,Haijie Yu,Zhiyu Lu,Changhao Zhao,Jiaguang Zheng,Tao Wei,Fuying Wu,Beibei Xiao
High hydrogen desorption temperature and sluggish reaction kinetics are the major limitations for the practical application of MgH 2 . In this study, Co particles with a face centered cubic (FCC) structure and a hexagonal close packed (HCP) structure were prepared facilely and proved to be good catalysts for magnesium hydride. Co particles with FCC structure presented better catalytic effect on MgH 2 than that with HCP structure. Both 7% (mass) Co FCC and HCP particle modified MgH 2 decreased the initial dehydrogenation temperature from 301.3 °C to approximately 195.0 °C, but 7% (mass) Co with FCC structure modified MgH 2 has a faster desorption rate, and around 6.5% (mass) H 2 was desorbed in 10 min at 325 °C. Hydrogen uptake was detected at 70 °C under 3.25 MPa hydrogen pressure and 6.0% (mass) H 2 was recharged in 40 min at 150 °C. The hydrogen desorption and absorption activation energy for 7% (mass) FCC Co modified MgH 2 was significantly decreased to (76.6±8.3) kJ·mol −1 and (68.3±6.0) kJ·mol −1 , respectively. Thermodynamic property was also studied, the plateau pressures of MgH 2 + 7% (mass) FCC Co were determined to be 0.14, 0.28, 0.53 and 0.98 MPa for 300 °C, 325 °C, 350 °C and 375°C. The decomposition enthalpy of hydrogen (Δ H ) for MgH 2 + 7% (mass) FCC Co was (80.6±0.1) kJ·mol −1 , 5.8 kJ·mol −1 lower than that of as-prepared MgH 2 . Moreover, cycling performance for the first 20 cycles revealed that the reaction kinetics and capacity of MgH 2 -FCC Co composite remained almost unchanged. The result of density functional theory calculation demonstrated that cobalt could extract the Mg H bond and reduced the decompose energy of magnesium hydride. Our paper can be presented as a reference for searching highly effective catalysts for hydrogen storage and other energy-related research fields.
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 Magnesium and Alloys
·
2026
·
IF 15.8
Bogu Liu,Shuo Liang,Xingqing Duan,Yawei Li,Haixiang Huang,Tingting Xu,Bao Zhang,Jianguang Yuan,Xiaohong Chen,Ying Wu
High entropy alloys (HEAs) have garnered considerable interest in catalysis owing to their unique characteristics, while transition metal oxides remain widely studied as classical catalysts. Herein, a novel core-shell FeCoNiCrCu/Fe 2 O 3 @C catalyst coated by a micro- and nano-scale amorphous carbon layer was prepared via a relatively facile synthesis method involving complexing multiple metal cations in organic solvents followed by calcination. Compared with MgH 2 , the initial hydrogen desorption temperature of MgH 2 with the FeCoNiCrCu/Fe 2 O 3 @C catalyst decreases significantly from 290 °C to 172 °C, and the peak temperature is reduced to 268 °C. Furthermore, the catalyzed MgH 2 enables hydrogen absorption even at room temperature under 3 MPa. It also demonstrates excellent cyclability, maintaining over 90% of its initial capacity after 50 cycles, along with progressively enhanced dehydrogenation kinetics. The excellent hydrogen storage performance of the catalyzed MgH 2 is contributed to the synergistic interplay of catalytic components collectively, including the “hydrogen diffusion channel” effect of the in-situ generated Co 3 Fe 7 , the “hydrogen pump effect” exhibited by the reversible catalytic phase pair Mg 2 Ni(Cu)/Mg 2 Ni(Cu)H 4 , as well as the multiphase interface composed of HEAs FeCoNiCrCu, Co 3 Fe 7 and MgH 2 . The amorphous carbon prevents particle agglomeration. This study demonstrates that the HEAs can exhibit significant catalytic effects through rational design.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Yana Liu,Yu Zhu,Qinke Tang,Xinkang Shen,Yunfeng Zhu,Jiguang Zhang,Jun Wang,Zhixin Ba,Wenrong Cai,Yuting Huang,Xiaohui Hu
(3DOM) LaNiO 3 catalysts were successfully synthesized and significantly improved the hydrogen storage kinetics of MgH 2 . MgH 2 -5 wt% 3DOM LaNiO 3 can rapidly absorb 5.91 wt% H 2 at 175 °C within 500 s and desorb 6.37 wt% H 2 within 500 s at 300 °C, its hydrogen absorption and desorption rates are 10 and 11 times higher than MgH 2 -5 wt% Nano LaNiO 3 , respectively. This remarkable enhancement is primarily due to its unique 3DOM structure and the synergistic effect of highly dispersed LaH 3 and Mg 2 Ni/Mg 2 NiH 4 formed in situ during the ball milling and first de/re-hydrogenation process. 3DOM structure catalysts are fragile which can make the catalyst distribution more uniform during ball milling process, giving rise to the significantly improved catalytic activity. The theoretical calculation results show that Mg 2 Ni/LaH 3 heterostructure can greatly reduce the hydrogen adsorption energy to −0.768 eV and the heterogeneous interface induces the charge redistribution between Mg 2 Ni and LaH 3 , resulting in a small amount of negative charge accumulating on the surface of Mg 2 Ni. Moreover, highly dispersed LaH 3 and Mg 2 Ni/Mg 2 NiH 4 in the MgH 2 matrix create a multiphase interface, which can provide more active sites and a variety of pathways for hydrogen diffusion. Above reasons contribute to the excellent synergistic catalytic performance of in situ formed LaH 3 and Mg 2 Ni/Mg 2 NiH 4 on MgH 2 . These discoveries hold scientific value for the design and preparation of highly active catalysts using 3DOM materials for hydrogen storage in light-metal hydrides, especially in MgH 2 .
研究领域:
材料科学
·
能源化学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Quanhui Hou,Jinhui Wang,Yang Zhou,Peng Jiang,Yuting Li,Zhao Ding,Qianyang Wang,Yonglian Xiong
Developing sustainable catalysts for magnesium-based hydrogen storage systems is crucial for advancing clean energy technologies. Here, we report a facile synthesis strategy for Co/C nanocomposites using renewable sugarcane bagasse as a carbon precursor, achieving uniform dispersion of Co nanoparticles (<200 nm) within a hierarchically porous carbon matrix. The optimized MgH 2 +10 wt% Co/C composite exhibits dramatically enhanced hydrogen storage performance, with a reduction in dehydrogenation onset temperature from 330.4 °C to 209.4 °C and a 26 % decrease in apparent activation energy. The composite achieves rapid hydrogen uptake (6.2 wt% within 10 min at 150 °C) and excellent cycling stability (6.28 wt% after 10 cycles at 300 °C). Mechanistic studies reveal that the superior performance originates from the synergistic effects between the in-situ formed CoMg 2 /CoMg 2 H 5 phases acting as "hydrogen pumps" and the porous carbon framework providing efficient pathways for mass/heat transfer. This work not only demonstrates an effective approach for developing high-performance hydrogen storage materials from renewable resources but also provides fundamental insights into the rational design of sustainable energy materials.
研究领域:
材料科学
·
能源科学
·
可持续发展
✓ 已验证
产品关联
DOI
高影响因子
RARE METALS
·
2024
·Vol. 43
·期 6
·2623-2635
·
IF 9.6
Hong Fei-Fan,Shi Wei-Tao,Zhao Ruo-Lin,Fan Yi,Liu Zi-Qi,Ding Si-Zhi,Liu Hai-Zhen,Zhou Wen-Zheng,Guo Jin,Lan Zhi-Qiang
Herein, the successful preparation of a single-atom catalyst V–N–C using vanadium-doped zeolitic imidazolate framework (ZIF)-8 as a precursor is reported. The experimental results showed that the V–N–C had a good promoting effect on the hydrogen storage performance of MgH 2 , and the optimal addition amount of V–N–C was 10 wt%. The hydrogenation and dehydrogenation apparent activation energies of 10 wt% V–N–C-catalyzed MgH 2 were reduced by 44.9 and 53.5 kJ·mol −1 , respectively, compared to those of additive-free MgH 2 . The 10 wt% V–N–C-catalyzed MgH 2 could reabsorb 5.92 wt% of hydrogen in 50 min at 150 °C, with a capacity retention rate of 99.1% after 30 cycles of hydrogen absorption and desorption. Mechanism analysis showed that V–N–C was partially transformed into VN and metallic V when it was milled with MgH 2 ; the in-situ-formed VN and metallic V played an important role in improving the hydrogen storage performance of MgH 2 . This approach provides a potential solution for obtaining high-performance Mg-based hydrogen storage materials through synergistic interactions between V, N and C. Graphical abstract
研究领域:
材料科学
·
氢能
·
纳米催化
·
金属有机框架（MOFs）
✓ 已验证
DOI
高影响因子
Nano Energy
·
2019
·
IF 15.548
Meijia Liu,Shuchun Zhao,Xuezhang Xiao,Man Chen,Chenghua Sun,Zhendong Yao,Zhencan Hu,Lixin Chen
Magnesium hydride (MgH 2 ) offers large capacity for hydrogen storage , but poor thermodynamics and kinetics for releasing hydrogen. In this work, the novel 1D bamboo-shaped carbon nanotubes (BCNTs) are firstly used as carriers for the self-assembly of MgH 2 (denoted as MgH 2 @BCNTs). The high specific surface area (262.3 m 2 g -1 ) and large diameter (over 80 nm) of BCNTs contribute to extremely high loading capacity (76.8 mass fraction), small particle size (15–20 nm) and uniform distribution of MgH 2 nanoparticles (NPs). The well-defined MgH 2 @BCNTs shows remarkably improved thermodynamics and kinetics for H 2 adsorption and desorption. In particular, it starts to release hydrogen at about 220 °C, near 170 °C lower than that of the commercial MgH 2 , as well it tends to be hydrogenated even at a relatively low temperature of 100 °C by absorbing 3.56 wt% H 2 . Moreover, a reversible capacity up to 5.79 wt%, including the “dead weight” of BCNTs, and is well maintained after 10 cycles. The dehydrogenation E a and Δ H of MgH 2 @BCNTs can be reduced to 97.97 kJ/mol and 68.92 kJ/mol, which are 111.24 kJ/mol and 6.07 kJ/mol lower than those of the commercial MgH 2 , respectively. By high pressure densification treatment, the MgH 2 @BCNTs system achieves an exceptional volumetric capacity up to 65.90 g/L without obvious performance degeneration, resulting from the special structure of BCNTs with inner intervals which works as supports under ultra-high pressure of 750 MPa. Our innovative design of 1D BCNTs supporting MgH 2 NPs with high loading weight offers new strategy to synchronously improve the gravimetric and volumetric capacity, as well as the hydrogen storage kinetics and thermodynamics of the nanoconfinement system in the future.
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
COMBUSTION AND FLAME
·
2022
·
IF 5.767
Hua Fang,Peng Deng,Rui Liu,Kehua Han,Pengfei Zhu,Jianxin Nie,Xueyong Guo
Metal hydride has been used as a potential energetic material due to its high hydrogen storage density, high reactivity, high mass calorific value and large gas production. But it was still a great challenge towards optimizing and enhancing the energy-releasing properties of metal hydride. In this work, a novel molecular perovskite energetic material (H 2 dabco)[NH 4 (ClO 4 ) 3 ] (DAP-4) was introduced as a high energy oxidant to fabricate metal hydride (MH 2 , M=Mg, Ti, and Zr) based energetic composites. The thermal decomposition, ignition and combustion characteristics of MH 2 -based energetic composites were studied. The results showed that molecular perovskite energetic material DAP-4 was beneficial as oxidant in MH 2 -based high-energy solid composites, which were originated from its high energy properties and strong oxidation capacity. The ignition and combustion reaction mechanisms of MH 2 with DAP-4 as oxidant were provided. This work offered an effective way to realize energy-releasing performance of MH 2 by molecular perovskite energetic materials introduced for their potential application.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Cong Peng,Yongtao Li,Qingan Zhang
Magnesium hydride is a promising hydrogen storage material and how to improve its sorption kinetics is one of challenges in practical applications. In this paper, a new approach is proposed to catalyze MgH 2 with highly dispersed Ni nanoparticles by in-situ hydrogenolysis of nickelocene (NiCp 2 ) in ball milling process. After ball milling under 4 MPa hydrogen atmosphere for 15 h, the MgH 2 –16.1 wt% NiCp 2 sample exhibits a homogeneous morphology where the in-situ formed Ni nanoparticles with size of ~8 nm are highly dispersed in MgH 2 matrix. During initial dehydrogenation , Ni would react with MgH 2 to form Mg 2 Ni which inherits the configuration of its high dispersion. In the subsequent hydrogen absorption and desorption cycles, the much fine and highly dispersed Ni-based catalytic phase contributes to the superior hydrogen desorption kinetics of MgH 2 with a high-capacity retention rate of ~96% after 50 cycles. This work demonstrates that the in-situ formation of highly dispersed catalytic species is beneficial for improving hydrogen storage properties of MgH 2 .
研究领域:
材料科学
·
无机化学
·
能源化学
·
纳米催化
·
氢储能
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 20
·12190-12197
·
IF 10.7
Fanqi Bu,Ali Wajid,Na Yang,Mengyue Gu,Xuewen Zhao,Lei Huang,Xin Ji,Shujiang Ding,Yonghong Cheng,Jinying Zhang
Magnesium hydrides are promising solid-state hydrogen storage materials due to their high gravimetric hydrogen storage density and low cost. However, the high temperature, slow kinetics, and poor cycle stability hinder the practical application of magnesium hydrides as hydrogen storage materials. Here, amorphous TiO2 was embedded into MgH2 particles as hydrogen conveying channels by atomic layer deposition followed by a ball-milling process to improve their hydrogen adsorption and desorption kinetics. The MgH2 particles embedded with amorphous TiO2 were then wrapped by graphene nanosheets (MgH2–20 nm TiO2@Gra) to enhance their cycle stability. The onset hydrogen desorption temperature of MgH2–20 nm TiO2@Gra has been reduced to 199 °C, which is about 100 °C lower than that of pristine MgH2 (290 °C). MgH2–20 nm TiO2@Gra has been demonstrated to rapidly release 6.04 wt% H2 at 275 °C in 10 min, where only 0.086 wt% H2 was released from pristine MgH2 at 300 °C in 10 min. MgH2–20 nm TiO2@Gra has been found to absorb 5.39 wt% H2 at a temperature as low as 50 °C (30 bar H2), where only 1.67 wt% H2 was absorbed by pristine dehydrogenated MgH2 at 200 °C in 20 min. Moreover, MgH2–20 nm TiO2@Gra has been demonstrated to still release 5.92 wt% of H2 after 50 cycles with a capacity retention of 95.5%. The multivalent Ti+ and abundant oxygen defects have been measured during different de/rehydrogenation states to explore the effects of amorphous TiO2 as hydrogen conveying channels. The amorphous TiO2 hydrogen channels with graphene wrappers have been demonstrated to be an effective strategy to enhance the hydrogen storage properties and cycle stability of MgH2, which is applicable for various solid-state hydrogen storage materials.
研究领域:
材料科学
·
氢能
·
纳米材料
·
能量存储
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Wen Li,Jiaxiang Xu,Yaoyu Du,Yana Liu,Yunfeng Zhu,Jiguang Zhang,Rui Shi,Jun Wang
To overcome the hydrogen storage kinetic limitations of magnesium hydride (MgH2), highly effective NiCu bimetallic MOFs with different Ni/Cu ratios were successfully synthesized and introduced into MgH2. The Ni3Cu1 MOF, featuring a distinctive flower-like structure assembled from thin nanosheets, demonstrates the most remarkable catalytic activity in enhancing the hydrogen storage properties of MgH2. The MgH2-8 wt % Ni3Cu1 MOF composite can initiate hydrogen desorption at 198.50 °C and exhibits a significantly reduced dehydrogenation peak temperature of 285.92 °C, in comparison with that of the ball-milled MgH2 (385.5 °C). This composite can rapidly release 6.18 wt % H2 at 300 °C and absorb 5.32 wt % H2 at 150 °C, both within 500 s. The activation energies for dehydrogenation and hydrogenation are reduced to 66.91 and 33.81 kJ/mol H2, respectively. Furthermore, the MgH2-8 wt % Ni3Cu1 MOF presents a capacity retention rate of 93% after 50 cycles, indicating excellent cycle stability. The enhancement in the hydrogen storage performance is mainly attributed to the following two aspects. The distinctive flower-like Ni3Cu1 MOF possesses a relatively large specific surface area, which provides more uniformly dispersed metal active sites and a larger contact area with MgH2. Moreover, the Mg2Ni(Cu)/Mg2Ni(Cu)H4 phases formed in situ during the initial hydrogen de/absorption cycle act as an enhanced “hydrogen pump” to facilitate the de/hydrogenation process of MgH2/Mg. The enhanced effect can be confirmed by theoretical calculations, which reveal a pronounced interfacial electron transfer (0.54 e–) and a marked elongation of the Mg–H bond (2.85 Å) at the MgH2–Mg2Ni(Cu) interface compared to that of the MgH2–Mg2Ni interface. These findings offer a strategy for the design and preparation of bimetallic MOF catalysts to improve the hydrogen storage properties of Mg-based materials.
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DOI
PubMed
高影响因子
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