ACS Applied Energy Materials
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2024
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IF 5.4
Jiajing Zhu,Hui Wang,Liangjun Huang,Liuzhang Ouyang,Lan Zhang,Min Zhu
Nanosized SrTiO3, a common photocatalyst that enhances water splitting for hydrogen production, has been synthesized to catalyze the reversible hydrogen gas–solid reaction of MgH2. Compared to the pure MgH2, the milled MgH2-SrTiO3 composite shows significantly enhanced hydrogen storage properties, absorbing 3.5 wt % H2 within 1 min at room temperature and releasing 6.1 wt % H2 within 9 min at 250 °C. The activation energy for dehydrogenation is 82.91 kJ/mol, which is 52.09 kJ/mol lower than that of as-milled MgH2. The composite retains a capacity of 5.47 wt % after 40 cycles of dehydrogenation at 250 °C. The catalytic mechanism of nanosized SrTiO3 was discussed. Therefore, like anatase TiO2 photocatalysts, SrTiO3 shows an excellent catalytic effect to enhance the hydrogen sorption of MgH2 at significantly lower temperatures. A significant number of photocatalytsts have great potential to enhance the hydrogen sorption of Mg, making them promising candidates for solid-state hydrogen storage materials.
研究领域:
材料科学
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能源科学
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DOI
高影响因子
Inorganics
·
2023
·Vol. 11
·期 6
·243
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IF 2.9
Xiantun Huang,Chenglin Lu,Yun Li,Haimei Tang,Xingqing Duan,Kuikui Wang,Haizhen Liu
MgH2has a high hydrogen content of 7.6 wt% and possesses good reversibility under normal conditions. However, pristine MgH2requires a high temperature above 300 °C to release hydrogen, with very slow kinetics. In this work, we utilized Ti3CN MXene to reduce the operating temperature and enhance the kinetics of MgH2. The initial temperature of MgH2decomposition can be lowered from 322 °C for pristine MgH2to 214 °C through the employment of Ti3CN. The desorbed MgH2+ 7.5 wt% Ti3CN can start absorption at room temperature, while the desorbed pristine MgH2can only start absorption at 120 °C. The employment of Ti3CN can significantly improve the hydrogen release kinetics of MgH2, with the desorption activation energy decreasing from 121 to 80 kJ mol−1. Regarding thermodynamics, the desorption enthalpy changes of MgH2and MgH2+ 7.5 wt% Ti3CN were 79.3 and 78.8 kJ mol−1, respectively. This indicates that the employment of Ti3CN does not alter the thermal stability of MgH2. Phase evolution studies through the use of X-ray diffraction and electron diffraction both confirm that Ti3CN remains stable during the hydrogen release and uptake process of the composite. This work will help understand the impact of a transition metal carbonitride on the hydrogen storage of MgH2.
研究领域:
材料科学
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能源存储
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高影响因子
ACS Applied Energy Materials
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2024
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IF 5.4
Jiajing Zhu,Hui Wang,Yuqi Zhai,Liangjun Huang,Jie Cui,Liuzhang Ouyang,Min Zhu,Jacques Huot
MgH2 is a promising solid-state hydrogen storage medium with a high hydrogen capacity and low cost, but it suffers from high hydrogen sorption temperatures. In this work, Cr-doped TiO2 solid solution nanocatalysts were synthesized and demonstrated to significantly reduce the hydrogen sorption temperatures and pressure of MgH2. The Ti(5Cr)O2 catalyzed MgH2 releases over 6.1 wt % of H2 at 200 °C, and even at 175 °C, 2.62 wt % H2 can be desorbed. The dehydrogenation activation energy is greatly reduced to 85.3 ± 8.7 kJ/mol, which is ∼49.7 kJ/mol less than that observed for pure MgH2. The dehydrogenated product can absorb 4.5 wt % of H2 within 10 s at a low temperature of −20 °C and back pressure of 30 bar, or the hydrogen uptake content can reach 4.81 wt % under 5 bar and 75 °C. The mechanism study indicates that the Cr-doped TiO2 can markedly reduce the adsorption energy and dissociation energy barrier of H2 molecules and greatly enhance the dissociation ability of H on the catalyst surface. This work demonstrates the potential of modified TiO2 as a cost-effective and efficient catalyst for Mg-based hydrogen storage materials.
研究领域:
材料科学
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能源存储
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高影响因子
Nanomaterials
·
2019
·Vol. 9
·期 10
·1370
·
IF 4.034
Liuting Zhang,Xiong Lu,Liang Ji,Nianhua Yan,Ze Sun,Xinqiao Zhu
Catalytic doping plays an important role in enhancing the hydrogen storage performance of MgH2, while finding an efficient and reversible catalyst remains to be a great challenge in enhancing the de/rehydrogenation properties of MgH2. Herein, a bidirectional nano-TiH1.971catalyst was prepared by a wet chemical ball milling method and its effect on hydrogen storage properties of MgH2was studied. The results showed that all the TiH1.971nanoparticles were effective in improving the de/rehydrogenation kinetics of MgH2. The MgH2composites doped with TiH1.971could desorb 6.5 wt % H2in 8 min at 300 °C, while the pure MgH2only released 0.3 wt % H2in 8 min and 1.5 wt % H2even in 50 min. It was found that the smaller the size of the TiH1.971particles, the better was the catalytic effect in promoting the performance of MgH2. Besides, the catalyst concentration also played an important role and the 5 wt %-c-TiH1.971modified system was found to have the best hydrogen storage performance. Interestingly, a significant hydrogen absorption amount of 4.60 wt % H2was evidenced for the 5 wt %-c-TiH1.971doped MgH2within 10 min at 125 °C, while MgH2absorbed only 4.11 wt% hydrogen within the same time at 250 °C. The XRD results demonstrated that the TiH1.971remained stable in cycling and could serve as an active site for hydrogen transportation, which contributed to the significant improvement of the hydrogen storage properties of MgH2.Keywords:hydrogen storage;MgH2;TiH1.971;catalytic effect;reversibility
研究领域:
材料科学
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化学工程
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PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Lina Qin,Guorong Zhang,Taigen Liang,Lixian Sun,Fen Xu,Yongpeng Xia,Sergey P. Verevkin,Sergey V. Vostrikov,Anton Lvovich Maximovi,Xuezhang Xiao,Lixin Chen,Hongge Pan
As a prominent catalyst in the development of MgH 2 hydrogen storage materials, MXene can significantly enhance hydrogen storage performance. In this study, we investigated the impact of using molten salts instead of HF to treat Ti 2 NTi x and its impact on the hydrogen storage properties of MgH 2 . MgH 2 -10 wt% Ti 2 NTi x composite has been prepared via ball milling. The results showed that adding 10 wt% Ti 2 NTi x largely lowered the initial dehydrogenation temperature of MgH 2 from 300.2 ℃ to 173.5 ℃. Under isothermal conditions at 350 ℃, the composite released 6.11 wt% H 2 within 4 minutes. Furthermore, after dehydrogenation, the MgH 2 -10 wt% Ti 2 NTi x composite absorbed 3.4 wt% H 2 in 60 minutes at 100 ℃ and 30 bar hydrogen pressure. EPR found that there is a large number of oxygen vacancies on the Ti 2 NTi x surface introduced by molten salt treatment, providing abundant active sites and accelerating electron transfer. Additionally, the in-situ formation of titanium nitride compounds, the synergistic multivalent catalytic effect of titanium, and the multiphase interfaces in MgH 2 -10 wt% Ti 2 NTi x contributed to the composite’s improved catalytic activity and stability. This work provided valuable insights into the application of oxygen vacancy-rich, incompletely etched Ti 2 NTi x materials in magnesium-based hydrogen storage, demonstrating their great potential in hydrogen storage technologies.
研究领域:
材料科学
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能源存储
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DOI
高影响因子
TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA
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2023
·
IF 4.5
Hao-yu ZHANG,Gui-bin TIAN,Fu-ying WU,Zhen-dong YAO,Jia-guang ZHENG,Liu-ting ZHANG
Two-dimensional Mo 2 TiC 2 MXenematerial was synthesized by etching Mo 2 TiAlC 2 and then doped into MgH 2 to tailor its hydrogen storage performance. The initial hydrogen desorption temperature of the Mo 2 TiC 2 -doped MgH 2 was significantly reduced from 330 °C (pristine MgH 2 ) to 187 °C. Isothermal dehydrogenation analysis indicated that the MgH 2 +9 wt.% Mo 2 TiC 2 composite rapidly discharged 6.4 wt.% H 2 at 300 °C within 4 min. For hydrogenation, the dehydrogenated MgH 2 +9 wt.% Mo 2 TiC 2 uptook 6.5 wt.% H 2 at 175 °Cwithin 5 min. By calculation, the activation energy for MgH 2 +9 wt.% Mo 2 TiC 2 was calculated to be (135.6±1.9) kJ/mol for the desorption reaction and (46.1±0.2) kJ/mol for the absorption reaction. After 20 cycles, 1.0 wt.% H 2 was lost for the MgH 2 +9 wt.% Mo 2 TiC 2 composite. Microstructure analysis results showed that the presence of Mo in Mo 2 TiC 2 enhanced the thermal stability of MXene and reduced the amount of active Ti during cycling, leading to poorer catalytic effect of the catalyst compared to Ti 3 C 2 .
研究领域:
材料科学
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能源存储
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催化化学
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Lingying Chen,Qinke Tang,Yichen Qi,Jiguang Zhang,Rui Shi,Yana Liu,Jun Wang,Yunfeng Zhu
Practical applications of magnesium hydride are hampered by high thermodynamic stability and slow kinetics. The design of highly active catalysts is essential to improve the kinetics of MgH 2 . Although studies concerned with the interaction between MgH 2 and catalyst have remained quite active, detailed investigation of the beneficial effect from the phase transformation is lacking. Herein, a high-activity VS 2 was designed and introduced to catalyze MgH 2 , and the MgH 2 -VS 2 system exhibited superior hydrogen desorption capabilities at comparatively low temperatures (3.5 wt% H 2 , 1800 s, 225 °C). This enhancement in the hydrogen storage performance of MgH 2 was attributed to the in-situ phase transformation of the catalytic species during hydrogen cycling. DFT calculations demonstrated the catalytic effect of VS 2 and in-situ formation of new species relative to MgH 2 . Our results provide a deeper insight into enhancing dehydrogenation mechanism on metal hydrides of the high-activity catalyst.
研究领域:
材料科学
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化学工程
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催化
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氢存储
✓ 已验证
DOI
高影响因子
Journal of Magnesium and Alloys
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2022
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IF 11.813
Haiguang Gao,Rui Shi,Yana Liu,Yunfeng Zhu,Jiguang Zhang,Liquan Li,Xiaohui Hu
Two-dimensional Ti 3 C 2 T x MXenes exposing different active facets are introduced into MgH 2 , and their catalytic effects are systematically investigated in depth through experimental and theoretical approaches. Excluding factors such as interlayer space, surface functional groups and experimental contingency, the exposed facets is considered to be the dominant factor for catalytic activity of Ti 3 C 2 T x towards MgH 2 . More exposed edge facets of Ti 3 C 2 T x displays higher catalytic activity than that with more exposed basal facets, which also leads to different rate-controlling steps of MgH 2 in the de/hydrogenation process. The low work function, strong hydrogen affinity and high content of in situ metallic Ti for the edge facet contribute the high catalytic activity. This work will give insights into the structural design of two-dimensional Ti 3 C 2 T x MXene used for enhancing the catalytic activity in various fields.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Yuhang Wang,Guangxin Fan,Dafeng Zhang,Yanping Fan,Baozhong Liu
The enhanced effect of metal catalysts is crucial to achieve advanced performance of hydrogen storage system. Rational design of catalysts with superior catalytic activity is significant to regulate the re-/hydrogenation kinetics of MgH 2 . Herein, Ti 3 C 2 -supported praseodymium(III) fluoride (PrF 3 ) nanoparticles (PrF 3 /Ti 3 C 2 ) composite was prepared by hydrothermal method , which exhibited superior catalytic activity toward hydrogen storage of MgH 2 . The onset temperature of dehydrogenation was reduced to 180 °C after adding 5 wt% PrF 3 /Ti 3 C 2 , corresponding to a reduction of 107 °C compared with pristine MgH 2 . About 7.0 wt% hydrogen was rapidly desorbed within 3 min at 260 °C and 6.6 wt% hydrogen was absorbed within 36 s at 200 °C for MgH 2 -5 wt% PrF 3 /Ti 3 C 2 . Moreover, MgH 2 -5 wt% PrF 3 /Ti 3 C 2 exhibited an excellent capacity retention of 92.5% even after 10 cycles. Experimental results reveal that the electron transfer among Ti-species (Ti 0 , Ti 2+ , and Ti 3+ ) occurred due to the striking enhanced effect of PrF 3 on Ti 3 C 2 MXene during the reaction process, and the synergistic action between Ti-species and PrF 3 are responsible for the markedly enhanced hydrogen storage properties of MgH 2 . This study is helpful to the design and optimization of hydrogen storage materials for mobile application.
研究领域:
材料科学
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能源存储
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高影响因子
Nanomaterials
·
2020
·Vol. 10
·期 9
·1745
·
IF 4.324
Ze Sun,Liuting Zhang,Nianhua Yan,Jiaguang Zheng,Ting Bian,Zongming Yang,Shichuan Su
Magnesium hydride (MgH2) has been considered as a potential material for storing hydrogen, but its practical application is still hindered by the kinetic and thermodynamic obstacles. Herein, Mn-based catalysts (MnCl2and Mn) are adopted and doped into MgH2to improve its hydrogen storage performance. The onset dehydrogenation temperatures of MnCl2and submicron-Mn-doped MgH2are reduced to 225 °C and 183 °C, while the un-doped MgH2starts to release hydrogen at 315 °C. Further study reveals that 10 wt% of Mn is the better doping amount and the MgH2+ 10 wt% submicron-Mn composite can quickly release 6.6 wt% hydrogen in 8 min at 300 °C. For hydrogenation, the completely dehydrogenated composite starts to absorb hydrogen even at room temperature and almost 3.0 wt% H2can be rehydrogenated in 30 min under 3 MPa hydrogen at 100 °C. Additionally, the activation energy of hydrogenation reaction for the modified MgH2composite significantly decreases to 17.3 ± 0.4 kJ/mol, which is much lower than that of the primitive MgH2. Furthermore, the submicron-Mn-doped sample presents favorable cycling stability in 20 cycles, providing a good reference for designing and constructing efficient solid-state hydrogen storage systems for future application.Keywords:hydrogen storage;MgH2;Mn-based catalysts;catalytic effect;reversibility
研究领域:
材料科学
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化学工程
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能源存储
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DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
·
IF 7.139
Han Yu,Ying Cheng,Yaokun Fu,Lu Zhang,Sanyang Guo,Yuan Li,Wei Zhang,Shumin Han
Carbon-based materials have been proposed as an ideal medium to reduce the reaction energy barriers and improve the (de)hydrogenation kinetics of magnesium-based hydrogen storage material (MgH 2 ) in term of their excellent dispersion. However, tedious preparation process and uneven distribution of carbon restrict the application. Therefore, in this paper, we cover MgH 2 by in-situ formed amorphous carbon via a facile approach of co-sintering Mg with fluorene followed by hydriding combustion and ball milling processes, named as MgH 2 -carbonization product of fluorene (MgH 2 -CPF). As a result, the MgH 2 -CPF composite prepared at 823 K initially dehydrogenates at 557 K, 94 K lower than the as-milled MgH 2 (651 K). Meanwhile, the composite can release 5.67 wt% H 2 within 1000 s at 623 K. Even at a lower temperature of 423 K, the MgH 2 -CPF composite still reabsorbs 5.62 wt% H 2 within 3600 s, while the as-milled Mg can hardly absorb hydrogen under a same condition. Furthermore, by addition of CPF, the apparent activation energy of the system is decreased from 161.2 kJ/mol to 87.2 kJ/mol. Our finding suggests that the carbon layer can keep the MgH 2 from aggregation, promote hydrogen transport and improve the efficiency of hydrogen absorption and desorption.
研究领域:
材料科学
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氢储存
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能源材料
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Yaokun Fu,Yu Wang,Lu Zhang,Yuan Li,Shumin Han
MgH 2 is one of the ideal hydrogen storage materials because of its high hydrogen storage density, but the thermodynamic stability and slow kinetics of Mg/MgH 2 system hinder its practical application. Transition metal catalyst doping has become an important strategy to improve the hydrogen storage kinetics of MgH 2 . In this work, FeNi 3 @CS was prepared by solvothermal method with carbon spheres (CS) as the support, and introduced into Mg/MgH 2 system to prepare MgH 2 –FeNi 3 @CS composite. The initial dehydrogenation temperature of MgH 2 –FeNi 3 @CS composite is 565 K, which is 100 K lower than additive-free MgH 2 . At 423 K, MgH 2 –FeNi 3 @CS composite could absorb 4.5 wt% H 2 , while the hydrogen absorption capacity of MgH 2 without additives is only 2.0 wt%. After 10 cycles, the hydrogenation and dehydrogenation capacity could be maintained at 5.6 wt% and 4.5 wt%, respectively. In addition, the activation energy of MgH 2 –FeNi 3 @CS composite decreased by 52 kJ/mol compared with MgH 2 . FeNi 3 was in situ converted to Mg 2 NiH 4 and Fe after hydrogenation-ball milling, which were considered as the catalytic active substances in Mg/MgH 2 system. The synergistic catalysis of Mg 2 Ni/Mg 2 NiH 4 , Fe and carbon materials has a positive effect on improving the hydrogen storage performance of Mg/MgH 2 system.
研究领域:
材料科学
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高影响因子
危险品化学品经营许可证（带存储）