ENERGY
·
2024
·
IF 9
Xiaoming Li,Zeming Yuan,Zhenyang Li,Chenxu Liu,Tingting Zhai,Yanghuan Zhang,Tao Li
Magnesium metal and its hydride have the characteristics of high hydrogen storage capacity, which is suitable for storing hydrogen energy. In this paper, VS 2 /NC catalyst supported on nanosheet carbon was synthesized by hydrothermal method with organic matter as raw material, then the MgH 2 + x wt.% VS 2 /NC ( x = 0, 3, 6, 9) composites were prepared by ball milling with MgH 2 . The phase characterization of the composite material showed that the VS 2 and MgH 2 phases in the composite material remain stable during ball milling and subsequently, the hydrogen absorption/desorption cycle. There were V 4+ and V 2+ ions (an atomic ratio of 3.77:1) in the catalyst. At 593 K, the capacities of the composites were 5.71, 6.11, 5.62, and 5.33 wt.% H 2 , respectively. The time to reach the maximum hydrogen desorption capacity of 95% was 190, 30, 20, and 23 min, respectively. The dehydrogenation activation energy of the material with x = 6 is reduced by nearly 50 kJ/mol H 2 . The initial dehydrogenation temperature of the material decreases to 323 K. Because of the valence state transition between V ions, the band gap of the composite material is narrowed, which significantly improves the hydrogen absorption and desorption reaction kinetics.
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Liang Dan,Hui Wang,Xiaobao Yang,Jiangwen Liu,Liuzhang Ouyang,Min Zhu
The practical applications of MgH2 as a high-density hydrogen carrier depend heavily on efficient and low-cost catalysts to accelerate the dehydriding/hydriding reactions at moderate temperatures. In the present work, this issue is addressed by synthesizing Nb-doped TiO2 solid-solution-type catalysts that dramatically improve the hydrogen sorption performances of MgH2. The catalyzed MgH2 can absorb 5 wt % of H2 even at room temperature for 20 s, release 6 wt % of H2 at 225 °C within 12 min, and the complete dehydrogenation can be achieved at 150 °C under a dynamic vacuum atmosphere. Density functional theory calculations reveal that Nb doping introduces Nb 4d orbitals with stronger interaction with H 1s into the density of states of TiO2. This considerably enhances both the adsorption and dissociation ability of the H2 molecule on the catalysts surface and the hydrogen diffusion across the specific Mg/Ti(Nb)O2 interface. The successful implementation of solid solution-type catalysts in MgH2 offers a demonstration and inspiration for the development of high-performance catalysts and solid-state hydrogen storage materials.
研究领域:
材料科学
·
催化化学
·
能源存储
✓ 已验证
DOI
高影响因子
Inorganics
·
2023
·Vol. 11
·期 5
·216
·
IF 2.9
Zhi-Kang Qin,Li-Qing He,Xiao-Li Ding,Ting-Zhi Si,Ping Cui,Hai-Wen Li,Yong-Tao Li
Realizing rapid and stable hydrogen sorption at low temperature is critical for magnesium-based hydrogen storage materials. Herein, liquid channels are built in magnesium hydride by introducing lithium borohydride ion conductors as an efficient route for improving its hydrogen sorption. For instance, the 5 wt% LiBH4-doped MgH2can release about 7.1 wt.% H2within 40 min at 300 °C but pure MgH2only desorbs less than 0.7 wt.% H2, and more importantly it delivers faster desorption kinetics with more than 10 times enhancement to pure MgH2. The hydrogen absorption capacity of LiBH4-doped MgH2can still be well kept at approximately 7.2 wt.% without obvious capacity degradation even after six absorption and desorption cycles. This approach is not only through building ion transfer channels as a hydrogen carrier for kinetic enhancement but also by inhibiting the agglomeration of MgH2particles to obtain stable cyclic performance, which brings further insights to promoting the hydrogen ab-/desorption of other metal hydrides.Keywords:hydrogen storage materials;magnesium hydrides;borohydrides;liquid channels;kinetics
研究领域:
材料科学
·
氢能研究
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2024
·
IF 11.2
Nuo Xu,Haoran Zhou,Mingqiang Zhang,Yuchuan Ye,Kaiwen Wang,Yingtang Zhou,Yunfeng Zhu,Yao Zhang
Hydrogen storage plays a pivotal role in the hydrogen industry, yet its current status presents a bottleneck. Diverse strategies have emerged in recent years to address this challenge. MgH 2 has stood out as a promising solid-state hydrogen storage material due to its impressive gravimetric and volumetric hydrogen density, but its practical application is hampered by elevated thermal stability and sluggish kinetics. In this study, we introduce a solution by synthesizing Pd metallene through a one-pot solvothermal method, revealing a distinctive highly curved lamellar structure with a thickness of around 1.6 nm. Incorporating this Pd metallene into MgH 2 results in a composite system wherein the starting dehydrogenation temperature is significantly lowered to 439 K and complete dehydrogenation occurs at 583 K, releasing 6.14 wt.% hydrogen. The activation energy of dehydrogenation for MgH 2 was reduced from 170.4 kJ mol –1 to 79.85 kJ mol –1 after Pd metallene decoration. The enthalpy of dehydrogenation of the MgH 2 –10 wt.% Pd sample was calculated to be 73 kJ mol –1 H 2 –1 and decreased by 4.4 kJ mol –1 H 2 –1 from that of dehydrogenation of pure MgH 2 (77.4 kJ mol –1 H 2 –1 ). Theoretical calculations show that the average formation energy and average adsorption energy of hydrogen vacancies can be significantly reduced in the presence of both Pd clusters and Pd single atoms on the surface of MgH 2 /Mg, respectively. It suggests that the synergistic effect of in situ formed Pd single atoms and clusters significantly improves the hydrogenation and dehydrogenation kinetics. The identified active sites in this study hold potential as references for forthcoming multi-sized active site catalysts, underscoring a significant advancement toward resolving hydrogen storage limitations.
研究领域:
材料科学
·
能源存储
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Nano Research
·
2024
·
IF 9.5
Zhao Yuan,Wang Qingshuang,Yin Dongming,Wang Xiaoli,Li Shouliang,Wang Chunli,Liang Long,Zhao Shaolei,Wang Limin,Cheng Yong
α-AlH 3 is regarded as one of the most promising hydrogen storage materials due to its high hydrogen storage capacity (10.1 wt.%, 148 kg·m −3 ). However, in practical applications, the associated hydrogen release temperature remains relatively high. To effectively address this issue, hollow structured Fe@C nanorods derived from Fe-MOF are introduced as highly efficient catalyst to optimize the dehydrogenation properties of α-AlH 3 . Comparatively, the initial hydrogen release temperature of α-AlH 3 + 3 wt.% Fe@C is reduced to 94.2 °C, which is significantly lower than that of pure α-AlH 3 (137.8 °C). At 100 and 120 °C, it exhibits hydrogen capacities of 5.38 wt.% and 7.47 wt.%, respectively, whereas pure α-AlH 3 only delivers hydrogen capacities of 0.24 wt.% and 5.94 wt.% under the same temperatures. The density functional theory (DFT) calculations further indicate that the existence of Fe@C catalyst can make the length of Al–H bond increase, which is more conducive to the release of hydrogen. The results show that the synergistic effect of Fe and porous carbon in Fe@C nanorods can improve the hydrogen desorption kinetics of α-AlH 3 , providing a good prospect for the application of α-AlH 3 in hydrogen storage fields.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Xu Huang,Xuezhang Xiao,Xuancheng Wang,Zhendong Yao,Jiahuan He,Xiulin Fan,Lixin Chen
Li–Mg–B–H reactive hydride composite (RHC) has attracted extensive attention over the past decades for its extremely high hydrogen storage capacity (11.5 wt%). But the sluggish desorption kinetics for the second step dehydrogenation reaction need to be further improved. Herein, short rod-like TMTiO 3 (TM = Co, Ni) bimetallic oxides , which contain two kinds of transition metal elements, were synthesized and introduced into Li–Mg–B–H RHC for the first time. The NiTiO 3 exhibits excellent catalytic effect on the hydrogen desorption kinetic performance of Li–Mg–B–H RHC, and the incubation period for the second step dehydrogenation reaction is eliminated completely by reducing the apparent activation energy for the generation of MgB 2 from 296 kJ/mol to 269 kJ/mol. The NiTiO 3 doped Li–Mg–B–H RHC can desorb about 9.0 wt% H 2 without obvious attenuation of kinetic performance in five cycles. Mechanism analyses reveal that the in-situ generated nano-sized MgNi 3 B 2 and TiB 2 species (∼5 nm) both meet the critical value ( < 10%) of the edge-to-edge matching model (5.77% for MgNi 3 B 2 and 2.22% for TiB 2 ), which play a significant role in supporting the nucleation of MgB 2 . Meanwhile, the extremely fine MgNi 3 B 2 and TiB 2 heterogeneous nucleation sites can inhibit the excessive growth for a single crystal nucleus of MgB 2 . The heterogeneous nucleation and grain refinement mechanisms caused by the novel bimetallic oxide could provide alternative insights into designing an in-situ generated nano-sized catalytic hydrogen storage system with enhanced kinetics and cyclic stability for hydrogen-fueled applications.
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
·
2024
·
IF 8.1
Chengguo Yan,Jiaguang Zheng,Ao Xia,Qingbo Zhang,Meiling Lv,Zhenxuan Ma,Chao Su,Zhendong Yao
Among conventional hydrogen storage materials , LiBH 4 has been regarded as one of the best hydrogen transporters due to its relatively large hydrogen capacities. However, because of its extraordinarily high dehydrogenation temperatures, LiBH 4 was not suitable for hydrogen storage due to its stable thermodynamic features. Herein, we present a novel approach to LiBH 4 that uses solid-state multi-hydroxyl mannitol as a reactant, regulating hydrogen release below 69.9 °C. More than 7 wt% H 2 could be released with ultra-fast rates at 140 °C from the LiBH 4 -mannitol composite. XRD , FTIR , and SEM tests revealed that the reaction between mannitol (H δ+ ) and LiBH 4 (H δ− ) to produce hydrogen was accompanied by the generation of large amounts of heat in situ, which further promoted the decomposition of LiBH 4 for hydrogen production , exceeding the theoretical dehydrogenation amount of H δ+ - H δ− reaction. This work indicates possibilities for the development of fast and easy high-capacity hydrogen generation systems based on complex hydrides.
研究领域:
材料科学
·
无机化学
·
能源化学
·
氢能源存储
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Kang Chen,Mili Liu,Zhuoyin Peng,Hao Zhong,Lang Gan,Jincheng Huang,Jing Zhao,Hui Wang,Jiangwen Liu,Huaiyu Shao,Liuzhang Ouyang
LiBH 4 (LB in short) with a hydrogen capacity as high as 18.5 wt% and a low molecular weight (21.78 g mol −1 ) is among the most promising candidates for the hydrogen-based economy. However, current major technologies in (re)generation of LB rely heavily on energy-intensive processes, which greatly prohibits practical scaling-up of applications. Here we report a sustainable and effective approach to (re)generate LB via converting renewable H + in crystalline water into H - , achieving a desirable yield of ∼50%. This one-step synthesis method relies on the reaction between spent fuels, specifically LiBO 2 · x H 2 O, and Mg-based alloys to form LB under ambient atmosphere. Notably, our approach surpasses the efficiency of other conventional method, such as LiH-B-H 2 and MgH 2 -LiBO 2 systems, which not only bypasses the energy-intensive dehydration procedure of LiBO 2 · x H 2 O (∼470 ℃) but also eliminates the use of costly hydrides or high-pressure H 2 . Our findings indicate that Mg participated in the regeneration process prior to Al in Mg-Al alloys and [BH 4 ] - is gradually evolved from other intermediate species [BH x (OH) 4- x ] - ( x = 0, 1, 2, 3). By combining hydrogen release and efficient storage of hydrogen-rich substrate in a closed materials cycle, this study may shed light on a promising step toward application of renewable hydrogen in a fuel cell-based hydrogen economy.
研究领域:
材料科学
·
能源科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
iScience
·
2023
·
IF 5.8
Fuhua Xu,Jiaying Yan,Yanlan Wang,Xiang Liu
Sodium formate (SF) is regarded as a technological additive to improve H 2 generation upon HCOOH dehydrogenation. The development of SF as a hydrogen storage material is still a challenge. Herein, we report the design and synthesis of carbon nanosphere-stabilized Pd nanoparticles (Pd/CNS) for the direct H 2 generation upon SF hydrolysis in the presence of Fe 3+ . The tandem reaction, isotopic mass spectrometry, and gas chromatograms result confirmed that SF hydrolysis generates H 2 with one H atom provided by SF and other H by H 2 O. The kinetic study and detailed mechanistic investigations have demonstrated that the concerted process between the cleavage of O-H bond in H 2 O and -O 2 C-H bond oxidative addition is the rate-controlling step in SF hydrolysis. This work offers a new chemical hydrogen storage material (HCOONa) for the high-efficiency generation, transport, and storage of H 2 .
研究领域:
化学
·
能源科学
·
催化科学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Zexuan Yang,Jiaao Wu,Yazhou Wang,Shunxiang Wang,Yongjin Zou,Cuili Xiang,Fen Xu,Lixian Sun,Yong Shen Chua
With rising energy demand for energy and the deterioration of the environment, the search for finding a sustainable energy material is crucial. Hydrogen energy has been widely recognized as a clean energy source, and magnesium-based hydrogen storage material (MgH 2 ) is a material with great potential, but some of its properties limit its practical application. In this study, we prepared flower-shaped niobium nitride (NbN) and 2D titanium carbide (Ti 3 C 2 ). Subsequently, the two materials were compounded to yield a NbN@Ti 3 C 2 composite material. Because of the synergistic effect of NbN and multivalent Ti as a catalytic pair, the addition of 7 wt% NbN@Ti 3 C 2 significantly reduced the dehydrogenation temperature of MgH 2 from 305 °C to 185 °C. Under isothermal dehydrogenation at 300 °C, 5.9 wt% of H 2 was dissociated within 180 s. The dehydrogenation activation energy was measured to be 44.82 ± 2.57 kJ/mol, considerably lower than that of ball-milled MgH 2 (126.04 ± 3.65 kJ/mol), representing a relative reduction of 64.4 %. The presence of carbon effectively avoids the reunification phenomenon during the cyclic testing; thus, the MgH 2 -7 wt% NbN@Ti 3 C 2 composite material maintained an effective H 2 capacity of approximately 95.5 % after 50 cycles at 300 °C, substantially enhancing the cyclic stability of 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
Energy Technology
·
2018
·Vol. 7
·期 3
·1800533
·
IF 3.175
Shiliang Zhang,Qilu Yao,Qingyang Li,Gang Feng,Zhang-Hui Lu
The synthesis of noble-metal-free recyclable catalysts with prominent catalytic performance for the complete hydrogen production from hydrazine borane (N 2 H 4 BH 3 , HB) is of great significance in achieving a hydrogen economy-based society. Herein, Raney Ni is synthesized using a rapidly quenched aluminum–nickel alloy under a typical alkali leaching condition and is used to catalytically convert hydrogen of N 2 H 4 BH 3 to H 2 via hydrolyzing BH 3 groups and decomposing the N 2 H 4 moiety in alkaline conditions. It is the first report of a noble-metal-free catalyst achieving a complete production of hydrogen from N 2 H 4 BH 3 at room temperature. This noble-metal-free catalyst might tremendously broaden the actual utilization of HB as a promising chemical hydrogen storage material. In addition, such a simple strategy can also be expanded to design and synthesize other porous metals for more applications.
研究领域:
能源化学
·
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
DALTON TRANSACTIONS
·
2020
·Vol. 49
·期 11
·3495-3502
·
IF 4.174
Yu Wang,Zhenmin Ding,Xinjun Li,Shuqin Ren,Shuhua Zhou,Hongming Zhang,Yuan Li,Shumin Han
Magnesium hydride is considered to be one of the most desirable hydrogen storage materials due to its high weight capacity (7.6 wt% H2) and low price. However, its relatively high operating temperatures and slow dynamics have always hampered its commercial applications. In this paper, nano-nickel particle coated nitrogen-doped carbon spheres (Ni@NCS) were synthesized by a chemical reduction method and then introduced into Mg to form an MgH2–Ni@NCS composite via hydriding combustion and subsequent high-energy ball milling processes. The results showed that the MgH2–Ni@NCS composite possessed high hydrogen storage capacity and fast absorbing/desorbing kinetics, absorbing 5.7 wt% H2 and desorbing 4.3 wt% H2 within 8 min at 623 K. Moreover, the capacity shows negligible degradation after 10 cycles, indicating that the MgH2–Ni@NCS composite has good cycling stability. Even at relatively low temperature (373 K), the MgH2–Ni@NCS composite still absorbed 4.2 wt% H2 within 60 min compared to 0.9 wt% H2 for milled MgH2. The improvement in hydrogen storage properties is ascribed to the in situ formed Mg2NiH4 induced dehydrogenation of MgH2 and effective prevention of the agglomeration of magnesium during the hydriding/dehydriding reaction by the carbon material.
研究领域:
材料科学
·
能源化学
·
纳米催化
·
储氢技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）