ACS Applied Nano Materials
·
2021
·
IF 5.097
Jianguang Yuan,Haixiang Huang,Zan Jiang,Yujie Lv,Bogu Liu,Bao Zhang,Youhua Yan,Ying Wu
Borohydride magnesium is widely studied as a promising hydrogen storage material due to its high gravimetric and volumetric density (14.9 wt % and 112 g/L, respectively). Different types of catalysts play a good catalytic role in enhancing the hydrogen desorption rates in borohydride systems. In the present paper, multiwalled carbon nanotubes supported Ni (Ni/MWCNTs) were synthesized by a chemical reduction method, and the catalyst was introduced into Mg(BH4)2 to enhance the dehydrogenation kinetics. The effect of Ni/MWCNTs on the microstructural evolution and hydrogen storage properties of Mg(BH4)2 is studied. The Mg(BH4)2-5wt% Ni/MWCNTs (95M@5NiMWCNTs) sample exhibits the best hydrogen storage performance; it starts to release hydrogen at 93 °C, which is 113 °C lower than that of the primary Mg(BH4)2 sample. Moreover, it takes only 3600 s to desorb hydrogen completely at 300 °C, showing a significant improvement on hydrogen desorption kinetics. In comparison with the primary Mg(BH4)2 sample, the dehydriding apparent activation energy of the 95M@5Ni3MWCNTs2 sample is significantly lowered to 119.5 kJ mol–1. Transmission electron microscopy analysis exhibits that the striking improvement of dehydriding properties of Mg(BH4)2 is mainly due to the synergistic catalysis of Ni and MWCNTs. This work provides a new method for designing and synthesizing high-performance catalysts in borohydride hydrogen storage materials, which is potentially utilized as a hydrogen supplier for hydrogen fuel cells.
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高影响因子
RARE METALS
·
2025
·
IF 11
Zhen-Xuan Ma,Jia-Guang Zheng,Mei-Ling Lv,Cong Li,Chang-Hai Wu,Pan-Pan Zhou,Chao Su,Lei Ge
en This research uncovered the influence of nitrogen-doped MXene Ti 3 CN on the reversible hydrogen storage properties of Mg(BH 4 ) 2 . The Mg(BH 4 ) 2 -20Ti 3 CN composite began releasing hydrogen at a temperature of 80°C. In addition, the composite discharged over 8.8 wt% hydrogen at a comparatively lower temperature of 270°C, whereas the pure Mg(BH 4 ) 2 emitted merely 5.9 wt% hydrogen under identical circumstances, which exhibited remarkably enhanced dehydrogenation kinetics. Furthermore, upon completion of four cycles, Mg(BH 4 ) 2 -20Ti 3 CN retained a reversible hydrogen storage capacity of 4.5 wt%, representing an 80% improvement over the undoped Mg(BH 4 ) 2 . In the course of the dehydrogenation phase, the boron atoms in Mg(BH 4 ) 2 were anchored by nitrogen atoms in Ti 3 CN to form B-N bonds, which helped suppress the formation of MgB 12 H 12 . During the subsequent rehydrogenation process, the B-N bonds broke, and the boron atoms reparticipated in the reversible transformation into [BH 4 ] − clusters. Meanwhile, the formation of Ti 0 by the reaction of Mg(BH 4 ) 2 with Ti 3 CN weakened the B-H bond energy, and the layered structure provided an effective way for hydrogen spillover. These factors collectively improved the reversible hydrogen storage capabilities of Mg(BH 4 ) 2 . 摘要 zh 本研究揭示了氮掺杂MXene Ti 3 CN对Mg(BH 4 ) 2 可逆储氢性能的影响。Mg(BH 4 ) 2 -20Ti 3 CN复合材料在温度80°C时开始放氢。此外,在270°C的较低温度下,该复合材料的氢排放量超过8.8 wt%,而在相同的条件下,纯Mg(BH 4 ) 2 的氢排放量仅为5.9 wt%,脱氢动力学显著增强。在完成四个循环后,Mg(BH 4 ) 2 -20Ti 3 CN保留了4.5 wt%的可逆储氢容量,比未掺杂的Mg(BH 4 ) 2 提高了80%。在脱氢过程中,Mg(BH 4 ) 2 中的硼原子被Ti 3 CN中的氮原子锚定形成B-N键,有助于抑制MgB 12 H 12 的形成。在随后的再氢过程中,B-N键断裂,硼原子重新参与可逆转化为[BH 4 ] − 簇。同时,Mg(BH 4 ) 2 与Ti 3 CN反应生成Ti 0 ,削弱了B-H键能,层状结构也为氢溢出提供了有效路径。这些因素共同提高了Mg(BH 4 ) 2 的可逆储氢能力。
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高影响因子
Journal of Magnesium and Alloys
·
2022
·
IF 11.813
Yongyang Zhu,Mili Liu,liming Zeng,Yin Wang,Daifeng Wu,Rui Li,Qing Zhou,Renheng Tang,Fangming Xiao
The hydrolysis of MgH 2 delivers high hydrogen capacity (15.2 wt%), which is very attractive for real-time hydrogen supply. However, the formation of a surface passivation Mg(OH) 2 layer and the large excess of H 2 O required to ensure complete hydrolysis are two key challenges for the MgH 2 hydrolysis systems. Now, a low-cost method is reported to synthesize MgH 2 @Mg(BH 4 ) 2 composite via ball-milling MgH 2 with cheap and widely available B 2 O 3 (or B(OH) 3 ). By adding small amounts of B 2 O 3 , the in-situ formed Mg(BH 4 ) 2 could significantly promote the hydrolysis of MgH 2 . In particular, the MgH 2 –10 wt% B 2 O 3 composite releases 1330.7 mL·g −1 H 2 (close to 80% theoretical hydrogen generation H 2 ) in H 2 O and 1520.4 mL·g −1 H 2 (about 95%) in 0.5 M MgCl 2 in 60 min at 26 °C with hydrolysis rate of 736.9 mL·g −1 ·min −1 and 960.9 mL·g −1 ·min −1 H 2 during the first minute of the hydrolysis, respectively. In addition, the MgCl 2 solution allows repeated use by filtering and exhibits high cycle stability (20 cycles), therefore leading to much reduced capacity loss caused by the excess H 2 O. We show that by introducing B 2 O 3 and recycling the 0.5 M MgCl 2 solution, the system hydrogen capacity can approach 5.9 wt%, providing a promising hydrogen generation scheme to supply hydrogen to the fuel cells.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Zhi Zhang,Dongqiang Gao,Jiaguang Zheng,Ao Xia,Qingbo Zhang,Li Wang,Liuting Zhang
For solid-state hydrogen storage, Mg(BH 4 ) 2 has long been recognized as a promising material. However, its higher thermal stability is distant from conditions for practical application. Herein, it is effectively established that VF 4 nanoparticles anchored on 2D Mxene Ti 3 C 2 (VF 4 @Ti 3 C 2 ) have efficiently catalytic effects towards the hydrogen storage process of Mg(BH 4 ) 2 . The MBH-VF 4 @Ti 3 C 2 sample started releasing hydrogen at 90 °C, which was 182 °C and 55 °C lower than those of additive-free Mg(BH 4 ) 2 and MBH-20Ti 3 C 2 composites. Additionally, the MBH-20VF 4 @Ti 3 C 2 composite desorbed more than 8 wt% H 2 at 275 °C. The activation energies of dehydrogenation were reduced, and the improved reversibility of VF 4 @Ti 3 C 2 -doped Mg(BH 4 ) 2 was also discussed. According to microstructural study, the heterostructural VF 4 @Ti 3 C 2 interacted with Mg(BH 4 ) 2 to produce VH 2.01 and metallic Ti during re/dehydrogenation, which worked as active species to improve hydrogen storage performance in Mg(BH 4 ) 2 .
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yujie Lv,Yifan Jing,Bao Zhang,Yingxue Li,Guanglin Xia,Xuebin Yu,Pengru Huang,Haixiang Huang,Bogu Liu,Jianguang Yuan,Ying Wu
Although Mg(BH 4 ) 2 has been widely studied in the hydrogen storage field for its high hydrogen density, its terrible dehydriding kinetics and cycling features remain impediments to practical applications. Herein, introducing different MXenes (Ti 3 C 2 , Ti 2 C, Nb 2 C) with novel two-dimensional structures as catalysts into Mg(BH 4 ) 2 has been demonstrated to be an efficient approach to boosting the hydrogen storage properties. 30 wt% MXenes in Mg(BH 4 ) 2 causes a considerable reduction in its hydrogen release temperature, remarkable increases in its dehydrogenation rate and capacity, and an enhancement to its reversibility. The Mg(BH 4 ) 2 -30Ti 2 C as the most excellent composite starts to liberate hydrogen from 132 °C, 143 °C lower than that of Mg(BH 4 ) 2 . Furthermore, at 260 °C, the Mg(BH 4 ) 2 -30Ti 2 C composite desorbs 10.2 wt% H 2 , which is much higher than that of Mg(BH 4 ) 2 (1.5 wt%). Theoretical calculations elucidate the weakening of B-H bonds caused by the electron transfer at the Mg(BH 4 ) 2 /MXenes interfaces, and the dehybridization effect between the B and H orbits. X-ray photoelectron spectroscopy (XPS) analyses prove the in-situ formation of multiphase interfaces resulting from the interaction of Mg(BH 4 ) 2 and MXenes during milling and dehydrogenation processes, which could increase electron conduction and facilitate hydrogen diffusion. These factors contribute to the outstanding dehydrogenation properties of Mg(BH 4 ) 2 .
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2018
·
IF 3.779
Jiaguang Zheng,Xuezhang Xiao,Yan He,Man Chen,Meijia Liu,Shouquan Li,Lixin Chen
The Mg(BH 4 ) 2 -AlH 3 - x LiH ( x = 0, 0.5, 1) novel ternary composites have been synthesized through mechanical ball milling, their favorable dehydrogenation properties and mechanism have been experimentally investigated. It can be found that during ball milling, a slight amount of Mg(BH 4 ) 2 would react with LiH and transform into LiBH 4 , while most Mg(BH 4 ) 2 remained stable after ball milling. Two major dehydrogenation steps can be detected in the Mg(BH 4 ) 2 -AlH 3 - x LiH composite, which belong to the decomposition of AlH 3 and Mg(BH 4 ) 2 , respectively. Remarkably, the onset hydrogen desorption temperature of Mg(BH 4 ) 2 -AlH 3 - x LiH composite can be reduced to 125.9 °C, with a total hydrogen desorption capacity of 10.3 wt%. It is worth emphasizing that the reversible dehydrogenation capacity is obviously improved to 3.8 wt%, compared to the Mg(BH 4 ) 2 -AlH 3 composite. This reversible capacity can be held for 3 cycles without obvious degeneration. Microstructural analysis on de/rehydrogenated composite has identified the regeneration of [BH 4 ] - in Mg(BH 4 ) 2 -AlH 3 -0.5LiH composite and revealed the role of LiH in the cycling hydrogen desorption and absorption processes. The formation of LiBH 4 and MgH 2 resulted from the rehydrogenation between MgAlB 4 and LiH could be helpful for the stability of reversible hydrogen storage performance.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
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IF 4.939
Xuelei Feng,Jianguang Yuan,Yujie Lv,Bogu Liu,Haixiang Huang,Bao Zhang,Youhua Yan,Shumin Han,Ying Wu
Magnesium borohydride (Mg(BH 4 ) 2 ) is an attractive materials for solid-state hydrogen storage due to its high hydrogen content (14.9 wt%). In the present work, the dehydrogenation performance of Mg(BH 4 ) 2 by adding different amounts (10, 20, 40, 60 wt%) of two-dimensional layered Ti 3 C 2 MXene is studied. The Mg(BH 4 ) 2 -40 wt% Ti 3 C 2 composite releases 7.5 wt% hydrogen at 260 °C, whereas the pristine Mg(BH 4 ) 2 only releases 2.9 wt% hydrogen under identical conditions, and the onset desorption temperature decreases from 210 °C to a relative lower temperature of 82 °C. The special layered structure of Ti 3 C 2 MXene and fluorine plays an important role in dehydrogenation process especially at temperatures below 200 °C. The main dehydrogenation reaction is divided into two steps, and activation energy of the Mg(BH 4 ) 2 -40 wt% Ti 3 C 2 composite is 151.3 kJ mol −1 and 178.0 kJ mol −1 , respectively, which is much lower than that of pure Mg(BH 4 ) 2 .
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Qingbo Zhang,Zhenxuan Ma,Jiaguang Zheng,Ao Xia,Cong Li,Panpan Zhou
This study presents the synthesis of novel Mg(BH 4 ) 2 @V 2 C, Mg(BH 4 ) 2 @Nb 2 C and Mg(BH 4 ) 2 @Ti 3 C 2 composites using a solution-based nanoconfinement strategy, achieving robust architecture of Mg(BH 4 ) 2 onto Mxene structures. Among these composites, the Mg(BH 4 ) 2 @V 2 C composite exhibited an initial dehydrogenation temperature of 76.4 °C and released 9 wt% hydrogen at 300 °C, which exhibited the optimal hydrogen release behavior. Its two-step dehydrogenation activation energies (104.44 kJ/mol and 118.52 kJ/mol) were significantly lower than those of pure Mg(BH 4 ) 2 , showing improved dehydrogenation kinetics. After four absorption-desorption cycles, the composite could still desorb 4.9 wt% hydrogen, demonstrating excellent cycling stability. Further structural investigations revealed that V 2 C actually acted as a “functionalized” matrix, which improved hydrogen storage through a combination of nanoconfinement and catalytic effects, promoting both hydrogen desorption and absorption. This work provides critical insights for designing high-performance hydrogen storage materials and advances the development of next-generation storage systems.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2018
·
IF 3.779
Zan Jiang,Jianguang Yuan,Huanqing Han,Ying Wu
As an important member of complex hydrides , Mg(BH 4 ) 2 has a high gravimetric capacity (14.9 wt%). In this study, the Mg(BH 4 ) 2 was synthesized by the ion exchange method. Afterwards, the Mg(BH 4 ) 2 composites with different amounts (2, 5, 10, 25 and 50 wt%) of carbon nanotubes (CNTs) were prepared by mechanical milling. Effects of the CNTs on the microstructural evolution and hydrogen storage properties were investigated. The onset desorption temperature of the Mg(BH 4 ) 2 -5 wt% CNTs is decreased to lower temperature around 120 °C from 275 °C. The desorption plateau of Mg(BH 4 ) 2 -5 wt% CNTs is the highest, which ascribes that CNTs causes the reaction pathway change. Additionally, the Mg(BH 4 ) 2 -5 wt% CNTs shows the best dehydriding kinetics properties, and can desorb 6.04 wt% hydrogen within 2000 s at 300 °C. The dehydrogenation activation energy of the Mg(BH 4 ) 2 -5 wt% CNTs is decreased to 130.2 kJ/mol H 2 , which is much lower than that of pure Mg(BH 4 ) 2 .
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高影响因子
Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 20
·9723-9732
·
IF 8.867
Jiaguang Zheng,Xuezhang Xiao,Liuting Zhang,Shouquan Li,Hongwei Ge,Lixin Chen
A remarkable improvement in the hydrogen desorption performance of Mg(BH4)2–NaBH4 eutectic composite is achieved by simply ball-milling with fluorographene (FG). It is found that the desorption temperature of Mg(BH4)2–NaBH4 (∼200 °C) is still too high and liquid phase appears during dehydrogenation. Particularly, the novel bowl-like 3D Mg(BH4)2–NaBH4–FG composite can be formed after ball-milling. The novel Mg(BH4)2–NaBH4–FG exhibits a low dehydrogenation temperature of 114.9 °C with 6.9 wt% of pure hydrogen in seconds. In-depth investigations show that such greatly improved hydrogen desorption properties of the Mg(BH4)2–NaBH4–FG composite could be ascribed to both the “novel bowl-like 3D structure” with large specific surface area and the “reactant destabilized modification” owing to the decrease of the reaction enthalpy caused by the formation of NaMgF3. This finding provides a facile preparation of complex borohydride composites with low dehydrogenation temperature and fast rate, which accelerates its practical application in fuel cells.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 9.2
Zheyu Zhang,Yuxiao Jia,Nuo Lei,Fei Chu,Liuhui Zhu,Mengdan Yu,Lixin Chen,Xuezhang Xiao
Developing a strategy for efficiently synthesizing borohydrides with high capacity and favorable reversibility is significant for promoting the development of next-generation energy materials. This work proposes a novel Mg(BH 4 ) 2 –TiNbNiCuO@graphene (Mg(BH 4 ) 2 –TiNbNiCuO@GR) high-entropy system, integrating nanoconfinement and catalytic strategies to significantly enhance the dehydrogenation kinetics and cycling stability of Mg(BH 4 ) 2 . TiNbNiCuO medium-entropy oxide (MEO) were synthesized in situ on a graphene carbon skeleton as catalyst (TiNbNiCuO@GR). Subsequently, Mg(BH 4 ) 2 was slowly infiltrated into the TiNbNiCuO@GR framework, which served as a carrier for nanoconfined Mg(BH 4 ) 2 , forming the Mg(BH 4 ) 2 –TiNbNiCuO@GR. It is demonstrated that the close contact between nanoconfined TiNbNiCuO MEO and Mg(BH 4 ) 2 creates abundant active sites, which facilitates electron transfer to improve dehydrogenation kinetics (dehydrogenation onset temperature at 63.5 °C) with a high capacity of 9.8 wt% H 2 . Notably, high-entropy effect and nanoconfinement boost the structure stability of TiNbNiCuO and prevent the agglomeration of Mg(BH 4 ) 2 , respectively, thereby jointly achieving an enhanced reversibility of the dehydrogenation kinetics, enabling a capacity retention of 81.5% after 10 cycles. The synergistic nanoconfinement-catalytic effect within the Mg(BH 4 ) 2 –TiNbNiCuO@GR offers new insights into the efficient dehydrogenation pathway of Mg-based borohydride systems.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2015
·
IF 3.313
Liuting Zhang,Jiaguang Zheng,Lixin Chen,Xuezhang Xiao,Teng Qin,Yiqun Jiang,Shouquan Li,Hongwei Ge,Qidong Wang
Mg(BH 4 ) 2 is considered as one of the most promising light metal complex hydrides because of its high volumetric and gravimetric hydrogen capacities and world-wide abundance. However, its higher major desorption temperatures (above 300 °C) and poor reaction kinetics have to be improved for the practical application. Herein, Mg(BH 4 ) 2 was successfully synthesized via wet-chemical technique and a significant enhancement in dehydrogenation performance of Mg(BH 4 ) 2 is achieved by the synergetic effect of fluorographite (FGi) and LiBH 4 . Under the effect of FGi, the hydrogen desorption of 6 Mg(BH 4 ) 2 -4FGi composite could be completed below 170 °C in seconds. However, the hydrogen released from 6 Mg(BH 4 ) 2 -4FGi suffers from impurities of B 2 H 6 and HF. More importantly, it is demonstrated that almost all the B 2 H 6 and HF impurities can be suppressed by synergetic modifying Mg(BH 4 ) 2 with FGi and LiBH 4 . The 3 Mg(BH 4 ) 2 –3LiBH 4 -4FGi composite exhibits a capacity over 8.0 wt% H 2 and starts to release hydrogen at 125.7 °C, which is 143.8 °C and 254.3 °C lower than that of pure Mg(BH 4 ) 2 and LiBH 4 , respectively. These significant improvements could be attributed to both the novel morphology that numerous nano-scale borohydride spots formed on the surface of FGi, and the formations of stable fluorides (MgF 2 and LiF) from the interaction between borohydrides and FGi.
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