APPLIED SURFACE SCIENCE
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2020
·
IF 6.182
Man Chen,Yiqi Wang,Xuezhang Xiao,Yunhao Lu,Meng Zhang,Jiaguang Zheng,Lixin Chen
Magnesium hydride (MgH 2 ) has attracted extensive attention over the past decades due to its highly reversible hydrogen storage density (7.6 wt%). But intrinsic high activation energy barriers for de/rehydrogenation of MgH 2 /Mg restrict its potential application as an on-board hydrogen carrier. Herein, ZrH 2 nanocatalyst homogeneously distributed on the surfaces of MgH 2 exhibits pronounced low temperature de/rehydrogenation kinetics, resulting from the vast lattice distortions between ZrH 2 and MgH 2 /Mg phases. The ZrH 2 doped MgH 2 composite (MgH 2 -ZrH 2 ) starts to release H 2 at 203 °C, 102 °C lower than that of undoped MgH 2 . Most importantly, MgH 2 -ZrH 2 quickly absorbs 5.90 wt% H 2 at the temperature as low as 65 °C. Further deep investigations found that H atoms preferentially accumulates around ZrH 2 , since the lower hydrogen dissociation energy on the surfaces of ZrH 2 (1.421 eV) than that of pure Mg (2.301 eV). Then, the large lattice disordered zone between ZrH 2 and Mg phases enables H atoms diffuse easily into the lattice of Mg nearby, thus triggering the formation of MgH 2 . These findings are critically important to understand the mechanism of other metal hydride catalysts, as well as offer an opportunity for the practical on-board fuel cell applications in the future.
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
CHEMICAL PHYSICS LETTERS
·
2018
·
IF 1.686
Huaiwei Zhang,Jianbo Qi,Zhenguo Ji
Synergic effects of rare earth-magnesium based hydrides (LaH 3 -MgH 2 ) on thermal dehydrogenation of potassium borohydride (KBH 4 ) are discussed in the paper. Comparing to above 675 K for the LaH 3 -MgH 2 or KBH 4 , the dehydrogenation temperature can be decreased to 346 K for the composites (LaH 3 -MgH 2 -KBH 4 ). The apparent activation energy of desorption process for the mixture is also greatly reduced. On the other hand, the products in the temperature programmed desorption process are also illustrated.
研究领域:
材料化学
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无机化学
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能源材料
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储氢材料
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固态化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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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.
研究领域:
材料科学
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能源存储
✓ 已验证
DOI
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.
研究领域:
材料科学
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能源化学
✓ 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
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无机化学
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能源化学
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氢能源存储
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Jiabao Bai,Yaoyu Du,Yana Liu,Yunfeng Zhu,Jiguang Zhang,Rui Shi,Jun Wang,Zhixin Ba,Wenrong Cai
In this work, a three-dimensional network LaCoO3 (3D LaCoO3) was successfully synthesized by the colloidal crystal template technique and used for optimizing the de/hydrogenation performance of magnesium hydride (MgH2). 3D LaCoO3 displays a unique three-dimensional network macroporous structure with interconnected pores, where LaCoO3 nanoparticles (10–20 nm) are homogeneously anchored on the macroporous pore walls. Remarkably, MgH2 doped with 5 wt % 3D LaCoO3 can quickly release 6.06 wt % H2 at 300 °C within 1200 s and absorb 6.13 wt % H2 at 175 °C within 1800 s. Furthermore, MgH2-5 wt % 3D LaCoO3 exhibits a capacity retention rate of 98.12% after 10 cycles, indicating excellent reversibility. The superior catalytic performance originates from the unique 3D network structure of 3D LaCoO3 and the in situ formed Co/La4Co3O9 heterostructure during the first dehydrogenation process. The 3D network structure can make a more uniform distribution of the catalyst during ball milling, leading to more catalytic active sites. The experimental results prove that the in situ formed Co/La4Co3O9 heterostructure plays a key role in enhancing the de/hydrogenation performance of MgH2. Additionally, the DFT calculation results confirm that the Co/La4Co3O9 heterostructure exhibits a higher hydrogen absorption ability due to significant electron transfer between the Co and La4Co3O9 interfaces, which can facilitate the hydrogen absorption and desorption of MgH2. These findings provide a fresh approach to designing and preparing catalysts with distinctive morphologies for MgH2-based systems.
研究领域:
材料科学
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能源存储
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纳米技术
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催化
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氢能
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Energy Chemistry
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2014
·
IF 0
Pei Yu,Yong Shen Chua,Hujun Cao,Zhitao Xiong,Guotao Wu,Ping Chen
Alkali metal hydroxide and hydride composite systems contain both protic (H bonded with O) and hydridic hydrogen. The interaction of these two types of hydrides produces hydrogen . The enthalpy of dehydrogenation increased with the increase of atomic number of alkali metals, i.e., −23 kJ/mol H 2 for LiOH-LiH, 55.34 kJ/mol H 2 for NaOH-NaH and 222 kJ/mol H 2 for KOH-KH. These thermodynamic calculation results were consistent with our experimental results. H 2 was released from LiOH-LiH system during ball milling . The dehydrogenation temperature of NaOH-NaH system was about 150 °C; whereas KOH and KH did not interact with each other during the heating process. Instead, KH decomposed by itself. In these three systems, NaOH-NaH was the only reversible hydrogen storage system, the enthalpy of dehydrogenation was about 55.65 kJ/mol H 2 , and the corresponding entropy was ca. 101.23 J/(mol H 2 ·K), so the temperature for releasing 1.0 bar H 2 was as high as 518 °C, showing unfavorable thermodynamic properties. The activation energy for hydrogen desorption of NaOH-NaH was found to be 57.87 kJ/mol, showing good kinetic properties.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
Materialia
·
2018
·
IF 0
Zhengyang Shen,Zeyi Wang,Min Zhang,Mingxia Gao,Jianjiang Hu,Fang Du,Yongfeng Liu,Hongge Pan
A novel solid-solution MXene (Ti 0.5 V 0.5 ) 3 C 2 is successfully synthesized by exfoliating a solid-solution MAX phase (Ti 0.5 V 0.5 ) 3 AlC 2 , and its catalytic effect on the hydrogen storage reaction of Mg is systemically evaluated for the first time. Typical layer morphology is observed for the prepared (Ti 0.5 V 0.5 ) 3 C 2 , which exhibits a better catalytic activity than that of Ti 3 C 2 . The addition of 10 wt% (Ti 0.5 V 0.5 ) 3 C 2 remarkably reduces the dehydrogenation onset temperature of MgH 2 by 70 °C, from 266 to 196 °C. At 250 °C, approximately 5.0 wt% H 2 is released from the 10 wt% (Ti 0.5 V 0.5 ) 3 C 2 -containing MgH 2 within 20 min. The dehydrogenated sample rapidly absorbs 4.8 wt% H 2 within 5 s at 120 °C; these hydrogenation kinetics are much more superior even to the well-studied Nb 2 O 5 catalyst. The apparent activation energy is calculated to be 77.3 kJ/mol for the MgH 2 -10 wt% (Ti 0.5 V 0.5 ) 3 C 2 sample, which is only around half of that of the pristine MgH 2 (153.8 kJ/mol). This is responsible for the remarkably reduced dehydrogenation operating temperature. Moreover, the chemical states of (Ti 0.5 V 0.5 ) 3 C 2 during dehydrogenation are also analysed and discussed.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2013
·Vol. 38
·期 25
·10932-10938
·
IF 3.548
H. Wang,J. Zhang,J.W. Liu,L.Z. Ouyang,M. Zhu
In this study, alkali hydroxides (NaOH, LiOH, KOH) were attempted as new-type catalytic additives to improve the hydrogen storage properties of MgH 2 by ball milling . It is shown that the additives readily react with the MgH 2 to form perovskite-structured NaMgH 3 and KMgH 3 , but not the LiMgH 3 . Although the in-situ formed perovskite hydrides remain stable during hydriding/dehydriding cycles, both NaMgH 3 and KMgH 3 show predominant catalytic role on the hydriding and dehydriding of MgH 2 . In contrast, the LiOH modified MgH 2 presents much inferior sorption kinetics because of the absence of LiMgH 3 . The catalytic mechanism of perovskite hydrides can be explained by the high hydrogen mobility in the perovskite structure . This study shows that such cheap hydroxides could be used as efficient catalysts to improve the hydrogen storage properties of high-capacity metal hydrides and complex hydrides .
研究领域:
材料科学
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无机化学
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能源化学
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氢能存储
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金属氢化物
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固态储氢
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催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Deyu Tang,Jiaguang Zheng,Chengguo Yan,Ao Xia,Wei Kong,Arkadii Proskurin,Xiuzhen Wang
Sodium borohydride (NaBH 4 ) has long been regarded as a cost-effective hydrogen storage material with a theoretical hydrogen storage capacity of 10.6 wt%. However, its practical application is hindered by thermodynamic stability, and traditional hydrogen production from NaBH 4 required excess water, which lowered its volumetric and gravimetric capacities. In this study, for the first time, solid-state glycolic acid (GA) was used to destabilize NaBH 4 for producing hydrogen. According to the results, NaBH 4 -GA started releasing hydrogen rapidly from room temperature and more than 3.6 wt% hydrogen was produced below 100 ℃ with efficient hydrogen utilization rate of 95 %. Moreover, NaBH 4 -GA composites maintained solid-state through the entire dehydrogenation process with high volumetric capacity above 39 g H 2 L −1 . Through the evolution of bonding structures and composition in NaBH 4 -GA composites, the dehydrogenation process was further confirmed as similar to the hydrolysis process of NaBH 4 , but with no liquid appearing. This chemical process “solid-state hydrolysis” may offer potential application and novel insights in low-temperature solid-state hydrogen storage using NaBH 4 .
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
·
2020
·
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 .
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Yanping Fan,Dandan Chen,Xianyun Liu,Guangxin Fan,Baozhong Liu
Two-dimensional layered material of Ti 3 C 2 has been used to improve the hydrogen desorption properties of LiBH 4 . The results of temperature-programmed dehydrogenation (TPD) and isotherm dehydrogenation (TD) demonstrate that adding the Ti 3 C 2 contributes to the hydrogen storage performance of LiBH 4 . The dehydrogenation temperature decreases and the dehydrogenation rate increases with increasing the adding amounts of Ti 3 C 2 . The onset dehydrogenation temperature of LiBH 4 + 40 wt% Ti 3 C 2 composite is 120 °C and approximately 5.37 wt% hydrogen is liberated within 1 h at 350 °C. Furthermore, the activation energy of LiBH 4 + wt.% Ti 3 C 2 is also greatly reduced to 70.3 kJ/mol, much lower than that of pure LiBH 4 . The remarkable dehydrogenation property of the LiBH 4 + 40 wt% Ti 3 C 2 may be due to the layered active Ti-containing Ti 3 C 2 and the high surface area of MXene .
研究领域:
材料科学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子