JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Xinyu Liu,Xixi Meng,Tao Zhong,Yuxin Wang,Fuying Wu,Hu Liu,Hong Li,Liuting Zhang
Magnesium hydride (MgH 2 ) with its high hydrogen storage capacity (7.6 wt%) and exceptional reversibility, has emerged as a promising solid-state hydrogen storage material. This study designed a polymeric carbon nitride (PCN) supported single-phase Ni catalyst with superior thermal stability and catalytic activity. The optimized PCN-Ni catalyst significantly reduced the initial dehydrogenation temperature of MgH 2 to 192 ºC. At 295 ºC, the composite released 6.10 wt% H 2 within 5 min, and it subsequently absorbed 5.50 wt% H 2 within 5 min at 150 ºC. Compared to pristine MgH 2 , the activation energies for dehydrogenation and hydrogen absorption were reduced by 31.6 % and 29.4 %, respectively. Moreover, the MgH 2 + 10 wt% PCN-Ni composite exhibited remarkable cycling stability, with capacity retention rates of 96.0 % and 96.7 % after 20 hydrogenation/dehydrogenation cycles. In conclusion, this work provides a new perspective on the heterogeneous synergy of transition metal and carbon nitride composite catalysts in promoting the dehydrogenation/rehydrogenation reactions of MgH 2 and lays the foundation for the design and fabrication of highly efficient catalysts in other energy storage related fields.
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
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Wenjie Xue,Hongxia Liu,Binbin Zhao,Lixia Ge,Shuai Yang,Minghuang Qiu,Jiong Li,Wei Han,Xinqing Chen
N-ethylcarbazole (NEC) has been considered one of the most prospective liquid organic hydrogen carriers (LOHCs) for hydrogen storage. However, designing single catalyst capable of driving both hydrogenation of NEC and dehydrogenation of dodecahydro-NEC (12 H-NEC) is of a big challenge. Herein, we develop an atomic-dispersion of Rh with the Co nanoparticles (NPs) to form a Rh 1 Co structure maximizing the Rh utilization, which boosts the reversible (de)hydrogenation of NEC, and enables multiple cycles of reversible hydrogen uptake and release. Significantly, a low temperature of 90 °C is realized for the complete hydrogenation (100%), representing one of the lowest temperatures yet reported for the total hydrogenation of NEC. The remarkable catalytic performance of Rh 1 Co catalysts is the result of the optimal electronic structure between atomic-dispersion of Rh and Co NPs confirmed by structural characterizations and density functional theory (DFT) calculations, which allowed fast interfacial electron transfer to intermediates.
研究领域:
化学
·
材料科学
·
能源研究
✓ 已验证
产品关联
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
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zhuanghe Ren,Xin Zhang,Zhenguo Huang,Jianjiang Hu,Yangzhong Li,Shiyou Zheng,Mingxia Gao,Hongge Pan,Yongfeng Liu
Nanosized titanium compounds are particularly effective in catalyzing hydrogen cycling by NaAlH 4 . Titanium hydride (TiH 2 ), as a catalyst, is highly interesting since it contributes hydrogen in addition to active Ti. However, it has been challenging to fabricate nanosized TiH 2 due to the strong affinity of Ti with oxygen. Herein, TiH 2 nanoflakes with a lateral size of ~10 nm and thickness of ~1 nm are successfully synthesized through a novel facile one-pot solvothermal process. In an anhydrous THF solution, LiH reacts with TiCl 4 rapidly at 100 °C forming TiH 2 and LiCl. The newly formed TiH 2 nucleates and grows epitaxially on the graphene surface due to the well-matched lattice parameters, giving rise to the formation of TiH 2 nanoflakes. Both theoretical calculations and experiments reveal the generation of Cl· radicals and unsaturated C C bonds when TiCl 4 reacts with THF, which promotes the formation of TiH 2 . The nanoflake-like TiH 2 on graphene enables an outstanding hydrogen storage performance of NaAlH 4 , i.e., full dehydrogenation at 80 °C and hydrogenation at 30 °C and under 100 bar H 2 , with a practical hydrogen capacity of 4.9 wt%, which has been never reported before.
研究领域:
材料科学
·
纳米化学
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能源化学
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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
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2011
·Vol. 36
·期 23
·15266-15272
·
IF 4.057
Pei Pei Yuan,Bin Hong Liu,Zhou Peng Li
A comparative study was performed on four LiBH 4 -based hydrogen storage composites 2LiBH 4 + MgX 2 and 6LiBH 4 + CaX 2 (X = H and F). The composites with fluorides and those with corresponding hydrides exhibited similar hydrogen storage properties. The dehydrogenation of 2LiBH 4 + MgF 2 demonstrated a strong dependence on the hydrogen back pressure , similar to that of 2LiBH 4 + MgH 2 . The reversible hydrogen storage of 2LiBH 4 + MgF 2 was achieved under a back pressure of 5 bar at 450 °C. Dehydrogenation under lower H 2 pressures resulted in the production of Mg and thus a partial reversibility. In contrast, both 6LiBH 4 + CaH 2 and 6LiBH 4 + CaF 2 revealed reversible hydrogen storage properties regardless of the hydrogen back pressure. The structural difference between MgB 2 and CaB 6 may account for the observed differences in hydrogen storage properties of the Mg- and Ca-containing LiBH 4 reactive composites.
研究领域:
材料科学
·
能源化学
·
固态储氢
·
无机化学
·
功能材料
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Weilai Wang,Junfeng Niu,Zhifeng Yang
Presence of unsaturated bonds and halogen-containing groups is the most common characteristic of toxic and harmful environmental pollutants. Herein, catalytic hydrogenation was chosen as a water quality control method for such contaminants. Considering the safety, availability and activity of the hydrogen source, electrochemical in situ hydrogen generation was introduced. Under the combined action of Raney Ni (R-Ni) and nascent hydrogen (Nas-H 2 ), three compounds (50 mg L −1 , 90 ml), i.e., acrylamide, 2, 6-dibromo-4-nitrophenol and 2-chloro-4-fluorobenzonitrile achieved complete hydrogenation reduction in a short time. The improved system realized the quantitative consumption of hydrogen source and the efficient operation of hydrogenation reaction under mild conditions. Additionally, the alkaline environment formed by hydrogen evolution reaction (HER) avoided secondary pollution caused by catalyst dissolution. Atomic hydrogen (H·) produced from R-Ni and Nas-H 2 was the active free radical of the reaction. The hydrogenation activities of different functional groups were obtained according to the following order: Ph-NO 2 ＞ -C = C- ＞ Ph-C≡N ＞ Ph-Br ＞ Ph-Cl ＞ Ph-F. This work indicates that the catalytic hydrogenation system consisting of R-Ni and Nas-H 2 is a promising technology to reduce unsaturated bonds and halogen-containing groups.
研究领域:
环境科学
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化学工程
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催化
·
水处理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
International Journal of Minerals Metallurgy and Materials
·
2025
·Vol. 32
·期 11
·2713-2722
·
IF 7.2
Wang Li,Wu Fuying,Chen Daifen,Bian Ting,Senin Petr,Zhang Liuting
Owing to the orbital hybridization between the transition metal and the B element and the electron-trapping effect of the B element, transition metal borides are considered very promising materials for energy catalysis. In this work, an amorphous scaly high-entropy boride (HEB) with electron traps was designed and fabricated via a facile reduction method to improve the hydrogen storage properties of magnesium hydride (MgH 2 ). For dehydrogenation, the onset temperature of MgH 2 + 10wt% HEB was dropped to 187.4°C; besides, the composite exhibited superior isothermal kinetics and the activation energy of the composite was reduced from (212.78 ± 3.93) to (65.04 ± 2.81) kJ/mol. In addition, MgH 2 + 10wt% HEB could absorb hydrogen at 21.5°C, and 5.02wt% H 2 was charged in 50 min at 75°C. For reversible hydrogen storage capacity tests, the composite maintained a retention rate of 97% with 6.47wt% hydrogen capacity after 30 cycles. Combining microstructure evidence with hydrogen storage performance, the catalytic mechanism was proposed. During ball milling, scaly high-entropy borides riveted a large number of heterogeneous active sites on the surface of MgH 2 . Driven by the cocktail effect as well as the orbital hybridization of metal borides, numerous active sites steadily enhanced the hydrogen storage reactions in MgH 2 .
研究领域:
材料科学
·
能源化学
·
纳米催化
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固态储能
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物理化学
✓ 已验证
DOI
高影响因子
SN Applied Sciences
·
2018
·Vol. 1
·期 1
·1-9
·
IF 0
Zhang Liuting,Ji Liang,Yao Zhendong,Cai Zeliang,Sun Ze,Yan Nianhua,Zhu Xinqiao
The hydrogen storage properties of MgH 2 – x wt%TiCN ( x = 5, 10, 15) composites were systematically investigated and the results show that the addition of TiCN can effectively improve the de/rehydrogenation kinetics of MgH 2 . Taken the onset dehydrogenation temperature and isothermal de/rehydrogenation kinetics into consideration, the MgH 2 –10 wt% TiCN composite was shown to have the best performance. It was found that the MgH 2 –10 wt% TiCN composite could release 4 wt% H 2 in 17.3 min at 300 °C while the as-synthesized MgH 2 could not release any hydrogen under the same condition. Besides, the MgH 2 –10 wt% TiCN composite could absorb 4.63 wt% H 2 under 3.2 MPa hydrogen pressure at 300 °C within 20 s. Compared with as-synthesized MgH 2 , the activation energy of the MgH 2 –10 wt% TiCN composite was significantly decreased from 183.76 ± 10 to 106.82 ± 5 kJ/mol. X-ray diffraction analysis revealed that the TiCN remained stable during the ball milling and the following de/rehydrogenation cycle. The catalytic mechanism was also proposed that the TiCN particles absorbed on MgH 2 not only served as charge transfer centers and accelerated the hydrogen incorporation and dissociation rate but also provided more diffusion channels for hydrogen, which contributed to the good de/rehydrogenation properties of MgH 2 .
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
ACS Applied Energy Materials
·
2020
·
IF 4.473
Jiuyi Zhu,Yuchen Mao,Hui Wang,Jiangwen Liu,Liuzhang Ouyang,Min Zhu
LiBH4 (lithium borohydride) is a promising high capacity hydrogen storage material but suffering from its high dehydrogenation temperature and poor reversibility. To solve this problem, surface-modified AlN (aluminum nitride) was prepared by the alcoholysis process of LiBH4 and composited with LiBH4. By controlling the temperature of the drying process, it can tune the sorts and quantities of the functional groups on AlN. The de/rehydrogenation of LiBH4 is greatly improved by compositing it with surface-modified AlN because oxygen atoms in functional groups promote the decomposition of intermediates of LiBH4 and Hδ+ (positive hydrogen atom) reacting with Hδ− (negative hydrogen atom) in LiBH4. Besides, AlN provides the pathway of H and Li atoms to improve the kinetics of the de/rehydrogenation of LiBH4. Freeze-dried AlN containing O–H and C–H groups shows the best catalytic effect on the hydrogen storage reaction of LiBH4. The optimized composite could release a stable capacity of more than 6.1 wt % after cycling, which has potential applications in high-temperature environment hydrogen storage.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
RARE METALS
·
2024
·Vol. 43
·期 9
·4387-4400
·
IF 9.6
Xia Ao,Zheng Jia-Guang,Zhang Qing-Bo,Shu Yu-Gang,Yan Cheng-Guo,Zhang Liu-Ting,Tao Zhan-Liang,Chen Li-Xin
The facile construction of nanoscale NbH x supported by Ti 3 C 2 (NbH x @Ti 3 C 2 ) was achieved using facile ball milling strategy to improve the hydrogen desorption kinetics and reversibility of magnesium borohydride (Mg(BH 4 ) 2 ). The doping of 30 wt% NbH x @Ti 3 C 2 catalyst reduced the onset dehydrogenation temperature of Mg(BH 4 ) 2 to 71.2 °C. Additionally, the Mg(BH 4 ) 2 + 30NbH x @Ti 3 C 2 composite achieved remarkable hydrogen release of over 9.2 wt% at a temperature as low as 230 °C, indicating unexpected dehydrogenation kinetics. Moreover, the reversibility of NbH x @Ti 3 C 2 doped Mg(BH 4 ) 2 was retained to more than 4.2 wt% after four cycles, which was increased by 68% compared to that of undoped Mg(BH 4 ) 2 . The strong catalysis of NbH x @Ti 3 C 2 catalyst could be attributed to the synergistic effect of NbH x and Ti 3 C 2 in hydrogen spillover and diffusion. NbH x acted as a “hydrogen pump” for effective hydrogen spillover, while Ti 3 C 2 created numerous diffusion channels for hydrogen dissolution and provided the active catalytic site to facilitate the re/dehydrogenation of Mg(BH 4 ) 2 . Graphical abstract
研究领域:
材料科学
·
能源储存
✓ 已验证
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
Small
·
2024
·
IF 13
Wenxuan Zhang,Linming Zhou,Xin Zhang,Zhenguo Huang,Fang Fang,Zijian Hong,Juan Li,Mingxia Gao,Wenping Sun,Hongge Pan,Yongfeng Liu
Nanostructured metal hydrides with unique morphology and improved hydrogen storage properties have attracted intense interests. However, the study of the growth process of highly active borohydrides remains challenging. Herein, for the first time the synthesis of LiBH 4 nanorods through a hydrogen-assisted one-pot solvothermal reaction is reported. Reaction of n-butyl lithium with triethylamine borane in n-hexane under 50 bar of H 2 at 40–100 °C gives rise to the formation of the [100]-oriented LiBH 4 nanorods with 500–800 nm in diameter, whose growth is driven by orientated attachment and ligand adsorption. The unique morphology enables the LiBH 4 nanorods to release hydrogen from ≈184 °C, 94 °C lower than the commercial sample (≈278 °C). Hydrogen release amounts to 13 wt% within 40 min at 450 °C with a stable cyclability, remarkably superior to the commercial LiBH 4 (≈9.1 wt%). More importantly, up to 180 °C reduction in the onset temperature of hydrogenation is successfully attained by the nanorod sample with respect to the commercial counterpart. The LiBH 4 nanorods show no foaming during dehydrogenation, which improves the hydrogen cycling performance. The new approach will shed light on the preparation of nanostructured metal borohydrides as advanced functional materials.
研究领域:
材料科学
·
化学工程
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）