JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2023
·
IF 10.9
Samuel Guemou,Liuting Zhang,Shuai Li,Yiqun Jiang,Tao Zhong,Zichuan Lu,Ren Zhou,Fuying Wu,Qian Li
The design of an excellent active catalyst to improve the sluggish kinetic and thermodynamic properties of magnesium hydride (MgH 2 ) remains a great challenge to achieve its practical application. In this study, a novel Ni-Nb/rGO nanocomposite catalyst was successfully prepared by one-spot hydrothermal and subsequent calcination methods. The novel Ni-Nb/rGO nanocomposite exhibits an exceptional catalytic effect on improving MgH 2 sorption properties. Specifically, the onset desorption temperature of MgH 2 + 10 wt% Ni-Nb/rGO composite is reduced to 198 °C, much lower than that of undoped MgH 2 (330 °C). Interestingly, the composite can release 5.0, 5.9, and 6.0 wt% H 2 within 10 min at 245, 260, and 275 °C, respectively. Furthermore, the dehydrogenated MgH 2 + 10 wt% Ni-Nb/rGO composite starts to absorb hydrogen even at room temperature with approximate 2.75 wt% H 2 uptake at 75 °C under 3 MPa H 2 pressure within 30 min and exhibits excellent stability by maintaining 6.0 wt% hydrogen content after 20 cycles at 300 °C. Chou's model suggests that the de/hydrogenation kinetics of Ni-Nb/rGO-modified MgH 2 switches from surface penetration model to diffusion model at lower temperatures. Additionally, the activation energies ( E a ) for the de/hydrogenation of MgH 2 + 10 wt% Ni-Nb/rGO are reduced to 57.8 kJ/mol and 33.9 kJ/mol, which are significantly lower than those of undoped MgH 2 . The work demonstrates that the addition of a novel ternary Ni-Nb/rGO catalyst is an effective strategy to not only boost the sorption kinetics of MgH 2 but also maintain its cycling property.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2022
·
IF 10.319
Xuelian Zhang,Xin Zhang,Lingchao Zhang,Zhenguo Huang,Fang Fang,Yaxiong Yang,Mingxia Gao,Hongge Pan,Yongfeng Liu
Nanoscaled catalysts have attracted much more attention due to their more abundant active sites and better dispersion than their bulky counterparts. In this work, VH x nanoparticles smaller than 10 nm in average size are successfully synthesized by a simple solid-state ball milling coupled with THF washing process, which are proved to be highly effective in enhancing the hydrogen absorption/desorption kinetics of MgH 2 at moderate temperatures. The nano-VH x -modified MgH 2 releases hydrogen from 182 °C, which is 88 °C lower than additive-free MgH 2 . The release of hydrogen amounts to 6.3 wt% H within 10 min at 230 °C and 5.6 wt% H after 30 min at 215 °C with initial vacuum. More importantly, the dehydrogenated MgH 2 +10 wt.% nano-VH x rapidly absorbs 5.2 wt% H within 3 min at 50 °C under 50 bar H 2 . It even takes up 4.3 wt% H within 30 min at room temperature (25 °C) under 10 bar H 2 , exhibiting superior hydrogenation kinetics to most of the previous reports. Mechanistic analyzes disclose the reversible transformation between V and V-H species during the hydrogen desorption-absorption process. The homogeneously distributed V-based species is believed to act as hydrogen pump and nucleation sites for MgH 2 and Mg, respectively, thus triggering fast hydrogenation/dehydrogenation kinetics.
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
Inorganics
·
2023
·Vol. 11
·期 6
·243
·
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
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2011
·Vol. 36
·期 14
·8203-8208
·
IF 4.057
Z.G. Zhang,H. Wang,M. Zhu
The major challenge of complex hydride for hydrogen storage is to release hydrogen at a moderate temperature with rapid kinetics. This paper reports a new composite system (NaBH 4 /ZnF 2 ) to generate hydrogen at a low temperature below 100 °C. The NaBH 4 and ZnF 2 mixture was prepared by a mechanical milling in a 2:1 M ratio. Dehydrogenation of the mixture during a heating process shows that the initial dehydrogenation temperature was below 100 °C with favorable kinetics. The structural analysis confirmed the formation of NaBF 4 and Zn in the reaction products. The study concerning the reaction mechanism reveals that ZnF 2 plays a role of reagent rather than catalyst. The produced intermediate of NaZnF 3 , however, affects the decomposition of the emitted B 2 H 6 . This work suggests that the extension of the decomposition mechanism of NaBH 4 /ZnF 2 composite system would favor the development of new catalysts for complex hydride systems.
研究领域:
材料科学
·
能源化学
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无机化学
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储氢技术
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纳米催化
✓ 已验证
DOI
高影响因子
Journal of Magnesium and Alloys
·
2024
·
IF 15.8
Meihong Wu,Mingxia Gao,Shanqing Qu,Yongfeng Liu,Wenping Sun,Xin Zhang,Chu Liang,Xiaoyu Zhang,Yaxiong Yang,Hongge Pan
MgH 2 is a promising solid–state hydrogen storage material. However, its high thermodynamics and sluggish kinetics hinder its practical application. Catalytic strategy is effective in improving its kinetic performance. Nevertheless, the highly efficient catalysts or additives are normally of low-yield in fabrication with high cost. In this work, a novel structural LaVO 4 fabricated by a low-cost method of spraying dry followed by a calcination is used as a catalytic additive for the hydrogen storage of MgH 2 . With an optimized addition of LaVO 4 , the overall hydrogen storage performances of MgH 2 are significantly improved. An onset dehydrogenation temperature of only 183°C is obtained after an initial activation of dehydrogenation and hydrogenation. The system can desorb 5.7 wt% H 2 at 250°C within 10 min and maintains a dehydrogenation capacity of 5.0 wt% H 2 after 50 cycles. It is found that LaVO 4 is transferred to lanthanum hydride and metallic vanadium in the initial dehydrogenation process, the former acts as a highly effective catalyst for the hydrogen storage of MgH 2 and the latter undergoes reversible hydrogenation and dehydrogenation in the subsequent cycles. The structural design of the catalyst and its scalable fabrication are highly valuable in realizing the practical application of catalytic strategy for the hydrogen storage of MgH 2 .
研究领域:
材料科学
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催化化学
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能源存储
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Jiaguang Zheng,Zhendong Yao,Xuezhang Xiao,Xuancheng Wang,Jiahuan He,Man Chen,Hao Cheng,Liuting Zhang,Lixin Chen
Novel porous hollow carbon nanospheres (HCNS) have been synthesized and utilized as scaffold for LiBH 4 –Mg(BH 4 ) 2 eutectic borohydride (LMBH). Large loading amounts of LMBH (33, 50 and 67 wt%) have been melt-infiltrated into HCNS, and the significantly improved dehydrogenation properties have been discovered. The LMBH@HCNS composites not only exhibit high actual dehydrogenation amounts and fast hydrogen desorption rates, but also an increased reversible hydrogen storage capacities after three cycles without obvious degradation. Further structural tests have revealed that the over-infiltrated LMBH covering the spherical surface of HCNS could also contribute to the improved hydrogen storage behaviors, due to a strong interfacial adhesion effect that avoid LMBH from aggregation during de/rehydrogenation cycles.
研究领域:
材料科学
·
化学工程
·
能源存储
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2024
·
IF 10.7
Zonglin Liu,Honglei Zhang,Dongyue Liu,Yujie Feng,Dechang Jia,Caicai Li,Qingfeng Sun,Yu Zhou,Zhenhui Kang,Baoqiang Li
The in-depth understanding of electrocatalysts is the key issue in the fields of clean energy and the chemical industry. Although various carbon-loaded active metal particle catalysts for the electrocatalytic hydrogen evolution reaction (HER) have been developed, the interaction between active metals and the substrate is still unclear. Herein, ruthenium (Ru) nanoparticles loaded on N-doped carbon dots (Ru/NCDs) were constructed to discover the critical roles of the carbon substrate as well as its interaction with Ru. Notably, we show the two critical functions of NCDs in a carbon-confined Ru system. First, the ultra-small Ru nanoparticles increase the hydrogen spillover channels. Second, the carbon substrate shows a Ru-like hydrogen adsorption capacity, supplying sufficient H sources for hydrogen spillover. Thus, the hydrogen spillover is enhanced and the HER process is accelerated. The Ru/NCDs catalyst shows superior HER activity and durability in both acidic and alkaline solutions. This work clarifies the critical role of carbon substrates in carbon-loaded catalysts.
研究领域:
电化学
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催化
·
清洁能源
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2018
·
IF 4.229
Zhao Jiang,Xiang Gong,Bin Wang,Zhiqiang Wu,Tao Fang
Liquid organic hydrogen carrier (LOHC) is considered as a promising candidate for large-scale hydrogen storage. In this work, we found that Pt/TiO 2 catalysts exhibited better catalytic activity and selectivity compared to Pd/TiO 2 and commercial Pd/Al 2 O 3 catalysts in the dehydrogenation of dodecahydro-N-ethylcarbazole (12H-NECZ) at 453 K. The catalytic activity of the noble metal catalysts followed the trend of Pt/TiO 2 > Pd/TiO 2 > Rh/TiO 2 > Au/TiO 2 > Ru/TiO 2 . Compared with the commercial Pd/Al 2 O 3 , Pt/TiO 2 greatly improved the selectivity and conversion rate, the reaction time was also shortened. In addition, kinetics calculation was carried out to obtain fundamental reaction parameters. It was found that the third step of 4H-NECZ dehydrogenation to NECZ was the rate-limiting step of the entire dehydrogenation reaction for all catalysts.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2022
·Vol. 52
·期 3
·609-620
·
IF 4.569
Samuel Guemou,Dongqiang Gao,Fuying Wu,Jiaguang Zheng,Tao Wei,Zhendong Yao,Danhong Shang,Liuting Zhang
As an ideal material for solid-state hydrogen storage, magnesium hydride (MgH2) has attracted enormous attention due to its cost-effectiveness, abundant resources, and outstanding reversibility. However, the high thermodynamics and poor kinetics of MgH2 still hinder its practical application. In this work, a simple stirring–hydrothermal method was used to successfully prepare bimetallic Mn3O4/ZrO2 nanoparticles, which were subsequently doped into MgH2 by mechanical ball milling to improve its hydrogen sorption performance. The MgH2 + 10 wt% Mn3O4/ZrO2 composite began discharging hydrogen at 219 °C, which was 111 °C lower compared to the as-synthesized MgH2. At 250 °C, the MgH2 + 10 wt% Mn3O4/ZrO2 composite released 6.4 wt% hydrogen within 10 min, whereas the as-synthesized MgH2 reluctantly released 1.4 wt% hydrogen even at 335 °C. Moreover, the dehydrogenated MgH2 + 10 wt% Mn3O4/ZrO2 sample started to charge hydrogen at room temperature. 6.0 wt% hydrogen was absorbed when heated to 250 °C under 3 MPa H2 pressure, and 4.1 wt% hydrogen was taken up within 30 min at 100 °C at the same hydrogen pressure. In addition, compared with the as-synthesized MgH2, the de/rehydrogenation activation energy values of the MgH2 + 10 wt% Mn3O4/ZrO2 composite were decreased to 64.52 ± 13.14 kJ mol−1 and 16.79 ± 4.57 kJ mol−1, respectively, which incredibly contributed to the enhanced hydrogen de/absorption properties of MgH2.
研究领域:
材料科学
·
氢能
·
纳米技术
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Jinlong Yang,Xinglin Yang,Feitao Fan,Qianqian Han,Quanhui Hou
MgH 2 is a promising energy storage material due to its high hydrogen capacity and cost-effectiveness. However, its practical application is limited by a high dehydrogenation temperature and sluggish kinetics. While doping with Fe 2 NiO 4 alone has been shown to lower the initial dehydrogenation temperature, its kinetic performance remains insufficient. To address this, this study synthesizes a novel Co 0.2 Ni 0.8 /Fe 2 NiO 4 (CNFO) bimetallic catalyst via hydrothermal treatment, calcination, and ultrasonic methods. The results demonstrate that 15 wt% CNFO is the optimal doping concentration, under which MgH 2 exhibits outstanding hydrogen desorption performance, delivering 5.82 wt% H 2 in just 10 min under 260 °C. In comparison, although 40 wt% is the optimal loading for Fe 2 NiO 4 alone, it releases merely 3.79 wt% H 2 in 60 min under 300 °C. Regarding absorption, MgH 2 + 15 wt% CNFO absorbs 4.94 wt% H 2 in 9 min under 120 °C and 3 MPa, whereas MgH 2 + 40 wt% Fe 2 NiO 4 absorbs only 4.50 wt% H 2 in 9 min under 300 °C and 4 MPa. Therefore, the incorporation of Co0.2Ni0.8 is thus shown to be highly effective. Comprehensive characterization suggests that this improvement arises from the synergistic interaction between Co and Ni dispersed on the matrix surface, which effectively facilitates the reversible transformation between Mg 2 Ni and Mg 2 NiH 4 , thereby intensifying the so-called “hydrogen pump” effect. Altogether, this finding opens up a new avenue for the fabrication of MgH 2 catalysts with enhanced efficiency.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Fei Li,Zhuonan Huang,Yuqi Wang,Le Wu,Sinan Guan,Yue Wang,Ying Liu,Shuang Cheng,Jinlei Wu,Jun Hu,Xin Ding
Magnesium hydride (MgH 2 ) has garnered substantial consideration mainly due to its high gravimetric density and reliable resource, whereas its poor thermodynamics and kinetics for absorbing/releasing hydrogen restricts the largescale application. Certain catalysts have demonstrated remarkable activity in enhancing the hydrogen storage capabilities of MgH 2 . In this work, the nanoparticle-cumulated flower-like CoFe@C coated catalysts (denoted as CoFe@C) are controllably synthesized as expected by the MOF (Metal-Organic Farmwork) in-suit decomposition method at 800 °C, which exhibits an average pore size of 18.63 nm. Meanwhile, the particle size for the as-prepared CoFe alloy coated in carbon layer are approximately 10–20 nm, and the as-prepared samples are introduced to promote the de/rehydrogenation properties of MgH 2 at relatively lower temperatures. Due to the synergistic interaction of CoFe alloy nanoparticles serving as active sites and agglomeration resistance of carbon layers, the MgH 2 composites doped with CoFe@C-800 could initialize its decomposition process at 175.9 °C, and may desorb 6.0 wt% H 2 at 300 °C in 400 s. Additionally, the peak temperature and apparent activation energy during dehydrogenation decline significantly (with 35 % and 38 %, respectively). Furthermore, theoretical analysis results indicate a higher catalytic activity for the carbon-coated CoFe alloy owing to the synergetic effect between CoFe nanocomposite & carbon layer, which can facilitate the bond extension and strength decrease of Mg-H bonding. In brief, using MOF may derive transition metal and carbon layer, which could be a promising approach to stimulating the hydrogen storage properties of MgH 2 .
研究领域:
材料科学
·
能源存储与转换
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Storage
·
2024
·
IF 8.9
Congwen Duan,Haimei Wang,Jinhui Wu,Ting Qu,Yuling Zhang,Dong Fu,Lianxi Hu,Fei Wang,Dongsheng Lai,Yueru Dai,Ying Wu
Mg/MgH 2 stands out as an excellent hydrogen storage material due to its abundant presence and its capacity for high hydrogen storage density. However, the sluggish hydrogenation/dehydrogenation kinetics make it unsuitable for solid-state hydrogen storage. To tackle these challenges, the MgH 2 -Co@Pd‑c arbon nanotubes composite was created through ball milling , and its hydrogenation/dehydrogenation behavior was examined. The inclusion of Co@Pd notably enhanced the kinetics of hydrogenation/dehydrogenation in Mg/MgH 2 . The Mg-Co@Pd‑c arbon nanotubes composite achieved an absorption of 7.30 wt% H 2 in just 8 h of milling. The study proposed an energy conversion model to investigate the enhanced properties of Mg/MgH 2 . The addition of Co@Pd substantially reduced the activation energy (Ea) for hydrogen desorption to 81.9 kJ/mol. Furthermore, Transmission Electron Microscope and Density Functional Theory simulations were employed to understand how Co@Pd enhances the properties of Mg/MgH 2 . The improved hydriding/dehydriding kinetics of Mg/MgH 2 are likely closely linked to both the confining impact of c arbon nanotubes and the synergistic interplay of the “spillover” and “hydrogen pump” effects facilitated by the Co@Pd bimetallic catalysts . The excellent hydriding/dehydriding behavior is ascribed to the electron spillover and the phase transformation of Mg 2 Co/Mg 2 CoH 5 and Mg 6 Pd/Pd. These findings offer new insights into the new insights into the rational design of Co@Pd bimetallic catalysts, which are expected to be an optimal solution for supported catalysts in Mg-based solid-state hydrogen storage systems.
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
危险品化学品经营许可证（带存储）