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
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化学工程
·
能源存储
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Han Yu,Ying Cheng,Yaokun Fu,Lu Zhang,Sanyang Guo,Yuan Li,Wei Zhang,Shumin Han
Carbon-based materials have been proposed as an ideal medium to reduce the reaction energy barriers and improve the (de)hydrogenation kinetics of magnesium-based hydrogen storage material (MgH 2 ) in term of their excellent dispersion. However, tedious preparation process and uneven distribution of carbon restrict the application. Therefore, in this paper, we cover MgH 2 by in-situ formed amorphous carbon via a facile approach of co-sintering Mg with fluorene followed by hydriding combustion and ball milling processes, named as MgH 2 -carbonization product of fluorene (MgH 2 -CPF). As a result, the MgH 2 -CPF composite prepared at 823 K initially dehydrogenates at 557 K, 94 K lower than the as-milled MgH 2 (651 K). Meanwhile, the composite can release 5.67 wt% H 2 within 1000 s at 623 K. Even at a lower temperature of 423 K, the MgH 2 -CPF composite still reabsorbs 5.62 wt% H 2 within 3600 s, while the as-milled Mg can hardly absorb hydrogen under a same condition. Furthermore, by addition of CPF, the apparent activation energy of the system is decreased from 161.2 kJ/mol to 87.2 kJ/mol. Our finding suggests that the carbon layer can keep the MgH 2 from aggregation, promote hydrogen transport and improve the efficiency of hydrogen absorption and desorption.
研究领域:
材料科学
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氢储存
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能源材料
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Yongqing Wang,Zhiqiang Lan,Xiantun Huang,Haizhen Liu,Jin Guo
Using a deposition-reduction method, Mg/MOF nanocomposites were prepared as composites of Mg and metal-organic framework materials (MOFs = ZIF-8, ZIF-67 and MOF-74). The addition of MOFs can enhance the hydrogen storage properties of Mg. For example, within 5000 s, 0.6 wt%, 1.2 wt%, 2.7 wt%, 3.7 wt% of hydrogen were released from Mg, Mg/MOF-74, Mg/ZIF-8, Mg/ZIF-67, respectively. Activation energy values of 198.9 kJ mol −1 H 2 , 161.7 kJ mol −1 H 2 , 192.1 kJ mol −1 H 2 were determined for the Mg/ZIF-8, Mg/ZIF-67, Mg/MOF-74 hydrides, which are 6 kJ mol −1 H 2 , 43.2 kJ mol −1 H 2 , and 12.8 kJ mol −1 H 2 lower than that of Mg hydride, respectively. Moreover, the cyclic stability characterizing Mg hydride was significantly improved when adding ZIF-67. The hydrogen storage capacity of the Mg/ZIF-67 nanocomposite remained unchanged, even after 100 cycles of hydrogenation/dehydrogenation. This excellent cyclic stability may have resulted from the core-shell structure of the Mg/ZIF-67 nanocomposite.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Frontiers in Chemistry
·
2020
·
IF 3.693
Zhang Xin,Zhang Xuelian,Ren Zhuanghe,Hu Jianjiang,Gao Mingxia,Pan Hongge,Liu Yongfeng
In this paper, we report amorphous-carbon-supported TiB2 nanoparticles having sizes of 2–4 nm (nano-TiB2@C) as highly active catalysts for hydrogen storage in NaAlH4. Nano-TiB2@C was synthesized by a simple calcination at 550°C with Cp2TiCl2 and MgB2 (molar ratio of 1:1) as precursors. The addition of 7 wt% nano-TiB2@C reduced the onset dehydrogenation temperature of NaAlH4 by 100 to 75°C. A practically available hydrogen capacity of 5.04 wt% could be desorbed at 140°C within 60 min, and completely hydrogenated at 100°C within 25 min under a hydrogen pressure of 100 bar. Notably, the hydrogen capacity was almost unchanged after 20 cycles, which shows the stable cyclability, considerably higher than those of structures catalyzed by Ti halides or TiO2. The stable catalytic function was closely related to the in-situ-formed Ti–Al alloy, which considerably facilitated the dissociation and recombination of H–H and Al–H bondings.
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2020
·
IF 4.65
Tianping Huang,Jianxin Zou,Huabing Liu,Wenjiang Ding
Three kinds of transition metal fluorides TMF x (TM = Nb, Co, Ti) were introduced into the 3NaBH 4 -GdF 3 hydrogen storage system via mechanical milling. Their effects on the hydrogen storage behaviors of 3NaBH 4 -GdF 3 were systematically investigated by means of DSC and volumetric methods. All TMF x exhibited promoting effect on hydrogen desorption properties of 3NaBH 4 -GdF 3 to different degrees, especially when NbF 5 or TiF 3 was added. For example, the hydrogen desorption peak temperature was decreased by 17 °C with doping 3 mol% of NbF 5 . Besides, TiF 3 improved also the hydrogen absorption capacity and reversibility of 3NaBH 4 -GdF 3 . Based on XRD analyses, the role of TMF x on the dehydrogenation and the promoting effect of TiF 3 on the reversibility of 3NaBH 4 -GdF 3 were clarified. This work helped to understand the combination effect of rare earth metal fluoride (GdF 3 ) and transition metal fluorides on the reversible hydrogen storage properties of 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
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Yuhang Wang,Guangxin Fan,Dafeng Zhang,Yanping Fan,Baozhong Liu
The enhanced effect of metal catalysts is crucial to achieve advanced performance of hydrogen storage system. Rational design of catalysts with superior catalytic activity is significant to regulate the re-/hydrogenation kinetics of MgH 2 . Herein, Ti 3 C 2 -supported praseodymium(III) fluoride (PrF 3 ) nanoparticles (PrF 3 /Ti 3 C 2 ) composite was prepared by hydrothermal method , which exhibited superior catalytic activity toward hydrogen storage of MgH 2 . The onset temperature of dehydrogenation was reduced to 180 °C after adding 5 wt% PrF 3 /Ti 3 C 2 , corresponding to a reduction of 107 °C compared with pristine MgH 2 . About 7.0 wt% hydrogen was rapidly desorbed within 3 min at 260 °C and 6.6 wt% hydrogen was absorbed within 36 s at 200 °C for MgH 2 -5 wt% PrF 3 /Ti 3 C 2 . Moreover, MgH 2 -5 wt% PrF 3 /Ti 3 C 2 exhibited an excellent capacity retention of 92.5% even after 10 cycles. Experimental results reveal that the electron transfer among Ti-species (Ti 0 , Ti 2+ , and Ti 3+ ) occurred due to the striking enhanced effect of PrF 3 on Ti 3 C 2 MXene during the reaction process, and the synergistic action between Ti-species and PrF 3 are responsible for the markedly enhanced hydrogen storage properties of MgH 2 . This study is helpful to the design and optimization of hydrogen storage materials for mobile application.
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
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Jingjing Chen,Chaoqun Li,Wei Chen,Xiaoyue Zhang,Xuebin Yu,Guanglin Xia
Despite of the moderate working temperature and relatively high hydrogen capacity of NaAlH 4 , the slow H 2 absorption and desorption kinetics and poor reversibility pose a major bottleneck hindering its practical application. Herein, porous NiTiO 3 nanorods is constructed to tailor reversible hydrogen storage performance of NaAlH 4 . It is theoretically and experimentally demonstrated that the building of NiTiO 3 nanorods effectively promotes the uniform distribution of catalytic Ni-based species and Ti-based species inside of NaAlH 4 matrix that are capable of synergistically weakening Al-H bonds of NaAlH 4 . As a result, under the catalysis of porous NiTiO 3 nanorods, the onset temperature for H 2 desorption from NaAlH 4 is decreased down to 89 °C, 91 °C lower than that of pure NaAlH 4 . In addition, NaAlH 4 under the catalysis of porous NiTiO 3 nanorods is capable of releasing 4.5 wt% H 2 within 60 min, 3.8 and 0.9 wt% higher than that of NaAlH 4 catalyzed by NiO and TiO 2 , respectively. More importantly, a reversible capacity of 4.6 wt% could be obtained for NaAlH 4 under the catalysis of porous NiTiO 3 nanorods after 5 cycles, corresponding to a capacity retention of 95%, while this value is significantly decreased to 42% for NaAlH 4 without the addition of NiTiO 3 nanorods. This work provides a new perspective for the development and design of high-performance catalysts for realizing reversible hydrogen storage of NaAlH 4 under moderate condition.
研究领域:
材料科学
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氢储存技术
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催化剂开发
✓ 已验证
DOI
高影响因子
Nanoscale
·
2019
·Vol. 11
·期 15
·7465-7473
·
IF 6.97
Meng Zhang,Xuezhang Xiao,Xinwei Wang,Man Chen,Yunhao Lu,Meijia Liu,Lixin Chen
Transition metal compounds are one of the highly efficient types of catalyst for improving the reaction kinetics of hydrogen storage materials. Among all the transition metals, titanium and its compounds show great catalytic effects on magnesium hydride. In this study, for the first time, TiO2 nanosheets with exposed {001} facets were synthesized and doped into MgH2. The TiO2 nanosheet (NS)-doped MgH2 showed superior kinetic performance and the lowest desorption temperature. The onset temperature of MgH2 + 5 wt% TiO2 NS for the release of hydrogen was 180.5 °C and the corresponding peak temperature was 220.4 °C, which are much lower than those of pure MgH2 and also distinctly lower than those of MgH2 + 5 wt% TiO2 nanoparticles (NP). For the isothermal dehydrogenation analysis, the MgH2 + 5 wt% TiO2 NS could release 6.0 wt% hydrogen within 3.2 min at 260 °C and desorb 5.8 wt% hydrogen within 6 min at 240 °C. It is worth noting that the MgH2 + 5 wt% TiO2 NS can even release 1.2 wt% hydrogen at a temperature as low as 180 °C within 300 min. The hydrogenation kinetics of MgH2 + 5 wt% TiO2 NS is also greatly improved, which could absorb hydrogen within only a few seconds at mild temperature. It can take up 3.3 wt% hydrogen at 50 °C and 5.4 wt% at 100 °C within 10 s. It is demonstrated that the tremendous enhancement in reaction kinetics of MgH2 can be ascribed to the nanometer size and highly active {001} facets of anatase TiO2. The higher average surface energy can significantly reduce the hydrogen desorption activation energy of MgH2 to 67.6 kJ mol−1, thus easily improving the hydrogen desorption properties.
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
Chemistry-An Asian Journal
·
2016
·Vol. 11
·期 24
·3541-3549
·
IF 4.592
Xin Zhang,Ruyan Wu,Zeyi Wang,Mingxia Gao,Hongge Pan,Yongfeng Liu
Graphical Boosting hydrogen storage : In situ-synthesized nanocrystalline ZrO 2 @C exhibits good catalytic activity for hydrogen storage in NaAlH 4 . The NaAlH 4 –7 wt % ZrO 2 @C sample releases hydrogen starting from 126 °C and reabsorbs hydrogen starting from 54 °C, and these temperatures are lower by 71 and 36 °C, respectively, than those for pristine NaAlH 4 (see figure). Sodium alanate (NaAlH 4 ) has attracted intense interest as a prototypical high-density hydrogen-storage material. However, poor reversibility and slow kinetics limit its practical applications. Herein, a nanocrystalline ZrO 2 @C catalyst was synthesized by using Uio-66(Zr) as a precursor and furfuryl alcohol (FA) as a carbon source. The as-synthesized ZrO 2 @C exhibits good catalytic activity for the dehydrogenation and hydrogenation of NaAlH 4 . The NaAlH 4 -7 wt % ZrO 2 @C sample released hydrogen starting from 126 °C and reabsorbed it starting from 54 °C, and these temperatures are lower by 71 and 36 °C, respectively, relative to pristine NaAlH 4 . At 160 °C, approximately 5.0 wt % of hydrogen was released from the NaAlH 4 -7 wt % ZrO 2 @C sample within 250 min, and the dehydrogenation product reabsorbed approximately 4.9 wt % within 35 min at 140 °C and 100 bar of hydrogen. The catalytic function of the Zr-based active species is believed to contribute to the significantly reduced operating temperatures and enhanced kinetics.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2023
·
IF 10.9
Yuxiao Jia,Xuancheng Wang,Leijie Hu,Xuezhang Xiao,Shuoqing Zhang,Jiahuan He,Jiacheng Qi,Ling Lv,Fen Xu,Lixian Sun,Lixin Chen
Ultrafine carbon-based transition metal compounds have been widely investigated as efficient catalysts for enhancing the hydrogen storage performance of magnesium hydride. In this work, the carbon thermal shock method is applied to synthesize the ultrafine carbon-encapsulated NbC nanoparticles with an average grain size of 17.3 nm. The MgH 2 –10 wt% NbC/C composites show excellent low-temperature hydrogen storage performance with the onset dehydrogenation temperature of 196.1 °C, which is 92.2 °C and 98 °C lower than that of MgH 2 –10 wt% NbC and undoped MgH 2 , respectively. Specifically, MgH 2 –10 wt% NbC/C can absorb 6.71 wt% H 2 at 100 °C within 30 min around and retain almost 100% reversible hydrogen desorption capacity after 10 cycles. For the catalytic mechanism, the electron transfer process between multi-valence Nb cations of in-situ formed NbH x and Mg, H atoms can greatly improve the cyclic de/rehydrogenation kinetics of MgH 2 -NbC/C. Besides, the enhancement of dehydrogenation kinetics can also be ascribed to MgH 2 particle refinement by NbC nanoparticles, and destabilization of the Mg-H bond caused by carbon substrate. This investigation not only proves that carbon-encapsulated NbC nanoparticles can greatly enhance the hydrogen storage performance of MgH 2 but provides an idea of preparing carbon-based transition metal carbides as effective catalysts for magnesium-based hydrogen storage materials.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
Energy & Environmental Science
·
2020
·Vol. 14
·期 4
·2302-2313
·
IF 30.289
Xin Zhang,Yongfeng Liu,Zhuanghe Ren,Xuelian Zhang,Jianjiang Hu,Zhenguo Huang,Yunhao Lu,Mingxia Gao,Hongge Pan
Using light metal hydrides as hydrogen carriers is of particular interest for safe and compact storage of hydrogen. Magnesium hydride (MgH2) has attracted significant attention due to its 7.6 wt% hydrogen content and the natural abundance of Mg. However, bulk MgH2 is stable (ΔHf ∼ 76 kJ mol−1) and releases hydrogen only at impractically high temperatures (>300 °C). Herein, we demonstrate a first attempt to achieve ambient-temperature reversibility of hydrogen storage for MgH2 by fabricating non-confined ultrafine nanoparticles. Taking advantage of the big discrepancies in the solubility of metal hydrides and chlorides in THF, a novel metathesis process of liquid–solid phase driven by ultrasound was proposed. Ultrafine MgH2 nanoparticles predominantly of around 4–5 nm in size were successfully obtained without scaffolds or supports. A reversible hydrogen storage capacity of 6.7 wt% at 30 °C was measured, which has never been achieved before, thanks to thermodynamic destabilization and decreased kinetic barriers. The bare nanoparticles exhibited a stable and rapid hydrogen cycling behaviour in 50 cycles at 150 °C, a remarkable improvement compared with bulk MgH2. Our finding brings MgH2 a step closer to practical applications and the methodology presented here opens new pathways for fabricating sensitive nanoparticles.
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
·
2023
·
IF 7.2
Shijie Wang,Shenghan Zhang,Zhenye Zhang,Yu Tan,Kexin Liang,Xinliang Guo,Xuhui Kong
Nitrogen heterocyclic organics are promising hydrogen storage carriers with the advantage of being capable of large-scale transportation over long distances using existing oil and gas facilities. However, traditional methods for the hydrogenation and dehydrogenation of organic hydrogen carriers usually require high temperature and pressure conditions and external hydrogen supplies, which hinder their large-scale applications, as well as having certain safety risks. In this paper, a reversible electrochemical hydrogen storage system using quinoxaline as a hydrogen carrier was developed with potential for use at room temperature and atmospheric pressure. Experiments revealed that the hydrogenation conversion of quinoxaline reached 95% within 120 min at −0.20 V vs. RHE, and the dehydrogenation conversion of 1,2,3,4-tetrahydroquinoxaline reached 100% within 30 min at 1.30 V vs. RHE. This means that the system achieved quick and efficient reversible hydrogen storage. The Pd/NF dual-function electrode prepared by spontaneous redox reaction still showed high catalytic activity after 8 cycles, indicating its good long-term stability. The proton donor in the electrochemical hydrogenation process of quinoxaline was water, which completely eliminates the safety risk from the use of external hydrogen. This work provides a simple and reliable strategy for efficient hydrogen storage using nitrogen heterocyclic organics.
研究领域:
材料科学
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能源化学
✓ 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）