孙大林
高性能贮氢材料的研发、氢与金属(金属薄膜)相互作用的基础和应用研究
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- 姓名:孙大林
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博士生导师,
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学科领域:
材料科学基础学科
- 研究兴趣:高性能贮氢材料的研发、氢与金属(金属薄膜)相互作用的基础和应用研究
孙大林,1992年于浙江大学材料科学与工程系获博士学位,毕业后任该校材料科学与工程系讲师、副教授。曾先后主持和参加了国家自然科学基金、青年基金、“863”高技术项目等有关高性能贮氢材料的研究项目。95年获法国科学研究中心的资助,于稀土冶金及其谱化学实验室任助理研究员,研究改善新型锆基Laves相合金氢化物电极材料的电化学活化性能。96年获得欧盟Brite/EURAM项目的资助,赴英国卢瑟福实验室和Salford 大学物理系利用中子散射技术研究镍-氢化物二次电池高速放电的动力学性能。1997年获日本通商产业省新能源产业技术综合开发机构的资助,任物质工学与工业技术研究所NEDO研究员,研究和开发高性能镁基复合贮氢材料。2000年受美国能源部“Hydrogen Program”的资助,赴夏威夷大学化学系研究和开发以NaAlH4为代表的新一代高性能贮氢材料。2003年任复旦大学材料科学系教授、博导。现从事高性能贮氢材料的研发、氢与金属(金属薄膜)相互作用的基础和应用研究。
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【期刊论文】Rehydrogenation and cycling studies of dehydrogenated NaAlH4
孙大林, Dalin Suna, *, Sesha S. Srinivasanb, Guorong Chena, Craig M. Jensenb
Journal of Alloys and Compounds 373(2004)265-269,-0001,():
-1年11月30日
/3Al+1/2H2↔1/3Na3AlH6+2/3Al+H2↔NaAlH4 was studied in the temperature range of 80-170℃ and the pressure range of 8-12MPa. It was found that under the pressure of 12MPa, an increase in the hydrogenation temperature from 100 to 170℃ causes a reduction in the amount of absorbed hydrogen. Under the constant pressure of 10MPa, the initial rate of hydrogenation increases when the temperature increases from 80 to 120℃, and reaches an optimum at 120℃; further increase in temperature leads to a decrease in the rate. It was also observed that at a constant temperature, the rate increases with the increase of applied hydrogen pressure. The cycling studies of titanium doped NaAlH4 have shown that the initial capacity was about 3.6wt.%, but after a few dehydrogenation-rehydrogenation cycles, the capacity decreases to 3.0wt.%. And this capacity was retained with no further deterioration in the following consecutive 100 cycles. However, the rates of the two-step dehydrogenation processes were found to reduce kinetically with the ongoing cycling.
Hydrogen absorbing materials, Hydride, Hydrogenation, Cycling stability, Sodium aluminum hydride
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【期刊论文】Improved kinetics by the multiphase alloys prepared from Laves phases and LaNi5
孙大林, M. Bououdina*, D.-L. Sunb, H. Enokib, E. Akibab
Journal of Alloys and Compounds 288(1999)229-237,-0001,():
-1年11月30日
We propose a new method to prepare hydrogen absorbing alloys from single phase intermetallic ones. The alloys, (100-x) Zr0.5Ti0.5Cr1.5Ni0.51x LaNi5 (x=5-20 mass%) as prepared by this method showed dramatic enhancement of the hydrogenation properties. The Rietveld analysis on XRD data revealed that pure Cr precipitated from the Laves phase and its relative amount was proportional to the nominal LaNi amount. The PCT curves measured at 313K showed a large hydrogen capacity, 1.4wt%.
Laves phases, Mixed phases, LaNi5, Hydriding kinetics
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孙大林, J.-M. Joubert, Dalin Sun, M. Latroche, A. Percheron-Guegan*
Journal of Alloys and Compounds 253-254(1997)564-569,-0001,():
-1年11月30日
Zr-based AB, (B=V, Cr, Mn) Laves phases are studied for their ability to reversibly store hydrogen and are potential negative electrode materials in Ni-MH batteries. The hydrides formed are too stable for electrochemical use and their thermodynamicat properties can be adapted by Ni substitution on the B sublattice. However, measured electrochemical reversible capacities are very low compared to solid-gas results. This phenomenon is related to passivation and surface corrosion in electrolytic medium. To overcome this problem, the role of secondary phases has been studied following two routes: precipitation of controlled amounts of Zr-Ni binary intermetallic compounds or addition of a rare earth (R) element leading to precipitation of RNi compound in the matrix. The consequences on the electrochemical behaviour are discussed in terms of the microstructure of the alloys which lead to composite electrodes by taking advantage of the bulk properties of the Laves phase and the surface properties of the secondary phase (s).
Zr-based Laves phases, Hydrides, Nickel-hydride batteries, Secondary phases, Activation
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【期刊论文】New approach for synthesizing Mg-based alloys
孙大林, Dalin Sun, Hirotoshi Enoki, Franz Gingl, Etsuo Akiba*
Journal of Alloys and Compounds 285(1999)279-283,-0001,():
-1年11月30日
Mg2Ni, Mg2Cu and MgZn2 were synthesized by means of ball-milling plus solid-state reactions. Firstly, the mixtures of the two elemental powders, corresponding to the compositions of Mg2Ni, Mg2Cu and MgZn2, were subject to ball-milling for 20 min. Then, they were pressed into pellets and sintered at temperatures below the melting points of the components. X-ray diffraction experiments show that the yields of the desired products are above 97wt%, higher than those prepared by the conventional metallurgical method. The hydrogenation properties of the Mg2Ni sample synthesized by solid-state reaction are in agreement with the previously published resultson alloys prepared by the conventional methods.
Mg-based alloys, solid-state reaction, hydride
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【期刊论文】In situ X-ray diffraction study of hydrogen-induced phase decomposition in LaMg12 and La2 Mg17
孙大林, Dalin Suna, Franz Gingla, Yumiko Nakamuraa, Hirotoshi Enokia, Mohomed Bououdinab, Etsuo Akibaa, *
Journal of Alloys and Compounds 333(2002)103-108,-0001,():
-1年11月30日
In situ X-ray diffraction (XRD) shows that LaMg and LaMg12 and thermally stable under argon upon heating to 330℃, while under hydrogen they decompose to LaH3 and MgH2 at about 290 and 270℃, respectively. The decomposition is believed to result from the large difference in enthalpy between the parent compounds and the resultants. Prior to the decomposition, the lattice parameters of LaMg12 and La2 Mg17 do not change, indicating that hydrogen does not dissolve into them to form solid solution of LaMg12 Hx and La2 Mg12 Hx. The enhanced mobility of La and/or Mg was observed in the presence of hydrogen, which might be related to the formation of the copious vacancy.
Rare earth compounds, Hydrogen-absorbing materials, X-ray diffraction
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孙大林, Dalin Suna, Tetsu Kiyobayashib, Hiroyuki T. Takeshitab, Nobuhiro Kuriyamab, Craig M. Jensena, *
Journal of Alloys and Compounds 337(2002)L8-L11,-0001,():
-1年11月30日
X-ray diffraction patterns of NaAlH4 doped with up to 10mol.% of either titanium or zirconium do not contain Bragg peaks for the 4 bulk metals or their aluminum alloys. Instead the hydride lattice parameters a and c undergo significant contraction upon 2mol.% doping and then expand as the doping level increases from 2 to 5mol.%. These results are explained by a model that entails substitution of sodium cations by variable valence transition metal cations and the creation of Na+ vacancies in the bulk hydride lattice.
Hydrogen absorbing materials, Metal hydrides, X-ray diffraction, Vacancy formation
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孙大林, D. SUN, F. GINGL, H. ENOKI, D. K. ROSS, and E. AKIBA†
Acta mater. 48(2000)2363-2372,-0001,():
-1年11月30日
Mg-x wt% LaNi5 (x =20-50) composite materials were prepared by sintering powder mixtures of magnesium and LaNi5 at 973 K for 1 h. The microstructures were studied using optical microscopy, X-ray diffraction and scanning electron microscopy. After sintering, the samples with x=20 and 30 consisted of Mg, Mg2Ni and LaMg12. As x increased to 40, the La2Mg17 phase started to form. With further increase in x to 50, Mg and LaMg12 vanished, and Mg2Ni and La2Mg17 were the major phases. The phase abundance as a function of composition was determined by Rietveld analysis. It is also found that LaMg12 is not a well-de.ned stoichiometric compound but exists within a composition range. Compared with pure magnesium, all samples were more easily activated under hydrogen pressure of 5 MPa at 623 K. From the viewpoint of pressure
Sintering, X-ray diffraction (, XRD), , Hydrides, Microstructure, Hydrogenatio
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孙大林, Sesha S. Srinivasan a, Hendrik W. Brinks b, Bjorn C. Hauback b, Dalin Sun a, , Craig M. Jensen a, *
Journal of Alloys and Compounds 377(2004)283-289,-0001,():
-1年11月30日
A simple and an efficient synthesis route, solvent mediated milling of NaH and Al with 2mol% of the dopant precursor, Ti (OBu)4 followed by hydrogenation, has been developed and employed to synthesize Ti-doped NaAlH4. The long-term hydrogenation and dehydrogenation, up to 100 cycles were carried out systematically. Reversibility of about 3.4 wt.% hydrogen release was obtained during the first dehydrogenation (160℃) run after the initial hydrogenation of Ti-doped (NaH+Al) at 150℃; 1.4MPa H2 for 12h. In the subsequent cycles, the storage capacity increased, reaching an optimum of 4.0wt.%. This capacity was retained for 40 cycles with the dehydrogenation kinetic curves showing remarkable reproducibility. Comparison of the X-ray diffraction profiles of Ti-doped (NaH+Al) from initial and final stages of the cycling study reveals a growing resistance to the hydrogenation of Na3AlH6 to NaAlH4.
Hydrogenation, Dehydrogenation, Cycling stability, Solvent mediated milling, Hydrogen storage capacity, Sodium aluminum hydride, Hydrogen absorbing materials, Metal hydrides, Mechanochemical processing, Gas-solid reactions
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【期刊论文】Rehydrogenation of Dehydrogenated NaAlH4 at Low Temperature and Pressure
孙大林, Dalin Sun, *, †, Sesha S. Srinivasan, Tetsu Kiyobayashi, ‡, Nobuhiro Kuriyama, and Craig M. Jensen†
,-0001,():
-1年11月30日
NaAlH4 is considered as a promising material for onboard storage of hydrogen. It is generally thought that high temperature (>120℃) and high pressure (>15 MPa) are needed for rehydrogenation of dehydrogenated NaAlH4. However, for practical application, reducing the rehydrogenation temperature and pressure as much as possible would be highly desirable. We have found that the dehydrogenated NaAlH4, in either the undoped or titanium-doped state, can be rehydrogenated at temperatures of 25-120℃ and pressures of 2-12MPa. This finding is confirmed by the subsequent dehydrogenation at 160℃. In addition to that, after rehydrogenation under the same conditions, the amount of evolved hydrogen from the titanium-doped NaAlH4 was much higher than that of the undoped NaAlH4. This clearly indicates that the addition of titanium species enhances kinetically not only the dehydrogenation, but also the reverse process, the rehydrogenation reaction of the dehydrogenated NaAlH4.
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孙大林, Tetsu Kiyobayashi, †, Sesha S. Srinivasan, ‡, Dalin Sun, and Craig M. Jensen*
,-0001,():
-1年11月30日
The rates of the dehydrogenation of the sodium alanates NaAlH4 and Na3AlH6 doped with 2mol% Tior Zr have been measured over the temperature range 363-423K. NaAlH4 and Na3AlH6 undergo dehydrogenation at equal rates upon direct doping with titanium. However, Na3AlH6 arising from the dehydrogenation of Ti-doped NaAlH4 undergoes dehydrogenation at much slower rates. Rate constants were determined from the slopes of the dehydrogenation profiles. On the basis of Eyring theory, the enthalpies of activation, △H‡, for the dehydrogenation reactions were determined to be ~100kJ-mol-1 for both Ti-doped NaAlH4 and Na3AlH6 and ~135kJ-mol-1 for both Zr-doped NaAlH4 and Na3AlH6. These results suggest that the dehydrogenation reaction pathways are highly sensitive to the nature and istribution of the dopant but not to differences in the Al-H bonding interactions in [AlH4]-and [AlH6]3-complex anions. Furthermore, we conclude that the kinetics are probably influenced by processes such as nucleation and growth and/or range atomic transport phenomenon.
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