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A new phenomenon is theoretically predicted, namely, that solid-solid transformation with a relatively large transformation strain can occur through virtual melting along the interface at temperatures significantly (more than 100 K) below the melting temperature. The energy of elastic stresses, induced by transformation strain, increases the driving force for melting and reduces the melting temperature. Immediately after melting, the stresses relax and the unstable melt solidifies. Fast solidification in a thin layer leads to nanoscale cracking, which does not affect the thermodynamics and kinetics of solid-solid transformation. Seven theoretical predictions are in quantitative agreement with experiments conducted on the beta-->delta transformation in the HMX energetic crystal. 相似文献
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Natan Bibelnik Sasha Gersten Alon B Henson Etay Lavert-Ofir Yuval Shagam Wojciech Skomorowski 《Molecular physics》2019,117(15-16):2128-2137
In many chemical reactions with more than one possible outcome, the branching ratio, which is the ratio between the different reaction paths, is nearly constant over a wide range of collision energies. In barrierless systems governed by long-range interactions, however, the branching ratio is more sensitive to collision energy, and its dependence on it can be useful for better understanding the dynamics and reconstructing interaction potentials. Here we present the reaction rates of Penning and associative ionisation of metastable neon and helium with argon atoms. We obtain reaction rates in merge beam experiments, over a wide range of collision energies corresponding to that of room temperature, all the way down to a few millikelvins. We observe a change of two orders of magnitude in the branching ratio in the measured collision energy range and explain these changes using theoretical calculations. 相似文献
65.
Baker RT Gordon JC Hamilton CW Henson NJ Lin PH Maguire S Murugesu M Scott BL Smythe NC 《Journal of the American Chemical Society》2012,134(12):5598-5609
Ammonia-borane (NH(3)BH(3), AB) has garnered interest as a hydrogen storage material due to its high weight percent hydrogen content and ease of H(2) release relative to metal hydrides. As a consequence of dehydrogenation, B-N-containing oligomeric/polymeric materials are formed. The ability to control this process and dictate the identity of the generated polymer opens up the possibility of the targeted synthesis of new materials. While precious metals have been used in this regard, the ability to construct such materials using earth-abundant metals such as Fe presents a more economical approach. Four Fe complexes containing amido and phosphine supporting ligands were synthesized, and their reactivity with AB was examined. Three-coordinate Fe(PCy(3))[N(SiMe(3))(2)](2) (1) and four-coordinate Fe(DEPE)[N(SiMe(3))(2)](2) (2) yield a mixture of (NH(2)BH(2))(n) and (NHBH)(n) products with up to 1.7 equiv of H(2) released per AB but cannot be recycled (DEPE = 1,2-bis(diethylphosphino)ethane). In contrast, Fe supported by a bidentate P-N ligand (4) can be used in a second cycle to afford a similar product mixture. Intriguingly, the symmetric analogue of 4 (Fe(N-N)(P-P), 3), only generates (NH(2)BH(2))(n) and does so in minutes at room temperature. This marked difference in reactivity may be the result of the chemistry of Fe(II) vs Fe(0). 相似文献
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TK Mukhopadhyay RK Feller FN Rein NJ Henson NC Smythe RJ Trovitch JC Gordon 《Chemical communications (Cambridge, England)》2012,48(69):8670-8672
The reduction of Triphos [PhP(CH(2)CH(2)PPh(2))(2)] iron halide complexes has been explored, yielding formally zerovalent (κ(3)-Triphos)Fe(κ(2)-Triphos) and (κ(3)-Triphos)Fe(κ(2)-Bpy). Electrochemical analysis, coupled with the metrical parameters of (κ(3)-Triphos)Fe(κ(2)-Bpy), reveal an electronic structure consistent with a π-radical monoanion bipyridine chelate that is antiferromagnetically coupled to a low spin, Fe(i) metal center. 相似文献
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Takahiro Ohkubo Yasuhiko Iwadate Yu Seung Kim Neil Henson Yoong-Kee Choe 《Theoretical chemistry accounts》2011,130(2-3):555-561
Sulfonated poly(arylene ether ether nitrile) (m-SPAEEN) copolymers are reported to have the property of reduced water uptake compared with other hydrocarbon membranes, such as sulfonated polysulfones or polyketones, with similar ion exchange capacity. It is believed that this difference is largely due to the nitrile group. In this study, to investigate the effect of the nitrile group on properties of polymer electrolyte membranes for fuel cell applications, we carried out a series of molecular dynamics (MD) simulations. We compared the results of MD simulations for m-SPAEEN and sulfonated poly(arylene ether sulfone)s (BPSH). We found that water molecules hydrate not only the sulfonate (SO3 ?) groups of m-SPAEEN but also other hydrophilic functional groups in the copolymers. Results showed that hydration around the nitrile group in m-SPAEEN and around the sulfone (SO2) group in BPSH differs in features related to water uptake: The former exhibits uptake of fewer water molecules than does the latter. This difference in hydration features causes m-SPAEEN to have a relatively low water-uptake level compared with BPSH. 相似文献
68.
Shandella M. Henson 《Journal of Difference Equations and Applications》2013,19(2):243-244
Difference Equations Theory and Applications by Ronald E. Mickens, CRZ: Press LLC, Eioca Iiaron, Florida, Second Edition, Publicarion Date: 01 /Oi /9l, 4-43 pages. ISBN: 0442001363, Price: $69.95 US. 相似文献
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