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J. Burgess R.D.W. Kemmitt N. Morton C.T. Mortimer M.P. Wilkinson 《Journal of organometallic chemistry》1980,191(2):477-480
Enthalpies, ΔH(1) ?94.8 ± 6.0 and ΔH(6) ?57.1 ± 5.1 kJ mol?1, of the following reactions have been measured calorimetrically [Pt(trans-stilbene)(PPh3)2](s) + dpcp(g) → (PPh3)2Pt(dpcb)(s) + trans-stilbene(g) (1) [Pt(trans-stilbene)(PPh3)2](s) + bcbd(g) → (PPh3)2Pt(bcpd)(s) + trans-stilbene (g) (6) where dpcp is diphenylcyclopropenone, (PPh3)2Pt(dpcb) is (1,1-bistriphenylphosphine)platinadiphenylcyclobutenone, (PPh3)2O, bcbd is benzocyclobutene-1,2-dione and (PPh3)2Pt(bcpd) is (1,1-bistriphenylphosphine)platinabenzocyclopentanedione, . It is concluded that the five-membered platinacyclo ring system in (PPh3)2Pt(dpcb) is not heavily strained. 相似文献
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Dimers of free nucleobases with their conjugate acid ions can be assigned to either of two categories: protonated dimers or proton-bound dimers. In the former, the extra proton attaches to a lone pair of a neutral dimer. In the latter, the extra proton is situated between two lone pairs and participates in a proton bridge. In general, proton-bound dimers are found to be more tightly held together than protonated dimers. While neutral adenine and its isomer 8-aminopurine (C(5)H(5)N(5)) are substantially more stable than their 7H tautomers, their conjugate acid ions and those of their respective 7H tautomers have nearly the same heats of formation. Correspondingly, the most stable (C(5)H(5)N(5))2H+ structures contain 7H tautomers as the neutral partner. Proton transit from one partner to the other within the most stable protonated dimer of 8-aminopurine has a low barrier (6 kJ mol(-1)). The potential energy curve for the NH stretch in that case is better fitted as a double minimum rather than as a harmonic potential. Purine-purine mismatches have been observed in nucleic acids, to which calculated (C(5)H(5)N(5))2H+ dimer geometries appear nearly isosteric. 相似文献
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Inspection games in arms control 总被引:1,自引:0,他引:1
Rudolf Avenhaus Morton Canty D. Marc Kilgour Bernhard von Stengel Shmuel Zamir 《European Journal of Operational Research》1996,90(3):383
An inspection game is a mathematical model of a situation in which an inspector verifies the adherence of an inspectee to some legal obligation, such as an arms control treaty, where the inspectee may have an interest in violating that obligation. The mathematical analysis seeks to determine an optimal inspection scheme, ideally one which will induce legal behavior, under the assumption that the potential illegal action is carried out strategically; thus a non-cooperative game with two players, inspector and inspectee, is defined. Three phases of development in the application of such models to arms control and disarmament may be identified. In the first of these, roughly from 1961 through 1968, studies that focused on inspecting a nuclear test ban treaty emphasized game theory, with less consideration given to statistical aspects associated with data acquisition and measurement uncertainty. The second phase, from 1968 to about 1985, involves work stimulated by the Treaty on the Non-Proliferation of Nuclear Weapons (NPT). Here, the verification principle of material accountancy came to the fore, along with the need to include the formalism of statistical decision theory within the inspection models. The third phase, 1985 to the present, has been dominated by challenges posed by such far-reaching verification agreements as the Intermediate Range Nuclear Forces Agreement (INF), the Treaty on Conventional Forces in Europe (CFE) and the Chemical Weapons Convention (CWC), as well as perceived failures of the NPT system in Iraq and North Korea. In this connection, the interface between the political and technical aspects of verification is being examined from the game-theoretic viewpoint. 相似文献
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Photoionization studies of (CH(3))(2)CHC(CH(3))(2)OH (tert-hexyl alcohol, also called thexyl alcohol) exhibit four fragmentations below 10 eV. As with other tertiary alcohols, no molecular ion is detected. The only ion observed at threshold corresponds to propane loss. Examination of a deuterated analogue, (CH(3))(2)CHC(CD(3))(2)OH, shows only loss of C(3)H(7)D, implying that the fragment ion has the structure of ionized acetone enol. There is no evidence for reversible deuterium transposition, as has been reported for isotopomers of the homologous secondary alcohol (CH(3))(2)CHCH(CH(3))OH. Propane loss from thexyl alcohol is attributed to intermediacy of ion-neutral complexes containing isopropyl radical and O-protonated acetone. Simple cleavage to give O-protonated acetone has an appearance energy 18 kJ mol(-1) higher than that of propane loss. Thermochemical estimates and ab initio calculations both predict that methyl loss should have a lower threshold than the fragmentation leading to isopropyl loss, but experiments show the appearance energy to be 6 kJ mol(-1) higher. This is consistent with previous reports of reverse activation barriers for methyl cleavages. Finally, formation of tert-hexyl cation, (CH(3))(2)CHC(CH(3))(2)(+), is observed with an appearance energy comparable to that of methyl loss, substantially below that predicted for OH radical expulsion from the molecular ion. The comparatively low threshold of this fragmentation is ascribed to ion-pair formation (concomitant with hydroxide ion) directly from an electronically excited neutral. Interactions between charged and neutral fragments (including energetics, bond orders <1, and electrical charges on molecular fragments) are explored using a combination of DFT and ab initio methods, along with topological analysis using the Atoms in Molecules approach. 相似文献