Periodic density functional theory（DFT） calculations are presented to describe the adsorption and decomposition of CH3OH on Ru（0001） surfaces with different coverages, including p（3 ×2）, p（2×2）, and ...Periodic density functional theory（DFT） calculations are presented to describe the adsorption and decomposition of CH3OH on Ru（0001） surfaces with different coverages, including p（3 ×2）, p（2×2）, and p（2× 1） unit cells, corresponding to monolayer（ML） coverages of 1/6, 1/4, and 1/2, respectively. The geometries and energies of all species involved in methanol dissociation were analyzed, and the initial decomposition reactions of methanol and the subsequent dehydrogenations reactions of CH3O and CH2OH were all computed at 1/2, 1/4, and 1/6 ML coverage on the Ru（0001） surface. The results show that coverage exerts some effects on the stable adsorption of CH30, CH2OH, and CH3, that is, the lower the coverage, the stronger the adsorption. Coverage also exerts effects on the initial decomposition of methanol. C-H bond breakage is favored at 1/2 ML, whereas C-H and O--H bond cleavages are preferred at 1/4 and 1/6 ML on the Ru（0001） surface, respectively. At 1/4 ML coverage on the Ru（0001） surface, the overall reaction mechanism can be written as 9CH3OH ,3CH30＋6CH2OH＋9H ,6CH20＋3CHOH＋18H , 7CHO＋COH＋CH＋OH＋26H → 8CO＋C＋O＋36H.展开更多
The Casimir effect for two parallel slabs immersed in an ideal Fermi sea is investigated at both zero and nonzero temperatures. It is found that the Casimir effect in a Fermi gas is distinctly different from that in a...The Casimir effect for two parallel slabs immersed in an ideal Fermi sea is investigated at both zero and nonzero temperatures. It is found that the Casimir effect in a Fermi gas is distinctly different from that in an electromagnetic field or a massive Bose gas. In contrast to the familiar result that the Casimir force decreases monotonically with the increase of the separation L between two slabs in an electromagnetic field and a massive Bose gas, the Casimir force in a Fermi gas oscillates as a function of L. The Casimir force can be either attractive or repulsive, depending sensitively on the magnitude of L. In addition, it is found that the amplitude of the Casimir force in a Fermi gas decreases with the increase of the temperature, which also is contrary to the case in a Bose gas, since the bosonic Casimir force increases linearly with the increase of the temperature in the region T 〈 Tc, where Tc is the critical temperature of the Bose Einstein condensation.展开更多
In the past, the planetary radiation balance served to quantify the atmospheric greenhouse effect by the difference between the globally averaged near-surface temperature of and the respective effective radiation temp...In the past, the planetary radiation balance served to quantify the atmospheric greenhouse effect by the difference between the globally averaged near-surface temperature of and the respective effective radiation temperature of the Earth without atmosphere of resulting in . Since such a “thought experiment” prohibits any rigorous assessment of its results, this study considered the Moon as a testbed for the Earth in the absence of its atmosphere. Since the angular velocity of Moon’s rotation is 27.4 times slower than that of the Earth, the forcing method, the force-restore method, and a multilayer-force-restore method, used in climate modeling during the past four decades, were alternatively applied to address the influence of the angular velocity in determining the Moon’s globally averaged skin (or slab) temperature, . The multilayer-force-restore method always provides?the highest values for , followed by the force-restore method and the forcing method, but the differences are marginal. Assuming a solar albedo of , a relative emissivity , and a solar constant of and applying the multilayer-force-restore method yielded and for the Moon. Using the same values for α, ε, and S, but assuming the Earth’s angular velocity for the Moon yielded and quantifying the effect of the terrestrial atmosphere by . A sensitivity study for a solar albedo of commonly assumed for the Earth in the absence of its atmosphere yielded , , and . This means that the atmospheric effect would be more than twice as large as the aforementioned difference of 33 K. To generalize the findings, twelve synodic months (i.e., 354 Earth days) and 365 Earth days, where , a Sun-zenith-distance dependent solar albedo, and the variation of the solar radiation in dependence of the actual orbit position and the tilt angle of the corresponding rotation axis to the ecliptic were considered. The case of Moon’s true angular velocity yielded and . Whereas Earth’s 27.4 times higher angular velocity yielded , and . In both cases, the effective radi展开更多
基金Supported by the Key Program of Natural Science of Tianjin, China（No. 13JCZDJC26800）, the National Natural Science Foundation of China（Nos.21503122, 21346002）, the Shanxi Province Science Foundation for Youths, China（No.2014021016-2）, the Scientific and Technological Programs in Shanxi Province, China（No.2015031017） and the Foundation of Key Laboratory of Advanced Energy Materials Chemistry of Ministry of Education of China.
文摘Periodic density functional theory（DFT） calculations are presented to describe the adsorption and decomposition of CH3OH on Ru（0001） surfaces with different coverages, including p（3 ×2）, p（2×2）, and p（2× 1） unit cells, corresponding to monolayer（ML） coverages of 1/6, 1/4, and 1/2, respectively. The geometries and energies of all species involved in methanol dissociation were analyzed, and the initial decomposition reactions of methanol and the subsequent dehydrogenations reactions of CH3O and CH2OH were all computed at 1/2, 1/4, and 1/6 ML coverage on the Ru（0001） surface. The results show that coverage exerts some effects on the stable adsorption of CH30, CH2OH, and CH3, that is, the lower the coverage, the stronger the adsorption. Coverage also exerts effects on the initial decomposition of methanol. C-H bond breakage is favored at 1/2 ML, whereas C-H and O--H bond cleavages are preferred at 1/4 and 1/6 ML on the Ru（0001） surface, respectively. At 1/4 ML coverage on the Ru（0001） surface, the overall reaction mechanism can be written as 9CH3OH ,3CH30＋6CH2OH＋9H ,6CH20＋3CHOH＋18H , 7CHO＋COH＋CH＋OH＋26H → 8CO＋C＋O＋36H.
基金Project supported by the National Natural Science Foundation of China(Grant No.10875100)the Natural Science Foundationof Fujian Province,China(Grant No.A1010016)
文摘The Casimir effect for two parallel slabs immersed in an ideal Fermi sea is investigated at both zero and nonzero temperatures. It is found that the Casimir effect in a Fermi gas is distinctly different from that in an electromagnetic field or a massive Bose gas. In contrast to the familiar result that the Casimir force decreases monotonically with the increase of the separation L between two slabs in an electromagnetic field and a massive Bose gas, the Casimir force in a Fermi gas oscillates as a function of L. The Casimir force can be either attractive or repulsive, depending sensitively on the magnitude of L. In addition, it is found that the amplitude of the Casimir force in a Fermi gas decreases with the increase of the temperature, which also is contrary to the case in a Bose gas, since the bosonic Casimir force increases linearly with the increase of the temperature in the region T 〈 Tc, where Tc is the critical temperature of the Bose Einstein condensation.
文摘In the past, the planetary radiation balance served to quantify the atmospheric greenhouse effect by the difference between the globally averaged near-surface temperature of and the respective effective radiation temperature of the Earth without atmosphere of resulting in . Since such a “thought experiment” prohibits any rigorous assessment of its results, this study considered the Moon as a testbed for the Earth in the absence of its atmosphere. Since the angular velocity of Moon’s rotation is 27.4 times slower than that of the Earth, the forcing method, the force-restore method, and a multilayer-force-restore method, used in climate modeling during the past four decades, were alternatively applied to address the influence of the angular velocity in determining the Moon’s globally averaged skin (or slab) temperature, . The multilayer-force-restore method always provides?the highest values for , followed by the force-restore method and the forcing method, but the differences are marginal. Assuming a solar albedo of , a relative emissivity , and a solar constant of and applying the multilayer-force-restore method yielded and for the Moon. Using the same values for α, ε, and S, but assuming the Earth’s angular velocity for the Moon yielded and quantifying the effect of the terrestrial atmosphere by . A sensitivity study for a solar albedo of commonly assumed for the Earth in the absence of its atmosphere yielded , , and . This means that the atmospheric effect would be more than twice as large as the aforementioned difference of 33 K. To generalize the findings, twelve synodic months (i.e., 354 Earth days) and 365 Earth days, where , a Sun-zenith-distance dependent solar albedo, and the variation of the solar radiation in dependence of the actual orbit position and the tilt angle of the corresponding rotation axis to the ecliptic were considered. The case of Moon’s true angular velocity yielded and . Whereas Earth’s 27.4 times higher angular velocity yielded , and . In both cases, the effective radi
