摘要
使用飞行时间反应器研究了环氧丙烷-石英催化体系,并且用实验直接证明该催化反应不是在表面上,而是在空间内完成的。实验的一次相遇反应概率随着飞行距离的缩短和反应压力的增大而逐渐减小,但是不因起始能量分布的改变而改变。用气固传能过程新处理法所进行的成功模拟再一次支持了所提新观点的适用性。
The catalytic system of propylene oxide-silica was studied in a time-of-flight reactor. By changing the flight distance of activated molecules it was directly proved for the first time that the catalytic reaction did not occur on the surface, but in the space of the reactor.The one encounter reaction probability decreased with shortening of the flight distance and enlarging of the reaction pressure, but did not change due to the difference of initial energy distributions. The existence of the desorption well greatly influenced the shape of the energy distribution of desorbed molecules, though the desorption energy E_d kept constant in the region of experimental errors when the data were simulated with two sorts of energy distribution modes (F_d and F_M). The best fit could be attained by means of the total distribution, which was the linear composition of F_d and F_m with the ratio of surface adsorption θ as composition coefficients. According to the new idea, the vibrational energy accommodation coefficients were much larger than 1 if they were still calculated on the basis of the Boltzmann distribution. The significant success of the theortical simulation supported the new point of view on gas-solid energy transfer magnificently.
基金
国家自然科学基金
关键词
飞行时间
反应器
气固分子传能
reactor, propylene oxide, energy transfer, catalysis, flight-time reactor, energy transfer efficiency.
