Gong Yubing, Hou Zhonghuai, Xin Houwen
Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, People's Republic of China.
J Phys Chem A. 2005 Mar 31;109(12):2741-5. doi: 10.1021/jp044664x.
We have studied the roles of internal noise in the oscillatory reaction kinetics during NO reduction by CO on low-index single crystal platinum surfaces using the chemical Langevin equation and the Poisson approximation algorithm. Considering that the surface is divided into small well-mixed cells, we have focused on the dynamical behavior inside a single cell. It is found that internal noise can induce rate oscillations and the performance of the stochastic rate oscillations undergoes a maximum with the variation of internal noise level for a given NO partial pressure, demonstrating the occurrence of internal noise stochastic resonance. Such a phenomenon is robust to the change of external parameters, such as NO pressures. Interestingly, it is also found that internal noise noticeably alters the oscillatory waveform and, hence, the reaction activity and oscillation signal intensity, but it nearly does not change the global reaction rate.
我们使用化学朗之万方程和泊松近似算法,研究了在低指数单晶铂表面上,一氧化碳还原一氧化氮的振荡反应动力学过程中内部噪声的作用。考虑到表面被划分为小的充分混合的单元,我们专注于单个单元内部的动力学行为。研究发现,对于给定的一氧化氮分压,内部噪声可引发速率振荡,且随机速率振荡的性能会随着内部噪声水平的变化而达到最大值,这表明发生了内部噪声随机共振。这种现象对外界参数(如一氧化氮压力)的变化具有鲁棒性。有趣的是,还发现内部噪声显著改变了振荡波形,进而改变了反应活性和振荡信号强度,但几乎不改变整体反应速率。