催化过程多尺度动态模拟方法的研究

项目名称： 催化过程多尺度动态模拟方法的研究

项目编号： No.91545118

项目类型： 重大研究计划

立项/批准年度： 2016

项目学科： 数理科学和化学

项目作者： 陈兆旭

作者单位： 南京大学

项目金额： 80万元

中文摘要： 由于温度、压力和反应气氛的影响，反应条件下固体催化剂表面结构和组成往往与非工作状态下的差别很大，甚至有些催化剂的活性相必须在反应条件下才能存在。此外，催化是非平衡过程，活性相结构不一定是热力学上稳定的结构。故研究催化剂随环境变化的动力学、从反应条件下催化剂组成和结构出发是正确认识催化过程的前提。本项目拟以催化甲醇水蒸气重整催化剂Pd/ZnO在不同气氛和温度压力下的变化为研究对象，将动力学Monte Carlo和反应性力场分子动力学相结合，理论模拟和原位表征(XPS、IR和Raman等)结果相参比，探索催化过程动态模拟的方法，编写多尺度模拟程序ReaxFF-MD/KMC，考察催化剂演变行为。该项目将深化固体表界面与环境气氛相互作用的认识、丰富柔性催化剂概念、架设从超真空和模型催化剂所得结果到实际条件下结果的桥梁，为今后研究提供合理的催化剂模型,也将为阐明甲醇水蒸气重整制氢机理提供重要信息。

中文关键词： 多尺度模拟；原位表征；动力学蒙特卡罗；分子动力学；甲醇水蒸气重整

英文摘要： The composition and structure of a catalyst under reactive environment differs significantly from that in UHV or under non-reaction condition, due to the effect of temperature, pressure and gas atmosphere. In some cases, catalytically active phases can only exist under reaction condition. Moreover, catalysis is a non-equilibrium process and active phases may not be the thermodynamically stable structures. In order to correctly understand catalytic processes, one should study the dynamics in catalysts and start from the information gathered for the catalyst under reaction. This proposal aims at combining kinetic Monte Carlo with reactive force field molecular dynamics and building a spatial and temporal multi-scale program called ReaxFF-MD/KMC to explore the changes of Pd/ZnO used to catalyze methanol steam reforming under different reactive environments. The simulated results will be compared with experimental results obtained by in-situ characterization techniques XPS, IR and Raman spectroscopy. This proposal will definitely help understand the interaction between the gas atmosphere and a solid catalyst, enrich the flexible concept of catalysts, bridge the material gap and pressure gap and provide information to build reasonable catalyst models for further studies. It surely will also help unravel methanol steam reforming mechanism.

英文关键词： Multi-scale simulation;In-situ characterization;Kinetic Monte Carlo;Molecular Dynamics;Methanol steam reforming