Ni-M(M=Cu, Ag, Au)双金属催化剂催化甲烷水蒸气重整制氢的理论研究

项目名称： Ni-M(M=Cu, Ag, Au)双金属催化剂催化甲烷水蒸气重整制氢的理论研究

项目编号： No.21203001

项目类型： 青年科学基金项目

立项/批准年度： 2013

项目学科： 物理化学

项目作者： 黄玉成

作者单位： 安徽师范大学

项目金额： 22万元

中文摘要： 能源和环境是当今的两大主题。氢能作为一种可再生能源越来越受到重视，而甲烷水蒸气重整(SRM)是各产氢途径中最为经济、应用最广泛的反应，其活性催化剂可分为非贵金属系及贵金属系。其中，镍系催化剂价格低廉、活性高，已被广泛用于工业生产。然而该体系易积碳，导致催化剂失活。添加M（M=Cu、Ag或Au）形成Ni-M合金是调变和改善镍系催化剂性能的有效途径，对其机理的研究则有助于揭示催化现象的本质。项目拟采用基于第一性原理的理论计算和模拟，先以CHx、H2O等物种的吸附、石墨碳的形成以及CH4活化反应的机理研究，探讨Ni-M合金催化SRM反应的活性相。选择其中一种合金（如Ni-Au），建立合理的底物模型，研究SMR过程在其表面的完整反应机理。基于第一性原理的动力学参数，进行蒙特卡罗模拟，得出重整反应的微观动力学特征，最终揭示Ni-M合金催化SRM的本质。

中文关键词： 第一性原理；甲烷水蒸气重整；石墨烯；密度泛函理论；催化机理

英文摘要： Nowadays energy and environment are the two main themes. As a renewable energy resource, hydrogen energy attracts more and more attention. Among each pathway for hydrogen production, steam reforming of methane (SRM) is the most economical and widely used reaction. The active catalyst for SRM can be divided into non-precious metals and precious metals. Nickel-based catalysts, due to inexpensive price and high activity, are widely used for industrial production. However, coke deposition is easy to form on this system, leading to catalyst deactivation. The effective means to tune and improve catalytic performance of Ni-based catalysts is to add another metal (Cu, Ag or Au) by forming Ni-M alloy. Investigation of the reaction mechanism of SRM on Ni-M surface can help us to reveal the essence of the catalytic phenomena. Using theoretical calculations based on first-principles and simulations, the project intends to firstly explore the active phase of the Ni-M alloy by investigating the adsorption features of CHx and H2O, the formation of graphitic carbon as well as the mechanism of methane activation. Select one of the alloys (e.g., Ni-Au) to establish the rational substrate model, the whole reaction mechanism of SRM would be suggested. Based on the kinetic parameters from the calculation results of the first princip

英文关键词： first-principles；methane steam reforming；graphene；density functional theory；catalyzing mechanism