论文标题
金纳米颗粒中的CO氧化中火山尺寸依赖性的电子模型
Electronic model of a volcano-shaped size dependence in CO oxidation by gold nanoparticles
论文作者
论文摘要
基于催化器的电子理论，金属簇的jellium模型和过渡金属中地层键的D波段模型，提出了CO氧化中非凡催化活性的火山型大小依赖性的理论模型。通过解离氧分子的解离性吸附，通过将电子步骤引入反应机制，该反应机制将电子步骤引入反应机制，该反应与弱化学和强度的互化状态之间的过渡相对应，从而考虑了电子氧化反应的一般机制的动力学，并通过对气相的CO分子的相互作用进行了催化的CO氧化反应的动力学。通过引入弱和强化学吸附的中间体的分数（O，CO2）对金属簇的大小相对于中间体的抗体能量水平的尺寸依赖性费米水平的指数依赖性，这是获得反应率对金纳米颗粒尺寸的火山型依赖性的火山型依赖性。通过将附加的能量项引入金属催化剂的费米水平，应考虑反应速率对支持的依赖性。
The theoretical model of a volcano-type size dependence of extraordinary catalytic activity of gold nanoparticles in CO oxidation is proposed based on the electronic theory of catalysis, the jellium model of metal clusters and the d-band model of formation bonds in transition metals. The kinetics of the general mechanism of CO oxidation reaction catalyzed by gold nanoparticles through dissociative adsorption of oxygen molecules and interaction with CO molecules from the gas-phase is considered by introducing electronic steps into 3-step mechanism of the reaction, corresponding to transitions between weak and strong chemisorbed states of intermediates. By introducing the exponential dependences of the fractions of weak and strong chemisorbed intermediates (O, CO2) on the size dependent Fermi level of the metal cluster with respect to antibonding energy levels of the intermediates, a volcano-type dependence of reaction rate on the size of gold nanoparticles is obtained. The dependence of the reaction rate upon the supports is taken into account by introducing the additional energy term into the Fermi level of the metal catalyst.
