金-钛等典型异核氧化物团簇催化氧化CO研究

项目名称： 金-钛等典型异核氧化物团簇催化氧化CO研究

项目编号： No.21303215

项目类型： 青年科学基金项目

立项/批准年度： 2014

项目学科： 数理科学和化学

项目作者： 李晓娜

作者单位： 中国科学院化学研究所

项目金额： 25万元

中文摘要： 担载金催化剂在一氧化碳（CO）催化氧化方面具有优异的低温催化活性。目前科学家对含金催化剂催化氧化CO的反应机理意见不一。团簇反应可以作为研究含金催化剂与CO反应的一条重要途径，它可以从分子水平上研究其反应过程，为了解体相催化剂的反应机理提供重要理论依据。二氧化钛（TiO2）担载的金颗粒是典型的低温催化氧化CO的催化剂，而分子水平上研究金-钛异核氧化物团簇与CO的反应却鲜有实验报道。本项目申请人提出研究金-钛等典型异核氧化物团簇与CO的反应，有望从分子水平了解担载金催化剂高活性的起因。本项目拟使用激光溅射、快速流动反应、四级杆选质反应、碰撞诱导解离反应以及高分辨率反射式飞行时间质谱测量含金异核氧化物团簇与CO的反应通道和速率，并结合理论模拟计算团簇的结构、成键以及与CO和O2分子反应的动力学数据，进而得到含金催化剂催化氧化CO以及活化O2分子过程中的活性位点和反应机理等相关信息。

中文关键词： 一氧化碳；贵金属；团簇；质谱；理论计算

英文摘要： Highly dispersed gold exhibits extraordinary catalytic activity in low-temperature oxidation of carbon monoxide(CO).However, contradictory hypotheses have been advanced on the nature of reaction mechanism in CO catalytic oxidation.Cluster reaction is an important way to study the reaction mechanism between supported gold and CO, which can uncover the elementary reactions at molecular level and provide theoretical support to further understand the reaction mechanism in condensed phase systems. TiO2 supported Au catalyst is an typical example, which has extraordinary catalytic activity in low-temperature oxidation of CO. However, the experimental studies between gold-titanium doped oxide clusters and CO at molecular level are rarely reported. This project is going to investigate the reaction between gold-titanium doped oxide clusters and CO, which is very important to understand the reaction mechanism of supported-gold under molecular level. Laser ablation, fast flow reaction, collision-induced dissociation reaction, quadrupole mass-selected setup, and high-resolution reflectron time-of-flight mass spectrometry will be used to obtain the reaction channels and rate constants for reactions between typical heteronuclear oxide clusters including gold doped titanium oxide clusters and CO. Based on the experimental data

英文关键词： CO；noble-metal；cluster；mass spectrometry；theoretical calculations