自由基修饰的黄铁矿表面催化性能的研究

项目名称： 自由基修饰的黄铁矿表面催化性能的研究

项目编号： No.21473015

项目类型： 面上项目

立项/批准年度： 2015

项目学科： 数理科学和化学

项目作者： 车丽

作者单位： 大连海事大学

项目金额： 96万元

中文摘要： 黄铁矿(FeS2)是地壳中分布最广的硫化物,其表面经氢原子轰击后会产生还原性的Fe(I)-S相,此发现激发了关于FeS2表面的催化活性的研究,因为Fe(I)-S相 与FeMo-固氮酶和FeFe-氢化酶的铁硫活化中心具有相似的结构.本项目拟采用程序升温脱附谱（超声分子束-表面散射仪）和飞行时间谱方法（通用型交叉分子束装置），在FeS2表面进行还原氮气合成氨气的催化活性的研究。首先，采用H原子或D原子将FeS2表面还原修饰，然后将高能氮气束入射到被还原修饰的FeS2表面上，在原子分子水平上理解氮气在二硫化铁表面的还原机理，并研究与这一催化过程紧密相关的N2，H2，N原子，H原子，以及H2S与FeS2表面相互作用的动力学。该还原修饰的表面的催化活性以及其机理的研究将开启异相催化研究领域（如氨气合成，CO还原）产生实用仿生催化剂的新方向。

中文关键词： 黄铁矿；表面科学；分子束；催化活性

英文摘要： Pyrite (FeS2) is the most abundant sulfide mineral in the world. The discovery of a reduced Fe(I)-S phase created by hydrogen-atom bombardment of an FeS2 surface has inspired research work on the catalytic activity of this surface, because the surface bears a structural similarity to the iron-sulfur center in FeMo-nitrogenases and FeFe-hydrogenases. In this project, we plan to study the potential catalytic activity of reduced pyrite surface for ammonia synthesis by using of Temperature Programmed Desorption(TPD) and Time of Flight technologies(TOF).At first,FeS2 is modified and and reduced by H atom or D atom. Then a beam of energetic nitrogen will be directed at hydrogenated and reduced pyrite surfaces, in the mean time, products scattered from surface will be monitored. The proposed work seeks to demonstrate unequivocally that the reduced iron-sulfur surface is an effective catalyst for nitrogen reduction and to gain insight into the details of the catalytic mechanism.The demonstration of significant catalytic activity on a reduced iron-sulfur surface, along with the initial mechanistic details to be uncovered via molecular beam scattering methods, would open a new area of research in the field of heterogeneous catalysis that could potentially lead to practical biomimetic catalysts for important reactions such as ammonia synthesis and carbon dioxide reduction.

英文关键词： pyrite;surface science;molecular beam;catalytic activity