基于相反脱汞特性对比的单质汞催化剂二氧化硫中毒机理及其改性研究

项目名称： 基于相反脱汞特性对比的单质汞催化剂二氧化硫中毒机理及其改性研究

项目编号： No.51306046

项目类型： 青年科学基金项目

立项/批准年度： 2014

项目学科： 能源与动力工程

项目作者： 张安超

作者单位： 河南理工大学

项目金额： 25万元

中文摘要： 燃煤烟气中汞对环境的危害日趋严重，必须得到有效控制。利用催化剂和O2将单质Hg转化为氧化态Hg后热解、收集、资源化的技术具有广泛的应用前景，但催化剂需克服SO2的毒化。目前，催化剂SO2中毒的机理尚不明确。本项目拟采用Ce/TiO2和Mn/TiO2两种典型单质汞催化剂，围绕SO2促进Ce/TiO2对单质Hg的氧化而抑制Mn/TiO2对单质Hg的氧化这一相反脱汞特性开展催化剂SO2中毒机理研究。通过DRIFTS、XAFS和XPS等必要手段研究SO2在催化剂表面的反应历程；探寻SO2对两种催化剂促进/抑制作用的各种影响因素和内在关联；明确催化剂表面沉积物的具体成分、主要元素的迁徙规律和配位环境；探明SO2在反应中的促进/抑制机理。通过过渡金属或稀土元素掺杂改性催化剂，改善表面基团和活性中心分布以提高其抗硫能力，为深层次阐明催化剂SO2中毒机制和设计抗硫催化剂提供重要理论基础和科学依据。

中文关键词： 单质汞脱除；SO2中毒机理；钌改性催化剂；硫酸盐化；协同作用

英文摘要： The harm to the environment caused by mercury from coal-fired flue gas is becoming more serious. Thus, the emission of mercury must be effectively controled. The technology for elemental mercury catalytic oxidation by using the catalyst and O2 to oxidized mercury which can be desorbed with pyrolysis and collected for reutilization has broad application prospects. However, the SO2 poisoning of the catalyst should be overcome. While at present, the mechanism of the catalyst deactivation caused by SO2 is not clear. In this project, focusing on the opposite Hg removal performance of how can SO2 promote the catalytic oxidation of Hg0 over Ce/TiO2 and inhibit over Mn/TiO2 catalyst, the SO2 poisoning mechanism analysis are carried out. The physicochemical properties of the catalysts are characterized by in situ DRIFTS, XAFS, XPS and other necessary characterization techniques. The reaction path of SO2 over the two catalysts are studied. The various influence factors and inherent correlation of promotion and inhibition caused by SO2 are also explored. Furthermore, to prove the mechanism of promotion and inhibition over the two catalysts in the process of Hg0 capture, the composition of sediment on the catalyst surface, the evolution and coordination environment of the main elements are investigated. Moreover, to impove

英文关键词： Elemental mercury removal；SO2 poisoning mechanism；Ruthenium modified catalysts；Sulfation；Synergistic effect