改性MnOx-CeO2/γ-A12O3复合催化剂低温催化还原脱硝、催化氧化脱汞机理研究

Transition Metal and Precious Metal Compounds Zr，Fe and Ag modified MnOx-CeO2/γ-A12O3 catalysts are carried out to remove mercury and NO of flue gas at low temperatures (100℃-200℃). This will renew the traditional SCR denitration technology at moderate temperature(300℃-420℃), and provide a new route for removal of mercury and NO of flue gas at low temperatures. Accounting for the lack of the basic research related to low temperature sorbents, sol-gel method is proposed to prepare the efficient, renewable catalyst sorbents with good abrasion resistance. The effects of additives loading values, preparation method on the efficiency of NOx/Hg removal by the sorbents are investigated. The DRIFTS method and microscopic analytical instruments are used to characterize the surface of catalyst. The surface adsorption/desorption kinetics models will be set up to reveal the mechanism of NOx reduction and Hg adsorption/oxidation by the catalysts at low temperature. Meanwhile, the regenerative process and mechanism for the catalysts are investigated in order to design the optimal treament method. The accomplishment of the project will put forward the new mechanism of NO catalytic reduction and Hg catalytic oxidation at low temperature and provide the foundation for the theory of multiple heterogeneous gas-solid catalytic reaction.

提出过渡金属或贵金属氧化物（Zr，Fe和Ag等）掺杂改性的MnOx-CeO2/γ-A12O3复合催化剂，实现对100℃-200℃低温燃煤烟气同时脱硝脱汞，这是对传统300℃-420℃中温SCR脱硝的更新，为低温联合脱硝脱汞提出一条新路径。采用溶胶-凝胶法制备高效可再生多元复合催化剂，其具备类纳米材料的良好孔隙结构、优良的活性组分分散度，从根本上解决催化剂的机械强度、活性和热稳定性等问题；研究并揭示不同催化剂组分、不同制备工艺、不同反应条件下的低温脱硝脱汞性能；研究复合催化剂再生方法与再生机理；采用原位红外在线分析和微观分析仪器，表征反应进程中催化剂表面物理化学特性，建立联合脱除过程中多相复杂反应流扩散-物理化学吸附-催化氧化或还原-解吸附过程反应动力学模型，揭示低温烟气条件下“NO催化还原”和“汞催化氧化” 关键反应进程的化学反应路径、相互作用和竞争机制，丰富多元非均相气固催化反应理论。

提出过渡金属或贵金属氧化物（Zr，Fe和Ag等）掺杂改性的MnOx-CeO2/γ-A12O3和MnSmCo/Ti复合催化剂，实现对100℃-200℃低温燃煤烟气同时脱硝脱汞，这是对传统300℃-420℃中温SCR脱硝的更新，为低温联合脱硝脱汞提出一条新路径。采用溶胶-凝胶法制备高效可再生多元复合催化剂，解决催化剂的机械强度、活性和热稳定性等问题；研究并揭示不同催化剂组分、不同制备工艺、不同反应条件下的低温脱硝脱汞性能；研究并揭示H2O/CO2/SO2/SO3等组分对催化剂性能的影响；研究复合催化剂中毒、再生机理与再生方法；采用微观分析仪器，表征反应进程中催化剂表面物理化学特性，建立联合脱除过程中多相复杂反应流扩散-物理化学吸附-催化氧化/还原-解吸附过程反应动力学模型；借助量子化学计算，揭示了低温烟气条件下“NO催化还原”和“汞催化氧化”关键反应进程的化学反应路径、相互作用和竞争机制，丰富多元非均相气固催化反应理论。