基于氮氧化物高效催化脱除的分子筛拓扑结构调控研究

本课题针对固定源氮氧化物的高效脱除而展开，探索新型分子筛体系（超微孔分子筛、介孔分子筛等）的特色合成，探寻分子筛孔道尺寸（超微孔分子筛：SSZ-13、SAPO-34、NU-3、UZM-12；中微孔分子筛：SUZ-4、ZSM-5；大微孔分子筛：Y、Beta；介孔分子筛：SBA-15、SBA-16、KIT-6）和酸性（酸浓度、酸强度）调控的有效策略，尝试离子交换、浸渍、化学气相沉积、骨架同晶取代等引入活性组分，制备一系列分子筛型催化剂用于氮氧化物选择性催化还原（SCR）。并通过红外、程序升温等谱学表征，辅以分子模拟手段，探索脱硝反应的微观机制，考察催化剂耐硫、耐水能力和中毒、再生机理，揭示分子筛拓扑结构-酸性-活性组分-废气净化效能间的内在必然，作为改良设计的指导原则，以获得综合性能优异（低温活性理想、活性温度窗口宽、具有一定耐硫耐水能力）的分子筛型脱硝催化剂，为其产业化推广奠定理论基础。

The applied proposal focuses on catalytic removal of nitrogen oxides coming from the stationary resource. A series of zeolite-typed catalysts for selectively catalytic reduction (SCR) of NOx would be achieved based on the synthesis of novel zeolites including supersmall microporous and mesoporous zeolites, the control of their pore sizes (small micropore: SSZ-13, SAPO-34, NU-3, UZM-12; medium micropore: SUZ-4, ZSM-5; large mircorpore: Y, Beta; mesopore: SBA-15, SBA-16, KIT-6) and acidic properties (acidic number and strength), and the introduction of active components by ion-exchange, impregnation, chemical vapor deposition, and isomorphic substitution. SCR mechanism is going to be investigated by means of infrared and temperature programmed techniques as well as molecular simulation based on DFT theory. The resistance towards SO2 and steam as well as the behaviors of poisoning and the corresponding recovery are also studied. The correlation among zeolite topology, acidity, active component, and SCR performance will be clarified. The zeolite-typed SCR catalysts with satisfactory performances (ideal low-temperature activity, wide temperature window with excellent SCR performance, good resistance to SO2 and steam) are highly expected. These planned researches can offer the theoretical supporting for the practical applications of the related zeolite-typed catalysts.