可控表面化学性MnOx@Ny-AC催化剂构建及其低温焦化烟气脱硝增强机制

焦化烟气脱硝（NOx）是钢铁行业实现超低排放的重要任务之一。然而，焦化烟气较低的温度（180-260℃）和复杂易波动的成分使得现有SCR脱硝催化剂难以稳定高效的工作，极大限制了焦化烟气的治理。调控催化剂表面化学性是提高其催化性能和稳定性的有效途径。本课题拟制备表面化学性（吸附性、酸碱性和氧化还原性等）可控的MnOx@Ny-AC催化剂，通过氮掺杂和活性金属MnOx负载调控催化剂所形成的含氮官能团种类、缺陷形态、酸性位和暴露晶面等，并借助多种表征技术深入分析其对催化剂表面化学性的单一影响和协同作用，利用原位表征手段和理论计算从分子原子层面探究其对催化剂低温SCR脱硝性能的增强机制。构建出具有可控表面化学性的MnOx@Ny-AC催化体系的普适性制备方法，并阐释主要催化剂表面化学性调控途径对其低温脱硝性能的贡献机制。本项目的完成有望为可控表面化学性催化剂在低温脱硝领域的进一步开发和应用提供新思路。

Coking flue gas de-NOx is one of the important tasks to achieve ultra-low emissions for the iron and steel industry. The emission characteristics of coking flue gas, such as low temperature (180-260℃) and complex and changeable composition, all make de-NOx difficult greatly. It is an efficient method to adjust surface chemical properties to improve catalytic performance of the catalyst. We will prepare MnOx@Ny-AC catalyst with controllable surface chemical properties (e.g., adsorption property, surface acidity, redox property, et al.). The species of nitrogen functional group and defect, acid sites and specific exposed crystal plane of catalyst is adjusted via doping nitrogen and supporting MnOx. Its single influence and synergistic effect on surface chemical properties are investigated deeply with various characterization techniques. Its enhanced low-temperature de-NOx mechanism is explored with in situ characterization means and theoretical calculation at molecular and atomic level. Besides, the common method is proposed to prepare MnOx@Ny-AC catalyst with controllable surface chemical properties, and the contribution of regulation approaches to the de-NOx performance of catalyst at low temperature are analyzed. The completion of this project will provide new ideas for developing and applying the catalyst with controllable surface chemistry in the field of low-temperature de-NOx.