煤基高活性脱硝多孔炭的制备、结构修饰及相关体系技术集成

This project provides a new approach to simultaneously use spherical activated carbon and honeycomb-like activated carbon (abbreviate AC) as catalyst supporter, which possess high surface area (1500m2/g), high strength and suitable for high space velocity operation. Based on the illuminating the active nature of AC (including adsorption potential energy, amount of defect carbon atom, active degree, etc.) and its respective contributions for de-NOx, we will further directionality modify the AC to increase its particularly activity for wide application, including de-NOx. Furthermore, the project focuses on summarizing the common principle that how to increase the activity of AC.. Also, Mn/Ce catalysis will be loaded on the functionalized AC to improve the de-NOx performance and reveal the mechanism through coupling effect between Mn/Ce and AC for high de-NOx efficiency obtained. On the basis of molecular gene characters of the materials mentioned above, the project will center upon designing and preparing AC/MnCe and AC/MnCe/melamine catalysis with even high activity, respectively, indicating their synergistic role for de-NOx. Moreover, the project aims at designing modular reactor using industrial tail gas based on the actual test results to realize the best matching between catalysis materials and reactor for constructing a new low NH3-non NH3 system for deep de-NOx.

课题拟采用具有自催化功效、高比表面积（1500m2/g）且适合高空速的煤基球状活性炭和蜂窝状活性炭为基体（AC），在阐明其表观活性本质（活性度、吸附势、缺陷位数量等）及其对脱硝活性贡献度基础上，进一步后期定向修饰，阐释出包括但不限于AC脱硝体系的AC活性度和活性位数量提升的普适性原则和技术手段。. 在此基础上，负载锰铈催化剂，在阐释锰铈彼此之间活性相互促进的机制下，继而揭示出其与AC界面耦合增强活性的关联性。力图从所采用材料的特质分子基因的角度出发，制备出高活性的AC/锰铈和AC/锰铈/三聚氰胺多组元催化材料体系，并分析确立多组元共存下对活性的贡献机制与贡献权重和最佳协同原理。结合多床层模块化反应器设计与实际工业侧线验证，实现材料-反应器最佳适配性及贫氨-无氨脱硝反应新体系。. 此课题的结果，将会衍生出多个炭材料学科生长点，对我国此领域有一定的引导性作用。

NOx引起的环境问题和对人体健康的危害主要表现为：对人体的致毒作用、对植物的损害、酸雨及酸雾的主要污染物、与碳氢化合物可形成光化学烟雾、参与臭氧层的破坏，当前巨大的氮氧化物（NOx）排放量严重制约社会和经济的可持续发展。.本研目制备出高性能的煤基球状活性炭(比表面积1500m2/g)、超级活性炭(比表面积(2000-4500m2/g))和蜂窝状活性炭，采用具有高强度、自催化、高比表面积和适合高空速运行的煤基活性炭材料（球形和蜂窝形）为基体，制备出高活性的CuO/AC，锰铈/AC和锰铈/AC/三聚氰胺多组元催化材料体系。CuO/AC催化剂具有优异的脱硫性能，穿透硫容高达55.16 mg/g。所制备锰铈/AC催化剂具有优越的NOx脱除效果，脱硝活性超过96%，发现MnOx-CeO2/AC催化剂的NH3-SCR反应遵循Eley-Rideal反应机理。所制备的MnOx-CeO2/AC/三聚氰胺催化剂具有优异的低温脱硝性能，其脱硝活性大于95%，阐明了该催化剂在有没有氨气条件下的脱硝反应机理。设计了三段式贫氨-无氨低温梯度脱硝反应器并进行了实验室验证，在120-180oC操作温度下，可以达到在排放尾气中NO浓度<20ppm、无氨逃逸现象、无催化剂中毒。CuO/AC催化剂作为第1段反应器，负责脱除少量的SO2，解决催化剂的硫中毒问题；MnOx-CeO2/AC催化剂作为第2段反应器，采用贫氨方式将高浓度 (500-1000ppm) NOx转化成低浓度 (<100ppm) NOx；MnOx-CeO2/AC/三聚氰胺催化剂作为第3段反应器，采用无氨方式脱除低浓度NOx，达到协同耦合的脱硝效果。.本项目所研制的高性能煤基活性炭、衍生的高性能脱硝催化剂以及所设计的贫氨-无氨低温梯度脱硝反应床层模块对于煤基材料的高附加值利用和发展深度脱硝体系有重要的理论意义和应用价值。