强抗碱金属中毒的氨选择性还原氮氧化物催化剂

This project is to study strong alkali-resistant and environment-friendly deNOx catalysts for selective catalytic reduction of NOx with NH3, and the objective is to synthesize a novel CeO2/TiO2@HMO (CTM)catalyst with separated catalytically active sites and alkali-trapping sites (HMO is Hollandite MnO2). The main work is as follows: 1. to synthesize the deNOx catalyst containing the active phase CeO2 and the hollandite MnO2 for alkali trapping, and CeO2 and MnO2 are separated with TiO2 by covering TiO2 layers on the surface of the MnO2; 2. to identify the locations of the catalytically active sites and alkali-trapping sites of the CTH catalyst; 3. to establish the relationship between the structure of alkali-trapping sites and the alkali-resistant property; 4. to investigate the alkali-resistant mechanism that the CTH catalyst trapps the alkali ions during the reactions. There are four expected results: i.the strong alkali-resistant and environment-friendly deNOx catalyst will be successfully developed,ii.the catalytically active sites and alkali-trapping sites of the CTH deNOx catalysts will be proven to be separated with each other,and the synergistic effect of two separate sites will be obtained，iii.the structure-property of the alkali-trapping sites of the CTH catalyst will be correlated, iv.the general alkaili-resistanct mechanism of the deNOx catalysts will be achieved according to these results of the project. It is of scientific and fundamental importance of the project to develop efficient deNOx catalysts specially suitable for controlling NOx emission from the stack gases of the plant (co-)fuelled by the biomass, and the results of this project will be technologically served as a solid base for thoroughly controlling the emission of the atmospheric fine particulate matters such as PM2.5.

本项目为强抗碱金属中毒的氨选择性还原氮氧化物催化剂的研究，拟开发一种催化活性位和碱金属捕获位分别独立的CeO2/TiO2@HMO（CTH）高效脱硝催化剂（HMO为Hollandite型MnO2）。研究内容：1.研发以催化活性的CeO2为外层、捕获碱金属的HMO为内层和TiO2为夹层的脱硝催化剂；2.证明CTH具有独立的催化活性位和碱金属捕获位；3.建立CTH碱金属捕获位的结构与抗中毒性能之间的构效关系；4.探索CTH的抗碱金属中毒机理。预期的重要成果：i.研制出强抗碱金属中毒的高效脱硝催化剂；ii.证明催化活性位和碱金属捕获位的独立存在性和相互协作原理；iii.构建CTH碱金属捕获位的构效关系；iv.建立脱硝催化剂普适性的抗碱金属中毒机理。本项目对研制以生物质(或与燃煤混合)为燃料的锅炉烟气脱硝催化剂具有重要的科学理论意义，对控制大气细颗粒污染物(如PM2.5)的排放具有重要的应用价值。

本项目为有关强抗碱金属催化剂脱硝催化剂的研究，探究hexagonal型三氧化钨（HWO）系列负载型催化剂抗碱金属的性能及其机理的研究。主要内容包括：(i) 研发强抗碱金属的高效的V2O5/HWO脱硝催化剂；(ii) 证明催化活性位和碱金属捕获位的独立存在性和相互协作原理；(iii) 构建催化剂碱金属捕获位的构效关系；(iv) 建立脱硝催化剂普适性的抗碱金属中毒机理。本项目获得了一些重要的研究成果：（1）制备合成了一种强抗碱金属中毒性能的V2O5/HWO新型脱硝催化剂；（2）证明了实际烟气条件下K+可以自发从催化剂表面扩散至HWO六方孔道中；（3）发现HWO六方孔道结构容纳K+并发生电子轨道杂化从而稳定K+是其抗碱金属的本质原因，且该结论具有普适性。本项目取得的研究成果发表了24篇SCI论文：五篇化学国际主流的杂志，即三篇Chem. Commun. (IF = 6.290)；和两篇Chem. Eur. J. (IF = 5.160)；九篇环境类国际顶尖杂志Environ. Sci. Technol. (IF = 6.653)；一篇Environ. Sci. Technol. Lett. (IF = 5.869)；一篇Catal. Sci. Technol. (IF = 5.365)；三篇ChemCatChem (IF = 4.674)；一篇Catal. Commun. (IF = 3.463)；一篇Chinese J. Catal. (IF = 3.525)；两篇Ind. Eng. Chem. Res. (IF = 3.141)；一篇Catal. Lett. (IF = 2.911)。总的IF =130.504，平均每篇文章的IF=5.4. 这样，88万元/24篇 = 3.67万元/篇，即每投资3.67万元可以获得科研成果为IF = 5.4的SCI论文一篇。