面向气相污染物一体化治理的催化膜制备与应用基础

Based on the multi-pollutant control of coal-fired flue gas, the catalytic membrane materials and the multifunctional membrane reactors will be studied.The theories of design, preparation and application of catalytic membranes will be restablished. These researches will consolidate the fundamental theories ofinorganic membrane in china, push the commercial applications of the high-temperature gas cleaning and gas-solid reaction, and provide fundamental knowledge for catalytic materials and new separation materials as well as processes. This study will involve the following tasks: (1) the preparation of multifunctional membrane materials based on the cooperative mechanisms between mass transmission and reaction: Through the research on the mass transmission performance of gas in the pores, gradient porous membrane materials with high porosity will be designed, and the membrane formation mechanism and the construction methods of high porosity in the membrane preparation process will be studied. With the introduction of high-performance catalysts, multifunctional membrane materials with both catalytic and separation properties will be prepared. (2) The high-temperature stability of membrane materials in the high-temperature.atmospheres: Research on the evolution rules of membrane materials at high-temperature corrosive environment, and reveal the failure mechanism of membrane materials. The bending strength of the membrane will be improved by adding inorganic nanofibers. A relationship on flexural strength and microstructure of ceramic membrane will be established. (3) Design and application of membrane reactors combined reaction and separation: The membrane reactors combined particle separation and hazardous gas removal will be studied using the.high-temperature exhaust gas as application objects.The mechanism of deactivation of catalysts and the fouling membranes will be studied, which could provide a base for running the membrane reactors stably.

本项目以燃煤烟气净化为应用对象，开发用于气相污染物的一体化治理的催化膜及多功能膜反应器，建立催化膜材料的设计、制备和应用的理论与方法，推动膜技术在煤炭高效清洁利用中的工业应用，为催化材料、新型分离材料及过程的研究提供基础。主要研究内容：（1）基于传递与反应协同机制的多功能膜材料制备：通过气体在微孔中传递性能的研究，设计具有高孔隙率的梯度孔膜材料，将高性能催化剂引入到膜孔道中，制备出具备催化-分离一体化的膜材料；（2）高温气相环境下多功能膜材料的稳定性：研究催化膜材料在高温腐蚀环境下的性能演变行为，揭示膜材料长久失效机理，提出采用无机纳米纤维提高强度的方法，建立膜微结构与抗折强度关系；（3）反应分离一体化的膜反应器设计与应用：以燃煤高温尾气净化为应用对象，设计同时脱除超细粉尘与气相污染物的膜反应器，发展污染膜与催化剂再生方法，为膜反应器的稳定运行奠定基础。

基于高温烟气高效净化的应用需求，以用于气相污染物一体化治理的催化膜及多功能膜反应器为研究对象，开展了基于传递与反应协同机制的多功能膜材料制备、复杂气相环境下多功能膜材料的稳定性、反应分离一体化的膜反应器设计与应用等三方面研究，建立了碳化硅支撑体、成膜理论与膜形成过程中高孔隙率的构建方法，设计并制备了高孔隙率的梯度孔碳化硅多孔支撑体，结合纳米修饰技术构建二次载体并嵌入高性能催化剂，制备了催化-分离一体化的催化膜材料；研究了复杂燃煤烟气环境下催化膜材料微观结构动态演变规律，揭示了膜材料长久失效机理，给出了碳化硅膜及碳化硅催化膜适宜的应用环境；以高温尾气净化为应用对象，设计同时脱除超细粉尘与气相污染物的膜反应器，采用CFD模拟分析了膜反应器内反应与分离过程的流场，优化了反应器结构，为膜反应器的稳定运行奠定基础。项目制备出两种高强度高孔隙率的碳化硅陶瓷膜及四种催化膜，展现出高渗透性和NOx、VOCs催化活性，并进行了放大制备；建成了1000m3/h高温陶瓷膜除尘脱硝一体化装置现场侧线实验装置，第三方检测机构的检测结果表明，该多功能膜反应器的烟气进口粉尘浓度为32 g/Nm3时，出口浓度为3.8mg/Nm3，NOx进口浓度为367 mg/Nm3，NOx出口浓度为6 mg/Nm3，实现了燃煤烟气中氮氧化物与粉尘的超低排放。研究成果进一步夯实我国无机膜的基础理论，推进了陶瓷膜材料在高温气体净化与气固相反应过程中的工业应用，也为催化材料、新型分离材料及过程的研究提供基础，可促进我国大气污染治理水平的提升。发表学术期刊论文32篇，申请专利23件，获教育部高等学校科学研究优秀成果奖（技术发明）二等奖中国石油和化学工业联合会赵永镐科技创新奖、江苏省创新争先奖和江苏省专利发明人奖；指导博士后1名，博士生6名，硕士生25名。