负载型钴基复合金属氧化物超薄多孔纳米片阵列催化柴油车碳烟消除研究

Diesel engine can increase the efficiency of energy conversion, and reduce the emission of greenhouse gas CO2. However, the diesel exhaust contains a large amounts of soot particles. The diesel soot may induce the formation of smog, which has great damage to the atmospheric environment and human health. Within the last decade, the combination of soot trap filter and combustion catalysts appeared to be the most promising technology for diesel emission after-treatment. The key is to develop practical and efficient diesel soot combustion catalysts. This project will adopt several kinds of chemical transformation methods to synthesize supported cobalt-based mixed metal oxide ultrathin porous nanosheet array with controlled oxygen vacancies, i.e. MCo2O4-x/Co3O4-y (M=Fe, Ni), for diesel soot catalysis oxidation. The dependence of ultrathin porous structure and concentration of oxygen vacancies on experimental parameters is systematically discussed. In addition, the ultrathin porous structure and concentration of oxygen vacancies will be studied in details to understand their effect on microscopic active oxygen species and macroscopic soot combustion performance. We aim to reveal the structure-performance relationship for the catalysts, and elucidate the dynamics and reaction mechanism for soot combustion. Our research will open up a new avenue for developing practical soot elimination catalysts with low cost and high efficiency.

柴油发动机相比于汽油发动机不仅提高了能量转换效率，还有效减少温室气体CO2排放。但是，柴油车尾气中含有大量不完全燃烧产生的碳烟颗粒(soot)，是近年来导致我国“雾霾天气”的主要元凶之一。催化再生的DPF技术被认为是目前最有前途的技术，研究的重点是开发实用、高效的soot氧化催化剂。本项目拟结合多种化学转化手段合成具有可控氧缺陷浓度的负载型钴基复合金属氧化物MCo2O4-x/Co3O4-y (M=Fe, Ni) 超薄多孔纳米片阵列，用于柴油车尾气中soot颗粒催化消除。系统考察材料的超薄多孔结构、氧空位浓度等与实验参数间的依赖关系，详细研究材料的氧空位浓度和超薄二维结构等与微观活化传递氧物种及宏观soot消除性能之间的关联性，建立催化剂的构效关系，进而加深对于soot催化消除机理和动力学的理解。为开发实用、高效的soot消除催化剂提供理论基础与实验依据。

发展高效的柴油车尾气净化催化剂并实现目标材料的精准合成是无机化学与环境催化化学领域的重要挑战。本项目提出结合多种化学转化手段合成具有可控氧缺陷浓度的负载型金属氧化物超薄多孔纳米片；系统考察材料的超薄多孔结构、氧空位浓度等与实验参数间的依赖关系；详细研究材料的氧空位浓度和超薄二维结构等与微观活化传递氧物种及宏观soot消除性能之间的关联性，建立催化剂的构效关系，进而加深对于soot催化消除机理和动力学的理解。为开发实用、高效的soot消除催化剂提供理论基础与实验依据。以第一/通讯作者在Nat Chem、Natl Sci Rev、EcoMat、Angew Chem Int Ed（2篇）、ACS Catal、Acc Chem Res等发表SCI论文20余篇，3篇论文入选ESI高被引论文。申请发明专利3项，出版1个英文书章节，受邀请在国内外做多个口头报告。担任JACS、Nature Commun等国际杂志的审稿人。在本项目的资助下，项目负责人入选国家海外引进高层次青年人才（2018年）、获得天津市杰出青年基金（2020）。培养博士毕业生2人、硕士毕业生2人。