基于分子氧还原活化的甲烷低温直接催化转化

项目名称： 基于分子氧还原活化的甲烷低温直接催化转化

项目编号： No.91545108

项目类型： 重大研究计划

立项/批准年度： 2016

项目学科： 数理科学和化学

项目作者： 曹勇

作者单位： 复旦大学

项目金额： 77万元

中文摘要： 以甲烷为主要成分的碳资源储量极其丰富，被认为是“后石油时代”的重要替代资源。本项目旨在寻求和发展甲烷直接转化新途径和新策略。拟以探索和开发甲烷直接制甲醇新工艺为目标，筛选和创制高性能催化体系；针对甲烷直接转化制甲醇及甲酸甲酯等高值化学品，探究本研究团队近年发展的具有“金属”及“表面酸/碱”等多活性位集成的复合催化材料的活性和选择性变化规律；建立以分子氧还原活化的甲烷直接制高值化学品的催化体系，研究其中的催化物理化学特点。系统认识催化剂表面多活性中心微/纳尺度上的协同/集成与甲烷直接制甲醇活性、选择性和稳定性的关系，催化体系中金属分散状态和金属-载体相互作用与甲烷活化或选择氧化反应的活性、选择性和稳定性的关系。明确相关催化反应体系的催化活性和选择转化作用的机理，拓展催化剂设计理念，发现和创制甲烷增值利用的高效催化体系，为发展相应催化新技术提供理论指导和科学基础。

中文关键词： 甲烷；直接转化；分子氧还原活化；反应耦合；协同催化

英文摘要： Given its tremendous abundance and availability, hydrocarbon gas mixture consisting primarily of methane has been considered a future alternative source for chemicals and materials in the post-oil era. The purpose of this project is to develop new catalytic routes for methane valorization. The objectives of this research were: 1) explore and develop new innovative processes that can deliver direct and selective catalytic conversion of methane to produce methanol; 2) demonstrate the feasibility to directly produce value-added methyl formate and its derivatives from simple feedstocks comprising methane and HCOOH. Special efforts will be dedicated to three aspects: investigate the catalytic behavior of the nanocomposite catalysts comprising both “metal” and “acid/base” surface species recently developed by our group for the selective reductive transformation of nitrobenzene using methane as the convenient and energy-efficient hydrogen source, establish several catalytic systems capable of producing value-added chemicals directly using methane as feedstock based on the concept of reductive activation of molecular O2, and conduct reaction/kinetic studies for understanding the essential physico-chemical aspects of the relevant processes. Efforts will also be directed to gain insight into the influence of metal dispersion, metal-support interactions, surface acidity/basicity and redox properties on the activity, selectivity and stability of the catalysts, understanding the mechanistic pathways involved in the relevant processes, exploiting the concepts of catalyst designing, seeking and fabricating new efficient catalytic system for methane valorization, thus providing the essential knowledge and skill required to develop a technically and economically feasible process.

英文关键词： methane;direct transformation;O2 molecule reductive-activation;reaction coupling;cooperative catalysis