铜基多元体系负载介孔材料上CO/CO2 共氢化合成甲醇研究

CO/CO2 co-hydrogenation to methanol has an important application in the fields of clean energy and environmental protection. However, an effective conversion of both carbons and high methanol yield are at present limited by a poor specific functionality of current catalysts. Herein, a new and efficient approach to Cu-based multi-component system supported on mesoporous materials for CO/CO2 co-hydrogenation to methanol has been proposed via component and surface/interface modification. The effects of synthesis conditions on catalysts functionality, the relationship between microstructure and catalytic performances of supported materials and the reaction mechanisms of co-hydrogenation will be studied. This work not only proposes a new idea for clean fuel preparation, but also has important theoretical significance for understanding scientific problems in catalytic system.

CO/CO2共氢化制备甲醇在洁净能源和环境保护领域有着重要的应用前景，但是现有催化材料不能同时有效的提高两种碳资源转化率及获得较高的甲醇产率。本项目通过组分及表面/界面调控，提出一种基于铜基多元体系负载介孔材料上CO/CO2共氢化合成甲醇的新方法。研究制备方法对材料功能调控的影响机制，探讨材料微结构与催化性能之间的构效关系，揭示CO/CO2共氢化合成甲醇反应机理，优化共氢化反应体系，建立CO/CO2共氢化合成甲醇技术的实验及理论基础。本项目不仅提供了一种制备清洁甲醇燃料的新思路，而且对解决复杂多相催化体系中的某些科学问题具有重要的理论意义。

CO/CO2共氢化合成甲醇是碳资源化利用和解决能源危机最经济的途径，基于铜基体系高效催化剂的深入理解和应用是这一途径实现工业化应用的关键因素。针对现有催化剂比表面积小、分散度差、活性组分易烧结和氢气解离吸附量不足等问题，项目采用浸渍-络合法获得高分散多组分铜基负载介孔催化剂，研究了载体材料表界面改性对催化剂结构和催化性能的影响，探讨了Cu、其他组分及载体之间的相互作用；结合热力学和原位红外等分析，揭示CO/CO2共氢化反应中中间产物类型及水汽变换反应对碳分子转化的影响，初步获得共氢化反应机理，最后开展了共氢化反应条件优化研究，获得CO/CO2共氢化合成甲醇技术的实验及理论基础。