重油浆态床加氢环境原位衍生碳载单原子钼高效催化体系的构筑及加氢转化机理

浆态床加氢是重油轻质化的有效途径之一。高性能催化剂的开发是实现重油高效转化、突破体系生焦技术瓶颈的关键。现有加氢催化体系油溶性钼催化剂在反应过程中活性物种易发生团聚，催化剂暴露的活性位逐渐减少，金属原子利用率不断降低，导致催化剂性能劣化和体系生焦。本项目旨在构筑浆态床加氢过程中沥青质原位衍生碳载单原子钼高效催化体系，深入认识螯合配体调变有机钼分子在沥青质上的“靶向”吸附及可控热转化衍生碳载单原子钼催化剂的制备过程机理，探明高转化频率的钼活性物种形态及其稳定存在机制；研究碳载单原子钼催化剂电子结构、原子配位环境影响加氢裂化与缩合反应的作用规律，建立碳载单原子钼催化剂微观结构与重油加氢转化的构效关系，阐明加氢转化反应机理，形成重油浆态床加氢环境原位衍生高转化频率和高原子利用率加氢催化剂的构建方法。项目研究从原子尺度上为重油浆态床加氢催化剂的发展提供了理论基础。

Slurry bed hydrogenation is one of the effective ways to lighten heavy oil. The development of high-performance catalyst is the key to realize high efficiency conversion of heavy oil and break through the technical bottleneck of coking. The active species of the current oil soluble molybdenum catalysts are easy to agglomerate during the hydrogenation reaction process, the exposed active sites of the catalyst are gradually reduced, and the utilization rate of metal atoms is constantly reduced, resulting in the degradation of catalyst performance and coking. The purpose of this project is to construct carbon supported single-atom molybdenum catalysts by in situ derivatization of asphaltene for highly efficient catalytic hydrogenation of heavy oil in slurry bed. Based on the understanding of the “targeted” adsorption of chelating ligand modified organomolybdenum molecules on asphaltenes and the preparation mechanism of carbon supported single-atom molybdenum catalysts derived from controlled thermal conversion, the active species of molybdenum with high turnover frequency and its stable existence mechanism will be explored. In addition, the effects of electronic structure and atomic coordination environment on hydrocracking and condensation of carbon supported single-atom molybdenum catalysts will be studied, the structure-activity relationship between the microstructure of carbon supported single-atom molybdenum catalysts and heavy oil hydrocracking will be established, and the law of hydrogenation conversion reaction will be clarified. Moreover, the in-situ derivatization construction method of hydrogenation catalysts with high conversion frequency and high atomic utilization in heavy oil slurry bed hydrogenation environment will be formed. The research of this project will provide a theoretical basis for the development of hydrogenation catalyst for highly efficient catalytic hydrogenation of heavy oil in slurry bed from the atomic scale.