新型多功能双金属纳米催化材料的构筑、结构及其催化加氢脱氧性能

Development and utilization of renewable and sustainable resources and energies are very important to address current problems derived from traditional resources and energies. Therefore, it is of great practical significance to obtain high value-added important chemicals and high-quality liquid bio-fuels through chemical conversions by hydrodeoxygenation process of oxygen-containing lignin-based bio-oils. The project aims to develop the most critical part of the process to achieve high-performance hydrodeoxygenation catalysts. New supported bimetallic (non-noble-metals and noble metals) nanocatalysts based on active composite precursors of multi-metal-based layered double hydroxide/nitrogen-doped carbon will be constructed. The precise control methods for supramolecular intercalation, composite assembly, structural topology transformation and self-reduction, as well as the stabilization method, will be developed and strengthened. As for multifunctional catalytically active sites, we will reveal multilevel synergistic effects between bimetallic components and between metals and surface structures (defects and acidic sites), as well as the stabilization effect of the support for active sites. Further, the mechanism of catalytic reactions will be clarified. And, both the hydrodeoxygenation performance and the stability of catalysts can be significantly improved. The project will provide an effective new approach for the structural design and the performance control of highly efficient and stable hydrodeoxygenation catalysts for the conversion of lignin-based bio-oils, and also provide a basis for the application of catalytic hydrodeoxygenation for biomass resource conversion.

可再生和可持续资源和能源开发与利用是解决传统资源和能源面临问题的重要途径，对高富氧木质素基生物质油进行加氢脱氧转化获得高附加值化学品和高品质生物液体燃料具有重要的现实意义。本项目旨在发展实现这一过程最关键一环的加氢脱氧催化剂，基于多金属组分层状双金属氢氧化物/氮掺杂碳型活性复合前体构筑新型双金属(非贵金属-贵金属)纳米催化材料，发展与强化超分子插层、复合组装、结构拓扑转变、自还原等过程的精确控制和结构稳定化方法，构建双金属活性位、表面缺陷位和表面酸性位等多功能催化活性位，揭示双金属组分间、金属活性位与表面缺陷位间、金属活性位与表面酸性位间多层次催化协同效应以及载体对活性位的稳定化机制，阐明催化作用机理，实现催化材料加氢脱氧性能和稳定性的显著提升。项目研究将为用于木质素基生物质油转化的高效稳定催化材料设计与性能调控提供一条新途径，为面向生物质资源转化的催化加氢脱氧技术应用提供一定的基础支撑。

可持续和可再生资源和能源开发与利用是解决传统资源和能源面临问题的重要途径，对高富氧木质素基生物质油进行加氢脱氧转化获得高附加值化学品和高品质生物液体燃料具有重要的现实意义。本项目基于此，开展了高性能加氢脱氧催化剂的构筑、结构及其催化生物质平台分子加氢脱氧性能的研究。重点通过多金属组分层状双金属氢氧化物或者氮掺杂碳复合的活性前体，构筑出了一系列新型双金属和单金属纳米催化材料，发展与强化了一系列复合组装、结构拓扑转变、还原过程的精确控制和结构稳定化方法，构建了双金属活性位、表面缺陷位和表-界面活性位等多功能催化活性位，通过系统深入的结构表征和理论计算揭示了双金属组分间、金属活性位与表面缺陷位间、金属活性位与表-界面活性位间多层次催化协同效应以及载体对活性位的稳定化机制，阐明了催化作用机理，实现了催化材料加氢脱氧性能和稳定性的显著提升。项目研究所得的研究成果为用于木质素基生物质油转化的高效稳定催化材料设计与性能调控提供了诸多的新思路和新途径，也为面向生物质资源转化的催化加氢脱氧技术应用提供了一定的基础支撑，具有一定的理论价值和实际意义。