介孔Mo-Al-Si催化剂酸位点定向调控及硫化氢资源化利用新途径与机理研究

煤洁净利用过程中产生的硫化氢是导致我国雾霾等大气污染的潜在原因之一。叔十二烷基硫醇（TDM）是合成树脂和橡胶等重要战略物资不可缺少的重要中间体。本项目针对硫化氢传统利用方法所获产品附加值低以及合成TDM过程存在关键科学技术问题尚未突破的难题，提出构筑过渡金属钼（Mo）协同硅（Si）-铝（Al）复合的介孔固体酸催化剂实现硫化氢高值资源化合成TDM的研究思路。拟通过构建多组分复杂作用下（Mo-Al-Si）的自组装体系，采用一步水热法精确调控介孔固体酸催化剂的酸位点性质和强度，建立固体酸位点结构与合成TDM催化性能之间的构效关系，揭示含硫物种之间的转化行为，阐明酸位点在合成TDM过程中的作用规律和反应机理。项目成果既可为合成TDM提供理论依据和技术支撑，也可为我国新型煤洁净利用过程产生的硫化氢脱除及资源化利用提供新途径。

Hydrogen sulfide produced during the clean utilization of coal is a potential cause for air pollution such as haze. Tertiary dodecyl mercaptan (TDM) is an indispensable important intermediate for resin, rubber and other important materials. In view of the fact that the products obtained by the current traditional desulfurization method for removing hydrogen sulfide is generally not high and the bottleneck in the TDM synthesis due to unsolved key scientific questions, this project proposed the construction of mesoporous solid acid catalyst assisted with a transition metal molybdenum (Mo) synergistic silicon (Si)-aluminum (Al) composite to realize the synthesis of TDM with high value from hydrogen sulfide. It is planned to build a multi-component complex action (Mo-Al-Si) self-assembly system and use a one-step hydrothermal method to precisely control the acid site properties and strength of the mesoporous solid acid catalyst. The project is mainly aimed to establish the structure-activity relationship between acid sites and the catalytic performance of synthesizing TDM, and to reveal the conversion behavior between sulfur-containing species as well as to clarify the action law and reaction mechanism in the process of synthesizing TDM. The project results can not only provide theoretical basis and technical support for the synthesis of TDM, but also provide an new way for the removal and the high-valued utilization of hydrogen sulfide generated by the clean coal utilization process in China.