原子级别非金属杂原子掺杂的介孔单层氮化硼的构建及其吸附脱硫性能研究

This project aims at adsorbing sulfur compounds from fuels to achieve a low-cost purification for fuels. The following scientific questions will be focused to be solved through the design of atomic level metal-free heteroatom doped mesoporous monolayer boron nitride (BN) materials and perform the related the oretical researches. (1) By the design of monolayer BN, more active sites can be exposed to improve the adsorption capacity. (2) Through the construction of mesoporous on the monolayer BN, the mass transfer limitations can be overcome as well as the adsorption rate and desorption regeneration ability can be increased. (3) By introducing the metal-free halogen heteroatoms, the electronic structure of BN can be adjusted, and the enhanced adsorption capacity of sulfide and higher selectivity can be achieved. (4) Based on the regulation of surface and interface along with the systematic characterizations and kinetic study, the adsorption desulfurization mechanism of atomically nonmetal heteroatom doped mesoporous monolayer BN materials was studied. The relationships between the structure and performance were also explored in details. It is hoped that through this research project, the study of novel adsorptive desulfurization materials and adsorptive desulfurization theory can have some innovations. And it is expected to provide a low-cost and highly efficient new technology for sulfur removal from fuel.

本项目采用吸附方法脱除燃油中的硫化物，实现低成本燃油净化。通过原子级别非金属杂原子掺杂的介孔单层BN吸附剂的设计并进行相关理论研究，着重解决下列科学问题：(1) 通过设计单层的BN脱硫吸附剂，暴露出更多的活性位点，增大吸附容量；(2) 通过设计具有介孔结构的单层BN吸附剂，克服传质限制，提高吸附速率和脱附再生能力；(3) 通过引入非金属卤素杂原子，调节BN的电子结构，实现吸附剂对含硫基团的吸附容量增大及选择性增强；(4) 通过系统表征和动力学研究，以界面和表面调控研究为出发点，研究原子级别非金属杂原子掺杂介孔单层BN吸附脱硫机理以及构效关系。期望通过本项目的研究，在新材料和吸附脱硫的理论研究方面有所创新，并为燃油脱硫净化提供低成本和高效新技术。

本课题针对传统的燃油加氢脱硫成本高的问题，开发常温常压条件下吸附脱硫技术，提出构建非金属杂原子掺杂的介孔单层BN吸附剂，并探究吸附剂吸附机理这一选题。在三年的实验过程中，本课题将不同的非金属共聚物引入到BN的合成中，通过控制合成温度，冷冻干燥等策略，来调节BN的孔径大小，表面官能团，以及电子结构。通过X射线衍射、扫描电镜、透射电镜以及X射线光电子能谱等方法对吸附材料的结构和组成进行了系统表征。再通过对吸附剂的吸附脱硫性能测试，筛选出高吸附性，高选择性的吸附材料，优化所得吸附剂能达到超深度脱硫（<10 ppm）。同时，本课题深入系统研究了暴露活性位点，增加微孔比例，以及缺陷对BN吸附剂吸附性能的影响，为燃油脱硫净化提供低成本的高效新技术。