Enhancing oxidative desulfurization of polyoxometalate by integrating with a self-reductive framework

通过与自还原框架结合增强多金属氧酸盐的氧化脱硫作用

With the strict control of sulfur content in fuels,oxidative desulfurization(ODS),a promising desulphurization technology,needs to be continuously developed.In this study,we integrated multiple approaches(fabricating a porous structure,increasing phosphomolybdic acid(PMo)loading,improving amphiphilicity,and enhancing the intrinsic activity of PMo using a reductive framework)into PAF-54 carriers to improve ODS catalytic ability.The catalytic performance suggested that PAF-54 was not simply used as a carrier for PMo by physical integration.During the binding process,electron transfer between PAF-54 and PMo formed Mo^(5+)with superior catalytic activity.Owing to the presence of PAF-54,the catalytic activity of PMo as the active component qualitatively improved to achieve rapid and efficient desulfurization.More importantly,we found that other nitrogen-rich porous organic polymers can also reduce some of Mo^(6+)in PMo during loading,and its formation mechanism was investigated.This work provides a feasible strategy for designing highly efficient DOS catalysts.

由于对燃油硫含量的控制日益严格,氧化脱硫(ODS)作为一种前景广阔的脱硫技术需要不断发展.本工作将构建多孔结构、提升磷钼酸(PMo)的负载量、提高两亲性以及利用载体的还原框架提高PMo的本征活性等策略整合实施,成功制备了具有出色ODS催化能力的PMo@PAF-54材料.在催化剂制备过程中,PAF-54不是简单地作为载体与PMo发生物理的结合,更是与PMo发生了电子转移,生成了具有更优催化活性的Mo^(5+).PAF-54的存在使PMo的催化活性得到了质的飞跃,实现了快速且高效的脱硫.我们还发现其他富氮多孔有机聚合物也可在负载过程中还原PMo中的部分Mo^(6+),并对其反应机理进行了探索研究.本工作为设计高效的ODS催化剂提供了一个切实可行的策略.