Boosting aerobic oxidative desulfurization performance in fuel oil via strong metal-edge interactions between Pt and h-BN
Boosting aerobic oxidative desulfurization performance in fuel oil via strong metal-edge interactions between Pt and h-BN
复制标题
通过 Pt 和 h-BN 之间强金属边缘相互作用提高燃油中的好氧氧化脱硫性能
DOI：
10.1016/j.cej.2019.122526
复制
发表时间：
2020
影响因子：
15.1
通讯作者：
Li Huaming
中科院分区：
文献类型：
--
作者：
Wu Peiwen;Wu Yingcheng;Chen Linlin;He Jing;Hua Mingqing;Zhu Fengxia;Chu Xiaozhong;Xiong Jun;He Minqiang;Zhu Wenshuai;Li Huaming
铂纳米颗粒（Pt NPs）长期以来被认为是许多催化过程的有效催化剂，包括催化氧化、氢化等。对于Pt催化，调整电子结构以提高催化性能和探索适当的纳米颗粒稳定化策略是两个中心问题。在这项工作中，我们在分散良好的Pt NP和六方氮化硼（h-BN）载体之间构建了强金属边缘相互作用（SMEI）。研究了h-BN与Pt纳米颗粒之间的电荷转移，发现h-BN中的B原子与Pt纳米颗粒之间存在电荷转移，而Pt纳米颗粒与h-BN中的N原子之间存在电荷转移。SMEI使Pt NPs带正电荷以增强好氧催化脱硫活性，对二苯并噻吩、4，6-二甲基二苯并噻吩、4-甲基苯并噻吩和苯并噻吩的硫去除率分别为98.3%、96.5%、93.7%和85.9%。此外，好氧氧化脱硫系统还表现出了良好的抗烯烃和芳烃性能。SMEI还产生了Pt NP的优异稳定性，而在反应后没有附聚。此外，催化剂可以循环使用5次而催化活性没有显著降低。此外，无论是几何结构和SMEI进行了很好的研究，以阐明构效关系。
Platinum nanoparticles (Pt NPs) have long been regarded as efficient catalysts for numerous catalytic process, including catalytic oxidation, hydrogenation, etc. For Pt catalysis, tuning the electronic structure for a boosted catalytic performance and exploring a proper strategy for stabilization of the nanoparticles are the two central issues. In this work, we constructed strong metal-edge interactions (SMEI) between well-dispersed Pt NPs and hexagonal boron nitride (h-BN) support. The charge transfer between h-BN and Pt NPs was carefully studied, and it was found that the charge transfers from B atoms in h-BN to Pt NPs and from Pt NPs to N atoms in h-BN. The SMEI makes the Pt NPs positively charged for a boosted aerobic catalytic desulfurization activity with sulfur removals of 98.3%, 96.5%, 93.7% and 85.9% to dibenzothiophene, 4, 6-dimethyldibenzothiophene, 4-methylbenzothiophene, and benzothiophene, respectively. Additionally, the aerobic oxidative desulfurization system showed an excellent resistance performance to olefins and aromatic hydrocarbons. The SMEI also gives rise to an excellent stabilization of the Pt NPs without agglomeration after the reaction. Moreover, the catalyst can be recycled 5 times without a significant decrease in catalytic activity. Additionally, both the geometric structure and the SMEI were well investigated to illuminate the structure-activity relationship.