Molybdenum Dioxide in Carbon Nanoreactors as a Catalytic Nanosponge for the Efficient Desulfurization of Liquid Fuels
Molybdenum Dioxide in Carbon Nanoreactors as a Catalytic Nanosponge for the Efficient Desulfurization of Liquid Fuels
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DOI：
10.1002/adfm.201808092
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发表时间：
2019-04-25
影响因子：
19
通讯作者：
Khlobystov, Andrei N.
中科院分区：
文献类型：
--
作者：
Astle, Maxwell A.;Rance, Graham A.;Khlobystov, Andrei N.
“催化纳米海绵”的原理，结合了有机硫氧化的催化和从反应混合物中的产物的螯合证明。VI族金属氧化物纳米颗粒（CrOx、MoOx、WOx）嵌入中空石墨化碳纳米纤维（GNF）中，其充当用于燃料净化中的氧化反应的纳米级反应容器。当浸入被有机硫化合物（苯并噻吩、二苯并噻吩、二甲基二苯并噻吩）污染的模型液体烷烃燃料中时，发现包含在GNF通道内生长的30 nm二氧化钼纳米颗粒的MoO2（R）GNF纳米反应器显示出上级氧化脱硫（ODS）能力，在仅5.9 mol%催化剂负载下提供超过98%的硫去除。碳纳米反应器在MoO2（R）GNF中的作用是在至少5个循环中增强催化中心的活性和稳定性。令人惊讶的是，纳米管空腔可以选择性地吸收和去除ODS产品（亚砜和砜）从几个模型燃料系统。这种效应与吸附脱硫（ADS）机制有关，该机制与同一材料中的ODS结合，产生“催化纳米海绵”MoO2（R）GNF。这种创新的ODS和ADS协同功能消除了燃料脱硫中溶剂萃取步骤的需要，并生产超低硫燃料。
The principle of a "catalytic nanosponge" that combines the catalysis of organosulfur oxidation and sequestration of the products from reaction mixtures is demonstrated. Group VI metal oxide nanoparticles (CrOx, MoOx, WOx) are embedded within hollow graphitized carbon nanofibers (GNFs), which act as nanoscale reaction vessels for oxidation reactions used in the decontamination of fuel. When immersed in a model liquid alkane fuel contaminated with organosulfur compounds (benzothiophene, dibenzothiophene, dimethyldibenzothiophene), it is found that MoO2 (R) GNF nanoreactors, comprising 30 nm molybdenum dioxide nanoparticles grown within the channel of GNFs, show superior abilities toward oxidative desulfurization (ODS), affording over 98% sulfur removal at only 5.9 mol% catalyst loading. The role of the carbon nanoreactor in MoO2 (R) GNF is to enhance the activity and stability of catalytic centers over at least 5 cycles. Surprisingly, the nanotube cavity can selectively absorb and remove the ODS products (sulfoxides and sulfones) from several model fuel systems. This effect is related to an adsorptive desulfurization (ADS) mechanism, which in combination with ODS within the same material, yields a "catalytic nanosponge" MoO2 (R) GNF. This innovative ODS and ADS synergistic functionality negates the need for a solvent extraction step in fuel desulfurization and produces ultralow sulfur fuel.