Perspectives on Advances in the Catalytic Desulfurization and Denitrogenation of Transportation Fuel Oils Using Graphitic Carbon Nitride and Boron Nitride
Abstract:Expulsion of sulfur-containing compounds as well as nitrogen-containing
compounds present in fuel oils is critical because it can cause numerous
environmental problems and catalyst deactivation. Because of the limitations
of the other catalysts and adsorbents used for desulfurization, a
new type of carbon material, i.e., graphitic carbon nitride (g-C3N4), has emerged. It is similar in morphology to
graphene having a two-dimensional structure and possessing a band
gap of 2.7 eV and is an attractive catalyst att… Show more
“…have been utilized over the past several decades to activate and cleave C–S bonds. However, these catalytic systems are expensive and often suffer from poor chemoselectivity, low catalytic efficiency, and low recyclability which greatly limits their long-term use as desulfurization catalysts …”
mentioning
confidence: 99%
“…However, these catalytic systems are expensive and often suffer from poor chemoselectivity, low catalytic efficiency, and low recyclability which greatly limits their long-term use as desulfurization catalysts. 16 Recently, our lab has shown that a covalent organic framework (COF) 17−19 containing dehydrobenzoannulene (DBA)-Ni(0) complexes can be used to reductively cleave the C(aryl)-S bonds of several organosulfur compounds utilizing hydrosilanes as the reducing agent. 20 While this catalytic system was recyclable and great for activating C(aryl)-S bonds of fused and unfused aryl thioethers, it is still unclear if this Ni(0)-based catalytic system is useful for the desulfurization of dibenzothiophenes (DBTs), a class of refractory sulfur compounds that are commonly found in sour crude oil.…”
mentioning
confidence: 99%
“…21 Unlike aryl thioethers, DBTs are not very reactive and they account for the highest percentage of sulfur compounds found in heavy and vacuum gas oil that must be removed to meet environmental standards. 2,16,21,22 Interestingly, Garcia and coworkers have shown that Ni catalysts like [(dippe)-NiH)] 2 are great for the desulfurization of DBTs in the presence of alkyl Grignards. 23,24 While the system is believed to proceed through a classical Ni(0)/Ni(II) pathway, the sulfur gets converted initially to MgS and then to H 2 S after an acidic workup.…”
The development of metalated porous organic polymers (POPs) is vital for producing recyclable heterogeneous catalytic systems that are useful for real-world applications. Herein, we report the synthesis, characterization, and catalytic desulfurization properties of an olefin-linked POP containing Ni-doped dehydrobenzoannulene (DBA) units. We show that a Ni-DBA-TMT-POP can be used to remove sulfur from dibenzothiophenes (DBTs) and benzothiophenes (BTs) in the presence of Grignard reagents and phosphine ligands. The Ni-DBA-TMT-POP catalytic system exhibits great recyclability and respectable yields. This work highlights a rare example of utilizing a Ni-doped DBA-POP for the desulfurization of refractory sulfur compounds that are commonly found in sour crude oil.
“…have been utilized over the past several decades to activate and cleave C–S bonds. However, these catalytic systems are expensive and often suffer from poor chemoselectivity, low catalytic efficiency, and low recyclability which greatly limits their long-term use as desulfurization catalysts …”
mentioning
confidence: 99%
“…However, these catalytic systems are expensive and often suffer from poor chemoselectivity, low catalytic efficiency, and low recyclability which greatly limits their long-term use as desulfurization catalysts. 16 Recently, our lab has shown that a covalent organic framework (COF) 17−19 containing dehydrobenzoannulene (DBA)-Ni(0) complexes can be used to reductively cleave the C(aryl)-S bonds of several organosulfur compounds utilizing hydrosilanes as the reducing agent. 20 While this catalytic system was recyclable and great for activating C(aryl)-S bonds of fused and unfused aryl thioethers, it is still unclear if this Ni(0)-based catalytic system is useful for the desulfurization of dibenzothiophenes (DBTs), a class of refractory sulfur compounds that are commonly found in sour crude oil.…”
mentioning
confidence: 99%
“…21 Unlike aryl thioethers, DBTs are not very reactive and they account for the highest percentage of sulfur compounds found in heavy and vacuum gas oil that must be removed to meet environmental standards. 2,16,21,22 Interestingly, Garcia and coworkers have shown that Ni catalysts like [(dippe)-NiH)] 2 are great for the desulfurization of DBTs in the presence of alkyl Grignards. 23,24 While the system is believed to proceed through a classical Ni(0)/Ni(II) pathway, the sulfur gets converted initially to MgS and then to H 2 S after an acidic workup.…”
The development of metalated porous organic polymers (POPs) is vital for producing recyclable heterogeneous catalytic systems that are useful for real-world applications. Herein, we report the synthesis, characterization, and catalytic desulfurization properties of an olefin-linked POP containing Ni-doped dehydrobenzoannulene (DBA) units. We show that a Ni-DBA-TMT-POP can be used to remove sulfur from dibenzothiophenes (DBTs) and benzothiophenes (BTs) in the presence of Grignard reagents and phosphine ligands. The Ni-DBA-TMT-POP catalytic system exhibits great recyclability and respectable yields. This work highlights a rare example of utilizing a Ni-doped DBA-POP for the desulfurization of refractory sulfur compounds that are commonly found in sour crude oil.
“…The problem of agglomeration is an urgent matter to be solved, as is the case with other TMOs. A feasible strategy is to select an appropriate porous carrier to construct supported catalysts. , Carbon nitride (g-C 3 N 4 ) has a simple preparation process and high yield and is often used as a carrier in supported catalysts . In comparison, three-dimensional porous carbon nitride (3D g-C 3 N 4 ) obtained by the supramolecular assembly method, with a rich pore structure and high specific surface area, is a more suitable carrier …”
mentioning
confidence: 99%
“…6,7 Carbon nitride (g-C 3 N 4 ) has a simple preparation process and high yield and is often used as a carrier in supported catalysts. 8 In comparison, three-dimensional porous carbon nitride (3D g-C 3 N 4 ) obtained by the supramolecular assembly method, with a rich pore structure and high specific surface area, is a more suitable carrier. 9 Ionic liquids (ILs) have many excellent properties, which have been widely studied by researchers since their discovery.…”
In this work, a series of supported catalysts V 2 O 5 / 3D g-C 3 N 4 were prepared by a solvothermal method and programmed calcination, where a vanadium-based ionic liquid (V-IL) [(C 8 H 17 ) 3 NCH 3 ] 3 H 3 V 10 O 28 was used as the vanadium source and 3D porous carbon nitride (3D g-C 3 N 4 ) acted as the carrier. The detailed structural and compositional characterization results show that the use of V-IL promotes the high dispersion of V 2 O 5 on the carrier and effectively avoids the problem of agglomeration. Therefore, the catalytic oxidative desulfurization activity of V 2 O 5 /3D g-C 3 N 4 is greatly enhanced, and the content of dibenzothiophene in model oil can be effectively reduced to 1.2 ppm under appropriate conditions. The recycling capacity and the possible process of the oxidative desulfurization were discussed.
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