Photocatalytic oxidative desulfurization and denitrogenation for fuels in ambient air over Ti3C2/g-C3N4 composites under visible light irradiation

Photocatalytic oxidative desulfurization and denitrogenation for fuels in ambient air over Ti3C2/g-C3N4 composites under visible light irradiation
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DOI:
10.1016/j.apcatb.2020.118845
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发表时间:
2020-07-15
影响因子:
22.1
通讯作者:
Wei, Lishan
Wei, Lishan
中科院分区:
化学1区
文献类型:
--
作者:
Li, Bolun;Song, Haiyan;Wei, Lishan

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制备了MXene Ti 3C 2改性g-C(3)N(4)复合材料,并将其用于可见光下的光催化氧化脱氮和脱硫。该系统适用于小分子吡啶和噻吩在环境空气中的氧化,而无需添加额外的H(2)O(2)或纯O-2氧化剂。对催化剂的结构和光电性能进行了表征和比较。在最佳的复合材料中,g-C3 N4纳米片被成功地插入Ti 3C 2层,形成界面效应和异质结。插层效应促进了光生电子从g-C3 N4向Ti 3C 2的转移,抑制了电子-空穴对的复合。Ti 3C 2/g-C3 N4复合材料在光催化降解吡啶和噻吩的过程中表现出更好的光催化性能、更高的矿化效率和更好的可循环性。机理和密度泛函理论研究表明,空穴是催化反应的主要活性物种,电子和O2-生成的超氧自由基对最终转化率有促进作用.
MXene Ti3C2 modified g-C(3)N(4 )composites were prepared and used in photocatalytic oxidative denitrogenation and desulfurization under visible light. The photocatalysis system adapted to oxidation of small molecular pyridine and thiophene for fuels in the ambient air without adding extra H(2)O(2 )or pure O-2 oxidants. Structural and photoelectric properties of the photocatalysts were characterized and compared. In an optimal composite, g-C3N4 nanosheets were successfully intercalated by Ti3C2 layers to form an interfacial effect and heterojunction. Intercalation effect accelerated the photogenerated electrons transferring from g-C3N4 to Ti3C2 , and inhibited the recombination of electron-hole pairs. Ti3C2/g-C3N4 composite exhibited enhanced photocatalytic performance, high mineralization efficiency, and good recyclability in the removal of pyridine and thiophene. Mechanism and DFT studies proposed that the holes acted as the major active species for the photocatalysis procedures to form the reactant intermediates, while the electrons and O-2 generated superoxide radicals provided a promotion effect on the final conversions.