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Amino-functionalized MIL-125(Ti) for photodenitrification of pyridine in fuels via coordination activation by unsaturated Ti4+ centers

文献类型: 外文期刊

作者: Wang, Shihui 1 ; He, Zhoujun 1 ; Wu, Ling 3 ; Wang, Deling 1 ; Si, Ruiru 4 ; Liu, Xiyao 2 ; Liang, Ruowen 1 ;

作者机构: 1.Ningde Normal Univ, Prov Univ Key Lab Green Energy & Environm Catalysi, Ningde 352100, Peoples R China

2.Ningde Normal Univ, Fujian Prov Key Lab Featured Mat Biochem Ind, Ningde 352100, Peoples R China

3.Fuzhou Univ, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350002, Peoples R China

4.Fujian Acad Agr Sci, Fujian Key Lab Agroprod Qual & Safety, Fuzhou 350003, Peoples R China

期刊名称:DALTON TRANSACTIONS ( 影响因子:4.0; 五年影响因子:3.7 )

ISSN: 1477-9226

年卷期: 2023 年 52 卷 11 期

页码:

收录情况: SCI

摘要: Due to their explicit structure, metal-organic frameworks (MOFs) have been supposed to be credible platforms to research the micro-mechanism of heterogeneous photocatalysis. In this study, amino-functionalized MOFs (MIL-125(Ti)-NH2 (denoted as MTi), UiO-66(Zr)-NH2 (denoted as UZr) and MIL-68(In)-NH2 (denoted as MIn)) with three different metal centers were synthesized and applied for the denitrification of simulated fuels under visible light irradiation, during which pyridine was used as a typical nitrogen-containing compound. The results showed that MTi had the best activity among the above three MOFs, and the denitrogenation rate increased to 80% after 4 h of visible light irradiation. On the grounds of the theoretical calculation of pyridine adsorption and actual activity experiments, it can be presumed that the unsaturated Ti4+ metal centers should be the key active sites. Meanwhile, the XPS and in situ infrared results verified that the coordinatively unsaturated Ti4+ sites facilitate the activation of pyridine molecules through the surface -NMIDLINE HORIZONTAL ELLIPSISTi- coordination species. The coordination-photocatalysis synergism promotes the efficiency of photocatalytic performance and the corresponding mechanism is proposed.

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