Amino-Modified Fe-Terephthalate Metal-Organic Framework as an Efficient Catalyst for the Selective Oxidation of H2S

Xiao Xiao Zheng; Li Juan Shen; Xiao Ping Chen; Xiao Hai Zheng; Chak Tong Au; Li Long Jiang

doi:10.1021/acs.inorgchem.8b01232

Amino-Modified Fe-Terephthalate Metal-Organic Framework as an Efficient Catalyst for the Selective Oxidation of H₂S

Xiao Xiao Zheng, Li Juan Shen, Xiao Ping Chen, Xiao Hai Zheng, Chak Tong Au, Li Long Jiang^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

87 Citations (Scopus)

Abstract

Classical amino-functionalized Fe-terephthalate metal-organic framework NH₂-MIL-53(Fe) and its parent framework MIL-53(Fe) were prepared via simple hydrothermal methods. The catalytic performaces of these two Fe-MOFs were explored for the selective oxidation of H₂S. The physicochemical properties of the fresh and used Fe-MOFs catalysts were investigated by XRD, BET, SEM, FT-IR, CO₂-TPD, and XPS techniques. It was found that the introduction of amino groups reduces the activation energies for H₂S oxidation and endows this catalyst surface with moderate basic sites. As a result, the NH₂-MIL-53(Fe) catalyst displays high H₂S conversion and near 100% S selectivity in the temperature range of 130-160 °C, outperforming commercial Fe₂O₃ and activated carbon. Moreover, a plausible reaction route for H₂S selective oxidation over NH₂-MIL-53(Fe) is proposed. This work opens up the possibility of utilizing MOFs as efficient catalyst for desulfuration reactions.

Original language	English
Pages (from-to)	10081-10089
Number of pages	9
Journal	Inorganic Chemistry
Volume	57
Issue number	16
DOIs	https://doi.org/10.1021/acs.inorgchem.8b01232
Publication status	Published - 20 Aug 2018
Externally published	Yes

Scopus Subject Areas

Physical and Theoretical Chemistry
Inorganic Chemistry

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@article{326468887fae4d3ba940cd77506ed72d,

title = "Amino-Modified Fe-Terephthalate Metal-Organic Framework as an Efficient Catalyst for the Selective Oxidation of H2S",

abstract = "Classical amino-functionalized Fe-terephthalate metal-organic framework NH2-MIL-53(Fe) and its parent framework MIL-53(Fe) were prepared via simple hydrothermal methods. The catalytic performaces of these two Fe-MOFs were explored for the selective oxidation of H2S. The physicochemical properties of the fresh and used Fe-MOFs catalysts were investigated by XRD, BET, SEM, FT-IR, CO2-TPD, and XPS techniques. It was found that the introduction of amino groups reduces the activation energies for H2S oxidation and endows this catalyst surface with moderate basic sites. As a result, the NH2-MIL-53(Fe) catalyst displays high H2S conversion and near 100% S selectivity in the temperature range of 130-160 °C, outperforming commercial Fe2O3 and activated carbon. Moreover, a plausible reaction route for H2S selective oxidation over NH2-MIL-53(Fe) is proposed. This work opens up the possibility of utilizing MOFs as efficient catalyst for desulfuration reactions.",

author = "Zheng, {Xiao Xiao} and Shen, {Li Juan} and Chen, {Xiao Ping} and Zheng, {Xiao Hai} and Au, {Chak Tong} and Jiang, {Li Long}",

note = "Funding Information: This work was supported by the Natural Science Foundation of China (21603034), the National Key Research and Development Program of China (2018YFA0209304), and the Natural Science Foundation of Fujian Province (2017J05022). Publisher copyright: {\textcopyright} 2018 American Chemical Society",

year = "2018",

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doi = "10.1021/acs.inorgchem.8b01232",

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journal = "Inorganic Chemistry",

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T1 - Amino-Modified Fe-Terephthalate Metal-Organic Framework as an Efficient Catalyst for the Selective Oxidation of H2S

AU - Zheng, Xiao Xiao

AU - Shen, Li Juan

AU - Chen, Xiao Ping

AU - Zheng, Xiao Hai

AU - Au, Chak Tong

AU - Jiang, Li Long

N1 - Funding Information: This work was supported by the Natural Science Foundation of China (21603034), the National Key Research and Development Program of China (2018YFA0209304), and the Natural Science Foundation of Fujian Province (2017J05022). Publisher copyright: © 2018 American Chemical Society

PY - 2018/8/20

Y1 - 2018/8/20

N2 - Classical amino-functionalized Fe-terephthalate metal-organic framework NH2-MIL-53(Fe) and its parent framework MIL-53(Fe) were prepared via simple hydrothermal methods. The catalytic performaces of these two Fe-MOFs were explored for the selective oxidation of H2S. The physicochemical properties of the fresh and used Fe-MOFs catalysts were investigated by XRD, BET, SEM, FT-IR, CO2-TPD, and XPS techniques. It was found that the introduction of amino groups reduces the activation energies for H2S oxidation and endows this catalyst surface with moderate basic sites. As a result, the NH2-MIL-53(Fe) catalyst displays high H2S conversion and near 100% S selectivity in the temperature range of 130-160 °C, outperforming commercial Fe2O3 and activated carbon. Moreover, a plausible reaction route for H2S selective oxidation over NH2-MIL-53(Fe) is proposed. This work opens up the possibility of utilizing MOFs as efficient catalyst for desulfuration reactions.

AB - Classical amino-functionalized Fe-terephthalate metal-organic framework NH2-MIL-53(Fe) and its parent framework MIL-53(Fe) were prepared via simple hydrothermal methods. The catalytic performaces of these two Fe-MOFs were explored for the selective oxidation of H2S. The physicochemical properties of the fresh and used Fe-MOFs catalysts were investigated by XRD, BET, SEM, FT-IR, CO2-TPD, and XPS techniques. It was found that the introduction of amino groups reduces the activation energies for H2S oxidation and endows this catalyst surface with moderate basic sites. As a result, the NH2-MIL-53(Fe) catalyst displays high H2S conversion and near 100% S selectivity in the temperature range of 130-160 °C, outperforming commercial Fe2O3 and activated carbon. Moreover, a plausible reaction route for H2S selective oxidation over NH2-MIL-53(Fe) is proposed. This work opens up the possibility of utilizing MOFs as efficient catalyst for desulfuration reactions.

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Amino-Modified Fe-Terephthalate Metal-Organic Framework as an Efficient Catalyst for the Selective Oxidation of H₂S

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