Synthesis of iron-based metal-organic framework MIL-53 as an efficient catalyst to activate persulfate for the degradation of Orange G in aqueous solution (2022)

A series of MIL-53(Fe) materials was synthesized using a solvothermal method under different temperature and time conditions and were used as catalysts to activate persulfate and degrade Orange G (OG). Influences of the above conditions on the crystal structure and catalytic behavior were investigated. Degradation of OG under different conditions was evaluated, and the possible activation mechanism was speculated. The results indicate that high synthesis temperature (larger than 170 °C) leads to poor crystallinity and low catalytic activity, while MIL-53(Fe) cannot fully develop at low temperature (100 or 120 °C). The extension of synthesis time from 5 h to 3 d can increase the crystallinity of the samples, but weakened the catalytic activity, which was caused by the reduction of BET surface area and the amount of Fe (II)-coordinative unsaturated sites. Among all the samples, MIL-53(Fe)-A possesses the best crystal structure and catalytic activity. In optimal conditions, OG solution can be totally decolorized after degradation for 90 min, and a removal rate of 74% for COD was attained after 120 min. The initial solution pH had great influence on OG degradation, with the greatest removal in acidic pH environment. ESR spectra showed that sulfate radical (SO4[rad]), hydroxyl radical (OH[rad]), persulfate radical (S2O8[rad]), and superoxide radical (O2[rad]) exist in this system under acidic conditions. Furthermore, with the increase of pH, the relative amount of O2[rad] increases while that of OH[rad] and SO4[rad] decreases, resulting in a reduced oxidizing capacity of the system.

Original languageEnglish (US)
Pages (from-to)82-92
Number of pages11
JournalApplied Catalysis A: General
Volume549
DOIs
StatePublished - 2018
  • Catalytic activity
  • Chemical oxidation
  • MIL-53(Fe)
  • Metal-organic frameworks
  • Persulfate
  • Sulfate radical
  • Catalysis
  • Process Chemistry and Technology
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Pu, M., Guan, Z., Ma, Y., Wan, J., Wang, Y., Brusseau, M. L., & Chi, H. (2018). Synthesis of iron-based metal-organic framework MIL-53 as an efficient catalyst to activate persulfate for the degradation of Orange G in aqueous solution. Applied Catalysis A: General, 549, 82-92. https://doi.org/10.1016/j.apcata.2017.09.021

Synthesis of iron-based metal-organic framework MIL-53 as an efficient catalyst to activate persulfate for the degradation of Orange G in aqueous solution. / Pu, Mengjie; Guan, Zeyu; Ma, Yongwen et al.

In: Applied Catalysis A: General, Vol. 549, 2018, p. 82-92.

Research output: Contribution to journalArticlepeer-review

Pu, M, Guan, Z, Ma, Y, Wan, J, Wang, Y, Brusseau, ML & Chi, H 2018, 'Synthesis of iron-based metal-organic framework MIL-53 as an efficient catalyst to activate persulfate for the degradation of Orange G in aqueous solution', Applied Catalysis A: General, vol. 549, pp. 82-92. https://doi.org/10.1016/j.apcata.2017.09.021

Pu M, Guan Z, Ma Y, Wan J, Wang Y, Brusseau ML et al. Synthesis of iron-based metal-organic framework MIL-53 as an efficient catalyst to activate persulfate for the degradation of Orange G in aqueous solution. Applied Catalysis A: General. 2018;549:82-92. https://doi.org/10.1016/j.apcata.2017.09.021

Pu, Mengjie ; Guan, Zeyu ; Ma, Yongwen et al. / Synthesis of iron-based metal-organic framework MIL-53 as an efficient catalyst to activate persulfate for the degradation of Orange G in aqueous solution. In: Applied Catalysis A: General. 2018 ; Vol. 549. pp. 82-92.

@article{d78a27a72d0f45c7ba8880014b894b17,

title = "Synthesis of iron-based metal-organic framework MIL-53 as an efficient catalyst to activate persulfate for the degradation of Orange G in aqueous solution",

abstract = "A series of MIL-53(Fe) materials was synthesized using a solvothermal method under different temperature and time conditions and were used as catalysts to activate persulfate and degrade Orange G (OG). Influences of the above conditions on the crystal structure and catalytic behavior were investigated. Degradation of OG under different conditions was evaluated, and the possible activation mechanism was speculated. The results indicate that high synthesis temperature (larger than 170 °C) leads to poor crystallinity and low catalytic activity, while MIL-53(Fe) cannot fully develop at low temperature (100 or 120 °C). The extension of synthesis time from 5 h to 3 d can increase the crystallinity of the samples, but weakened the catalytic activity, which was caused by the reduction of BET surface area and the amount of Fe (II)-coordinative unsaturated sites. Among all the samples, MIL-53(Fe)-A possesses the best crystal structure and catalytic activity. In optimal conditions, OG solution can be totally decolorized after degradation for 90 min, and a removal rate of 74% for COD was attained after 120 min. The initial solution pH had great influence on OG degradation, with the greatest removal in acidic pH environment. ESR spectra showed that sulfate radical (SO4−[rad]), hydroxyl radical (OH[rad]), persulfate radical (S2O8−[rad]), and superoxide radical (O2[rad]) exist in this system under acidic conditions. Furthermore, with the increase of pH, the relative amount of O2[rad] increases while that of OH[rad] and SO4−[rad] decreases, resulting in a reduced oxidizing capacity of the system.",

keywords = "Catalytic activity, Chemical oxidation, MIL-53(Fe), Metal-organic frameworks, Persulfate, Sulfate radical",

author = "Mengjie Pu and Zeyu Guan and Yongwen Ma and Jinquan Wan and Yan Wang and Brusseau, {Mark L.} and Haiyuan Chi",

note = "Funding Information: This study was supported by the National Natural Science Foundation of China (Grant Nos. 31570568 , 31670585 ), the State Key Laboratory of Pulp and Paper Engineering in China (No. 201535 ), the Science and Technology Planning Project of Guangzhou City , China (Nos. 201607010079 , 201607020007 ), the Science and Technology Planning Project of Guangdong Province , China (No. 2016A020221005 ) and SCUT Doctoral Student Short-Term Overseas Visiting Study Funding Project . The contribution of Mark L. Brusseau was supported by the NIEHS SRP (P42 ES04940 ). Publisher Copyright: {\textcopyright} 2017",

year = "2018",

doi = "10.1016/j.apcata.2017.09.021",

language = "English (US)",

volume = "549",

pages = "82--92",

journal = "Applied Catalysis A: General",

issn = "0926-860X",

publisher = "Elsevier",

}

TY - JOUR

T1 - Synthesis of iron-based metal-organic framework MIL-53 as an efficient catalyst to activate persulfate for the degradation of Orange G in aqueous solution

AU - Pu, Mengjie

AU - Guan, Zeyu

AU - Ma, Yongwen

AU - Wan, Jinquan

AU - Wang, Yan

AU - Brusseau, Mark L.

AU - Chi, Haiyuan

N1 - Funding Information:This study was supported by the National Natural Science Foundation of China (Grant Nos. 31570568 , 31670585 ), the State Key Laboratory of Pulp and Paper Engineering in China (No. 201535 ), the Science and Technology Planning Project of Guangzhou City , China (Nos. 201607010079 , 201607020007 ), the Science and Technology Planning Project of Guangdong Province , China (No. 2016A020221005 ) and SCUT Doctoral Student Short-Term Overseas Visiting Study Funding Project . The contribution of Mark L. Brusseau was supported by the NIEHS SRP (P42 ES04940 ). Publisher Copyright:© 2017

PY - 2018

Y1 - 2018

N2 - A series of MIL-53(Fe) materials was synthesized using a solvothermal method under different temperature and time conditions and were used as catalysts to activate persulfate and degrade Orange G (OG). Influences of the above conditions on the crystal structure and catalytic behavior were investigated. Degradation of OG under different conditions was evaluated, and the possible activation mechanism was speculated. The results indicate that high synthesis temperature (larger than 170 °C) leads to poor crystallinity and low catalytic activity, while MIL-53(Fe) cannot fully develop at low temperature (100 or 120 °C). The extension of synthesis time from 5 h to 3 d can increase the crystallinity of the samples, but weakened the catalytic activity, which was caused by the reduction of BET surface area and the amount of Fe (II)-coordinative unsaturated sites. Among all the samples, MIL-53(Fe)-A possesses the best crystal structure and catalytic activity. In optimal conditions, OG solution can be totally decolorized after degradation for 90 min, and a removal rate of 74% for COD was attained after 120 min. The initial solution pH had great influence on OG degradation, with the greatest removal in acidic pH environment. ESR spectra showed that sulfate radical (SO4−[rad]), hydroxyl radical (OH[rad]), persulfate radical (S2O8−[rad]), and superoxide radical (O2[rad]) exist in this system under acidic conditions. Furthermore, with the increase of pH, the relative amount of O2[rad] increases while that of OH[rad] and SO4−[rad] decreases, resulting in a reduced oxidizing capacity of the system.

AB - A series of MIL-53(Fe) materials was synthesized using a solvothermal method under different temperature and time conditions and were used as catalysts to activate persulfate and degrade Orange G (OG). Influences of the above conditions on the crystal structure and catalytic behavior were investigated. Degradation of OG under different conditions was evaluated, and the possible activation mechanism was speculated. The results indicate that high synthesis temperature (larger than 170 °C) leads to poor crystallinity and low catalytic activity, while MIL-53(Fe) cannot fully develop at low temperature (100 or 120 °C). The extension of synthesis time from 5 h to 3 d can increase the crystallinity of the samples, but weakened the catalytic activity, which was caused by the reduction of BET surface area and the amount of Fe (II)-coordinative unsaturated sites. Among all the samples, MIL-53(Fe)-A possesses the best crystal structure and catalytic activity. In optimal conditions, OG solution can be totally decolorized after degradation for 90 min, and a removal rate of 74% for COD was attained after 120 min. The initial solution pH had great influence on OG degradation, with the greatest removal in acidic pH environment. ESR spectra showed that sulfate radical (SO4−[rad]), hydroxyl radical (OH[rad]), persulfate radical (S2O8−[rad]), and superoxide radical (O2[rad]) exist in this system under acidic conditions. Furthermore, with the increase of pH, the relative amount of O2[rad] increases while that of OH[rad] and SO4−[rad] decreases, resulting in a reduced oxidizing capacity of the system.

KW - Catalytic activity

KW - Chemical oxidation

KW - MIL-53(Fe)

KW - Metal-organic frameworks

KW - Persulfate

KW - Sulfate radical

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U2 - 10.1016/j.apcata.2017.09.021

DO - 10.1016/j.apcata.2017.09.021

M3 - Article

AN - SCOPUS:85030156244

VL - 549

SP - 82

EP - 92

JO - Applied Catalysis A: General

JF - Applied Catalysis A: General

SN - 0926-860X

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