Metallic Active Sites on MoO2(110) Surface to Catalyze Advanced Oxidation Processes for Efficient Pollutant Removal

Advanced oxidation processes (AOPs) based on sulfate radicals (SO4⋅−) suffer from low conversion rate of Fe(III) to Fe(II) and produce a large amount of iron sludge as waste. Herein, we show that by using MoO2 as a cocatalyst, the rate of Fe(III)/Fe(II) cycling in PMS system accelerated significantl...

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Published iniScience Vol. 23; no. 2; p. 100861
Main Authors Ji, Jiahui, Aleisa, Rashed M., Duan, Huan, Zhang, Jinlong, Yin, Yadong, Xing, Mingyang
Format Journal Article
LanguageEnglish
Published Elsevier Inc 21.02.2020
Elsevier
Subjects
Catalysis
Inorganic Chemistry
Water Resources Engineering
Water Resources Engineering
Inorganic Chemistry
Catalysis
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Abstract Advanced oxidation processes (AOPs) based on sulfate radicals (SO4⋅−) suffer from low conversion rate of Fe(III) to Fe(II) and produce a large amount of iron sludge as waste. Herein, we show that by using MoO2 as a cocatalyst, the rate of Fe(III)/Fe(II) cycling in PMS system accelerated significantly, with a reaction rate constant 50 times that of PMS/Fe(II) system. Our results showed outstanding removal efficiency (96%) of L-RhB in 10 min with extremely low concentration of Fe(II) (0.036 mM), outperforming most reported SO4⋅−-based AOPs systems. Surface chemical analysis combined with density functional theory (DFT) calculation demonstrated that both Fe(III)/Fe(II) cycling and PMS activation occurred on the (110) crystal plane of MoO2, whereas the exposed active sites of Mo(IV) on MoO2 surface were responsible for accelerating PMS activation. Considering its performance, and non-toxicity, using MoO2 as a cocatalyst is a promising technique for large-scale practical environmental remediation. [Display omitted] •The degradation rate of PMS/Fe(II)/MoO2 system is 50 times higher than that without MoO2•Fe(III)/Fe(II) cycle on (110) surface of MoO2 in PMS/Fe(II)/MoO2 system was confirmed•The metal active sites exposed to MoO2 (110) surface are responsible for PMS activation•Compared with MoS2, MoO2 co-catalytic system has less toxicity and no release of H2S Inorganic Chemistry; Catalysis; Water Resources Engineering
AbstractList Advanced oxidation processes (AOPs) based on sulfate radicals (SO4⋅−) suffer from low conversion rate of Fe(III) to Fe(II) and produce a large amount of iron sludge as waste. Herein, we show that by using MoO2 as a cocatalyst, the rate of Fe(III)/Fe(II) cycling in PMS system accelerated significantly, with a reaction rate constant 50 times that of PMS/Fe(II) system. Our results showed outstanding removal efficiency (96%) of L-RhB in 10 min with extremely low concentration of Fe(II) (0.036 mM), outperforming most reported SO4⋅−-based AOPs systems. Surface chemical analysis combined with density functional theory (DFT) calculation demonstrated that both Fe(III)/Fe(II) cycling and PMS activation occurred on the (110) crystal plane of MoO2, whereas the exposed active sites of Mo(IV) on MoO2 surface were responsible for accelerating PMS activation. Considering its performance, and non-toxicity, using MoO2 as a cocatalyst is a promising technique for large-scale practical environmental remediation. : Inorganic Chemistry; Catalysis; Water Resources Engineering Subject Areas: Inorganic Chemistry, Catalysis, Water Resources Engineering
Advanced oxidation processes (AOPs) based on sulfate radicals (SO4⋅−) suffer from low conversion rate of Fe(III) to Fe(II) and produce a large amount of iron sludge as waste. Herein, we show that by using MoO2 as a cocatalyst, the rate of Fe(III)/Fe(II) cycling in PMS system accelerated significantly, with a reaction rate constant 50 times that of PMS/Fe(II) system. Our results showed outstanding removal efficiency (96%) of L-RhB in 10 min with extremely low concentration of Fe(II) (0.036 mM), outperforming most reported SO4⋅−-based AOPs systems. Surface chemical analysis combined with density functional theory (DFT) calculation demonstrated that both Fe(III)/Fe(II) cycling and PMS activation occurred on the (110) crystal plane of MoO2, whereas the exposed active sites of Mo(IV) on MoO2 surface were responsible for accelerating PMS activation. Considering its performance, and non-toxicity, using MoO2 as a cocatalyst is a promising technique for large-scale practical environmental remediation. [Display omitted] •The degradation rate of PMS/Fe(II)/MoO2 system is 50 times higher than that without MoO2•Fe(III)/Fe(II) cycle on (110) surface of MoO2 in PMS/Fe(II)/MoO2 system was confirmed•The metal active sites exposed to MoO2 (110) surface are responsible for PMS activation•Compared with MoS2, MoO2 co-catalytic system has less toxicity and no release of H2S Inorganic Chemistry; Catalysis; Water Resources Engineering
Advanced oxidation processes (AOPs) based on sulfate radicals (SO 4 ⋅− ) suffer from low conversion rate of Fe(III) to Fe(II) and produce a large amount of iron sludge as waste. Herein, we show that by using MoO 2 as a cocatalyst, the rate of Fe(III)/Fe(II) cycling in PMS system accelerated significantly, with a reaction rate constant 50 times that of PMS/Fe(II) system. Our results showed outstanding removal efficiency (96%) of L-RhB in 10 min with extremely low concentration of Fe(II) (0.036 mM), outperforming most reported SO 4 ⋅− -based AOPs systems. Surface chemical analysis combined with density functional theory (DFT) calculation demonstrated that both Fe(III)/Fe(II) cycling and PMS activation occurred on the (110) crystal plane of MoO 2 , whereas the exposed active sites of Mo(IV) on MoO 2 surface were responsible for accelerating PMS activation. Considering its performance, and non-toxicity, using MoO 2 as a cocatalyst is a promising technique for large-scale practical environmental remediation. • The degradation rate of PMS/Fe(II)/MoO 2 system is 50 times higher than that without MoO 2 • Fe(III)/Fe(II) cycle on (110) surface of MoO 2 in PMS/Fe(II)/MoO 2 system was confirmed • The metal active sites exposed to MoO 2 (110) surface are responsible for PMS activation • Compared with MoS 2 , MoO 2 co-catalytic system has less toxicity and no release of H 2 S Inorganic Chemistry; Catalysis; Water Resources Engineering
Advanced oxidation processes (AOPs) based on sulfate radicals (SO4⋅-) suffer from low conversion rate of Fe(III) to Fe(II) and produce a large amount of iron sludge as waste. Herein, we show that by using MoO2 as a cocatalyst, the rate of Fe(III)/Fe(II) cycling in PMS system accelerated significantly, with a reaction rate constant 50 times that of PMS/Fe(II) system. Our results showed outstanding removal efficiency (96%) of L-RhB in 10 min with extremely low concentration of Fe(II) (0.036 mM), outperforming most reported SO4⋅--based AOPs systems. Surface chemical analysis combined with density functional theory (DFT) calculation demonstrated that both Fe(III)/Fe(II) cycling and PMS activation occurred on the (110) crystal plane of MoO2, whereas the exposed active sites of Mo(IV) on MoO2 surface were responsible for accelerating PMS activation. Considering its performance, and non-toxicity, using MoO2 as a cocatalyst is a promising technique for large-scale practical environmental remediation.Advanced oxidation processes (AOPs) based on sulfate radicals (SO4⋅-) suffer from low conversion rate of Fe(III) to Fe(II) and produce a large amount of iron sludge as waste. Herein, we show that by using MoO2 as a cocatalyst, the rate of Fe(III)/Fe(II) cycling in PMS system accelerated significantly, with a reaction rate constant 50 times that of PMS/Fe(II) system. Our results showed outstanding removal efficiency (96%) of L-RhB in 10 min with extremely low concentration of Fe(II) (0.036 mM), outperforming most reported SO4⋅--based AOPs systems. Surface chemical analysis combined with density functional theory (DFT) calculation demonstrated that both Fe(III)/Fe(II) cycling and PMS activation occurred on the (110) crystal plane of MoO2, whereas the exposed active sites of Mo(IV) on MoO2 surface were responsible for accelerating PMS activation. Considering its performance, and non-toxicity, using MoO2 as a cocatalyst is a promising technique for large-scale practical environmental remediation.
ArticleNumber 100861
Author Zhang, Jinlong
Aleisa, Rashed M.
Ji, Jiahui
Duan, Huan
Yin, Yadong
Xing, Mingyang
AuthorAffiliation 3 School of Chemistry and Chemical Engineering, Southwest University, Chongqing 400715, China
1 Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai 200237, China
2 Department of Chemistry, University of California, Riverside, Riverside, CA 92521, USA
AuthorAffiliation_xml – name: 3 School of Chemistry and Chemical Engineering, Southwest University, Chongqing 400715, China
– name: 2 Department of Chemistry, University of California, Riverside, Riverside, CA 92521, USA
– name: 1 Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai 200237, China
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  surname: Ji
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  organization: Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai 200237, China
– sequence: 2
  givenname: Rashed M.
  surname: Aleisa
  fullname: Aleisa, Rashed M.
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  surname: Duan
  fullname: Duan, Huan
  organization: School of Chemistry and Chemical Engineering, Southwest University, Chongqing 400715, China
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  givenname: Jinlong
  surname: Zhang
  fullname: Zhang, Jinlong
  organization: Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai 200237, China
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  fullname: Yin, Yadong
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  givenname: Mingyang
  surname: Xing
  fullname: Xing, Mingyang
  email: mingyangxing@ecust.edu.cn
  organization: Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai 200237, China
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SSID ssj0002002496
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Snippet Advanced oxidation processes (AOPs) based on sulfate radicals (SO4⋅−) suffer from low conversion rate of Fe(III) to Fe(II) and produce a large amount of iron...
Advanced oxidation processes (AOPs) based on sulfate radicals (SO4⋅-) suffer from low conversion rate of Fe(III) to Fe(II) and produce a large amount of iron...
Advanced oxidation processes (AOPs) based on sulfate radicals (SO 4 ⋅− ) suffer from low conversion rate of Fe(III) to Fe(II) and produce a large amount of...
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SubjectTerms Catalysis
Inorganic Chemistry
Water Resources Engineering
Title Metallic Active Sites on MoO2(110) Surface to Catalyze Advanced Oxidation Processes for Efficient Pollutant Removal
URI https://dx.doi.org/10.1016/j.isci.2020.100861
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