π-π conjugation driving peroxymonosulfate activation for pollutant elimination over metal-free graphitized polyimide surface

Cao, Wenrui; Luo, Yongxiang; Cai, Xuanying; Wang, Shuguang; Hu, Chun; Lyu, Lai

doi:10.1016/j.jhazmat.2021.125191

Cited by 19 publications

(5 citation statements)

References 47 publications

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“…As shown in Figure d, the signal of the fresh catalyst was centered at g = 2.212, while it changed to g = 2.108 after the reaction, suggesting the existence of electron exchanges between the catalyst, DO, and pollutants. The relative intensity was increased after the reaction, which confirmed the electron-donating process of pollutants around the EPCs . Electrons accumulated around the ERCs and led to the microactivation of DO.…”

Section: Resultsmentioning

confidence: 64%

“…The relative intensity was increased after the reaction, which confirmed the electrondonating process of pollutants around the EPCs. 51 Electrons accumulated around the ERCs and led to the microactivation of DO. For the samples after reaction in a N 2 environment, the g value was further shifted to g = 2.095, and the relative intensity was further increased, indicating that more electrons accumulated around the ERCs without consumption.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

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Efficient Decomposition of Organic Pollutants over nZVI/FeO_x/FeN_y-Anchored NC Layers via a Novel Dual-Reaction-Centers-Based Wet Air Oxidation Process under Natural Conditions

Cao

Lyu

2021

ACS EST Eng.

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The wet air oxidation (WAO) process is a promising advanced oxidation process used for the degradation of organic pollutants; however, severe reaction conditions, including high temperature and high pressure, have significantly limited its application. In this report, we describe a new discovery that nZVI/FeO x /FeN y -anchored NC composites (nZVI/FeN5.5O7.2/C) exhibit an excellent catalytic performance for organic pollutant removal through natural dissolved oxygen (DO) microactivation at room temperature and atmospheric pressure. Characterization techniques reveal the key structural information: a special kind of construction of dual-reaction-centers (DRCs) with electron-rich Fe microcenters (ERCs) and electron-poor C(π)/N microcenters (EPCs) is successfully constructed on the surface of the catalyst through bonding of nZVI, FeO x , and FeN y , which is responsible for the novel DRCs-WAO process. During the reaction, DO obtains electrons and is rapidly activated into active oxygen species at the ERCs. Pollutants, as electron donors, lose electrons at EPCs and are oxidized. Electron transfer between EPCs and ERCs is achieved through the constructed Fe–O–C and Fe–N bonding bridges. This process is even free from the interference of inorganic ions, pH, or natural organic matter in the water environment. Our findings address the key limitation of the classical WAO process and are of positive significance for developing new wastewater treatment technologies with low energy consumption and high efficiency.

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Section: Resultsmentioning

confidence: 64%

Section: ■ Results and Discussionmentioning

confidence: 99%

Efficient Decomposition of Organic Pollutants over nZVI/FeO_x/FeN_y-Anchored NC Layers via a Novel Dual-Reaction-Centers-Based Wet Air Oxidation Process under Natural Conditions

Cao

Lyu

2021

ACS EST Eng.

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“…The process of preparing the composite is illustrated in Figure a. Upon mixing graphite and dopamine, dopamine molecules are adsorbed onto the graphite surface through intermolecular π–π interaction, resulting in an enrichment of functional groups on the graphite surface . The Zn 2+ are effectively immobilized through complexation with the hydroxyl groups in dopamine .…”

Section: Resultsmentioning

confidence: 99%

“…Upon mixing graphite and dopamine, dopamine molecules are adsorbed onto the graphite surface through intermolecular π−π interaction, resulting in an enrichment of functional groups on the graphite surface. 18 The Zn 2+ are effectively immobilized through complexation with the hydroxyl groups in dopamine. 19 Simultaneously, the nitrogen atoms in MBI and Zn 2+ interact with the dopamine molecule through ligand interaction, leading to their immobilization.…”

Section: Characterization Of Mzpg Materialmentioning

confidence: 99%

High-Loading Smart Carrier Containing 2-Mercaptobenzimidazole-Zn²⁺-Polydopamine with pH-Responsive Function to Fabricate High-Performance Waterborne Epoxy Anticorrosion Coatings

Liu,

Li,

Kong

et al. 2024

ACS Appl. Mater. Interfaces

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Corrosion inhibitor additives are considered to be one of the effective methods to slow down the corrosion of metals, but the corrosion inhibitors will decompose and lose their effect in a long-term corrosive environment. In this work, a smart corrosion inhibitor carrier 2-mercaptobenzimidazole-Zn 2+ -polydopamine@ graphite (MZPG) with excellent pH response was designed and synthesized using a one-pot method. This corrosion inhibitor carrier not only has a very high 2-mercaptobenzimidazole (MBI) loading capacity (38.0%) but also maintains a very low MBI activity to inhibit the decomposition of MZPG in the environment as much as possible. The MZPG/epoxy (MZPG/EP) coatings prepared by the spraying method showed excellent mechanical properties. Electrochemical and salt spray tests showed that the MZPG/EP coatings (1.20 × 10 10 Ω•cm 2 ) have excellent corrosion resistance with R p values up to 3 orders of magnitude higher than that of the EP coating (1.25 × 10 7 Ω•cm 2 ). Notably, the MZPG/EP coatings maintained good corrosion resistance under acidic conditions due to the pH-responsive release of corrosion inhibitors. This is of great significance for the future development of coatings for highly corrosive environments.

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“…Our previous work proposed dual-reaction-center (DRC) catalysts using lattice doping and organic complexation to induce the redistribution of free electrons on the catalyst surface, forming electron rich/poor microregions. − In addition to H 2 O 2 , pollutants and dissolved oxygen (DO) in the aquatic environment act as electron donors and acceptors, indicating that effective utilization of internal energy in the reaction system can be achieved by constructing the surface electron polarization of the catalyst. ,− Compared to the conventional heterogeneous Fenton system, DRC catalysts greatly reduce the dependence of the reaction on external resources and energy. ,− However, it remains a challenge to further construct DRC catalysts with strong surface polarity to efficiently utilize pollutant energy and reduce the dependence of the reaction system on H 2 O 2 .…”

Section: Introductionmentioning

confidence: 99%

Enhanced Water Purification Efficiency Induced by Trace H₂O₂ on the Electron Distribution-Polarized Unequilibrium Surface of CuS/ZnO Nanosheets

Gao

Wang

et al. 2022

ACS EST Water

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Excessive chemical reagents and energy are necessary to maintain electron recycling in advanced oxidation processes, resulting in high-energy consumption for water purification. Here, we present a new dual-reaction center catalyst consisting of CuS/ZnO nanosheets (CS/ZO NSs) with a cluster-like flower structure to reduce the energy consumption of Fenton reaction. The characterization results revealed that the simultaneous lattice doping of ZnO by Cu and S successfully induced the surface polarization distribution of free electrons, forming electronrich/poor microregions over CS/ZO NSs. The CS/ZO NSs/H 2 O 2 system showed excellent performance for refractory pollutant removal including ciprofloxacin, with a removal efficiency of 99.2% in 60 min, and achieved rapid and efficient removal of refractory organic matters and natural organic matter in wastewater in 120 min. Dissolved oxygen can act as an electron acceptor to gain electrons directly on the catalyst surface to be activated to superoxide radicals (HO 2• /O 2 •− ) without external energy input in CS/ZO NSs suspension. Just trace hydrogen peroxide (H 2 O 2 ) can stimulate the electron-donation effect from pollutants to the electron-deficient microregions. H 2 O 2 can also be reduced to hydroxyl radicals ( • OH) in the electron-rich microregions to destroy the contaminants. The synergistic linkage of the surface electron-poor and electron-rich microregions achieves excellent purification performance with a high efficiency and low energy.

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π-π conjugation driving peroxymonosulfate activation for pollutant elimination over metal-free graphitized polyimide surface

Cited by 19 publications

References 47 publications

Efficient Decomposition of Organic Pollutants over nZVI/FeO_x/FeN_y-Anchored NC Layers via a Novel Dual-Reaction-Centers-Based Wet Air Oxidation Process under Natural Conditions

Efficient Decomposition of Organic Pollutants over nZVI/FeO_x/FeN_y-Anchored NC Layers via a Novel Dual-Reaction-Centers-Based Wet Air Oxidation Process under Natural Conditions

High-Loading Smart Carrier Containing 2-Mercaptobenzimidazole-Zn²⁺-Polydopamine with pH-Responsive Function to Fabricate High-Performance Waterborne Epoxy Anticorrosion Coatings

Enhanced Water Purification Efficiency Induced by Trace H₂O₂ on the Electron Distribution-Polarized Unequilibrium Surface of CuS/ZnO Nanosheets

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π-π conjugation driving peroxymonosulfate activation for pollutant elimination over metal-free graphitized polyimide surface

Cited by 19 publications

References 47 publications

Efficient Decomposition of Organic Pollutants over nZVI/FeOx/FeNy-Anchored NC Layers via a Novel Dual-Reaction-Centers-Based Wet Air Oxidation Process under Natural Conditions

Efficient Decomposition of Organic Pollutants over nZVI/FeOx/FeNy-Anchored NC Layers via a Novel Dual-Reaction-Centers-Based Wet Air Oxidation Process under Natural Conditions

High-Loading Smart Carrier Containing 2-Mercaptobenzimidazole-Zn2+-Polydopamine with pH-Responsive Function to Fabricate High-Performance Waterborne Epoxy Anticorrosion Coatings

Enhanced Water Purification Efficiency Induced by Trace H2O2 on the Electron Distribution-Polarized Unequilibrium Surface of CuS/ZnO Nanosheets

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Efficient Decomposition of Organic Pollutants over nZVI/FeO_x/FeN_y-Anchored NC Layers via a Novel Dual-Reaction-Centers-Based Wet Air Oxidation Process under Natural Conditions

Efficient Decomposition of Organic Pollutants over nZVI/FeO_x/FeN_y-Anchored NC Layers via a Novel Dual-Reaction-Centers-Based Wet Air Oxidation Process under Natural Conditions

High-Loading Smart Carrier Containing 2-Mercaptobenzimidazole-Zn²⁺-Polydopamine with pH-Responsive Function to Fabricate High-Performance Waterborne Epoxy Anticorrosion Coatings

Enhanced Water Purification Efficiency Induced by Trace H₂O₂ on the Electron Distribution-Polarized Unequilibrium Surface of CuS/ZnO Nanosheets