Nitrogen-doped carbon nanotubes enhanced Fenton chemistry: Role of near-free iron(III) for sustainable iron(III)/iron(II) cycles

Zhou, Chenying; Zhou, Peng; Sun, Minglu; Liu, Yang; Zhang, Heng; Xiong, Zhengwei; Liang, Juan; Duan, Xiaoguang; Lai, Bo

doi:10.1016/j.watres.2021.117984

Cited by 90 publications

(19 citation statements)

References 52 publications

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“…Recent studies have demonstrated the electron transfer activation process between metal-free nanocarbons and persulfate/peroxymonosulfate, highlighting that the catalytic performance strongly depends on the electronic properties of the oxygen functional groups on the nanocarbon surface. − In the present study, considering the significant difference in catalytic performance between FeOCl/CC@GO and FeOCl/CC@rGO (Figure a), the species and abundance of oxygen-containing functional groups on the surface of the corresponding GO and rGO layers were thus speculated to have a significant influence on the directional transfer of enriched electrons to H 2 O 2 . In view of this, the H 2 O 2 decomposition behavior of FeOCl/CC before and after being encapsulated by GO or rGO was systematically studied to obtain detailed information about the modulation properties of the enriched electrons by the carbon shell during electron penetration.…”

Section: Resultsmentioning

confidence: 99%

Overcoming the Activity–Stability Trade-Off in Heterogeneous Electro-Fenton Catalysis: Encapsulating Carbon Cloth-Supported Iron Oxychloride within Graphitic Layers

Cui

Zhao

Xie³

et al. 2022

ACS Catal.

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Maintaining a long-term service life of catalytic materials under the established configuration and design concept is a key focus in catalytic process research and development, especially for iron-functionalized cathode-based heterogeneous electro-Fenton (EF) processes operated under harsh conditions. Herein, a versatile and robust encapsulation engineering strategy is proposed based on the concept of tightly covering the surface of conventional iron-functionalized cathodes with an ultrathin carbon layer to significantly improve the stability of composite cathodes without causing activity loss. Taking carbon cloth-supported iron oxychloride (FeOCl/CC) as a model cathode catalyst, it was successfully encapsulated in a reduced graphene oxide protective shell (FeOCl/CC@rGO) using an electrophoretic deposition method, thereby achieving high stability due to negligible iron leaching (only 0.57% of FeOCl/CC), while maintaining almost unaffected activity due to electron penetration effect. Experimental analysis of the structure–activity relationship and theoretical calculations were used to establish the underlying molecular mechanism of electron penetration-triggered H2O2 activation on the outermost surface of rGO. This study uses an effective approach to overcome the activity–stability trade-off of integrated cathodes in heterogeneous EF processes, providing theoretical guidance for the rational design of high-performance cathodes with an encapsulated structure.

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Section: Resultsmentioning

confidence: 99%

Overcoming the Activity–Stability Trade-Off in Heterogeneous Electro-Fenton Catalysis: Encapsulating Carbon Cloth-Supported Iron Oxychloride within Graphitic Layers

Cui

Zhao

Xie³

et al. 2022

ACS Catal.

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“…It has been reported that nitrogen-doped carbocatalysts (e.g., N-CNTs, N-rGO) exhibit good catalytic performance when accelerating TrOCs removal by AOPs (e.g., Fenton, persulfate-based oxidation) owing to the role of doping. 23,31,37 However, in this study, the as-prepared N-rGO only slightly enhanced the oxidation of SSX compared to Mn(VII) alone (Figure 1b), suggesting the introduction of oxygen functional groups was more effective than nitrogen for catalyzing Mn(VII) reactions with SSX. It has also been well documented that carbocatalysts can serve as both catalysts and adsorbents for organic contaminants.…”

Section: Removal Of Pollutants Bymentioning

confidence: 92%

Carbocatalysts for Enhancing Permanganate Oxidation of Sulfisoxazole

Wang

Strathmann

2023

Environ. Sci. Technol.

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Permanganate (Mn(VII)) is extensively applied in water purification due to its stability and ease of handling, but it is a mild oxidant for trace organic contaminants (TrOCs). Hence, there is significant interest in strategies for enhancing reaction kinetics, especially in combination with efficient and economical carbocatalysts. This study compared the performance of four carbocatalysts (graphite, graphene oxide (GO), reduced-GO (rGO), and nitrogen-doped rGO (N-rGO)) in accelerating sulfisoxazole (SSX) oxidation by Mn(VII) and found that GO exhibited the greatest catalytic performance. Besides, the Mn-(VII)/GO system shows desirable capacities to remove a broad spectrum of TrOCs. We proposed that the degradation of SSX in Mn(VII)-GO suspensions follows two routes: (i) direct oxidation of SSX by Mn species [both Mn(VII) and in situ formed MnO 2(s) ] and (ii) a carbocatalyst route, where GO acts as an electron mediator, accepting electrons from SSX and transferring them to Mn(VII). We developed a mathematical model to show the contribution of each parallel pathway and found one-electron transfer is primarily responsible for accelerating SSX removal in the Mn(VII)/GO system. Findings in this study showed that GO provides a simple and effective strategy for enhancing the reactivity of Mn(VII) and provided mechanistic insights into the GO-catalyzed redox reaction between SSX and Mn(VII).

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“…36 Zhou et al reported that N-doped carbon materials could elevate the oxidation potential of Fe(III), thus promoting the cycle of Fe(III)/ Fe(II). 37 However, to date, the identification of active sites on N-doped cocatalysts remains unclear and most of the above carbonaceous cocatalysts are still high-cost, which limited the feasibility of their practical application in water treatment. 21 Herein, an eco-friendly N/C cocatalyst was fabricated via a facile one-pot pyrolytic strategy by mixing lignin (the massive "waste" in the pulp and paper industry) 38,39 and dicyandiamide (N source) in a specific proportion.…”

Section: ■ Introductionmentioning

confidence: 99%

Eco-Friendly Lignin-Based N/C Cocatalysts for Ultrafast Cyclic Fenton-Like Reactions in Water Purification via Graphitic N-Mediated Interfacial Electron Transfer

et al. 2022

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Herein, an eco-friendly lignin-based N-doped cocatalyst (N/C) was fabricated to enhance Fenton-like oxidation capacity. The N/ C-assisted Fe(III)/H 2 O 2 system showed ultrafast pollutant oxidation activity via an accelerated Fe(III)/Fe(II) cycle, exhibiting 16.9 times better caffeine removal efficiency than equivalent quantities of the classical Fenton system. N/C cocatalysts exhibited extraordinary stability and generality in the decontamination and disinfection of complex solution matrixes. Both experimental and theoretical calculation results demonstrated that graphitic N was the active site on N/C cocatalysts, which could elevate the reactivity of Fe(III) and make the interfacial electron transfer more feasible. In the N/C-mediated Fe(III)/H 2 O 2 system, an increase in electron transfer on the surface of N/C facilitated the formation of surface-bound Fe(II), thereby activating H 2 O 2 to produce hydroxyl radicals, the main active species for contaminant degradation. Notably, practical continuous water purification could be achieved by assembling N/C into fixed-bed reactors or membrane treatment units. These findings provide novel insights into N-doped carbonaceous cocatalysts and a promising green strategy for practical water treatment.

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Nitrogen-doped carbon nanotubes enhanced Fenton chemistry: Role of near-free iron(III) for sustainable iron(III)/iron(II) cycles

Cited by 90 publications

References 52 publications

Overcoming the Activity–Stability Trade-Off in Heterogeneous Electro-Fenton Catalysis: Encapsulating Carbon Cloth-Supported Iron Oxychloride within Graphitic Layers

Overcoming the Activity–Stability Trade-Off in Heterogeneous Electro-Fenton Catalysis: Encapsulating Carbon Cloth-Supported Iron Oxychloride within Graphitic Layers

Carbocatalysts for Enhancing Permanganate Oxidation of Sulfisoxazole

Eco-Friendly Lignin-Based N/C Cocatalysts for Ultrafast Cyclic Fenton-Like Reactions in Water Purification via Graphitic N-Mediated Interfacial Electron Transfer

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