Simultaneously accelerating the regeneration of FeII and the selectivity of 2e- oxygen reduction over sulfide iron-based carbon aerogel in electro-Fenton system

Tian, Qingling; Xiao, Fan; Zhao, Hongying; Fei, Xianbin; Shen, Xuqian; Postole, G.; Zhao, Guohua

doi:10.1016/j.apcatb.2020.119039

Cited by 79 publications

(25 citation statements)

References 59 publications

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“…The ESR experiments were conducted to reveal the continuous ·OH generation performance of Fe 2+ /NDCA-EF and Fe 2+ /H 2 O 2 -F systems. As shown in Figure c, the specific quartet line with an intensity of 1:2:2:1 was detected in both EF (above) and F (below) systems, corresponding to the DMPO-•OH adduct. , In the Fe 2+ /NDCA-EF system, the production of ·OH was promoted with an increasing reaction time to 60 min, revealing the continuous regeneration of Fe 2+ in the presence of the NDCA cathode. In contrast, in the Fe 2+ /H 2 O 2 -F process, the intensity of DMPO-•OH decreased since Fe 2+ could not be efficiently regenerated.…”

Section: Resultsmentioning

confidence: 85%

“…As shown in Figure 1c, the specific quartet line with an intensity of 1:2:2:1 was detected in both EF (above) and F (below) systems, corresponding to the DMPO-•OH adduct. 42,43 In the Fe 2+ /NDCA-EF system, the production of •OH was promoted with an increasing reaction time to 60 min, revealing the continuous regeneration of Fe 2+ in the presence of the NDCA cathode. In contrast, in the Fe 2+ / The evolution of iron species was detected to investigate the role of NDCA cathode in Fe 2+ regeneration.…”

Section: ■ Results and Discussionmentioning

confidence: 96%

“…Detoxification of the DMP solution was achieved after 90 min, which was confirmed by the quickly decreasing inhibition ratio from initial 50.1% to zero.The ESR experiments were conducted to reveal the continuous •OH generation performance of Fe 2+ /NDCA-EF and Fe 2+ /H 2 O 2 -F systems. As shown in Figure1c, the specific quartet line with an intensity of 1:2:2:1 was detected in both EF (above) and F (below) systems, corresponding to the DMPO-•OH adduct 42,43. In the Fe 2+ /NDCA-EF system, the production of •OH was promoted with an increasing reaction time to 60 min, revealing the continuous regeneration of Fe 2+ in the presence of the NDCA cathode.…”

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confidence: 84%

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Accelerated Fe²⁺ Regeneration in an Effective Electro-Fenton Process by Boosting Internal Electron Transfer to a Nitrogen-Conjugated Fe(III) Complex

Liu

Feng

Luan

et al. 2021

Environ. Sci. Technol.

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171

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The regeneration rate of Fe 2+ from Fe 3+ dictates the performance of the electro-Fenton (EF) process, represented by the amount of produced hydroxyl radicals (•OH). Current strategies for the acceleration of Fe 2+ regeneration normally require additional chemical reagents, to vary the redox potential of Fe 2+ /Fe 3+ . Here, we report an attempt at using the intrinsic property of the electrode to our advantage, i.e., nitrogen-doped carbon aerogel (NDCA), as a reducing agent for the regeneration of Fe 2+ without using foreign reagents. Moreover, the pyrrolic N in NDCA provides unpaired electrons through the carbon framework to reduce Fe 3+ , while the graphitic and pyridinic N coordinate with Fe 3+ to form a C−O−Fe− N 2 bond, facilitating electron transfer from both the external circuit and pyrrolic N to Fe 3+ . Our Fe 2+ /NDCA-EF system exhibits a 5.8 ± 0.3 times higher performance, in terms of the amount of generated •OH, than a traditional Fenton system using the same Fe 2+ concentration. In the subsequent reaction, the Fe 2+ /NDCA-EF system demonstrates 100.0% removal of dimethyl phthalate, 3chlorophenol, bisphenol A, and sulfamethoxazole with a low specific energy consumption of 0.17−0.36 kW•h•g −1 . Furthermore, 90.1 ± 0.6% removal of dissolved organic carbon and 83.3 ± 0.9% removal of NH 3 -N are achieved in the treatment of domestic sewage. The purpose of this work is to present a novel strategy for the regeneration of Fe 2+ in the EF process and also to elucidate the role of different N species of the carbonaceous electrode in contributing to the redox cycle of Fe 2+ /Fe 3+ .

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Section: Resultsmentioning

confidence: 85%

Section: ■ Results and Discussionmentioning

confidence: 96%

mentioning

confidence: 84%

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Accelerated Fe²⁺ Regeneration in an Effective Electro-Fenton Process by Boosting Internal Electron Transfer to a Nitrogen-Conjugated Fe(III) Complex

Liu

Feng

Luan

et al. 2021

Environ. Sci. Technol.

Self Cite

171

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“…Another possibility for the performance decline is that the generated H 2 O 2 was further chemically reduced, especially for Fe-based catalysts. As heterogenous Fenton has been reported on the Fe compound-functionalized carbonaceous catalysts, [203,204] Fe contamination combined with • OH radical etch finally causes the severe decay of H 2 O 2 yields. Therefore, in addition to avoiding using materials containing Fe and reducing Fe contamination, introducing radical scavengers (e.g., N-oxides or peracids) may be an effective strategy to inhibit these deleterious radicals and cascade reactions.…”

Section: Catalyst Degradation Caused By Produced H 2 Omentioning

confidence: 99%

Tuning Two‐Electron Oxygen‐Reduction Pathways for H₂O₂ Electrosynthesis via Engineering Atomically Dispersed Single Metal Site Catalysts

et al. 2022

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The hydrogen peroxide (H2O2) generation via the electrochemical oxygen reduction reaction (ORR) under ambient conditions is emerging as an alternative and green strategy to the traditional energy‐intensive anthraquinone process and unsafe direct synthesis using H2 and O2. It enables on‐site and decentralized H2O2 production using air and renewable electricity for various applications. Currently, atomically dispersed single metal site catalysts have emerged as the most promising platinum group metal (PGM)‐free electrocatalysts for the ORR. Further tuning their central metal sites, coordination environments, and local structures can be highly active and selective for H2O2 production via the 2e− ORR. Herein, recent methodologies and achievements on developing single metal site catalysts for selective O2 to H2O2 reduction are summarized. Combined with theoretical computation and advanced characterization, a structure–property correlation to guide rational catalyst design with a favorable 2e− ORR process is aimed to provide. Due to the oxidative nature of H2O2 and the derived free radicals, catalyst stability and effective solutions to improve catalyst tolerance to H2O2 are emphasized. Transferring intrinsic catalyst properties to electrode performance for viable applications always remains a grand challenge. The key performance metrics and knowledge during the electrolyzer development are, therefore, highlighted.

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“…As the transition metals species immobilized on the surface of heterogeneous EF catalysts in solid form, both the catalytic formation and decomposition of H 2 O 2 mainly occur on the liquid-solid interfaces of catalysts. [8] Within this context, the heterogeneous EF catalysts require considerable activity for both H 2 O 2 generation and decomposition, [9][10][11] which consequently increase the difficulty in catalyst design and fabrication due to the higher structural complexity of the catalyst. Currently, carbon matrix (C) supported transition metal (TM) materials (TM/C) still majored in the preparation of heterogeneous EF catalyst , [12][13][14] where TM and carbon matrix could serves as the heterogeneous Fenton and 2e − oxygen reduction reaction (ORR) actives sites, [15] respectively.…”

Section: Ho Ohmentioning

confidence: 99%

Hierarchical Iron Phosphides Composite Confined in Ultrathin Carbon Layer as Effective Heterogeneous Electro‐Fenton Catalyst with Prominent Stability and Catalytic Activity

Cheng

Zheng

Shen

et al. 2021

Adv Funct Materials

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The heterogeneous electro-Fenton (EF) process is a promising wastewater treatment technology for the onsite production of H 2 O 2 and avoidance of iron sludge. However, the preparation of the cathode catalysts remains a challenge. Not only must the catalyst surface possesses active sites for both 2e − oxygen reduction reaction and heterogeneous Fenton reaction, preventing active metals from continuous leaching is also crucial to maintain its catalytic activity. Herein, a heterogeneous catalyst (rGO@Fe x P/C) with a vacuumized package-like structure, where carbon-supported iron phosphides (Fe x P/C) are tightly covered within interconnected reduced graphene oxide (rGO) sheets, is successfully prepared. The concentration of iron that dissolved from rGO@ Fe x P/C after the reaction is only 3.37% of bare Fe x P/C (14.6 mg L −1 ), while rGO@Fe x P/C achieves better performance towards sulfamethoxazole (10 mg L −1 ) degradation than Fe x P/C. Investigation on rGO@Fe x P/C with different thicknesses of outer rGO layer and diverse morphologic structures demonstrate that the unique structure of rGO@Fe x P/C played a decisive role in the simultaneously enhanced activity and stability.

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Simultaneously accelerating the regeneration of FeII and the selectivity of 2e- oxygen reduction over sulfide iron-based carbon aerogel in electro-Fenton system

Cited by 79 publications

References 59 publications

Accelerated Fe²⁺ Regeneration in an Effective Electro-Fenton Process by Boosting Internal Electron Transfer to a Nitrogen-Conjugated Fe(III) Complex

Accelerated Fe²⁺ Regeneration in an Effective Electro-Fenton Process by Boosting Internal Electron Transfer to a Nitrogen-Conjugated Fe(III) Complex

Tuning Two‐Electron Oxygen‐Reduction Pathways for H₂O₂ Electrosynthesis via Engineering Atomically Dispersed Single Metal Site Catalysts

Hierarchical Iron Phosphides Composite Confined in Ultrathin Carbon Layer as Effective Heterogeneous Electro‐Fenton Catalyst with Prominent Stability and Catalytic Activity

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Simultaneously accelerating the regeneration of FeII and the selectivity of 2e- oxygen reduction over sulfide iron-based carbon aerogel in electro-Fenton system

Cited by 79 publications

References 59 publications

Accelerated Fe2+ Regeneration in an Effective Electro-Fenton Process by Boosting Internal Electron Transfer to a Nitrogen-Conjugated Fe(III) Complex

Accelerated Fe2+ Regeneration in an Effective Electro-Fenton Process by Boosting Internal Electron Transfer to a Nitrogen-Conjugated Fe(III) Complex

Tuning Two‐Electron Oxygen‐Reduction Pathways for H2O2 Electrosynthesis via Engineering Atomically Dispersed Single Metal Site Catalysts

Hierarchical Iron Phosphides Composite Confined in Ultrathin Carbon Layer as Effective Heterogeneous Electro‐Fenton Catalyst with Prominent Stability and Catalytic Activity

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Accelerated Fe²⁺ Regeneration in an Effective Electro-Fenton Process by Boosting Internal Electron Transfer to a Nitrogen-Conjugated Fe(III) Complex

Accelerated Fe²⁺ Regeneration in an Effective Electro-Fenton Process by Boosting Internal Electron Transfer to a Nitrogen-Conjugated Fe(III) Complex

Tuning Two‐Electron Oxygen‐Reduction Pathways for H₂O₂ Electrosynthesis via Engineering Atomically Dispersed Single Metal Site Catalysts