A carbon nanotube-confined iron modified cathode with prominent stability and activity for heterogeneous electro-Fenton reactions

Su, Pei; Zhou, Minghua; Ren, Gang; Lu, Xiaoye; Du, Xuedong; Song, Ge

doi:10.1039/c9ta07491k

Cited by 92 publications

(42 citation statements)

References 68 publications

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“…For traditional TM/C catalysts, TM species are directly exposed to the electrolyte, catalysts are vulnerable to deactivation due to the oxidation, shedding, or dissolution of TM species. [ 20 ] Therefore, it is crucial to develop heterogeneous EF catalysts with prominent chemical and physical stability.…”

Section: Introductionmentioning

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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Section: Introductionmentioning

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 contribution of Cu(II) was not only attributed to decomposition of H 2 O 2 but also to the reaction of Cu(I) with Fe(III) resulting in Cu(II) and Fe(II) due to the difference in electrochemical potential of these atoms [70,73]. This mechanism was adapted from J. Wang et al [73] that proposed this sequence of reactions while working with a bimetallic heterogeneous catalyst mainly composed by zero-valent iron and zero-valent copper, which are highly reactive in comparison to iron oxides [74]. Then, the role of Cu(II) as an electron transfer to Fe(III)/Fe(II) sites for reduction of Fe(III) to Fe(II) in the surface seems to be essential in this setting for successful heterogeneous generation of •OH radical in the particles.…”

Section: Heterogeneous Catalyst As Particlesmentioning

confidence: 99%

“…The coating of the cathode with a solid catalyst combines convenience of heterogeneous process, such as extended range of working pH and reuse of catalyst with possible enhancement in the electroactivity of the cathode and then in the performance of electro-mediated oxidation of pollutants in the heterogeneous electro-Fenton systems. Most of the studies are based on coating the cathode with a secondary iron-supporting material such as iron minerals (pyrite [77], magnetite [78][79][80] and hematite [15,81,82]), zero-valent iron nanoparticles [74], chitosan [83] or zeolite [84] impregnated with iron oxide. More recently, cathodic materials with a three-dimensional porous structure able to support iron oxides in their composition referred to as Fe-carbon aerogel achieved remarkable performance in the degradation of pollutants under circumneutral conditions, but their multistep preparation involving complex techniques, such as supercritical drying, still prevents their practical application as a heterogeneous catalyst in the electro-Fenton process [14,15].…”

Section: Heterogeneous Catalyst Upon Cathodementioning

confidence: 99%

Review: Clay-Modified Electrodes in Heterogeneous Electro-Fenton Process for Degradation of Organic Compounds: The Potential of Structural Fe(III) as Catalytic Sites

et al. 2021

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Advanced oxidation processes are considered as a promising technology for the removal of persistent organic pollutants from industrial wastewaters. In particular, the heterogeneous electro-Fenton (HEF) process has several advantages such as allowing the working pH to be circumneutral or alkaline, recovering and reusing the catalyst and avoiding the release of iron in the environment as a secondary pollutant. Among different iron-containing catalysts, studies using clay-modified electrodes in HEF process are the focus in this review. Fe(III)/Fe(II) within the lattice of clay minerals can possibly serve as catalytic sites in HEF process. The description of the preparation and application of clay-modified electrodes in the degradation of model pollutants in HEF process is detailed in the review. The absence of mediators responsible for transferring electrons to structural Fe(III) and regenerating catalytic Fe(II) was considered as a milestone in the field. A comprehensive review of studies investigating the use of electron transfer mediators as well as the mechanism behind electron transfer from and to the clay mineral structure was assembled in order to uncover other milestones to be addressed in this study area.

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“…The calculations were performed in the density functional theory (DFT) with the DMol 3 package [35,36] using the GGA-PBE method [37,38], which can successfully consider the weak interactions between chemical functional groups. Considering the relativistic effects, the functional semicore pseudopotential (DSPP) was employed for the Fe, Co and Ni atom and other nonmetal atoms were used by all-electron basis sets.…”

Section: Computational Detailsmentioning

confidence: 99%

Theoretical Study on the Structures of Single-Atom M (M=Fe, Co and Ni) Adsorption Outside and Inside the Defect Carbon Nanotubes

Wang

Nan

Liu

et al. 2021

Preprint

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Single-atom confinement inside carbon nanotubes has attracted much attention in many fields. This class of materials may not only serve as a catalyst but also as a support material for certain reactions. In this paper, we have studied the single-walled carbon nanotubes (SWCNT), single vacancy defect (SV) and Stone-Wales defect (SW) carbon nanotubes with Fe, Co and Ni atom by both inside and outside adsorption structures in density function theory (DFT). Our results reveal that the binding abilities of atomic Fe, Co, Ni onto the internal and external surfaces of the SWCNT, SV and SW are in following orders by metals: Ni>Co>Fe. The adsorption energies of SV toward Fe, Co and Ni are more stable than those of SWCNT and SW, which can be attributed to the three active carbon sites created by a C atom removing, while the SWCNT and SW demonstrate similar adsorption energy due to the similar structure. Generally, the stability of external adsorption structures is stronger than those of internal adsorption structures, but as for the SW, the stability of internal and external adsorption structures is close, which means that the defects have improved the confinement of carbon nanotubes to M (M=Fe, Co Ni).

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A carbon nanotube-confined iron modified cathode with prominent stability and activity for heterogeneous electro-Fenton reactions

Abstract: We demonstrate the importance of confinement catalysis in selectively controlling the position and valence of iron on CNTs, which could effectively increase heterogeneous electro-Fenton activity and decrease iron leaching to improve cathode stability.

Cited by 92 publications

References 68 publications

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

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

Review: Clay-Modified Electrodes in Heterogeneous Electro-Fenton Process for Degradation of Organic Compounds: The Potential of Structural Fe(III) as Catalytic Sites

Theoretical Study on the Structures of Single-Atom M (M=Fe, Co and Ni) Adsorption Outside and Inside the Defect Carbon Nanotubes

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