Highly efficient degradation of emerging contaminants by magnetic CuO@FexOy derived from natural mackinawite (FeS) in the presence of peroxymonosulfate

RuoHan, Zhang; Chen, Maolian; Xiong, Zhaokun; Guo, Yong; Lai, Bo

doi:10.1016/j.cclet.2021.07.029

Cited by 45 publications

(7 citation statements)

References 26 publications

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“…Furthermore, 5,5-dimethyl-1-pyrroline- N -oxide (DMPO) and 2,2,6,6-tetramethyl-4-piperidinyloxy (TEMP) were selected as trapping agents for radicals ( • OH and SO 4 •– ) and 1 O 2 , respectively. – Signals of • OH and SO 4 •– in all Fe–N x C 4– x /PMS systems were negligible (Figure S27), confirming the absence of radicals. When TEMP was added, an enhanced triplet EPR signal ascribed to 1 O 2 emerged in all Fe–N x C 4– x /PMS systems but was low-intensity in control systems (Figure g,h), demonstrating the generation of 1 O 2 .…”

Section: Resultsmentioning

confidence: 79%

Facilely Tuning the First-Shell Coordination Microenvironment in Iron Single-Atom for Fenton-like Chemistry toward Highly Efficient Wastewater Purification

Wu,

Huang,

Wang

et al. 2023

Environ. Sci. Technol.

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Precisely identifying the atomic structures in single-atom sites and establishing authentic structure–activity relationships for single-atom catalyst (SAC) coordination are significant challenges. Here, theoretical calculations first predicted the underlying catalytic activity of Fe–N x C4–x sites with diverse first-shell coordination environments. Substituting N with C to coordinate with the central Fe atom induces an inferior Fenton-like catalytic efficiency. Then, Fe-SACs carrying three configurations (Fe–N2C2, Fe–N3C1, and Fe–N4) fabricate facilely and demonstrate that optimized coordination environments of Fe–N x C4–x significantly promote the Fenton-like catalytic activity. Specifically, the reaction rate constant increases from 0.064 to 0.318 min–1 as the coordination number of Fe–N increases from 2 to 4, slightly influencing the nonradical reaction mechanism dominated by 1O2. In-depth theoretical calculations unveil that the modulated coordination environments of Fe-SACs from Fe–N2C2 to Fe–N4 optimize the d-band electronic structures and regulate the binding strength of peroxymonosulfate on Fe–N x C4–x sites, resulting in a reduced energy barrier and enhanced Fenton-like catalytic activity. The catalytic stability and the actual hospital sewage treatment capacity also showed strong coordination dependency. This strategy of local coordination engineering offers a vivid example of modulating SACs with well-regulated coordination environments, ultimately maximizing their catalytic efficiency.

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Section: Resultsmentioning

confidence: 79%

Facilely Tuning the First-Shell Coordination Microenvironment in Iron Single-Atom for Fenton-like Chemistry toward Highly Efficient Wastewater Purification

Wu,

Huang,

Wang

et al. 2023

Environ. Sci. Technol.

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“…To investigate the reaction pathway and mechanism, we employed free radical scavenging experiments to determine the types of generated ROS during PMS activation. The effects of radical scavengers including tert -butyl alcohol (TBA, the probe for • OH), methanol (MeOH, the probe for • OH and SO 4 •– ), superoxide dismutase (SOD, the probe for O 2 •– ), dimethyl sulfoxide (DMSO, the probe for Co(IV)O), furfuryl alcohol (FFA), and β-carotene (the probe for 1 O 2 ) were used to investigate the presence of various ROS. − The reaction of different scavengers with PMS is shown in Figure S13, and the rate constants for the probe compounds with different ROS are listed in Table S4. As shown in Figures e and S14, there was little influence in the presence of TBA and MeOH compared with the control condition, indicating that • OH and SO 4 •– were hardly produced during the reaction.…”

Section: Resultsmentioning

confidence: 99%

Modulating Electronic Structure Engineering of Atomically Dispersed Cobalt Catalyst in Fenton-like Reaction for Efficient Degradation of Organic Pollutants

Huang,

Ren,

Zhao

et al. 2023

Environ. Sci. Technol.

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Currently, the lack of model catalysts limits the understanding of the catalytic essence. Herein, we report the functional group modification of model single atom catalysts (SACs) with an accurately regulated electronic structure for accelerating the sluggish kinetics of the Fenton-like reaction. The amino-modified cobalt phthalocyanine anchored on graphene (CoPc/G-NH2) shows superior catalytic performance in the peroxymonosulfate (PMS) based Fenton-like reaction with Co mass-normalized pseudo-first-order reaction rate constants (k obs, 0.2935 min –1 ), which is increased by 4 and 163 times compared to those of CoPc/G (0.0737 min –1 ) and Co3O4/G (0.0018 min –1 ). Density functional theory (DFT) calculations demonstrate that the modification of the −NH2 group narrows the gap between the d-band center and the Fermi level of a single Co atom, which strengthens the charge transfer rate at the reaction interface and reduces the free energy barrier for the activation of PMS. Moreover, the scale-up experiment realizes 100% phenol removal at 7200-bed volumes during 240 h continuous operation without obvious decline in catalytic performance. This work provides in-depth insight into the catalytic mechanism of Fenton-like reactions and demonstrates the electronic engineering of SACs as an effective strategy for improving the Fenton-like activity to achieve the goal of practical application.

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“…At present, the common water treatment technologies are mainly physical separation (adsorption and membrane separation), biodegradation (membrane bioreactor), chemical oxidation (ozone oxidation, Fenton oxidation, etc. ), and their coupling technologies. − Among them, the adsorption method is mild and simple to apply, but it can only separate pollutants and cannot degrade them . Membrane separation and membrane bioreactor are effective but both are prone to membrane fouling and cannot be used for a long time .…”

Section: Application Of Fe–mn-based Materials In Wastewater Decontami...mentioning

confidence: 99%

Synthesis of Fe–Mn-Based Materials and Their Applications in Advanced Oxidation Processes for Wastewater Decontamination: A Review

Dong

Shi

et al. 2023

Ind. Eng. Chem. Res.

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With the development of industry and agriculture, the increasingly serious problems of environmental pollution and water quality deterioration that affect human health need to be solved. Materials containing both Fe and Mn, the two most abundant metal elements, have been widely used for wastewater decontamination since they are nontoxic, low-cost, easy to prepare, and highly efficient. This review systematically summarizes the synthesis methods of Fe–Mn-based unloaded materials (such as spinel-type, perovskite-type, layered double hydroxides, metal–organic framework, and its derivatives) and loaded materials (carbon materials, oxides, and other loaded materials). Furthermore, the progress and problems of the application of Fe–Mn-based materials in the fields of Fenton, photo-Fenton, electro-Fenton, persulfate, and sulfite catalysis processes are analyzed. Different activation mechanisms of Fe–Mn-based materials, such as radical pathways and nonradical pathways (like direct electron transfer pathways, singlet oxygen, and high valence metals, etc.) are described. Finally, the application potential of Fe–Mn-based materials in environmental remediation is clarified and the future research directions are pointed out. It is expected that this review can provide new inspiration for subsequent research on the application of Fe–Mn based materials for wastewater treatment.

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Highly efficient degradation of emerging contaminants by magnetic CuO@FexOy derived from natural mackinawite (FeS) in the presence of peroxymonosulfate

Cited by 45 publications

References 26 publications

Facilely Tuning the First-Shell Coordination Microenvironment in Iron Single-Atom for Fenton-like Chemistry toward Highly Efficient Wastewater Purification

Facilely Tuning the First-Shell Coordination Microenvironment in Iron Single-Atom for Fenton-like Chemistry toward Highly Efficient Wastewater Purification

Modulating Electronic Structure Engineering of Atomically Dispersed Cobalt Catalyst in Fenton-like Reaction for Efficient Degradation of Organic Pollutants

Synthesis of Fe–Mn-Based Materials and Their Applications in Advanced Oxidation Processes for Wastewater Decontamination: A Review

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