Rapid pollutant degradation by peroxymonosulfate <i>via</i> an unusual mediated-electron transfer pathway under spatial-confinement

Shao, Siting; Cui, Jiahao; Li, Lina; Wang, Mingqi; Zhang, Peng; Cui, Jianguo; Hu, Chun; Zhao, Yubao

doi:10.1039/d1ra08954d

Cited by 9 publications

(10 citation statements)

References 66 publications

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“…The spike of BPA in the reaction system might modify the electron transfer pathway: in the absence of BPA, there was direct electron transfer between nanoconfined Co 0 and PMS, leading to the diffusion of Co 2+ into the solvent, while in the presence of BPA, the nanoconfined Co nanocrystal was no longer the electron donor, but it might have switched to a new role of electron mediator, transferring the electrons coming from BPA to PMS. The attenuated PMS decomposition in the presence of pollutants was also observed in other Cu- and Co-catalyzed reaction systems. , Meanwhile, the oxidation states of Co in Co- i -CNC after the reaction was evaluated by XPS (Figure S10). The binding energy of Co 2p 3/2 electron was slightly higher than that of the fresh catalyst, for example, 778 and 780.3 eV for the fresh and spent catalyst, respectively.…”

Section: Resultsmentioning

confidence: 75%

“…The attenuated PMS decomposition in the presence of pollutants was also observed in other Cu-and Co-catalyzed reaction systems. 59,60 Meanwhile, the oxidation states of Co in Co-i-CNC after the reaction was evaluated by XPS (Figure S10). The binding energy of Co 2p 3/2 electron was slightly higher than that of the fresh catalyst, for example, 778 and 780.3 eV for the fresh and spent catalyst, respectively.…”

Section: Mechanistic Insights Into Pms Activation Over Co-i-cnc and C...mentioning

confidence: 99%

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Nanoconfinement-Regulated Peroxymonosulfate Activation via an Anomalously Efficient Mediated Electron-Transfer Pathway on Cobalt

Cui

Shao

et al. 2022

ACS EST Eng.

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In a nanoconfined space, the chemical/physical properties of molecules/ions can be fundamentally changed; the strategy of nanoconfinement thus offers rich opportunities for the development of an efficient catalytic process. Peroxymonosulfate (PMS) involved in advanced oxidation processes is a promising technology for efficient abatement of recalcitrant pollutants. Radical, singlet oxygen, and high-valent cobalt species are, hitherto, reckoned as the predominant reactive species for pollutant degradation in cobalt-catalyzed reaction systems. Herein, a distinctive mediated electron-transfer mechanism of cobalt was substantiated in a nanoconfined space. Moreover, an unusual pollutant-dependent PMS consumption behavior was revealed; the presence of pollutant unexpectedly attenuated the PMS consumption, which was contrary to the knowledge in the usual mediated electron-transfer mechanism of noble metals or carbon. By nanoconfinement regulation, the reaction system afforded an unprecedently efficient catalytic performance for pollutant degradation, for example, rapid elimination of bisphenol A and 2-chlorophenol with a high concentration of 100 ppm within 1 min and 40 s, respectively.

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Section: Resultsmentioning

confidence: 75%

Section: Mechanistic Insights Into Pms Activation Over Co-i-cnc and C...mentioning

confidence: 99%

Nanoconfinement-Regulated Peroxymonosulfate Activation via an Anomalously Efficient Mediated Electron-Transfer Pathway on Cobalt

Cui

Shao

et al. 2022

ACS EST Eng.

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“…Ibuprofen, a nonsteroidal anti-inflammatory drug with an electron-withdrawing group connected to the aromatic ring, shows stronger resistance to oxidation . On m-CN, there is almost no degradation performance under visible light in the presence of O 2 , while in the presence of 5 ppm of O 3 in O 2 , ibuprofen could be eliminated in 120 min, affording a pseudo-first-order reaction rate constant of 0.0283 min –1 .…”

Section: Resultsmentioning

confidence: 99%

Polymeric Carbon Nitride from Inorganic Precursor in Eutectic Salts: Enhanced Exciton Dissociation and Photocatalytic H₂O₂ Production

Zeng

Yang

et al. 2022

J. Phys. Chem. C

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Photocatalysis is one of the environmental-friendly approaches toward the sustainable production of the versatile hydrogen peroxide. Polymeric carbon nitride (PCN) frameworks are especially favorable for the photocatalytic 2e– oxygen reduction reaction. High crystallinity of the PCN is favorable for enhancing the solar-to-chemical conversion efficiency. Employing the ionic compound of ammonium thiocyanate (NH4SCN) as the precursor, the crystallinity of AT-CN was significantly improved as compared to its counterpart synthesized with the organic melamine as the precursor (m-CN). Spectroscopic investigations revealed that the exciton dissociation was remarkably enhanced for the crystalline AT-CN. AT-CN thus exhibited remarkable photocatalytic performance in the H2O2 production and pollutant degradation. This work demonstrates a novel approach of tuning the miscibility of the precursor in the molten salt for enhancing the crystallinity of the polymeric carbon nitride framework.

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“…The solution with 10 ppm BPA and 0.5 mM PMS was pumped into the reactor by a peristaltic pump, and the flow rate was 24 mL h –1 . The effluent was sampled at a specified interval and mixed with an equal amount of methanol for analysis. , …”

Section: Methodsmentioning

confidence: 99%

Efficient and Durable Single-Atom Fe Catalyst for Fenton-like Reaction via Mediated Electron-Transfer Mechanism

et al. 2022

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Efficient approaches toward selective removal of the emerging organic pollutants are of critical importance to the well-being of the human health and the eco-system. Peroxymonosulfate-involved advanced oxidation process is promising in water treatment due to a couple of intrinsic advantages of the reaction system, and the development of an efficient catalyst is essential to the real application of this technique. In this work, a series of single-atom Fe catalysts were fabricated via a facile method, and the single-atom center was identified to be in a Fe–N4 configuration by Fe K-edge X-ray absorption spectroscopy. On the optimum catalyst with 4.8 wt % Fe single atom, 22 ppm BPA could be eliminated within 40 s under mild reaction conditions, affording a remarkable pseudo-first-order reaction rate constant of 8.4 min–1. The durability of the catalyst was tested with a fixed-bed flow reactor, and 55.2 L of polluted water with 10 ppm BPA could be treated with a removal rate of >95% by 1 g of catalyst. Through a series of probe reactions and spectroscopic analysis, the mediated electron-transfer mechanism was identified to be dominant during the pollutant degradation process.

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Rapid pollutant degradation by peroxymonosulfate via an unusual mediated-electron transfer pathway under spatial-confinement

Abstract: A highly efficient mediated-electron transfer process of PMS activation on Co was achieved by construction of a spatially-confined reaction environment.

Cited by 9 publications

References 66 publications

Nanoconfinement-Regulated Peroxymonosulfate Activation via an Anomalously Efficient Mediated Electron-Transfer Pathway on Cobalt

Nanoconfinement-Regulated Peroxymonosulfate Activation via an Anomalously Efficient Mediated Electron-Transfer Pathway on Cobalt

Polymeric Carbon Nitride from Inorganic Precursor in Eutectic Salts: Enhanced Exciton Dissociation and Photocatalytic H₂O₂ Production

Efficient and Durable Single-Atom Fe Catalyst for Fenton-like Reaction via Mediated Electron-Transfer Mechanism

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Rapid pollutant degradation by peroxymonosulfate via an unusual mediated-electron transfer pathway under spatial-confinement

Abstract: A highly efficient mediated-electron transfer process of PMS activation on Co was achieved by construction of a spatially-confined reaction environment.

Cited by 9 publications

References 66 publications

Nanoconfinement-Regulated Peroxymonosulfate Activation via an Anomalously Efficient Mediated Electron-Transfer Pathway on Cobalt

Nanoconfinement-Regulated Peroxymonosulfate Activation via an Anomalously Efficient Mediated Electron-Transfer Pathway on Cobalt

Polymeric Carbon Nitride from Inorganic Precursor in Eutectic Salts: Enhanced Exciton Dissociation and Photocatalytic H2O2 Production

Efficient and Durable Single-Atom Fe Catalyst for Fenton-like Reaction via Mediated Electron-Transfer Mechanism

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Product

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Polymeric Carbon Nitride from Inorganic Precursor in Eutectic Salts: Enhanced Exciton Dissociation and Photocatalytic H₂O₂ Production