Generating dual-active species by triple-atom sites through peroxymonosulfate activation for treating micropollutants in complex water

Proceedings of the National Academy of Sciences, Journal Year: 2023, Volume and Issue: 120(13)

Published: March 23, 2023

The peroxymonosulfate (PMS)-triggered radical and nonradical active species can synergistically guarantee selectively removing micropollutants in complex wastewater; however, realizing this on heterogeneous metal-based catalysts with single sites remains challenging due to insufficient electron cycle. Herein, we design asymmetric Co-O-Bi triple-atom Co-doped Bi2O2CO3 facilitate PMS oxidation reduction simultaneously by enhancing the transfer between sites. We propose that result an density increase Bi decrease Co sites, thereby undergoes a reaction generate SO4•- •OH at site 1O2 site. suggest synergistic effect of SO4•-, •OH, enables efficient removal mineralization without interference from organic inorganic compounds under environmental background. As result, achieves almost 99.3% sulfamethoxazole degradation 3 min k-value as high 82.95 min-1 M-1, which is superior existing reported so far. This work provides structural regulation approach control catalytic function, will guide rational Fenton-like catalysts.

Language: Английский

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A comprehensive review on persulfate activation treatment of wastewater

The Science of The Total Environment, Journal Year: 2022, Volume and Issue: 831, P. 154906 - 154906

Published: March 30, 2022

Language: Английский

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Outlook on Single Atom Catalysts for Persulfate-Based Advanced Oxidation

ACS ES&T Engineering, Journal Year: 2022, Volume and Issue: 2(10), P. 1776 - 1796

Published: Sept. 7, 2022

Single atom catalysts (SACs) have emerged as a promising catalyst material architecture for energy, chemical, and environmental applications. In the past several years, SACs been increasingly explored persulfate-based advanced oxidation processes (AOPs) due to their superior persulfate activation pollutant degradation performance compared benchmark dissolved ion nanoparticle catalysts. However, there still exist uncertainties on mechanism of by SACs, which involves complex interplay sulfate hydroxyl radicals, singlet oxygen, high-valent metal species, and/or mediated electron transfer. Questions also remain how ions molecularly align single site, are converted into reactive what design parameters lead higher efficiency degradation. this critical review, we examine SAC materials employed AOPs discuss they function differently counterparts. We further our discussion current limitations, opportunities, future research needs in (i) filling knowledge gaps mechanisms persulfate-SAC interactions; (ii) augmenting fundamental with theoretical simulation situ characterization techniques; (iii) improving tailored applications; (iv) proactively considering challenges associated engineering practices water matrixes.

Language: Английский

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Single-atom Mo–Co catalyst with low biotoxicity for sustainable degradation of high-ionization-potential organic pollutants

Proceedings of the National Academy of Sciences, Journal Year: 2023, Volume and Issue: 120(29)

Published: July 10, 2023

Single-atom catalysts (SACs) are a promising area in environmental catalysis. We report on bimetallic Co–Mo SAC that shows excellent performance activating peroxymonosulfate (PMS) for sustainable degradation of organic pollutants with high ionization potential (IP > 8.5 eV). Density Functional Theory (DFT) calculations and experimental tests demonstrate the Mo sites – Co SACs play critical role conducting electrons from to sites, leading 19.4-fold increase rate phenol compared CoCl 2 PMS group. The exhibit catalytic even under extreme conditions show long-term activation 10-d experiments, efficiently degrading 600 mg/L phenol. Moreover, catalyst has negligible toxicity toward MDA-MB-231, Hela, MCF-7 cells, making it an environmentally friendly option water treatment. Our findings have important implications design efficient remediation other applications biology medicine.

Language: Английский

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Switching of radical and nonradical pathways through the surface defects of Fe3O4/MoO S in a Fenton-like reaction

Science Bulletin, Journal Year: 2023, Volume and Issue: 68(6), P. 603 - 612

Published: Feb. 25, 2023

Language: Английский

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Site Engineering of Covalent Organic Frameworks for Regulating Peroxymonosulfate Activation to Generate Singlet Oxygen with 100 % Selectivity

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(43)

Published: Sept. 5, 2023

Singlet oxygen (1 O2 ) is an excellent reactive species (ROSs) for the selective conversion of organic matter, especially in advanced oxidation processes (AOPs). However, due to huge dilemma synthesizing single-site type catalysts, control and regulation 1 generation AOPs still challenging underlying mechanism remains largely obscure. Here, taking advantage well-defined flexibly tunable sites covalent frameworks (COFs), we report first achievement precisely regulating ROSs peroxymonosulfate (PMS)-based by site engineering COFs. Remarkably, COFs with bipyridine units (BPY-COFs) facilitate PMS activation via a nonradical pathway 100 % , whereas biphenyl-based (BPD-COFs) almost identical structures activate produce radicals (⋅OH SO4.- ). The BPY-COFs/PMS system delivers boosted performance degradation target pollutants from water, which ca. 9.4 times that its BPD-COFs counterpart, surpassing most reported PMS-based systems. Mechanism analysis indicated highly electronegative pyridine-N atoms on BPY-COFs provide extra adsorb terminal H PMS, resulting simultaneous adsorption O one pyridine ring, facilitates cleavage S-O bond generate .

Language: Английский

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Strategies based on electron donors to accelerate Fe(III)/Fe(II) cycle in Fenton or Fenton-like processes

Chemical Engineering Journal, Journal Year: 2022, Volume and Issue: 454, P. 140096 - 140096

Published: Nov. 1, 2022

Language: Английский

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Single-atom Ni-N4 sites coordinate dual nonradical oxidation pathways via peroxymonosulfate activation: Computational insights and in situ spectroscopic analyses

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 346, P. 123752 - 123752

Published: Jan. 21, 2024

In this work, we revealed a dual-pathway nonradical oxidation (NRO) system catalyzed by Ni single atom catalyst (NiN4) accommodated in the carbon nitride substrate. The monatomic coordinated with four N atoms (Ni-N4) is determined as dynamic catalytic center for peroxymonosulfate (PMS) activation, showing an exceptional specific rate constant of 3.34 min-1 g-2 L-2 (29.7 times that CN/PMS system) oxidizing bisphenol A and other refractory organics. situ Raman, X-ray absorption, electrochemical analyses well theoretical simulations demonstrate Ni-N4 sites exhibit strong interaction PMS benefited from modulated electronic structures, resulting surface-bonding active complexes (NiN4-PMS*) deuterogenic high-valent Ni(IV)-Oxo species. NRO process will spontaneously coordinate both electron transfer via CN matrix direct selective organic excellent anti-interference ability adaptability.

Language: Английский

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Wastewater flocculation substrate derived three-dimensional ordered macroporous Co single-atom catalyst for singlet oxygen-dominated peroxymonosulfate activation

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 335, P. 122886 - 122886

Published: May 19, 2023

Language: Английский

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Effective green treatment of sewage sludge from Fenton reactions: Utilizing MoS ₂ for sustainable resource recovery

Proceedings of the National Academy of Sciences, Journal Year: 2024, Volume and Issue: 121(9)

Published: Feb. 20, 2024

Effectively managing sewage sludge from Fenton reactions in an eco-friendly way is vital for technology’s viability pollution treatment. This study focuses on across various treatment stages, including generation, concentration, dehydration, and landfill, employs chemical composite MoS 2 to facilitate green resource utilization of all types sludge. , with exposed Mo 4+ low-coordination sulfur, enhances iron cycling creates acidic microenvironment the surface. The -modified exhibits outstanding (>95%) phenol pollutant degradation hydrogen peroxide peroxymonosulfate-based systems, unlike unmodified modified maintains excellent activity water conditions multiple anions, allowing extended over 14 d. Notably, generated oxygen demand (COD) modification process can be efficiently eliminated through reaction, ensuring effluent COD compliance enabling utilization.

Language: Английский

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