Rational Regulation of Co–N–C Coordination for High-Efficiency Generation of ¹O₂ toward Nearly 100% Selective Degradation of Organic Pollutants

Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(12), P. 8833 - 8843

Published: May 26, 2022

Single oxygen-based advanced oxidation processes (1O2-AOPs) exhibit great prospects in selective degradation of organic pollutants. However, efficient production 1O2 via tailored design catalysts to achieve contaminants remains challenging. Herein, we develop a simple strategy regulate the components and coordination Co–N–C at atomic level by adjusting Zn/Co ratio bimetallic zeolitic imidazolate frameworks (ZnxCo1-ZIFs). Zn4Co1–C demonstrates 98% removal phenol mixed phenol/benzoic acid (phenol/BA) solutions. Density functional theory calculations experiments reveal that more active CoN4 sites are generated Zn4Co1–C, which beneficial peroxymonosulfate activation generate 1O2. Furthermore, correlation between origin selectivity well-defined is systematically investigated electron paramagnetic resonance test quenching experiments. This work may provide novel insights into target pollutants complicated water matrix.

Language: Английский

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Fe, N-doped carbonaceous catalyst activating periodate for micropollutant removal: Significant role of electron transfer

Applied Catalysis B Environment and Energy, Journal Year: 2021, Volume and Issue: 303, P. 120880 - 120880

Published: Nov. 1, 2021

Language: Английский

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Oxygen doping of cobalt-single-atom coordination enhances peroxymonosulfate activation and high-valent cobalt–oxo species formation

Proceedings of the National Academy of Sciences, Journal Year: 2023, Volume and Issue: 120(16)

Published: April 11, 2023

The high-valent cobalt-oxo species (Co(IV)=O) is being increasingly investigated for water purification because of its high redox potential, long half-life, and antiinterference properties. However, generation Co(IV)=O inefficient unsustainable. Here, a cobalt-single-atom catalyst with N/O dual coordination was synthesized by O-doping engineering. O-doped (Co-OCN) greatly activated peroxymonosulfate (PMS) achieved pollutant degradation kinetic constant 73.12 min-1 g-2, which 4.9 times higher than that Co-CN (catalyst without O-doping) those most reported single-atom catalytic PMS systems. Co-OCN/PMS realized dominant oxidation pollutants increasing the steady-state concentration (1.03 × 10-10 M) 5.9 compared Co-CN/PMS. A competitive kinetics calculation showed contribution to micropollutant 97.5% during process. Density functional theory calculations influenced charge density (increased Bader transfer from 0.68 0.85 e), optimized electron distribution Co center d-band -1.14 -1.06 eV), enhanced adsorption energy -2.46 -3.03 eV, lowered barrier key reaction intermediate (*O*H2O) formation 1.12 0.98 eV. Co-OCN fabricated on carbon felt flow-through device, continuous efficient removal micropollutants (degradation efficiency >85% after 36 h operation). This study provides new protocol activation elimination through heteroatom-doping metal-oxo purification.

Language: Английский

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Sulfide-modified zero-valent iron activated periodate for sulfadiazine removal: Performance and dominant routine of reactive species production

Water Research, Journal Year: 2022, Volume and Issue: 220, P. 118676 - 118676

Published: May 26, 2022

Language: Английский

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Tetracycline degradation by peroxymonosulfate activated with CoNx active sites: Performance and activation mechanism

Chemical Engineering Journal, Journal Year: 2021, Volume and Issue: 431, P. 133477 - 133477

Published: Nov. 9, 2021

Language: Английский

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Recent advances in the applications of encapsulated transition-metal nanoparticles in advanced oxidation processes for degradation of organic pollutants: A critical review

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 342, P. 123401 - 123401

Published: Oct. 18, 2023

Language: Английский

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Single-Atom Cobalt Incorporated in a 2D Graphene Oxide Membrane for Catalytic Pollutant Degradation

Environmental Science & Technology, Journal Year: 2021, Volume and Issue: 56(2), P. 1341 - 1351

Published: Dec. 29, 2021

We introduce a new graphene oxide (GO)-based membrane architecture that hosts cobalt catalysts within its nanoscale pore walls. Such an would not be possible with in nanoscale, the current benchmark, since they block pores or alter structure. Therefore, we developed synthesis procedure to load atomically dispersed fashion, theoretical limit material downsizing. The use of vitamin C as mild reducing agent was critical Co atoms (Co1), preserving well-stacked 2D structure GO layers. With addition peroxymonosulfate (PMS), Co1-GO efficiently degraded 1,4-dioxane, small, neutral pollutant passes through nanopores single-pass treatment. observed 1,4-dioxane degradation kinetics were much faster (>640 times) than suspension and highest among reported persulfate-based destruction. capability reject large organic molecules alleviated their effects on radical scavenging. Furthermore, advanced oxidation also mitigated fouling. findings this study present advance toward developing catalytic membranes which two distinctive complementary processes, filtration oxidation, can combined into single-step

Language: Английский

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Facilitating Redox Cycles of Copper Species by Pollutants in Peroxymonosulfate Activation

Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(4), P. 2637 - 2646

Published: Jan. 28, 2022

The redox behavior of metal active sites determines the rate heterogeneous catalysis in peroxymonosulfate activation. Previous reports focused on construction catalysts for accelerating interfacial electron transfer. In this work, a new strategy was proposed facilitating valence cycles Cu+/Cu2+ by using pollutants. 2.5Cu/CeO2/PMS system capable achieving efficient removal pollutants, including tetracycline, oxytetracycline, and rhodamine B, wide pH working range. presence Cu-N bond formed between -NH2 group tetracycline Cu site catalyst, showing that coordination changed to CuO4N1. charge CuO4N1 rearranged, making it easier obtain electrons promote PMS oxidation, thereby reduction Cu2+ Cu+ activation showed excellent sustainability selectivity organic This study provides novel routine utilizing pollutants accelerate species.

Language: Английский

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Rational design of donor-acceptor conjugated polymers with high performance on peroxydisulfate activation for pollutants degradation

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 316, P. 121611 - 121611

Published: June 9, 2022

Language: Английский

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Catalyst-Free Periodate Activation by Solar Irradiation for Bacterial Disinfection: Performance and Mechanisms

Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(7), P. 4413 - 4424

Published: March 22, 2022

Periodate (PI)-based advanced oxidation process has recently attracted great attention in the water treatment processes. In this study, solar irradiation was used for PI activation to disinfect waterborne bacteria. The PI/solar system could inactivate Escherichia coli below limit of detection (LOD, 10 CFU mL-1) with initial concentrations 1 × 106, 107, and 108 mL-1 within 20, 40, 100 min, respectively. •O2- •OH radicals contributed bacterial disinfection. These reactive attack penetrate cell membrane, thereby increasing amount intracellular oxygen species destroying defense system. damage membrane caused leakage K+ DNA (that be eventually degraded). Excellent disinfection performance systems achieved a wide range solution pH (3-9), coexisting humic acid (0.1-10 mg L-1) broad ionic strengths (15-600 mM). also efficiently Gram-positive Bacillus subtilis. Moreover, activated by natural sunlight 107 viable E. LOD river sea waters working volume L 40 50 Clearly, potentially applied bacteria water.

Language: Английский

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