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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Long‐Range Interactions in Diatomic Catalysts Boosting Electrocatalysis

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(52)

Published: Oct. 6, 2022

Abstract The simultaneous presence of two active metal centres in diatomic catalysts (DACs) leads to the occurrence specific interactions between sites. Such interactions, referred as long‐range (LRIs), play an important role determining rate and selectivity a reaction. optimal combination must be determined achieve targeted efficiency. To date, various types DACs have been synthesised applied electrochemistry. However, LRIs not systematically summarised. Herein, regulation, mechanism, electrocatalytic applications are comprehensively summarised discussed. In addition basic information above, challenges, opportunities, future development proposed order present overall view reference for research.

Language: Английский

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Atomically dispersed materials: Ideal catalysts in atomic era

Nano Research, Journal Year: 2023, Volume and Issue: 17(1), P. 18 - 38

Published: May 25, 2023

Language: Английский

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Microenvironment Engineering of Single/Dual‐Atom Catalysts for Electrocatalytic Application

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(31)

Published: Feb. 23, 2023

Single/dual-metal atoms supported on carbon matrix can be modulated by coordination structure and neighboring active sites. Precisely designing the geometric electronic uncovering structure-property relationships of single/dual-metal confront with grand challenges. Herein, this review summarizes latest progress in microenvironment engineering single/dual-atom sites via a comprehensive comparison single-atom catalyst (SACs) dual-atom catalysts (DACs) term design principles, modulation strategy, theoretical understanding structure-performance correlations. Subsequently, recent advances several typical electrocatalysis process are discussed to get general reaction mechanisms finely-tuned SACs DACs. Finally, full-scaled summaries challenges prospects given for This will provide new inspiration development atomically dispersed electrocatalytic application.

Language: Английский

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Single-atom copper embedded in two-dimensional MXene toward peroxymonosulfate activation to generate singlet oxygen with nearly 100% selectivity for enhanced Fenton-like reactions

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 324, P. 122245 - 122245

Published: Dec. 1, 2022

Language: Английский

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Almost 100 % electron transfer regime over Fe−Co dual-atom catalyst toward pollutants removal: Regulation of peroxymonosulfate adsorption mode

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 339, P. 123178 - 123178

Published: Aug. 15, 2023

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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Ultrathin porous Bi2WO6 with rich oxygen vacancies for promoted adsorption-photocatalytic tetracycline degradation

Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 464, P. 142694 - 142694

Published: March 30, 2023

Language: Английский

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Fenton-like activity and pathway modulation via single-atom sites and pollutants comediates the electron transfer process

Proceedings of the National Academy of Sciences, Journal Year: 2024, Volume and Issue: 121(3)

Published: Jan. 8, 2024

The studies on the origin of versatile oxidation pathways toward targeted pollutants in single-atom catalysts (SACs)/peroxymonosulfate (PMS) systems were always associated with coordination structures rather than perspective pollutant characteristics, and analysis mechanism commonality is lacking. In this work, a variety (M-SACs, M: Fe, Co, Cu) fabricated via pyrolysis process using lignin as complexation agent substrate precursor. Sixteen kinds commonly detected various references selected, their ln k obs values M-SACs/PMS correlated well ( R 2 = 0.832 to 0.883) electrophilic indexes (reflecting electron accepting/donating ability pollutants) energy gap 0.801 0.840) between complexes. Both transfer (ETP) radical can be significantly enhanced systems, while was overwhelmed by ETP lower indexes. contrast, higher represented weaker electron-donating capacity complexes, which resulted accompanied noticeable oxidation. addition, different regulated gaps complexes pollutants. As result, Fenton-like activities could modulated reaction pathways, determined both sites. This work provided strategy establish PMS-based AOP tunable capacities for high-efficiency organic decontamination.

Language: Английский

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Exploring the Ni 3d Orbital Unpaired Electrons Induced Polarization Loss Based on Ni Single‐Atoms Model Absorber

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 33(7)

Published: Nov. 28, 2022

Abstract Single‐atoms (SAs) strategies have been proved to be effective in modulating electromagnetic wave (EMW) absorption, however, the establishment of a definitive relationship between metal SAs electronic configurations and physical loss mechanisms has still absent, especially on atomic scale. Herein, stable Ni‐SAs x /N‐doped carbon (NC) absorbers are fabricated with strategy ligand polymerization. The morphology, composition, electrical conductivity, defects, interactions material can well tailored by Ni species modulation engineering. Theoretical experimental results show that atomically dispersed individual atoms contribute enhanced EMW absorption performance through excess 3 d orbital unpaired electron induced polarization loss. Benefiting from it, Ni‐SAs3/NC highest SA y ‐N ( > 1, 1) polar/defect centers exhibit excellent an bandwidth 7.08 GHz at matched thickness 2.50 mm. Radar cross‐section simulations further demonstrate its potential for practical application as absorber. This study reveals continuous evolution microscopic mechanism (i.e., conduction loss→ unique loss) first time, which provides insight into deep design atom‐scale view.

Language: Английский

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