Origins of Electron-Transfer Regime in Persulfate-Based Nonradical Oxidation Processes

Environmental Science & Technology, Journal Year: 2021, Volume and Issue: 56(1), P. 78 - 97

Published: Dec. 21, 2021

Persulfate-based nonradical oxidation processes (PS-NOPs) are appealing in wastewater purification due to their high efficiency and selectivity for removing trace organic contaminants complicated water matrices. In this review, we showcased the recent progresses of state-of-the-art strategies electron-transfer regimes PS-NOPs, including design metal metal-free heterogeneous catalysts, situ/operando characterization/analytical techniques, insights into origins mechanisms. a typical process (ETP), persulfate is activated by catalyst form surface complexes, which directly or indirectly interact with target pollutants finalize oxidation. We discussed different analytical techniques on fundamentals tactics accurate analysis ETP. Moreover, demonstrated challenges proposed future research ETP-based systems, such as computation-enabled molecular-level investigations, rational real-scenario applications environment. Overall, review dedicates sharpening understanding ETP PS-NOPs presenting promising remediation technology green chemistry.

Language: Английский

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Single-atom catalysts for photocatalytic energy conversion

Joule, Journal Year: 2022, Volume and Issue: 6(1), P. 92 - 133

Published: Jan. 1, 2022

Artificial photocatalytic energy conversion represents a highly intriguing strategy for solving the crisis and environmental problems by directly harvesting solar energy. The development of efficient photocatalysts is central task pushing real-world application reactions. Due to maximum atomic utilization efficiency distinct advantages outstanding catalytic activity, single-atom catalysts (SACs) have emerged as promising candidates photocatalysts. In current review, recent progresses challenges on SACs systems are presented. Fundamental principles focusing charge separation/transfer molecular adsorption/activation photocatalysis systemically explored. We outline how isolated reactive sites facilitate photogenerated electron–hole transfer promote construction photoactivation cycles. widespread adoption in diverse reactions also comprehensively introduced. By presenting these advances addressing some future with potential solutions related integral over SACs, we expect shed light forthcoming research conversion.

Language: Английский

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Metal-based catalysts for persulfate and peroxymonosulfate activation in heterogeneous ways: A review

Chemical Engineering Journal, Journal Year: 2021, Volume and Issue: 429, P. 132323 - 132323

Published: Sept. 9, 2021

Language: Английский

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Degradation of antibiotic pollutants by persulfate activated with various carbon materials

Chemical Engineering Journal, Journal Year: 2021, Volume and Issue: 429, P. 132387 - 132387

Published: Sept. 10, 2021

Language: Английский

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Identification of Fenton-like active Cu sites by heteroatom modulation of electronic density

Proceedings of the National Academy of Sciences, Journal Year: 2022, Volume and Issue: 119(8)

Published: Feb. 14, 2022

Developing heterogeneous catalysts with atomically dispersed active sites is vital to boost peroxymonosulfate (PMS) activation for Fenton-like activity, but how controllably adjust the electronic configuration of metal centers further improve kinetics still remains a great challenge. Herein, we report systematic investigation into heteroatom-doped engineering tuning structure Cu-N4 by integrating electron-deficient boron (B) or electron-rich phosphorus (P) heteroatoms carbon substrate PMS activation. The electron-depleted Cu-N4/C-B found exhibit most oxidation capacity among prepared single-atom catalysts, which at top rankings Cu-based and superior state-of-the-art catalysts. Conversely, electron-enriched Cu-N4/C-P induces decrease in Both experimental results theoretical simulations unravel that long-range interaction B atoms decreases density Cu down-shifts d-band center, thereby optimizes adsorption energy This study provides an approach finely control atomic level expected guide design smart

Language: Английский

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Activation of peroxymonosulfate by single-atom Fe-g-C3N4 catalysts for high efficiency degradation of tetracycline via nonradical pathways: Role of high-valent iron-oxo species and Fe–Nx sites

Chemical Engineering Journal, Journal Year: 2021, Volume and Issue: 427, P. 130803 - 130803

Published: June 12, 2021

Language: Английский

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Unveiling the Origins of Selective Oxidation in Single-Atom Catalysis via Co–N₄–C Intensified Radical and Nonradical Pathways

Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(16), P. 11635 - 11645

Published: July 11, 2022

Single-atom catalysts (SACs)-based peroxymonosulfate (PMS) systems are highly selective to the type of organic pollutants while mechanisms remain ambiguous. In this work, we carried out experimental and theoretical investigations reveal origins selectivity radical nonradical pathways in a designated Co–N4–C/PMS system. Two typical [bisphenol A (BPA) metronidazole (MNZ)] with different molecular structures were employed for comparison. We found that oxidation (SO4•– HO•) electron-transfer pathway (ETP) co-existed Pollutants (e.g., MNZ) high redox potential degraded primarily by free radicals rather than ETP, oxidization low-redox BPA) was dominated ETP at surface region Co–N4–C which overwhelmed contributions homogeneous phase. Intriguingly, could be manipulated PMS loading, simultaneously increased population elevated Co–N4–C-PMS* complexes ETP. Findings from work will unravel mysterious behavior SACs/PMS micropollutants.

Language: Английский

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Activation of peroxymonosulfate via mediated electron transfer mechanism on single-atom Fe catalyst for effective organic pollutants removal

Applied Catalysis B Environment and Energy, Journal Year: 2021, Volume and Issue: 299, P. 120714 - 120714

Published: Sept. 14, 2021

Language: Английский

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Emerging low-nuclearity supported metal catalysts with atomic level precision for efficient heterogeneous catalysis

Nano Research, Journal Year: 2022, Volume and Issue: 15(9), P. 7806 - 7839

Published: June 2, 2022

Language: Английский

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Effect of phosphate on peroxymonosulfate activation: Accelerating generation of sulfate radical and underlying mechanism

Applied Catalysis B Environment and Energy, Journal Year: 2021, Volume and Issue: 298, P. 120532 - 120532

Published: July 13, 2021

Language: Английский

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