A critical review on correlating active sites, oxidative species and degradation routes with persulfate-based antibiotics oxidation

Water Research, Год журнала: 2023, Номер 235, С. 119926 - 119926

Опубликована: Март 27, 2023

Язык: Английский

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The optimized Fenton-like activity of Fe single-atom sites by Fe atomic clusters–mediated electronic configuration modulation

Proceedings of the National Academy of Sciences, Год журнала: 2023, Номер 120(15)

Опубликована: Апрель 3, 2023

The performance optimization of isolated atomically dispersed metal active sites is critical but challenging. Here, TiO2@Fe species-N-C catalysts with Fe atomic clusters (ACs) and satellite Fe-N4 were fabricated to initiate peroxymonosulfate (PMS) oxidation reaction. AC-induced charge redistribution single atoms (SAs) was verified, thus strengthening the interaction between SAs PMS. In detail, incorporation ACs optimized HSO5- SO5·- desorption steps, accelerating reaction progress. As a result, Vis/TiFeAS/PMS system rapidly eliminated 90.81% 45 mg/L tetracycline (TC) in 10 min. process characterization suggested that PMS as an electron donor would transfer species TiFeAS, generating 1O2. Subsequently, hVB+ can induce generation electron-deficient species, promoting circulation. This work provides strategy construct multiple atom assembly-enabled composite for high-efficiency PMS-based advanced processes (AOPs).

Язык: 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, Год журнала: 2022, Номер 324, С. 122245 - 122245

Опубликована: Дек. 1, 2022

Язык: 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, Год журнала: 2023, Номер 342, С. 123401 - 123401

Опубликована: Окт. 18, 2023

Язык: 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, Год журнала: 2023, Номер 339, С. 123178 - 123178

Опубликована: Авг. 15, 2023

Язык: Английский

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Generation and identification of 1O2 in catalysts/peroxymonosulfate systems for water purification

Water Research, Год журнала: 2023, Номер 245, С. 120614 - 120614

Опубликована: Сен. 11, 2023

Язык: Английский

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CoN₁O₂ Single‐Atom Catalyst for Efficient Peroxymonosulfate Activation and Selective Cobalt(IV)=O Generation

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(27)

Опубликована: Апрель 26, 2023

High-valent metal-oxo (HVMO) species are powerful non-radical reactive that enhance advanced oxidation processes (AOPs) due to their long half-lives and high selectivity towards recalcitrant water pollutants with electron-donating groups. However, high-valent cobalt-oxo (CoIV =O) generation is challenging in peroxymonosulfate (PMS)-based AOPs because the 3d-orbital occupancy of cobalt would disfavor its binding a terminal oxygen ligand. Herein, we propose strategy construct isolated Co sites unique N1 O2 coordination on Mn3 O4 surface. The asymmetric configuration able accept electrons from 3d-orbital, resulting significant electronic delocalization at for promoted PMS adsorption, dissociation subsequent CoIV =O species. CoN1 /Mn3 exhibits intrinsic activity activation sulfamethoxazole (SMX) degradation, highly outperforming counterpart CoO3 configuration, carbon-based single-atom catalysts CoN4 commercial oxides. effectively oxidize target contaminants via atom transfer produce low-toxicity intermediates. These findings could advance mechanistic understanding molecular level guide rational design efficient environmental catalysts.

Язык: Английский

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Fe-Mn oxycarbide anchored on N-doped carbon for enhanced Fenton-like catalysis: Importance of high-valent metal-oxo species and singlet oxygen

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 340, С. 123204 - 123204

Опубликована: Авг. 22, 2023

Язык: 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, Год журнала: 2023, Номер 62(43)

Опубликована: Сен. 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 .

Язык: Английский

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Derivatives of two-dimensional MXene-MOFs heterostructure for boosting peroxymonosulfate activation: Enhanced performance and synergistic mechanism

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 323, С. 122136 - 122136

Опубликована: Ноя. 1, 2022

Язык: Английский

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