Single-Atom MnN₅ Catalytic Sites Enable Efficient Peroxymonosulfate Activation by Forming Highly Reactive Mn(IV)–Oxo Species

Environmental Science & Technology, Год журнала: 2023, Номер 57(10), С. 4266 - 4275

Опубликована: Фев. 27, 2023

Four-nitrogen-coordinated transitional metal (MN4) configurations in single-atom catalysts (SACs) are broadly recognized as the most efficient active sites peroxymonosulfate (PMS)-based advanced oxidation processes. However, SACs with a coordination number higher than four rarely explored, which represents fundamental missed opportunity for chemistry to boost PMS activation and degradation of recalcitrant organic pollutants. We experimentally theoretically demonstrate here that five-nitrogen-coordinated Mn (MnN5) more effectively activate MnN4 sites, by facilitating cleavage O–O bond into high-valent Mn(IV)–oxo species nearly 100% selectivity. The high activity MnN5 was discerned be due formation higher-spin-state N5Mn(IV)═O species, enable two-electron transfer from organics through lower-energy-barrier pathway. Overall, this work demonstrates importance numbers informs design next-generation environmental catalysts.

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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Transition metal single-atom embedded on N-doped carbon as a catalyst for peroxymonosulfate activation: A DFT study

Chemical Engineering Journal, Год журнала: 2022, Номер 437, С. 135428 - 135428

Опубликована: Фев. 23, 2022

Язык: Английский

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

Environmental Science & Technology, Год журнала: 2021, Номер 56(2), С. 1341 - 1351

Опубликована: Дек. 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

Язык: Английский

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Single atom Fe-dispersed graphitic carbon nitride (g-C3N4) as a highly efficient peroxymonosulfate photocatalytic activator for sulfamethoxazole degradation

Chemical Engineering Journal, Год журнала: 2021, Номер 430, С. 132937 - 132937

Опубликована: Окт. 14, 2021

Язык: Английский

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