Accelerating Fe(III)/Fe(II) cycle via Fe(II) substitution for enhancing Fenton-like performance of Fe-MOFs

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F46747885%3A24620%2F21%3A00008215" target="_blank" >RIV/46747885:24620/21:00008215 - isvavai.cz</a>

Výsledek na webu

<a href="https://www.sciencedirect.com/science/article/pii/S0926337320312765?via=ihub" target="_blank" >https://www.sciencedirect.com/science/article/pii/S0926337320312765?via=ihub</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1016/j.apcatb.2020.119859" target="_blank" >10.1016/j.apcatb.2020.119859</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Accelerating Fe(III)/Fe(II) cycle via Fe(II) substitution for enhancing Fenton-like performance of Fe-MOFs

Popis výsledku v původním jazyce

Metal-organic frameworks (MOFs), especially iron-based MOFs (Fe-MOFs), are deemed as promising Fenton-like catalysts due to their well-developed pores and accessible active sites. However, the Fenton-like performance of Fe-MOFs is limited by the relatively low redox rate of Fe(III)/Fe(II) couples and density of coordinatively unsaturated iron centers (CUICs), which depend on the intrinsic structure of iron-oxo nodes in Fe-MOFs. Herein, we manipulated the structure of iron-oxo nodes in MIL-53(Fe) via a Fe(II) substitution method, affording a mixed-valence (i.e., Fe(III)/Fe(II)) material (denoted as Fe-II-MIL-53(Fe)) with highly improved Fenton-like performance. The substituted Fe(II) centers could serve as stronger active sites, where Fe(III)→Fe(II) half-reaction occurs, over original Fe(III) centers to rapidly activate H2O2 for efficient destruction of 4-nitrophenol (4-NP). Meanwhile, Fe(II) substitution induced the formation of a larger amount of Fe(III) CUICs, which was proven by the increased Lewis acidity of MIL-53(Fe). The increased density of Fe(III) CUICs promoted the interaction between Fe(III) centers and H2O2 and thus rendered another half-reaction, Fe(III)→Fe(II), with a greater rate. Accordingly, the accelerated cycle of Fe(III)/Fe(II) couples favored radical dotOH generation for improving 4-NP degradation. As a result, the 4-NP degradation and rate on FeII-MIL-53(Fe) were 1.39 and 9.48 times higher than that on pristine MIL-53(Fe). Moreover, FeII-MIL-53(Fe) showed a good stability and reusability over multiple cycles. Our work provides insights into the rational design of Fe-MOFs as promising Fenton-like catalysts for advanced water/wastewater treatment.

Název v anglickém jazyce

Accelerating Fe(III)/Fe(II) cycle via Fe(II) substitution for enhancing Fenton-like performance of Fe-MOFs

Popis výsledku anglicky

Metal-organic frameworks (MOFs), especially iron-based MOFs (Fe-MOFs), are deemed as promising Fenton-like catalysts due to their well-developed pores and accessible active sites. However, the Fenton-like performance of Fe-MOFs is limited by the relatively low redox rate of Fe(III)/Fe(II) couples and density of coordinatively unsaturated iron centers (CUICs), which depend on the intrinsic structure of iron-oxo nodes in Fe-MOFs. Herein, we manipulated the structure of iron-oxo nodes in MIL-53(Fe) via a Fe(II) substitution method, affording a mixed-valence (i.e., Fe(III)/Fe(II)) material (denoted as Fe-II-MIL-53(Fe)) with highly improved Fenton-like performance. The substituted Fe(II) centers could serve as stronger active sites, where Fe(III)→Fe(II) half-reaction occurs, over original Fe(III) centers to rapidly activate H2O2 for efficient destruction of 4-nitrophenol (4-NP). Meanwhile, Fe(II) substitution induced the formation of a larger amount of Fe(III) CUICs, which was proven by the increased Lewis acidity of MIL-53(Fe). The increased density of Fe(III) CUICs promoted the interaction between Fe(III) centers and H2O2 and thus rendered another half-reaction, Fe(III)→Fe(II), with a greater rate. Accordingly, the accelerated cycle of Fe(III)/Fe(II) couples favored radical dotOH generation for improving 4-NP degradation. As a result, the 4-NP degradation and rate on FeII-MIL-53(Fe) were 1.39 and 9.48 times higher than that on pristine MIL-53(Fe). Moreover, FeII-MIL-53(Fe) showed a good stability and reusability over multiple cycles. Our work provides insights into the rational design of Fe-MOFs as promising Fenton-like catalysts for advanced water/wastewater treatment.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

20701 - Environmental and geological engineering, geotechnics

Projekt

<a href="/cs/project/EF16_025%2F0007293" target="_blank" >EF16_025/0007293: Modulární platforma pro autonomní podvozky specializovaných elektrovozidel pro dopravu nákladu a zařízení</a><br>

Návaznosti

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Rok uplatnění

2021

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

APPLIED CATALYSIS B-ENVIRONMENTAL

ISSN

0926-3373

e-ISSN

—

Svazek periodika

286

Číslo periodika v rámci svazku

6

Stát vydavatele periodika

NL - Nizozemsko

Počet stran výsledku

34

Strana od-do

—

Kód UT WoS článku

000621624500005

EID výsledku v databázi Scopus

2-s2.0-85100058816