Mxene-decorated spinel oxides as innovative activators of
peroxymonosulfate for degradation of caffeine in WWTP
effluents: Insights into mechanisms

J 2024

Mxene-decorated spinel oxides as innovative activators of peroxymonosulfate for degradation of caffeine in WWTP effluents: Insights into mechanisms

ATRI, Shalu, František ZAŽÍMAL, Sridhar Gowri SANKARAN, Zuzana DYRCIKOVA, Maria CAPLOVICOVA et. al.

Basic information

Original name

Mxene-decorated spinel oxides as innovative activators of peroxymonosulfate for degradation of caffeine in WWTP effluents: Insights into mechanisms

Authors

ATRI, Shalu, František ZAŽÍMAL (203 Czech Republic, belonging to the institution), Sridhar Gowri SANKARAN, Zuzana DYRCIKOVA, Maria CAPLOVICOVA, Tomas ROCH, Dana DVORANOVA, Tomáš HOMOLA (703 Slovakia, belonging to the institution), Gustav PLESCH, Marcello BRIGANTE and Olivier MONFORT

Edition

Chemical Engineering Journal, Elsevier B.V. 2024, 1385-8947

Other information

Language

English

Type of outcome

Článek v odborném periodiku

Field of Study

21001 Nano-materials

Country of publisher

Switzerland

Confidentiality degree

není předmětem státního či obchodního tajemství

References:

URL

Impact factor

Impact factor: 15.100 in 2022

Organization unit

Faculty of Science

DOI

http://dx.doi.org/10.1016/j.cej.2024.157814

UT WoS

001365970300001

Keywords in English

MXene; Ferrite; Composites; Catalyst; Persulfate; Wastewater

Abstract

V originále

In the frame of the environmental issues related to the efficiency of wastewaters treatment, the generation of advanced oxidation processes (AOPs) by 2D materials appears one of the most promising solutions. In this study, a novel catalytic system for peroxymonosulfate activation (PMS) was designed based on MXene (Ti3C2Tx) decorated with spinel oxides Co3O4, Fe3O4 and CoFe2O4 catalysts. Their efficiency in caffeine (CAF) degradation via PMS activation was assessed. The insertion of spinel oxides inside the multilayer structure of MXene along with their uniform surface decoration was demonstrated by SEM and TEM analyses and it also avoided the aggregation of the magnetic particles, thus increasing their efficiency. Among the different catalysts, the MXene/CoFe2O4 (MXCF) stood out as the most effective, mainly due to the Fe and Co redox cycles. The complete degradation of CAF was achieved in the dark within 10 min at natural pH using 0.2 g/L of MXCF and 0.5 mM of PMS. The novelty of current study lies in the efficient activation of PMS by, for the first time, MXCF in the dark along with mechanistic elucidation of PMS activation. The important role of Co3+/Co2+ and Fe3+/Fe2+ redox cycles alongside surface bound functional groups were highlighted. Radical scavenging and EPR experiments confirmed •OH and 1O2 as the main ROS involved in the CAF degradation. The CAF degradation pathways pointed to hydroxylation and imidazole ring opening mechanisms and MXCF catalyst also exhibited high efficiency in the degradation of sulfamethoxazole and phenol via PMS activation. To further highlight the relevance of the obtained results, treatment of tertiary effluents of wastewaters treatment plant (WWTP) in Bratislava contaminated by CAF exhibited a complete pollutant degradation after 3 h by supplying 0.2 g/L of catalyst and 2 mM PMS in the dark.

Links

LM2023039, research and development project

Name: Centrum výzkumu a vývoje plazmatu a nanotechnologických povrchových úprav

Investor: Ministry of Education, Youth and Sports of the CR

90251, large research infrastructures

Name: CzechNanoLab II

Citovat

ATRI, Shalu, František ZAŽÍMAL, Sridhar Gowri SANKARAN, Zuzana DYRCIKOVA, Maria CAPLOVICOVA, Tomas ROCH, Dana DVORANOVA, Tomáš HOMOLA, Gustav PLESCH, Marcello BRIGANTE and Olivier MONFORT. Mxene-decorated spinel oxides as innovative activators of peroxymonosulfate for degradation of caffeine in WWTP effluents: Insights into mechanisms. Chemical Engineering Journal. Elsevier B.V., 2024, vol. 502, December, p. 157814-157826. ISSN 1385-8947. Available from: https://dx.doi.org/10.1016/j.cej.2024.157814.

@article{2453929,
   author = {Atri, Shalu and Zažímal, František and Sankaran, Sridhar Gowri and Dyrcikova, Zuzana and Caplovicova, Maria and Roch, Tomas and Dvoranova, Dana and Homola, Tomáš and Plesch, Gustav and Brigante, Marcello and Monfort, Olivier},
   article_number = {December},
   doi = {http://dx.doi.org/10.1016/j.cej.2024.157814},
   keywords = {MXene; Ferrite; Composites; Catalyst; Persulfate; Wastewater},
   language = {eng},
   issn = {1385-8947},
   journal = {Chemical Engineering Journal},
   title = {Mxene-decorated spinel oxides as innovative activators of peroxymonosulfate for degradation of caffeine in WWTP effluents: Insights into mechanisms},
   url = {https://www.sciencedirect.com/science/article/pii/S1385894724093057},
   volume = {502},
   year = {2024}
}

TY  - JOUR
ID  - 2453929
AU  - Atri, Shalu - Zažímal, František - Sankaran, Sridhar Gowri - Dyrcikova, Zuzana - Caplovicova, Maria - Roch, Tomas - Dvoranova, Dana - Homola, Tomáš - Plesch, Gustav - Brigante, Marcello - Monfort, Olivier
PY  - 2024
TI  - Mxene-decorated spinel oxides as innovative activators of peroxymonosulfate for degradation of caffeine in WWTP effluents: Insights into mechanisms
JF  - Chemical Engineering Journal
VL  - 502
IS  - December
SP  - 157814
EP  - 157814
PB  - Elsevier B.V.
SN  - 13858947
KW  - MXene
KW  - Ferrite
KW  - Composites
KW  - Catalyst
KW  - Persulfate
KW  - Wastewater
UR  - https://www.sciencedirect.com/science/article/pii/S1385894724093057
N2  - In the frame of the environmental issues related to the efficiency of wastewaters treatment, the generation of advanced oxidation processes (AOPs) by 2D materials appears one of the most promising solutions. In this study, a novel catalytic system for peroxymonosulfate activation (PMS) was designed based on MXene (Ti3C2Tx) decorated with spinel oxides Co3O4, Fe3O4 and CoFe2O4 catalysts. Their efficiency in caffeine (CAF) degradation via PMS activation was assessed. The insertion of spinel oxides inside the multilayer structure of MXene along with their uniform surface decoration was demonstrated by SEM and TEM analyses and it also avoided the aggregation of the magnetic particles, thus increasing their efficiency. Among the different catalysts, the MXene/CoFe2O4 (MXCF) stood out as the most effective, mainly due to the Fe and Co redox cycles. The complete degradation of CAF was achieved in the dark within 10 min at natural pH using 0.2 g/L of MXCF and 0.5 mM of PMS. The novelty of current study lies in the efficient activation of PMS by, for the first time, MXCF in the dark along with mechanistic elucidation of PMS activation. The important role of Co3+/Co2+ and Fe3+/Fe2+ redox cycles alongside surface bound functional groups were highlighted. Radical scavenging and EPR experiments confirmed •OH and 1O2 as the main ROS involved in the CAF degradation. The CAF degradation pathways pointed to hydroxylation and imidazole ring opening mechanisms and MXCF catalyst also exhibited high efficiency in the degradation of sulfamethoxazole and phenol via PMS activation. To further highlight the relevance of the obtained results, treatment of tertiary effluents of wastewaters treatment plant (WWTP) in Bratislava contaminated by CAF exhibited a complete pollutant degradation after 3 h by supplying 0.2 g/L of catalyst and 2 mM PMS in the dark.
ER  -

ATRI, Shalu, František ZAŽÍMAL, Sridhar Gowri SANKARAN, Zuzana DYRCIKOVA, Maria CAPLOVICOVA, Tomas ROCH, Dana DVORANOVA, Tomáš HOMOLA, Gustav PLESCH, Marcello BRIGANTE and Olivier MONFORT. Mxene-decorated spinel oxides as innovative activators of peroxymonosulfate for degradation of caffeine in WWTP effluents: Insights into mechanisms. \textit{Chemical Engineering Journal}. Elsevier B.V., 2024, vol.~502, December, p.~157814-157826. ISSN~1385-8947. Available from: https://dx.doi.org/10.1016/j.cej.2024.157814.

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