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Facile Pyrolysis Treatment for the Synthesis of Single-Atom Mn Catalysts Derived from a Hyperaccumulator
https://orcid.org/0000-0002-3837-6279
https://orcid.org/0000-0003-1883-8015
https://orcid.org/0000-0002-9887-2784
https://orcid.org/0000-0002-0921-0122
Advanced oxidation processes (AOPs) have revealed wide prospects in the application of the degradation of organic contaminants in ground water and soil. High-performance, environmentally friendly, and low-cost single-atom catalysts (SACs) are promising approaches to active persulfate in AOPs. However, the practical application of SACs is restricted by high preparation costs and tedious procedures. Herein, a manganese (Mn) hyperaccumulator, Phytolacca americana, was successfully exploited as a precursor to synthesize a novel Mn SAC (SPBC-700N) via a one-step pyrolysis method. In SPBC-700N, Mn atoms are dispersed atomically upon the carbon matrix and coordinate with four N atoms to form Mn–N4 active sites, which exhibits an extraordinary catalytic activity for peroxymonosulfate (PMS) activation. A large number of reactive oxygen species are formed during the reaction, and over 90% of the antibiotic (chloroquine phosphate/CQP) could be removed within 30 min. The superior catalytic performance of the Mn SAC/PMS system for CQP degradation is ascribed to the synergistic effect of the maximized utilization of Mn atoms and the neighboring pyrrolic N sites, as identified by X-ray absorption fine structure spectroscopy and density function theory calculations. This work not only provides a green and low-cost strategy for synthesizing SACs but also gives an atomic-level insight into the catalytic activity of the Mn–N4 sites for PMS activation.
Facile Pyrolysis Treatment for the Synthesis of Single-Atom Mn Catalysts Derived from a Hyperaccumulator
https://orcid.org/0000-0002-3837-6279
https://orcid.org/0000-0003-1883-8015
https://orcid.org/0000-0002-9887-2784
https://orcid.org/0000-0002-0921-0122
Advanced oxidation processes (AOPs) have revealed wide prospects in the application of the degradation of organic contaminants in ground water and soil. High-performance, environmentally friendly, and low-cost single-atom catalysts (SACs) are promising approaches to active persulfate in AOPs. However, the practical application of SACs is restricted by high preparation costs and tedious procedures. Herein, a manganese (Mn) hyperaccumulator, Phytolacca americana, was successfully exploited as a precursor to synthesize a novel Mn SAC (SPBC-700N) via a one-step pyrolysis method. In SPBC-700N, Mn atoms are dispersed atomically upon the carbon matrix and coordinate with four N atoms to form Mn–N4 active sites, which exhibits an extraordinary catalytic activity for peroxymonosulfate (PMS) activation. A large number of reactive oxygen species are formed during the reaction, and over 90% of the antibiotic (chloroquine phosphate/CQP) could be removed within 30 min. The superior catalytic performance of the Mn SAC/PMS system for CQP degradation is ascribed to the synergistic effect of the maximized utilization of Mn atoms and the neighboring pyrrolic N sites, as identified by X-ray absorption fine structure spectroscopy and density function theory calculations. This work not only provides a green and low-cost strategy for synthesizing SACs but also gives an atomic-level insight into the catalytic activity of the Mn–N4 sites for PMS activation.
Facile Pyrolysis Treatment for the Synthesis of Single-Atom Mn Catalysts Derived from a Hyperaccumulator
https://orcid.org/0000-0002-3837-6279
https://orcid.org/0000-0003-1883-8015
https://orcid.org/0000-0002-9887-2784
https://orcid.org/0000-0002-0921-0122
Advanced oxidation processes (AOPs) have revealed wide prospects in the application of the degradation of organic contaminants in ground water and soil. High-performance, environmentally friendly, and low-cost single-atom catalysts (SACs) are promising approaches to active persulfate in AOPs. However, the practical application of SACs is restricted by high preparation costs and tedious procedures. Herein, a manganese (Mn) hyperaccumulator, Phytolacca americana, was successfully exploited as a precursor to synthesize a novel Mn SAC (SPBC-700N) via a one-step pyrolysis method. In SPBC-700N, Mn atoms are dispersed atomically upon the carbon matrix and coordinate with four N atoms to form Mn–N4 active sites, which exhibits an extraordinary catalytic activity for peroxymonosulfate (PMS) activation. A large number of reactive oxygen species are formed during the reaction, and over 90% of the antibiotic (chloroquine phosphate/CQP) could be removed within 30 min. The superior catalytic performance of the Mn SAC/PMS system for CQP degradation is ascribed to the synergistic effect of the maximized utilization of Mn atoms and the neighboring pyrrolic N sites, as identified by X-ray absorption fine structure spectroscopy and density function theory calculations. This work not only provides a green and low-cost strategy for synthesizing SACs but also gives an atomic-level insight into the catalytic activity of the Mn–N4 sites for PMS activation.
Facile Pyrolysis Treatment for the Synthesis of Single-Atom Mn Catalysts Derived from a Hyperaccumulator
Yang, Qiang (author) / Wang, Weixuan (author) / Zhou, Yiyi (author) / Hao, Jiachen (author) / Fang, Guodong (author) / Liu, Cun (author) / Cui, Peixin (author) / Wang, Yujun (author)
ACS ES&T Engineering ; 3 ; 616-626
2023-05-12
Article (Journal)
Electronic Resource
English
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