Unsaturated single-atom CoN3 sites for improved fenton-like reaction towards high-valent metal species

Song, Junsheng; Hou, Nannan; Liu, Xiaocheng; Antonietti, Markus; Wang, Yan; Mu, Yang

doi:10.1016/j.apcatb.2023.122368

Cited by 37 publications

(17 citation statements)

References 48 publications

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“…Phenol removal was slightly inhibited in the presence of SOD, indicating the potential production of O 2 ·– as a minor contributor to phenol oxidation. In addition, KI (surface reaction scavenger) is also used as a quencher to evaluate the role of high-valent Co species and surface free radicals . As can be seen from Figure a, the addition of KI does not significantly inhibit the degradation efficiency of phenol, which shows that the high-valent Co species and surface free radicals combined on the surface are not the main contributors to degradation.…”

Section: Resultsmentioning

confidence: 99%

Single-Atom Cobalt Catalysts Encapsulating Cobalt Nanoparticles with Built-In Electric Field for Ultrafast and Lasting Peroxymonosulfate Activation

Zou,

Wang,

Sun

et al. 2024

ACS EST Water

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Cobalt single-atom catalysts (Co-SAs) are rising stars in persulfate chemistry for their well-defined coordination, reduced metal usage, and exceptional activity. However, the simultaneous formation of cobalt nanoparticles (Co-NPs) with Co-SAs raises questions about their complex interplay and synergy in catalysis. In this study, we synthesized Co-SAs-encapsulated Co-NPs (CoNP@NC/Co-SA) using the laserinduced carbonization strategy of high entropy synthesis technology. The results show that 93.23% of phenol can be removed in 15 min and 91.60% in 3 min in the CoNP@NC/Co-SA/PMS system. Simulation results showed that Co-NPs fine-tune the electronic structure of Co-SA sites, optimizing PMS adsorption and activation to generate confined reactive species. The surface-activated PMS-catalyst complex directly attacked adsorbed pollutants on the catalyst surface via an electron-transfer regime. CoNP@NC/Co-SA catalyzes PMS oxidation through a nonradical pathway with high selectivity toward target organics. The findings emphasize the synergistic effect of Co-SAs and Co-NPs in promoting Fenton-like catalysis, enlightening the rational design of advanced composite materials via synergistic molecular and interfacial engineering for fast and long-lasting catalytic oxidation. At the same time, this work provides insights into the electronic structure regulation of metal centers at the atomic level.

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Section: Resultsmentioning

confidence: 99%

Single-Atom Cobalt Catalysts Encapsulating Cobalt Nanoparticles with Built-In Electric Field for Ultrafast and Lasting Peroxymonosulfate Activation

Zou,

Wang,

Sun

et al. 2024

ACS EST Water

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“…Recent studies have identified that Co(IV)O species, a powerful active species, can be formed by the oxidation of the coordination of Co and N -based ligands in the PMS system. , Thus, the degradation of TC in the Co–NC-900/PMS system may involve high-valent cobalt species. To discern this, dimethyl sulfoxide (DMSO), a scavenger for high-valent cobalt-oxo species ( k (DMSO,Co(IV)) = 2.40 × 10 6 M –1 s –1 ), was added to the degradation system and displayed a vigorous inhibitory for TC degradation (dropped from 97.3 to 14.5%), indicating that Co(IV)O probably plays a crucial role for TC degradation in the Co–NC-900/PMS system.…”

Section: Resultsmentioning

confidence: 99%

“…Comparatively, heterogeneous catalysts have been developed for PMS activation. Recently, several Co-based heterogeneous catalysts (e.g., Co 3 O 4 , Co-doped g-C 3 N 4, and Co-SACs) – have been constructed to activate PMS, and Co(IV)O is the dominant reactive species for micropollutants degradation. For instance, a single atom Co–N 4 catalyst was prepared to activate PMS, and the generation Co(IV)O instead of radicals exhibited selective reactivity for the oxidation of emerging micropollutants .…”

Section: Introductionmentioning

confidence: 99%

Manipulating High-Valent Cobalt-Oxo Generation on Co/N Codoped Carbon Beads via PMS Activation for Micropollutants Degradation

Pei,

Fu,

et al. 2023

ACS EST Eng.

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Manipulating high-valent cobalt-oxo [Co(IV)O] species in a catalytic system is pivotal; however, it is challenging due to the inefficiency and unsustainability of Co(IV)O generation. In this study, we fabricated macroscopic porous Co/N codoped carbon beads (Co–NC) and identified Co(IV)O as the prominent species in peroxymonosulfate (PMS) activation. Specifically, Co(IV)O species on a Co–NC-900/PMS system was regarded as the crucial driver of tetracycline (TC) removal (with a degradation efficiency of 97.3% and an initial concentration of 20 mg L–1) through quenching experiments, methyl phenyl sulfoxide (PMSO) degradation, and methyl phenyl sulfone (PMSO2) generation. Importantly, Co–N x active sites are responsible for the formation of Co(IV)O species, which contribute as much as 98.33% to TC degradation based on the calculation of the steady-state concentration. In addition, the relative contributions of Co(IV)O toward various micropollutants are substrate-specific and related to their ionization potential (IP). The practical application of Co–NC-900 was further evaluated in the continuous flow mode, and it showed excellent durability and performance. Overall, we have aroused the importance of Co(IV)O on micropollutants removal in heterogeneous systems and provided an alternative macroscopic catalyst that can be potentially exploited in real water decontamination scenarios.

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“…Researchers have applied different strategies like coordination design, low-dimensional graphene chemistry, vacancy/defect design, and spatial confinement to stabilize single metal atoms. 72,79,81,85,86,[89][90][91][92][93][94]…”

Section: àmentioning

confidence: 99%

Single atom catalyst-mediated generation of reactive species in water treatment

Sharma,

Ma,

Zboril

2023

Chem. Soc. Rev.

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Unsaturated single-atom CoN3 sites for improved fenton-like reaction towards high-valent metal species

Cited by 37 publications

References 48 publications

Single-Atom Cobalt Catalysts Encapsulating Cobalt Nanoparticles with Built-In Electric Field for Ultrafast and Lasting Peroxymonosulfate Activation

Single-Atom Cobalt Catalysts Encapsulating Cobalt Nanoparticles with Built-In Electric Field for Ultrafast and Lasting Peroxymonosulfate Activation

Manipulating High-Valent Cobalt-Oxo Generation on Co/N Codoped Carbon Beads via PMS Activation for Micropollutants Degradation

Single atom catalyst-mediated generation of reactive species in water treatment

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