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Carbon–Iodine Coordination Activates Co–N4 Sites for Efficient Peroxymonosulfate Activation toward Mass-Transfer-Accelerated Singlet Oxygen Oxidation of Electron-Rich Pollutants
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PRE
AI
J
X
K
K
S
余
J
DOI：10.1021/acs.est.6c04882.png)
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Abstract
En 中文
Mass transfer limitations and inefficient nonradical oxidant generation often constrain the practical performance of Fenton-like catalysts for micropollutant removal. Here, we develop a synergistic architectural strategy to construct carbon-supported cobalt single-atom catalysts (Co-INC) via ammonium iodide-assisted chemical vapor deposition, integrating atomically dispersed Co–N4 sites with carbon–iodine (C–I) coordination motifs to simultaneously enhance reactant transport and singlet oxygen (1O2) production. Benefiting from in situ NH3-mediated etching, the architecture enhances active-site accessibility while achieving a high Co density of 0.165 mmol g–1, facilitating peroxymonosulfate (PMS) diffusion. Additionally, iodine incorporation creates an asymmetric Co–N4/C–I coordination environment that upshifts Co d-band center to −0.54 eV, strengthening PMS adsorption (−2.54 eV). This configuration promotes interfacial electron transfer and reduces the rate-determining energy barrier to −0.84 eV, substantially boosting 1O2 generation and achieving a steady-state concentration of 0.295 mM. Furthermore, the optimized pore architecture alleviates mass-transfer constraints, enabling efficient 1O2 utilization and a 2.3-fold increase in the ciprofloxacin mass-transfer coefficient. Consequently, Co-INC exhibits an exceptional normalized rate constant of 507 min–1·M–1 for ciprofloxacin degradation, outperforming pristine Co-NC by 10.3 times and surpassing most PMS-based catalysts. This study demonstrates that coupling active-site coordination with mass-transfer enhancement is pivotal for maximizing nonradical oxidation pathways in water treatment.
Keywords:
Adsorption
Catalysts
Cobalt
Oxidation
Particulate matter
single-atom catalyst
asymmetric coordination
mass transfer enhancement
peroxymonosulfate activation
singlet oxygen-dominated oxidation
Journal
E
IF:
11.3
Papers:
1.9K
Citations:
1
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Cited Papers