The enhanced peroxymonosulfate activation ability and mechanism on low-coordinated Fe-N3 single sites for organic pollutant degradation in wastewater
Source abstract
Abstract
For boosting the intrinsic peroxymonosulfate (PMS) catalytic activity of single atom catalysts (SACs), we fabricate zeolitic imidazolate framework (ZIF)-derived Fe SAC with different nitrogen coordination numbers (denoted as Fe-N x /C) to boost organic pollutant oxidation. X-ray absorption fine structure (XAFS) spectroscopy was undertaken to determine the coordination configuration of Fe–N path. As expected, the resultant Fe-N 3 /C exhibited more excellent PMS catalysis activity with a p-nitrophenol (4-NP) degradation kinetic rate constant (k obs ) of 0.061 min −1 that is 2.4-fold enhancement relative to the Fe-N 4 /C. Electron paramagnetic resonance (EPR) measurements and quenching tests confirmed the 1 O play the main role associated with high-valent Fe–oxo and a small amount of OH and SO 4 − species. Density functional calculations revealed that low coordinated Fe–N 3 sites prefer to form a bridge coordination bond structure of O-Fe-O with the adsorption sites of O2 and O1 in PMS molecule, exhibiting stronger interaction with the oxidant and better electron donating capability to enhance PMS activation comparing to common Fe-N 4 structure based on charge deformation density, electron localization function (ELF) and projected density of state (PDOS) analysis. These findings indicate that microstructure modulation is a useful avenue to prepare a high-performance Fenton-like SACs.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Advanced oxidation water treatment · Advanced Photocatalysis Techniques · Environmental remediation with nanomaterials
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (44)
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1. Review of organic wastewater compound concentrations and removal in onsite wastewater treatment systems10.1021/acs.est.6b04778 ↗
2. Pharmaceuticals and personal care products (PPCPs) in the freshwater aquatic environment10.1016/j.emcon.2016.12.004 ↗
3. Removal of pharmaceuticals and personal care products (PPCPs) from wastewater: a review10.1016/j.jenvman.2016.07.049 ↗
4. Challenges and prospects of advanced oxidation water treatment processes using catalytic nanomaterials10.1038/s41565-018-0216-x ↗
5. Critical review of advanced oxidation processes in organic wastewater treatment10.1016/j.chemosphere.2021.130104 ↗
6. Activation of persulfate (PS) and peroxymonosulfate (PMS) and application for the degradation of emerging contaminants10.1016/j.cej.2017.11.059 ↗
7. Persulfate-based advanced oxidation: critical assessment of opportunities and roadblocks10.1021/acs.est.9b07082 ↗
8. New insights into the generation of singlet oxygen in the metal-free peroxymonosulfate activation process: Important role of electron-deficient carbon atoms10.1021/acs.est.9b05856 ↗
9. Mn− O Covalency Governs the Intrinsic Activity of Co-Mn Spinel Oxides for Boosted Peroxymonosulfate Activation10.1002/anie.202010828 ↗
10. Different crystallographic one-dimensional MnO2 nanomaterials and their superior performance in catalytic phenol degradation10.1021/es400878c ↗
11. Catalytic reactivity of Co3O4 with different facets in the hydrogen abstraction of phenol by persulfate10.1016/j.apcatb.2020.118819 ↗
12. FexCo3− xO4 nanocages derived from nanoscale metal–organic frameworks for removal of bisphenol A by activation of peroxymonosulfate10.1016/j.apcatb.2015.08.050 ↗
13. Spatial confinement of a Co3O4 catalyst in hollow metal–organic frameworks as a nanoreactor for improved degradation of organic pollutants10.1021/es505014z ↗
14. A new magnetic nano zero-valent iron encapsulated in carbon spheres for oxidative degradation of phenol10.1016/j.apcatb.2015.02.016 ↗
15. Iron encapsulated in boron and nitrogen codoped carbon nanotubes as synergistic catalysts for Fenton-like reaction10.1016/j.watres.2016.05.065 ↗
16. Design of N-coordinated dual-metal sites: a stable and active Pt-free catalyst for acidic oxygen reduction reaction10.1021/jacs.7b10385 ↗
17. Engineering isolated Mn–N2C2 atomic interface sites for efficient bifunctional oxygen reduction and evolution reaction10.1021/acs.nanolett.0c01925 ↗
18. Single-Atom Iron Anchored Tubular g-C3N4 Catalysts for Ultrafast Fenton-Like Reaction: Roles of High-Valency Iron-Oxo Species and Organic Radicals10.1002/adma.202202891 ↗
19. Engineering low-coordination single-atom cobalt on graphitic carbon nitride catalyst for hydrogen evolution10.1021/acscatal.2c01253 ↗
20. Photoinduction of Cu single atoms decorated on UiO-66-NH2 for enhanced photocatalytic reduction of CO2 to liquid fuels10.1021/jacs.0c09599 ↗
21. MOF derived high-density atomic platinum heterogeneous catalyst for C-H bond activation10.1039/D0QM00040J ↗
22. Single-atomic-site cobalt stabilized on nitrogen and phosphorus co-doped carbon for selective oxidation of primary alcohols10.1039/C9NH00036D ↗
23. Single-atom Co-NC catalysts for high-efficiency reverse water-gas shift reaction10.1016/j.apcatb.2022.122298 ↗
24. Single-atom catalysis toward efficient CO2 conversion to CO and formate products10.1021/acs.accounts.8b00478 ↗
25. Matching the kinetics of natural enzymes with a single-atom iron nanozyme10.1038/s41929-021-00609-x ↗
26. Harvesting the Gas Molecules by Bioinspired Design of 1D/2D Hybrids Toward Sensitive Acetone Detecting10.1002/sstr.202200248 ↗
27. Single cobalt atoms anchored on porous N-doped graphene with dual reaction sites for efficient Fenton-like catalysis10.1021/jacs.8b05992 ↗
28. Almost 100% peroxymonosulfate conversion to singlet oxygen on single-atom CoN2+2 sites10.1002/ange.202014472 ↗
29. Unraveling the high-activity origin of single-atom iron catalysts for organic pollutant oxidation via peroxymonosulfate activation10.1021/acs.est.1c01131 ↗
30. Single Mn atom anchored on N-doped porous carbon as highly efficient Fenton-like catalyst for the degradation of organic contaminants10.1016/j.apcatb.2020.119363 ↗
31. Coordination number regulation of molybdenum single-atom nanozyme peroxidase-like specificity10.1016/j.chempr.2020.10.023 ↗
32. Engineering unsymmetrically coordinated Cu-S1N3 single atom sites with enhanced oxygen reduction activity10.1038/s41467-020-16848-8 ↗
33. Simultaneous diffusion of cation and anion to access N, S co-coordinated Bi-sites for enhanced CO2 electroreduction
34. Single cobalt atoms with precise N-coordination as superior oxygen reduction reaction catalysts10.1002/ange.201604802 ↗
35. Ionic exchange of metal–organic frameworks to access single nickel sites for efficient electroreduction of CO210.1021/jacs.7b02736 ↗
36. Uncoordinated amine groups of MOFs to anchor single Ru sites as chemoselective catalysts towards the hydrogenation of quinoline10.1021/jacs.7b01686 ↗
37. Isolated single iron atoms anchored on N-doped porous carbon as an efficient electrocatalyst for the oxygen reduction reaction10.1002/anie.201702473 ↗
38. Ab-initio simulations of materials using VASP: Density-functional theory and beyond10.1002/jcc.21057 ↗
39. Atoms, molecules, solids, and surfaces: Applications of the generalized gradient approximation for exchange and correlation10.1103/PhysRevB.46.6671 ↗
40. Transition metal single-atom embedded on N-doped carbon as a catalyst for peroxymonosulfate activation: A DFT study10.1016/j.cej.2022.135428 ↗
41. Metal–organic-framework-derived Fe-N/C electrocatalyst with five-coordinated Fe-N x sites for advanced oxygen reduction in acid media10.1021/acscatal.6b02966 ↗
42. Enhanced photocatalytic activity of aerogel composed of crooked carbon nitride nanolayers with nitrogen vacancies10.1021/acsami.9b10123 ↗
43. Defect graphene as a trifunctional catalyst for electrochemical reactions10.1002/adma.201602912 ↗
44. Core–shell ZIF-8@ ZIF-67-derived CoP nanoparticle-embedded N-doped carbon nanotube hollow polyhedron for efficient overall water splitting10.1021/jacs.7b12420 ↗