Precise coordination of high-loading Fe single atoms with sulfur boosts selective generation of nonradicals

Proceedings of the National Academy of Sciences, Год журнала: 2024, Номер 121(4)

Опубликована: Янв. 17, 2024

Nonradicals are effective in selectively degrading electron-rich organic contaminants, which unfortunately suffer from unsatisfactory yield and uncontrollable composition due to the competitive generation of radicals. Herein, we precisely construct a local microenvironment carbon nitride–supported high-loading (~9 wt.%) Fe single-atom catalyst (Fe SAC) with sulfur via facile supermolecular self-assembly strategy. Short-distance S coordination boosts peroxymonosulfate (PMS) activation generates high-valent iron–oxo species IV =O) along singlet oxygen ( 1 O 2 ), significantly increasing yield, PMS utilization, p -chlorophenol reactivity by 6.0, 3.0, 8.4 times, respectively. The nonradicals is controllable simply changing content. In contrast, long-distance both radicals nonradicals, could not promote reactivity. Experimental theoretical analyses suggest that short-distance upshifts d -band center atom, i.e., being close Fermi level, changes binding mode between atom site generate =O high yield. S-coordinated SAC exhibits excellent application potential various water matrices. These findings can guide rational design robust SACs toward selective utilization.

Язык: Английский

---

Modified nickel–cobalt tailing activated PMS for highly efficient degradation of organic pollutants: Multiple-scale effect and active sites

Chemical Engineering Journal, Год журнала: 2024, Номер 482, С. 149196 - 149196

Опубликована: Янв. 29, 2024

Язык: Английский

---

Metal sulfides as emerging materials for advanced oxidation of wastewater: Recent developments, challenges, and prospects

Coordination Chemistry Reviews, Год журнала: 2024, Номер 509, С. 215765 - 215765

Опубликована: Март 20, 2024

Язык: Английский

---

Graphene oxide-induced CuO reduction in TiO2/CaTiO3/Cu2O/Cu composites for photocatalytic degradation of drugs via peroxymonosulfate activation

Applied Surface Science, Год журнала: 2024, Номер 656, С. 159698 - 159698

Опубликована: Фев. 13, 2024

Contamination of water bodies is a global environmental and human health issue. Conventional treatment systems cannot efficiently eliminate organic contaminants, particularly drugs. Photocatalysis promising, environmentally friendly oxidation process for the removal such compounds. A key point choice material to be used as photocatalyst. Here, TiO2/CaTiO3/Cu2O/Cu composites were fabricated by adding different amounts (x) graphene oxide (GO) (x wt% = 1, 3, 5%) CaCu3Ti4O12 powder using solid-state synthesis method. The produced pellets sintered under inert nitrogen atmosphere at 1100°C 3h. X-ray diffraction analysis showed that Cu metal amount was increased upon GO addition, UV–Vis diffuse reflectance spectroscopy spectral response extended visible range. Then, high performance liquid chromatography assessment paracetamol degradation photocatalytic cell with efficiency introduction 0.5 mM peroxymonosulfate (PMS) active component generate ●SO4‾ radicals. After 3 hours light, 96% 10 ppm degraded composite 3% (1 cm2 surface photocatalyst) compared 50% without in same experimental conditions (PMS 210 mL aqueous solution). Free radical trapping acute toxicity potential by-products also investigated. Our results indicate displays long-term stability durability pharmaceutical pollutants from wastewater.

Язык: Английский

---

Nano-island-encapsulated cobalt single-atom catalysts for breaking activity-stability trade-off in Fenton-like reactions

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Янв. 2, 2025

Язык: Английский

---

Unprecedented Relay Catalysis of Curved Fe₁–N₄ Single-Atom Site for Remarkably Efficient ¹O₂ Generation

ACS Catalysis, Год журнала: 2022, Номер 13(1), С. 681 - 691

Опубликована: Дек. 23, 2022

The design of catalysts and catalytic processes for high efficiency selectivity important singlet oxygen (1O2) active species generation in oxidation reactions is still challenging, especially utilizing abundant environmental O2 without photoelectric field or extra thermal condition. Herein, a curved Fe1–N4 single-atom site developed by incorporating isolated Fe single atom into nanodiamond with high-curvature surface. It leads to an unprecedented relay catalysis route, which the activation coupled peroxymonosulfate (PMS) activation, efficiently generate 1O2 species. In detail, PMS first activated on electron donation atom, accompanied 1/2 equiv production. More importantly, due compressive strain higher energy level 3dz2 orbital, charge acquisition can directly transfer molecule consequently trigger additional 1 1O2. Taking advantage this tandem process, remarkable near 100% are achieved, ultrahigh metal 0.77 min–1 tetracycline oxidative degradation outstanding performance benzene alcohol selective oxidation. This work, one hand, opens up efficient way peroxide-based oxidations, other develops bifunctional rapid gain loss ability, sheds light further improving via mechanism.

Язык: Английский

---

Amorphous zirconium oxide activates peroxymonosulfate for selective degradation of organic compounds: Performance, mechanisms and structure-activity relationship

Water Research, Год журнала: 2022, Номер 228, С. 119363 - 119363

Опубликована: Ноя. 16, 2022

Язык: Английский

---

Efficient carbamazepine degradation by modified copper tailings and PMS system: Performance evaluation and mechanism

Journal of Hazardous Materials, Год журнала: 2023, Номер 465, С. 133198 - 133198

Опубликована: Дек. 10, 2023

Язык: Английский

---

Bimetallic (Cu, Zn) ZIF-derived S-scheme heterojunction for efficient remediation of aqueous pollutants in visible light/peroxymonosulfate system

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 330, С. 122539 - 122539

Опубликована: Фев. 26, 2023

Язык: Английский

---

High-valent cobalt-oxo species triggers singlet oxygen for rapid contaminants degradation along with mild peroxymonosulfate decomposition in single Co atom-doped g-C3N4

Chemical Engineering Journal, Год журнала: 2023, Номер 471, С. 144531 - 144531

Опубликована: Июнь 30, 2023

Язык: Английский

---