Single-atom copper embedded in two-dimensional MXene toward peroxymonosulfate activation to generate singlet oxygen with nearly 100% selectivity for enhanced Fenton-like reactions

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 324, P. 122245 - 122245

Published: Dec. 1, 2022

Language: Английский

---

Single-Atom MnN₅ Catalytic Sites Enable Efficient Peroxymonosulfate Activation by Forming Highly Reactive Mn(IV)–Oxo Species

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(10), P. 4266 - 4275

Published: Feb. 27, 2023

Four-nitrogen-coordinated transitional metal (MN4) configurations in single-atom catalysts (SACs) are broadly recognized as the most efficient active sites peroxymonosulfate (PMS)-based advanced oxidation processes. However, SACs with a coordination number higher than four rarely explored, which represents fundamental missed opportunity for chemistry to boost PMS activation and degradation of recalcitrant organic pollutants. We experimentally theoretically demonstrate here that five-nitrogen-coordinated Mn (MnN5) more effectively activate MnN4 sites, by facilitating cleavage O–O bond into high-valent Mn(IV)–oxo species nearly 100% selectivity. The high activity MnN5 was discerned be due formation higher-spin-state N5Mn(IV)═O species, enable two-electron transfer from organics through lower-energy-barrier pathway. Overall, this work demonstrates importance numbers informs design next-generation environmental catalysts.

Language: Английский

---

Almost 100 % electron transfer regime over Fe−Co dual-atom catalyst toward pollutants removal: Regulation of peroxymonosulfate adsorption mode

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 339, P. 123178 - 123178

Published: Aug. 15, 2023

Language: Английский

---

Fe-Mn oxycarbide anchored on N-doped carbon for enhanced Fenton-like catalysis: Importance of high-valent metal-oxo species and singlet oxygen

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 340, P. 123204 - 123204

Published: Aug. 22, 2023

Language: Английский

---

Selective degradation of organic micropollutants by activation of peroxymonosulfate by Se@NC: Role of Se doping and nonradical pathway mechanism

Journal of Hazardous Materials, Journal Year: 2023, Volume and Issue: 452, P. 131202 - 131202

Published: March 15, 2023

Language: Английский

---

Facilely Tuning the First-Shell Coordination Microenvironment in Iron Single-Atom for Fenton-like Chemistry toward Highly Efficient Wastewater Purification

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(37), P. 14046 - 14057

Published: Sept. 2, 2023

Precisely identifying the atomic structures in single-atom sites and establishing authentic structure-activity relationships for catalyst (SAC) coordination are significant challenges. Here, theoretical calculations first predicted underlying catalytic activity of Fe-NxC4-x with diverse first-shell environments. Substituting N C to coordinate central Fe atom induces an inferior Fenton-like efficiency. Then, Fe-SACs carrying three configurations (Fe-N2C2, Fe-N3C1, Fe-N4) fabricate facilely demonstrate that optimized environments significantly promote activity. Specifically, reaction rate constant increases from 0.064 0.318 min-1 as number Fe-N 2 4, slightly influencing nonradical mechanism dominated by 1O2. In-depth unveil modulated Fe-N2C2 Fe-N4 optimize d-band electronic regulate binding strength peroxymonosulfate on sites, resulting a reduced energy barrier enhanced The stability actual hospital sewage treatment capacity also showed strong dependency. This strategy local engineering offers vivid example modulating SACs well-regulated environments, ultimately maximizing their

Language: Английский

---

Enhanced Interfacial Electron Transfer by Asymmetric Cu‐O_v‐In Sites on In₂O₃ for Efficient Peroxymonosulfate Activation

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(11)

Published: Jan. 17, 2023

Enhancing the peroxymonosulfate (PMS) activation efficiency to generate more radicals is vital promote Fenton-like reaction activity, however, how PMS adsorption and accelerate interfacial electron transfer boost its kinetics remains a great challenge. Herein, we prepared Cu-doped defect-rich In2 O3 (Cu-In2 /Ov ) catalysts containing asymmetric Cu-Ov -In sites for in water purification. The intrinsic catalytic activity that side-on configuration of O-O bond (Cu-O-O-In) at significantly stretches length. Meanwhile, increase density near Fermi energy level, promoting faster generating SO4 ⋅- ⋅OH. degradation rate constant tetracycline achieved by Cu-In2 31.8 times than , it shows possibility membrane reactor practical wastewater treatment.

Language: Английский

---

High-efficiency degradation of carbamazepine by the synergistic electro-activation and bimetals (FeCo@NC) catalytic-activation of peroxymonosulfate

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 338, P. 123064 - 123064

Published: July 3, 2023

Language: Английский

---

Were Persulfate-Based Advanced Oxidation Processes Really Understood? Basic Concepts, Cognitive Biases, and Experimental Details

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(24), P. 10415 - 10444

Published: June 7, 2024

Persulfate (PS)-based advanced oxidation processes (AOPs) for pollutant removal have attracted extensive interest, but some controversies about the identification of reactive species were usually observed. This critical review aims to comprehensively introduce basic concepts and rectify cognitive biases appeals pay more attention experimental details in PS-AOPs, so as accurately explore reaction mechanisms. The scientifically summarizes character, generation, different species. It then highlights complexities analysis electron paramagnetic resonance, uncertainties use probes scavengers, necessities determination scavenger concentration. importance choice buffer solution, operating mode, terminator, filter membrane is also emphasized. Finally, we discuss current challenges future perspectives alleviate misinterpretations toward mechanisms PS-AOPs.

Language: Английский

---

Cu-doped CoOOH activates peroxymonosulfate to generate high-valent cobalt-oxo species to degrade organic pollutants in saline environments

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 340, P. 123224 - 123224

Published: Aug. 25, 2023

Language: Английский

---