Constructing Nano‐Heterostructure with Dual‐Site to Boost H2O2 Activation and Regulate the Transformation of Free Radicals DOI

Denghui Shang,

Siyu Wang, Jialu Li

et al.

Small, Journal Year: 2024, Volume and Issue: 20(31)

Published: March 10, 2024

Abstract A major issue with Fenton‐like reaction is the excessive consumption of H 2 O caused by sluggish regeneration rate low‐valent metal, and how to improve activation efficiency has become a key in current research. Herein, nano‐heterostructure catalyst (1.0‐MnCu/C) based on nano‐interface engineering constructed supporting Cu MnO carbon skeleton, its kinetic for degradation tetracycline hydrochloride 0.0436 min −1 , which 2.9 times higher than that Cu/C system (0.0151 ). The enhancement removal results from introduced Mn species can aggregate transfer electrons sites through electron bridge Mn−N/O−Cu, thus preventing 2+ oxidizing form •− facilitating reduction generating more reactive oxygen ( 1 ·OH) stronger oxidation ability, resulting utilization 1.9 as much Cu/C. Additionally, good stable practical application capacity different bodies demonstrates it great potential environmental remediation.

Language: Английский

Nanoconfinement steers nonradical pathway transition in single atom fenton-like catalysis for improving oxidant utilization DOI Creative Commons
Yan Meng,

Yu-Qin Liu,

Chao Wang

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: June 22, 2024

Abstract The introduction of single-atom catalysts (SACs) into Fenton-like oxidation promises ultrafast water pollutant elimination, but the limited access to pollutants and oxidant by surface catalytic sites intensive consumption still severely restrict decontamination performance. While nanoconfinement SACs allows drastically enhanced reaction kinetics, detailed regulatory mechanisms remain elusive. Here, we unveil that, apart from local enrichment reactants, pathway shift is also an important cause for reactivity enhancement nanoconfined SACs. electronic structure cobalt site altered confining it within nanopores mesostructured silica particles, which triggers a fundamental transition singlet oxygen electron transfer 4-chlorophenol oxidation. changed accelerated interfacial mass render system up 34.7-fold higher degradation rate raised peroxymonosulfate utilization efficiency (from 61.8% 96.6%) relative unconfined control. It demonstrates superior other electron-rich phenolic compounds, good environment robustness, high stability treating real lake water. Our findings deepen knowledge catalysis may inspire innovations in low-carbon purification technologies heterogeneous applications.

Language: Английский

Citations

48
Application of 3D hierarchical porous NiCo-spinel nanosheet array for enhancement of synergistic activation of peroxymonosulfate: Degradation, Intermediates, mechanism and degradation pathway of tetracycline DOI
Yuan Pan, Xiansheng Zhang, Ting Wu

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 481, P. 148506 - 148506

Published: Jan. 4, 2024

Language: Английский

Citations

40
Ce-doped CuCoO2 delafossite with switchable PMS activation pathway for tetracycline degradation DOI

Fan Li,

Jiahao Wei,

Dongbo Wang

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 481, P. 148633 - 148633

Published: Jan. 12, 2024

Language: Английский

Citations

37
Atomic‐Level Engineered Cobalt Catalysts for Fenton‐Like Reactions: Synergy of Single Atom Metal Sites and Nonmetal‐Bonded Functionalities DOI

Zhong‐Shuai Zhu,

Yantao Wang, Xiaoguang Duan

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(32)

Published: April 30, 2024

Abstract Single atom catalysts (SACs) are atomic‐level‐engineered materials with high intrinsic activity. Catalytic centers of SACs typically the transition metal (TM)–nonmetal coordination sites, while functions coexisting non‐TM‐bonded functionalities usually overlooked in catalysis. Herein, scalable preparation carbon‐supported cobalt‐anchored (CoCN) controlled Co─N sites and free functional N species is reported. The role metal‐ nonmetal‐bonded for peroxymonosulfate (PMS)‐driven Fenton‐like reactions first systematically studied, revealing their contribution to performance improvement pathway steering. Experiments computations demonstrate that 3 C plays a vital formation surface‐confined PMS* complex trigger electron transfer promote kinetics because optimized electronic state Co centers, nonmetal‐coordinated graphitic act as preferable pollutant adsorption additional PMS activation accelerate transfer. Synergistically, CoCN exhibits ultrahigh activity p ‐hydroxybenzoic acid oxidation, achieving complete degradation within 10 min an turnover frequency 0.38 −1 , surpassing most reported materials. These findings offer new insights into versatile inspire rational design high‐performance complicated heterogeneous systems.

Language: Английский

Citations

30
Oxygen Doping Cooperated with Co‐N‐Fe Dual‐Catalytic Sites: Synergistic Mechanism for Catalytic Water Purification within Nanoconfined Membrane DOI Creative Commons
Ziwei Wang,

Zhigang Yi,

Lok Wing Wong

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(30)

Published: May 14, 2024

Abstract Atom‐site catalysts, especially for graphitic carbon nitride‐based represents one of the most promising candidates in catalysis membrane water decontamination. However, unravelling intricate relationships between synthesis‐structure–properties remains a great challenge. This study addresses impacts coordination environment and structure units metal central sites based on Mantel test, correlation analysis, evolution sites. An optimized unconventional oxygen doping cooperated with Co‐N‐Fe dual‐sites (OCN Co/Fe) exhibits synergistic mechanism efficient peroxymonosulfate activation, which benefits from significant increase charge density at active regulation natural population orbitals, leading to selective generation SO 4 •− . Building upon these findings, OCN‐Co/Fe/PVDF composite demonstrates 33 min −1 ciprofloxacin (CIP) rejection efficiency maintains over 96% CIP removal (over 24 h) an average permeance 130.95 L m −2 h work offers fundamental guide elucidating definitive origin catalytic performance advance oxidation process facilitate rational design separation improved enhanced stability.

Language: Английский

Citations

24
Overcoming metals redox rate limitations in spinel oxide-driven Fenton-like reactions via synergistic heteroatom doping and carbon anchoring for efficient micropollutant removal DOI
Jinwen Hu,

Huabo Gong,

Kaixing Fu

et al.

Water Research, Journal Year: 2024, Volume and Issue: 261, P. 122020 - 122020

Published: June 29, 2024

Language: Английский

Citations

20
Pilot-scale and large-scale Fenton-like applications with nano-metal catalysts: from catalytic modules to scale-up applications DOI

Haoyun Lu,

Lifei Hou, Yang Zhang

et al.

Water Research, Journal Year: 2024, Volume and Issue: 266, P. 122425 - 122425

Published: Sept. 10, 2024

Language: Английский

Citations

20
Highly efficient micropollutant decomposition by ultrathin amorphous cobalt-iron oxide nanosheets in peroxymonosulfate-mediated membrane-confined catalysis DOI
Muhammad Bilal Asif, Seok‐Jin Kim, Thien S. Nguyen

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 485, P. 149352 - 149352

Published: Feb. 14, 2024

Language: Английский

Citations

19
Polymeric products deactivate carbon-based catalysts in catalytic oxidation reactions DOI
Pijun Duan,

Jiu-Yun Liu,

Lei Chen

et al.

Nature Water, Journal Year: 2025, Volume and Issue: 3(2), P. 178 - 190

Published: Jan. 17, 2025

Language: Английский

Citations

3
Data‐Driven Accelerated Discovery Coupled with Precise Synthesis of Single‐Atom Catalysts for Robust and Efficient Water Purification DOI Creative Commons

Kengqiang Zhong,

Feng Yu, Di Zhang

et al.

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 31, 2025

Abstract The development of advanced catalysts frequently employs trial‐and‐error methods and is lack highly controlled synthesis, resulting in unsatisfactory efficiency performance. Here we propose a data‐driven prediction coupled with precise synthesis strategy to accelerate the single‐atom (SACs) for efficient water purification. approach enables rapid screening high‐performance SACs from 43 metals‐N 4 structures comprising transition main group metal elements, followed by validation structural modulation improved performance through controllable hard‐template method. Impressively, well‐designed Fe‐SAC high loading Fe‐pyridine‐N sites (~3.83 wt %) mesoporous structure, exhibits ultra‐high decontamination (rate constant 100.97 min −1 g −2 ), representing best Fenton‐like activities sulfonamide antibiotics date. Furthermore, optimized shows excellent robust environmental resistance cyclic stability almost 100 % degradation 100‐h continuous operation. Density functional theory calculations reveal that can reduce energy barrier intermediate O* formation, rate‐determining step, selective generation singlet oxygen. integration method provides novel paradigm field as well other important fields including sustainable catalysis.

Language: Английский

Citations

2