Thermodynamic and Kinetic Behaviors of Persulfate-Based Electron-Transfer Regime in Carbocatalysis DOI

Yanhua Peng,

Qiming Zhang, Wei Ren

и другие.

Environmental Science & Technology, Год журнала: 2023, Номер 57(47), С. 19012 - 19022

Опубликована: Авг. 21, 2023

A carbon-based advanced oxidation process is featured for the nonradical electron-transfer pathway (ETP) from electron-donating organic compounds to activated persulfate complexes, enabling it as a green technology selective of pollutants in complex water environments. However, thermodynamic and kinetic behaviors regime had been ambiguous due neglect influence pH on mechanisms. In this study, three kinds were divided ETP regime: (i) physio-adsorption, (ii) adsorption-dominated (oxidation rate slightly surpasses adsorption rate), (iii) oxidation-dominated outpaces rate). The differential attributed physicochemical properties pollutants. For example, hydrophobicity, molecular radius, positive electrostatic potential controlled mass-transfer stage reactants (peroxydisulfate (PDS) organics). Meanwhile, other descriptors, including Fukui index, potential, electron cloud density regulated processes thus kinetics oxidation. Most importantly, pathways these could be altered by adjusting chemistry. This study reveals principles developing efficient systems selectively remove recycle wastewater.

Язык: Английский

Waste-derived biochar for water pollution control and sustainable development DOI
Mingjing He, Zibo Xu, Deyi Hou

и другие.

Nature Reviews Earth & Environment, Год журнала: 2022, Номер 3(7), С. 444 - 460

Опубликована: Июнь 21, 2022

Язык: Английский

Процитировано

471

Biochar co-doped with nitrogen and boron switching the free radical based peroxydisulfate activation into the electron-transfer dominated nonradical process DOI
Jibo Dou, Jie Cheng, Zhijiang Lu

и другие.

Applied Catalysis B Environment and Energy, Год журнала: 2021, Номер 301, С. 120832 - 120832

Опубликована: Окт. 19, 2021

Язык: Английский

Процитировано

315

Heterogeneous activation of persulfate by metal and non-metal catalyst for the degradation of sulfamethoxazole: A review DOI
Daniel T. Oyekunle,

Eman A. Gendy,

Jerosha Ifthikar

и другие.

Chemical Engineering Journal, Год журнала: 2022, Номер 437, С. 135277 - 135277

Опубликована: Фев. 16, 2022

Язык: Английский

Процитировано

246

Nitrogen Vacancy-Modulated Peroxymonosulfate Nonradical Activation for Organic Contaminant Removal via High-Valent Cobalt-Oxo Species DOI
Jingjing Jiang, Ziqing Zhao, Jiaying Gao

и другие.

Environmental Science & Technology, Год журнала: 2022, Номер 56(9), С. 5611 - 5619

Опубликована: Апрель 20, 2022

Rapid generation of high-valent cobalt-oxo species (Co(IV)═O) for the removal organic contaminants has been challenging because low conversion efficiency Co(III)/Co(II) and high activation energy barrier Co(II)-oxidant complex. Herein, we introduced nitrogen (N) vacancies into graphite carbon nitride imbedded with cobalt carbonate (CCH/CN–Vn) in a peroxymonosulfate (PMS)/visible light system to break limitations conventional two-electron transfer path. These N enhanced electron distribution Co 3d orbital lowered cleave O–O bond PMS Co(II)-PMS complex, achieving modulation major active from 1O2 Co(IV)═O. The developed synergistic that exhibited adsorption oxidation showed remarkable selectivity contaminant performance inorganic (Cl–, NO3–, HCO3–, HPO4–) (HA) even practical aqueous matrices (tap water secondary effluent). This study provides novel mechanistic perspective modulate nonradical path refractory treatment via defect engineering.

Язык: Английский

Процитировано

207

A critical review on correlating active sites, oxidative species and degradation routes with persulfate-based antibiotics oxidation DOI
Ning Li, Jingya Ye,

Haoxi Dai

и другие.

Water Research, Год журнала: 2023, Номер 235, С. 119926 - 119926

Опубликована: Март 27, 2023

Язык: Английский

Процитировано

204

Sustainable Fe(III)/Fe(II) cycles triggered by co-catalyst of weak electrical current in Fe(III)/peroxymonosulfate system: Collaboration of radical and non-radical mechanisms DOI
Xianhu Long, Zhaokun Xiong, Rongfu Huang

и другие.

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 317, С. 121716 - 121716

Опубликована: Июль 8, 2022

Язык: Английский

Процитировано

176

Degradation of Organic Contaminants in the Fe(II)/Peroxymonosulfate Process under Acidic Conditions: The Overlooked Rapid Oxidation Stage DOI
Hongyu Dong, Qinghua Xu,

Lushi Lian

и другие.

Environmental Science & Technology, Год журнала: 2021, Номер 55(22), С. 15390 - 15399

Опубликована: Ноя. 3, 2021

The iron(II)-activated peroxymonosulfate [Fe(II)/PMS] process is effective in degrading organic contaminants with a rapid oxidation stage followed by slow one. Nevertheless, prior studies have greatly underestimated the degradation rates of and ignored differences kinetics mechanism these two stages. In this work, we investigated mechanisms under acidic conditions combining stopped-flow spectrophotometric method batch experiments. were rapidly oxidized rate constants 0.18–2.9 s–1 stage. Meanwhile, both Fe(IV) SO4•– active oxidants contributed differently to different Additionally, presence Cl– promoted phenol estradiol but effects Br– humic acid on differed from those contrast, was amounts generated small This work updates fundamental understanding process.

Язык: Английский

Процитировано

173

Degradation of organic pollutants from water by biochar-assisted advanced oxidation processes: Mechanisms and applications DOI
Tao Jiang, Bing Wang, Bin Gao

и другие.

Journal of Hazardous Materials, Год журнала: 2022, Номер 442, С. 130075 - 130075

Опубликована: Сен. 29, 2022

Язык: Английский

Процитировано

168

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

Peizhen Yang,

Yuhan Long, Wenli Huang

и другие.

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 324, С. 122245 - 122245

Опубликована: Дек. 1, 2022

Язык: Английский

Процитировано

155

Origin of the Excellent Activity and Selectivity of a Single-Atom Copper Catalyst with Unsaturated Cu-N2 Sites via Peroxydisulfate Activation: Cu(III) as a Dominant Oxidizing Species DOI
Fan Li,

Zhicong Lu,

Tong Li

и другие.

Environmental Science & Technology, Год журнала: 2022, Номер 56(12), С. 8765 - 8775

Опубликована: Май 12, 2022

As an efficient active oxidant for the selective degradation of pollutants in wastewater, high-valent copper species Cu(III) with persulfate activation has attracted substantial attention some Cu-based catalysts. However, systematic study a catalyst structure and mechanism about peroxydisulfate (PDS) is challenging owing to coexistence multiple Cu structural symmetry PDS. Herein, we anchored atom two pyridinic N atoms synthesize single-atom (CuSA-NC). Experimental characterizations theoretical calculations complemented each other well because uniform atomic sites. The was identified as site, unsaturated Cu-N2 configuration more conductive PDS than saturated Cu-N4 configuration. Benefiting from generation Cu(III), CuSA-NC exhibited obvious anti-interference performance pollutant complex matrix. superior catalytic activity compared that reported catalysts good durability continuous-flow experiment further revealed potential practical applications. This work strongly deepens understanding sites under develops approach actual water purification.

Язык: Английский

Процитировано

148