SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Xue Zhang,Bo Yang,Hui Quan,Haoran Pei,Sheng-Qi Guo
The efficient removal of organic pollutants using singlet oxygen ( 1 O 2 ) represents a pivotal advancement in environmental purification. Despite its potential, the controlled generation of 1 O 2 remains a challenging endeavor. In this study, we present a novel approach whereby methyl/methylene are utilized to modulate the production of 1 O 2 by tungsten trioxide (WO 3 ), thereby enhancing the photocatalytic degradation of persistent pollutants through deep oxidation. Employing a dodecyltrimethylammonium bromide (DTAB)-assisted hydrothermal synthesis, we successfully fabricated WO 3 capable of generating 1 O 2 . This modified WO 3 demonstrates superior performance in the photocatalytic degradation of chloroquine phosphate by facilitating the rapid separation of photo-generated electron-hole pairs, thereby accelerating the degradation process. Furthermore, WO 3 augmented with 1 O 2 exhibits enhanced efficacy in decomposing other challenging organic contaminants, compared to its untreated counterpart. Our findings not only contribute to the advancement of photocatalytic design principles centered on 1 O 2 but also underscore the critical role of controlled 1 O 2 production in the effective eradication of pollutants.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Jian Wei,Zhaokun Xiong,Mengmeng Ao,Zhuang Guo,Jiali Zhang,Bo Lai,Yonghui Song
Fe-based catalysts activating peroxymonosulfate (PMS) for the generation of hydroxyl radicals ( OH) and sulfate radicals (SO 4 − ) have attracted widespread interest to efficient degrade contaminants. However, their limitations, including the leaching of metals and the instability of free radicals, are still thorny issues that plague researchers. In this study, an N-doped graphite catalyst (Fe-NC-4) was developed to activate PMS for the degradation of sulfamethoxazole (SMX). Transmission electron microscopy, X-ray diffraction and Raman spectroscopy found that Fe N active site was evenly distributed in the catalyst, and the iron leached under any experimental conditions was far below the instrument detection limit. Fe-NC-4 performed superior capacity in PMS activation, as evidenced by approximately 100% degradation of SMX after 10 min of treatment. Multiple experiments confirmed that OH, SO 4 − , and superoxide radical (O 2 − ) exerted negligible contribution. The Fe-NC-4/PMS system degraded SMX mainly through non-radical pathway of singlet radical ( 1 O 2 ) and high-valent iron-oxo species ( Fe(Ⅳ) O). Moreover, the Fe-NC-4/PMS system had satisfactory stability in natural water and showed excellent selective oxidation of different contaminants. This work will shed new light on effective PMS activation by Fe-based catalysts to efficiently degrade aqueous contaminants via the non-radical pathway.
研究领域:
环境科学
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催化化学
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Environmental Science-Nano
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2020
·Vol. 7
·期 10
·2982-2994
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IF 7.683
Weijian Duan,Jinglei He,Ziliang Wei,Zongren Dai,Chunhua Feng
The heteroatom-doped, carbon-activated peroxymonosulfate (PMS) system proceeding via the non-radical oxidation pathway involving singlet oxygen (1O2) represents a promising advanced oxidation process (AOP) due to the resistance of 1O2 to background anions in solution. However, the performance level of pollutant removal is not yet satisfied, and the mechanism of 1O2 generation remains elusive. Herein, we report the development for the first time of a unique Si-engaged heteroatom (i.e., N)-doped carbon (Si/N–C) nanomaterial for PMS activation, which exhibits outstanding performance in the removal of various kinds of pollutants and an appreciably wide working pH range of 2.5 to 11. Taking rhodamine B (RhB) as an example, the Si/N–C@PMS system achieved a much higher reaction rate (0.64 min−1) than the Si–C (0.047 min−1), N–C (0.017 min−1), SiO2 (0.021 min−1), and Co3O4 (0.026 min−1; a standard catalyst) systems. In addition, the results of electron spin resonance (ESR) and scavenging experiments solidly support the conclusion that the mechanism of 1O2 generation in this system is via the recombination of superoxide radicals O2˙−, a pathway seldom reported for metal-free, catalyst-activated PMS systems. More importantly, we observed apparent inhibition effects of the anions (e.g., HCO3−, HPO42−, and PO43−) on the degradation performance, inconsistent with many previous reports suggesting that the 1O2-mediated oxidative system possesses a high selectivity toward pollutant degradation in the presence of these anions. Further studies with the anions, including Cl−, HCO3−, and HxPO4(3−x) (x = 0, 1, 2), suggest that the reaction between O2˙− and these anions is the main reason for the abnormal salt effect. This work will deepen the understanding of 1O2 formation via the intermediate of O2˙− and provide a new insight into its salt resistance capacity.
研究领域:
环境化学
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材料科学
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催化
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水处理
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
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IF 9.6
Tancheng Dong,Yang Xiao,Wei Guo,Baojun Liu,Jincheng Mu
Biochar-induced interfacial defects modulate electronic structure of Mn Co spinel. • Complete IBU was removed in 5 min with an apparent reaction rate of 1.08 min −1 . • Interfacial structural defects accelerated redox cycles for boosted 1 O 2 generation. • The micropollutant was removed through a 1 O 2 dominated non-radical pathway. Spinel-based transition metal oxides are potential activators for peroxymonosulfate-based advanced oxidation processes (PMS-AOPs) in water purification, yet their sluggish redox cycling, stemming from poor conductivity, remains a critical limitation. In this work, a distiller's grain-derived porous biochar (BC)-decorated Mn Co spinel nanosheet catalyst (MnCoO x @BC) is developed and applied for PMS activation. The catalyst exhibits high efficacy in degrading ibuprofen (IBU), achieving complete removal within 5 min with an apparent reaction rate constant of 1.08 min −1 ([IBU] = 10 mg L −1 , [catalyst] = 200 mg L −1 , [PMS] = 200 mg L −1 ), which is 18 and 15 times for pristine BC and unsupported MnCoO x , respectively. Characterization and DFT calculation results indicate that the introduction of biochar could improve the conductivity and induce the formation of abundant oxygen defects, which accelerate the redox cycles of Co (III)/Co (II) and Mn (IV)/Mn (III) catalytic centers. This interfacial configuration facilitates the conversion of PMS into peroxysulfate radical (SO 5 • − ) and superoxide radical (O 2 • − ) species, and finally towards singlet oxygen ( 1 O 2 ), establishing a non-radical dominant pathway where 1 O 2 accounts for over 95% of the reactive species contribution. This work presents an effective strategy for developing defect-controlled catalytic interfaces to modulate the d-band center of metal sites and steer the interfacial electron transfer pathway, offering profound insights into non-radical-dominated mechanisms for the degradation of emerging micropollutants. Download: Download high-res image (312KB) Download: Download full-size image
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Xinyuan Wang,Zhuohang Wu,Taozhen Li,Xiaoning Wang,Pijun Duan,Jingwen Pan,Lei Wang
Sulfonamide antibiotics are highly toxic, persistent, and environmentally hazardous, necessitating effective remediation technologies for their removal from aquatic systems. Singlet oxygen ( 1 O 2 ), a selective and pH-tolerant reactive species, has emerged as a key oxidant in persulfate-based advanced oxidation processes (PS-AOPs). Herein, the systematic and novel pathway formation for the 1 O 2 on single Cu atom during PS-AOPs was elucidated. Nitrogen-doped biochar-supported single-atom Cu catalysts featuring low-coordination Cu-N 2 sites (SACu-N 2 @C) were synthesized via calcinating straw biomass, which showed remarkable catalytic efficiency towards sulfamethoxazole (SMX) oxidation even under high-salinity conditions. Results and further elucidated the 1 O 2 formation pathway, where the Cu-N 2 sites adsorbed and interacted the oxygen atom in S O group at the end of peroxymonosulfate (PMS) with lower adsorption energy. This process was accompanied by the generation of two SO 5 •− molecular intermediates, ultimately leading to the formation of 1 O 2 with the lowest energy barrier. Moreover, toxicity tests showed that the degraded SMX solution was ecologically safe with no significant toxic effects on zebrafish, rice and Escherichia coli ( E. coli ). This study provides atomic-level insights into 1 O 2 generation via Cu-N 2 coordination, advancing the design of efficient and environmentally benign Fenton-like systems for antibiotic wastewater treatment.
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
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2026
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IF 5.2
Yuqing Feng,Ziyan Tang,Jiaxian Tan,Hongxia Liu,Yingsen Fang,Shumei Gao,Ping Sun,Hui Wang,Hui Liu
Non-metallic photocatalysts represent a promising avenue for the green remediation of organic wastewater. In this study, O-doped g-C 3 N 4 (OCN) was synthesized using a one-step calcination strategy and synergistically coupled with periodate (PI) under visible light to develop a novel non-radical OCN/PI/Vis photo-Fenton-like system for the efficient degradation of Acid Orange 7 (AO7). Systematic characterization techniques, including transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), ultraviolet-visible diffuse reflectance spectroscopy (UV-Vis DRS) and photoluminescence (PL), along with density functional theory (DFT) calculations, were employed to elucidate the catalyst properties, oxidant adsorption, and reaction mechanisms. The OCN/PI/Vis system achieved a 93.9% removal of AO7 within 20 min and exhibited a reaction rate constant ( k = 1.48 × 10 −1 min −1 ) that was 4.4 times higher than that of the OCN/Vis system, significantly outperforming traditional oxidant-coupled systems (PMS/PDS/H 2 O 2 ). DFT calculations indicated that OCN exhibited an ultra-strong PI adsorption affinity ( E ads = −2.541 eV), leading to the elongation of the PI I-O bond and facilitating its activation. Quenching and electron paramagnetic resonance (EPR) experiments confirmed that singlet oxygen ( 1 O 2 ) is the dominant reactive species. Notably, the system demonstrated excellent anti-interference performance. This work establishes a high-efficiency, metal-free photo-Fenton-like system for dye wastewater treatment and provides a theoretical and experimental foundation for the rational design of g-C 3 N 4 -based PI activators, thereby opening new avenues for PI-based advanced oxidation processes (AOPs) in environmental remediation.
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FOOD CHEMISTRY
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2022
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IF 9.231
Xinxin Zheng,Qing Huang
Astaxanthin (AST) is a natural antioxidant and has been widely applied as a food supplement. While astaxanthin has many isomers, there are few studies comparing its physicochemical properties. In this work, we were concerned about their antioxidant activities against external oxidative stresses, and specifically, the singlet oxygen ( 1 O 2 ) quenching capacities of the representative optical and geometric isomers of astaxanthin were examined. Methylene blue (MB) was used as the photosensitizer to produce 1 O 2 , and 1,3-diphenylisobenzofuran (DPBF) was used to probe 1 O 2 . Our results showed that the 1 O 2 quenching capacities of the optical isomers, including 3 S ,3 ′S , 3 R ,3 ′S , and 3 R ,3 ′R all- trans -astaxanthin, are identical. In contrast, the 1 O 2 quenching capacity of cis -astaxanthin is higher than that of all- trans -astaxanthin. As such, this work provides an effective spectroscopic approach to assessing the antioxidant activities of various forms of astaxanthin against singlet oxygen, and demonstrates the remarkable difference among the geometric isomers.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Junjie You,Chengyang Zhang,Zelin Wu,Zhimin Ao,Weiyi Sun,Zhaokun Xiong,Shijun Su,Gang Yao,Bo Lai
In this paper, a type of Ni metal and Ni 3 ZnC 0.7 alloy nanoparticle catalyst encapsulated in N-doped graphite (NiZn@N-G-900), obtained by derivatization of metal–organic frameworks (MOF), was applied to activate peroxymonosulfate (PMS) to degrade Bisphenol A (BPA) in water. Characterizations and DFT calculations demonstrated that the encapsulation of graphite layer or N-doped graphite layer can not only adjust the surface charge distribution of the catalysts, but also improve the charge transfer ability between the catalyst and the adsorbate. These modifications were beneficial for the adsorption and activation of PMS. Based on the results of the modified radicals scavenging experiments and EPR, a typical 1 O 2 dominated non-radical system was proposed. Due to the characteristics of 1 O 2 , the NiZn@N-G-900/PMS system had strong inorganic anion resistance, high selectivity and satisfactory practical application. Moreover, two pathways of BPA degradation were put forward.
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CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Ningjie Du,Ying Liu,Qiuju Li,Wei Miao,Dandan Wang,Shun Mao
Single-atom catalysts have drawn increasing attention in advanced oxidation due to their unique structure and significant promise in heterogeneous catalysis. Herein, single-atom iron anchored on nitrogen-doped carbon (SAFe-N-C) was synthesized with iron phthalocyanine (FePc) and metal-organic framework (ZIF-8). With thermal treatment and acid leaching, atomically-dispersed Fe-N x sites were successfully formed on the surface of N-C support derived from ZIF-8. The prepared catalyst was demonstrated to activate peroxydisulfate (PDS) for chloramphenicol (CAP) degradation. Compared with N-C, the SAFe-N-C shows 6 times enhanced removal efficiency (from 15.3% to 93.1%) for CAP. Moreover, the catalyst shows high catalytic activity in a wide pH range of 5 to 9 and good resistance to inorganic anions, in which a singlet oxygen-dominated process is found. This study reveals the role of single-atom site in singlet oxygen evolution and offers a new catalytic approach for selective removal of organic pollutants in complex water matrix.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Chencheng Dong,Yan Bao,Tian Sheng,Qiuying Yi,Qiaohong Zhu,Bin Shen,Mingyang Xing,Irene M.C. Lo,Jinlong Zhang
Sulfate-radical (SO 4 − ) based Advanced Oxidation Process (SR-AOP), which is mainly generated from peroxymonosulfate (PMS) activation, is an excellent route for water treatment. Bimetallic nanoparticles have been widely applied in electronic, chemical, biological, and mechanical fields, etc.; however, few researchers have attempted to adopt bimetallic nanoparticles in environmental remediation. Further, in recent years, element molybdenum (Mo) has addressed much more environmental field attention than ever. Although singlet oxygen ( 1 O 2 ) generated commonly in SR-AOPs, its generation mechanism remains controversial. Hence, in this work, bimetallic MoFe/TiO 2 nanospheres were rationally constructed via a facile two-step methodology. Undoubtedly, it exhibited superior performance for the degradation of organic pollutants (e.g., rhodamine, phenol, 4-chlorophenol and sulfadiazine) irradiated by simulated solar light. Both photo-generated electrons and transition metallic redox couples (i.e., Mo 6+ /Mo 4+ , Fe 3+ /Fe 2+ and Mo 4+ /Fe 3+ ) play vital roles in the PMS activation. Distinct from conventional SR-AOPs, sulfate radicals (SO 4 − ), hydroxyl radicals ( OH) and peroxymonosulfate radicals (SO 5 − ) indeed participate in the transformation and generation of singlet oxygen ( 1 O 2 ). With the combination of DFT calculation, the Mo sites on the bimetallic MoFe (110) facet are more favorable to adsorb PMS molecules, then followed by the dissociation of PMS progressing on the Mo sites. Electrons transferring from the Mo atoms to the Fe atoms facilitated the adsorption of the negatively charged HSO 5 - anions, resulting in enhanced PMS activation efficiency. Considering its novelty and generation mechanism, this work highlights the mechanism of 1 O 2 generation from PMS reduction and oxidation simultaneously and furnishes theoretical support for further relevant studies.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Shishu Zhu,Chao Jin,Xiaoguang Duan,Shaobin Wang,Shih-Hsin Ho
Nonradical reactions induced by nanocarbon-driven peroxydisulfate (PDS) activation recently emerge a promising strategy of groundwater remediation or wastewater treatment, whereas the involved reaction pathways remain controversial. We here investigate and differentiate the two representative nonradical mechanisms of PDS activation on graphene-like nanosheets (GNS). The template-induced GNS exhibited a high porosity of over 1200 m 2 g −1 and a few-layered turbostratic structure with graphitic microcrystals. The nonradical oxidation system (aqueous 1 O 2 and nonaqueous electron transfer) of GNS/PDS was highly-reactive, and outperformed graphene- or metal-based activators. Although singlet oxygen ( 1 O 2 ) was detected in the bulk solution, the contribution of 1 O 2 to the entire oxidation were limited (0.004–0.43% and ~6% at neutral and alkaline pH, respectively), determined by chemical probes and steady-state kinetics. Different to the reference product (benzoquinone) of phenol oxidation by photosensitive singlet oxygenation, intermediate product in GNS/PDS was benzoic acid which barely resulted from 1 O 2 oxidation. Furthermore, surface-confined electron transfer was the major oxidation pathway verified by electronic measurement. Surface adsorption rather than hydrophobic effect of organic substrates on GNS accelerated a two-electron transfer. The nonradical oxidation exhibited a dissociation constant ( p Ka)-dependent mechanism because of competitive adsorption with S 2 O 8 2− anions. The findings facilitate a thorough understanding of carbon-catalyzed persulfate activation during in situ chemical oxidation (ISCO) and provide novel insights for the selective removal of aqueous organic contaminants in a nonradical manner.
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ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Jinling Xie,Xiaofang Pan,Chenming Jiang,Li Zhao,Xiaobo Gong,Yong Liu
The activation of persulfate technology using carbon-based materials doped with heteroatoms has been extensively researched for the elimination of refractory pollutants in wastewater. In this study, metal-organic frameworks were utilized as precursors to synthesize P, N dual-doped carbon material (PNC), which was employed to activate peroxymonosulfate (PMS) for the degradation of tetracycline hydrochloride (TCH). The results demonstrated a 90.2% removal efficiency of total organic carbon within 60 min. The significant increase of surface defects on the nitrogen self-doped porous carbon materials anchored with phosphorus promoted the conversion of superoxide radical to singlet oxygen during PMS activation , which was identified as the key active species of PNC/PMS system. Additionally, the enhanced direct electron transfer also facilitated the degradation of TCH. Consequently, TCH was successfully degraded into nontoxic and harmless inorganic small molecules. The findings of this research provide valuable insights into improving the performance of heteroatom-doped carbon materials for pollutant degradation by activating PMS and transforming the non-radical pathway. The results highlight the potential of metal-organic frameworks derived heteroatoms dual-doped porous carbon catalysts for the development of advanced treatment technologies in wastewater treatment .
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