APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Yuxuan Bai,Ganbing Zhang,Mingwang Liu,Shenghuai Hou,Shuang Zheng,Shu Yang,Chengzhou Zhu,Hui Xu
The electronic state modulation of catalytic active sites governs the oxidation/reduction activation pathway of peroxymonosulfate (PMS), however, directional singlet oxygen ( 1 O 2 ) generation via establishing electron-depleted active center remains challenging. Herein, we propose an innovative axial coordination strategy to engineer atomically dispersed Co-N x moieties on MXene substrates, creating a Co SA -N 2 O 1 /MXene catalyst with precisely modulated electron-depleted sites. The tailored electronic configuration redirects 2,4-dichlorophenol degradation from radical-dominated pathway (Co SA -N 4 counterpart without axial O modulation) to 1 O 2 -driven mechanism with 90.5% contribution, achieving up to 5.1-fold activity enhancement, even outperforming most state-of-the-art Fenton-like systems. The charge density redistribution and greater density of states near Fermi level accelerate PMS activation to selective generation of 1 O 2 . It also demonstrates exceptional environment robustness and high stability for treating real lake water. Our findings advance atomic-level insights into PMS activation and establish a novel paradigm of axial coordination engineering for designing next-generation single-atom catalysts.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Quanzhi Zhang,Tianlin Zhou,Xinchun Ye,Zhi-Xia Zhang,Shaolin Wu,Dezhi Chen
Persulfate-based advanced oxidation process dominated by singlet oxygen ( 1 O 2 ) shows potential for targeted degradation of organic pollutants but the regulation of 1 O 2 generation is still challenging. In this study, N-doped carbon polyhedron-modified Co@N-doped carbon nanotube (NCP/Co@NCNT) were successfully fabricated. The as-obtained NCP/Co@NCNT demonstrated a much enhanced 1 O 2 production in activating peroxymonosulfate (PMS) because of the nanoconfinement effect of metallic Co nanoparticles encapsulated in NCNT, which was further confirmed by density functional theory calculations. The NCP/Co@NCNT/PMS system has excellent catalytic performance and is capable of removing 97 % of carbamazepine (CBZ) in 55 min (Catalyst: 0.1 g/L, CBZ: 20 mg/L, PMS: 0.5 g/L). Quantitative structure–activity relationship (QSAR) analysis uncovered a positive correlation between the oxidation kinetics of organic pollutants and their E HOMO . Specifically, pollutants with higher E HOMO are more easily oxidized in the 1 O 2 -dominated NCP/Co@NCNT/PMS system. Furthermore, the generated intermediates exhibited low toxicity in the system with 1 O 2 as the primary active species. This study offers an effective approach to prepare catalysts for the selective elimination of organic micropollutants in complex water environments.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
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IF 19.7
Xuefei Li,Cheng Cheng,Lixia Yang,Zhenglin Chen,Shuqu Zhang,Jianping Zou
Bi 3+ doping enhances the singlet oxygen ( 1 O 2 ) lifetime. • Oxygen vacancy-rich Bi-Co 3 O 4 catalyst. • Under irradiation, Bi-Co 3 O 4 can efficiently degrade toluene and sterilize bacteria. • Bi-Co 3 O 4 exhibits efficient antibacterial activity, providing new insights for practical indoor air purification Developing efficient materials with excellent adsorption properties and photoactivity is pivotal for photocatalytic abatement of VOCs and bacteria in the air. Herein, Bi 3+ -doped Co 3 O 4 (Bi-Co 3 O 4 ) photocatalysts were successfully synthesized via a one-step hydrothermal-calcination method. Incorporation of Bi 3+ ions induces lattice distortion in Co 3 O 4 , generating oxygen vacancies (OVs), which subsequently modulates the electronic structure of Co 3 O 4 and produces singlet oxygen species ( 1 O 2 ) with a lifetime of 30 min. The Bi-Co 3 O 4 , with a geometric area of 24 cm 2 , achieves complete degradation (100%) of 50 ppm toluene within 30 min and a high mineralization rate of 93.4%. It retains outstanding photocatalytic activity even after multiple usage cycles. Notably, high-reactivity oxygen species at the Bi-Co 3 O 4 interface can effectively eliminate Escherichia coli ( E. coli ) and Staphylococcus aureus ( S. aureus ). This work offers theoretical insights for the design of stable and efficient photocatalysts aimed at improving indoor air quality. Download: Download high-res image (212KB) Download: Download full-size image
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DOI
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2021
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IF 6.789
Huajing Zhou,Dongxiu Lu,Shangquan Fang,Chang Liu,Yuancai Chen,Yongyou Hu,Qijin Luo
A novel heteroatomic N, P and S co-doped core-shell material (MnFe 3 O 4 @PZS) was synthesized by a simple polycondensation hydro-thermal method, and used as the cathode to cooperate with electron-catalysis to activate persulfate (S 2 O 8 2− ) (E-MnFe 3 O 4 @PZS-PDS) for tetracycline (TTC) degradation. Radical scavenger studies demonstrated that non-radicals including atomic H* and singlet oxygen ( 1 O 2 ) rather than sulfate and hydroxyl radicals were the crucial reactive oxygen species (ROS). Electrochemical analysis indicated that Mn doping could promote electro-catalytic process via diverting pathway from four/two-electron to one-electron to generate non-radical H*/ 1 O 2 at the cathode, including one-electron oxygen reduction reaction (1e-ORR) ( O 2 → 1 O 2 ), and one-electron hydrogen reduction reaction (1e-HRR) ( H 2 O + e − → H ∗ ) , as evidenced by the lowest onset potential (0.072 V) together with electron transfer number (n = 1.65). Besides, the regeneration/reduction of Fe Ⅱ/Ⅲ /Mn Ⅱ/Ⅲ/Ⅳ and persulfate will not cause excessive consumption of electron and chemicals due to that could directly get the electron individually from the cathode and anode , and finally TTC could be completely degraded with low energy consumption (0.655 kWh m −3 ). This study provides new insights into the direct single electron activating PDS to produce non-radical H*/ 1 O 2 via core-shell catalytic MnFe 3 O 4 @PZS, and displays a promising application in wastewater treatment .
研究领域:
环境科学
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电化学
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催化材料
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Tianyao Shen,Xiaojing Wang,Jiaqin Li,Peng Xu,Chunyan Yang,Peng Wang,Guangshan Zhang
Antibiotics in surface water adversely affect food safety and aquatic ecosystem, which hinder biological water treatment , and advanced oxidation technology (AOPs) is of great significance. This study achieved nitroimidazole antibiotic metronidazole (MNZ) removal in a dielectric barrier discharge plasma (DBDP) process. A ternary Bi 2 Mn 4 O 10 /NiF (BMON) was synthesized via microwave-assistant to enhance the DBDP process. Compared with Bi 2 Mn 4 O 10 , BMON has a more stable structure with lower ion dissolution but higher oxygen vacancy (Vö) content. The DBDP process generates active species, and O 2 ⋅ − acts as an intermediate in forming 1 O 2 ⋅ − to degrade MNZ through multipath. The cycle of lattice oxygen (O L )/O 2 and M n+ /M (n−1)+ maintain the charge balance on the BMON surface, during which the transformation of Vö and 1 O 2 improve the catalytic efficiency. Furthermore, MNZ possible degradation pathways were proposed by DFT calculations and ESI-QTOF-MS detection. The DBDP/BMON process exhibited great potential for heterogeneous catalytic in nitroimidazole antibiotic degradation.
研究领域:
环境科学
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化学工程
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等离子体技术
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DOI
高影响因子
WATER RESEARCH
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2022
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IF 13.4
Wenxiao Zheng,Yingkai Chen,Hengyi Fu,Zhang Yan,Zhenchao Lei,Weijian Duan,Chunhua Feng
The generation of chlorinated byproducts during the electrochemical oxidation (EO) of Cl − -laden wastewater is a significant concern. We aim to propose a concept of converting reactive species (e.g., reactive chlorines and HO • resulting from electrolysis) into 1 O 2 via the addition of H 2 O 2 , which substantially alleviates chlorinated organic formation. When phenol was used as a model organic compound, the results showed that the H 2 O 2 -involving EO system outperformed the H 2 O 2 -absent system in terms of higher rate constants (5.95 × 10 −2 min −1 vs. 2.97 × 10 −2 min −1 ) and a much lower accumulation of total organic chlorinated products (1.42 mg L −1 vs. 8.18 mg L −1 ) during a 60 min operation. The rate constants of disappearance of a variety of phenolic compounds were positively correlated with the Hammett constants ( σ ), suggesting that the reactive species preferred oxidizing phenols with electron-rich groups. After the identification of 1 O 2 that was abundant in the bulk solution with the use of electron paramagnetic resonance and computational kinetic simulation, the routes of 1 O 2 generation were revealed. Despite the consensus as to the contribution of reaction between H 2 O 2 and ClO − to 1 O 2 formation, we conclude that the predominant pathway is through H 2 O 2 reaction with electrogenerated HO • or chlorine radicals (Cl • and Cl 2 • − ) to produce O 2 • − , followed by self-combination. Density functional theory calculations theoretically showed the difficulty in forming chlorinated byproducts for the 1 O 2 -initiated phenol oxidation in the presence of Cl − , which, by contrast, easily occurred for the Cl • -or HO • -initiated phenol reaction. The experiments run with real coking wastewater containing high-concentration phenols further demonstrated the superiority of the H 2 O 2 -involving EO system. The findings imply that this unique method for treating Cl − -laden organic wastewater is expected to be widely adopted for generalizing EO technology for environmental applications.
研究领域:
环境科学
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化学工程
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Sainan Wang,Chao Yuan,Wei Chen,Yifan Niu,Yexi Yan,Fan Li,Hongmei Jiang
A series of CuO@g-C 3 N 4 composites with different contents of g-C 3 N 4 and different morphologies of CuO have been designed and prepared by hydrothermal method and applied to activate peroxymonosulfate (PMS) for the removal 2,4,6-trichlorophenol (2,4,6-TCP). The results showed that 3D spherical shape CuO-1@g-C 3 N 4 -3, being able to activate PMS to produce a large amount of singlet oxygen ( 1 O 2 ), not only had good catalytic performance, but also reduced the dissolution of Cu 2+ . By comparing the morphological characteristics, catalytic performance, free radical species, decomposition rate of PMS and surface properties of three kinds of CuO, the generation mechanism of 1 O 2 and key reasons of CuO for producing 1 O 2 were deeply explored and finally deduced. Besides, under the conditions of initial pH 7.0, catalyst dosage 50 mg·L −1 , PMS dosage 0.3 mmol·L −1 and initial concentration of 2,4,6-TCP 10 mg·L −1 , the removal rate of 2,4,6,-TCP reached 94 % at 25 min in the first cycle, and 85 % in the fifth cycle. When CuO-1@g-C 3 N 4 was applied in actual water samples, 65 % of 2,4,6-TCP was removed in the Yangtze River, and 60 % of 2,4,6-TCP in Xuanwu and Yueya Lake in 40 min. Quenching experiments and electron paramagnetic resonance (EPR) were used to indentify active species during degradation process and the degradation intermediates of 2,4,6-TCP and possible degradation pathways were determined and proposed by high performance liquid chromatography-time of flight-mass spectrometry (HPLC-TOF-MS 2 ). This study shed light on the 1 O 2 generation mechanism of catalyst and provided theoretical basis and guidance for the design of 1 O 2 catalysts rich in non-radical active species.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Peidong Hong,Zijian Wu,Dandan Yang,Kaisheng Zhang,Junyong He,Yulian Li,Chao Xie,Wu Yang,Ya Yang,Lingtao Kong,Jinhuai Liu
Singlet oxygen ( 1 O 2 ) is an electrophilic species that has great selectivity for breaking down electron-rich refractory organic pollutants. However, in most cases, 1 O 2 plays a minor role in the Fenton-like process due to its low yield, the contributions of which are usually covered by free radicals. Here, we provide the first report on a type of hollow amorphous Co/C composites prepared for the efficient generation of 1 O 2 to degrade oxytetracycline (OTC) selectively in the Fenton-like system. The optimized Co/C samples (Co/C-3) obtained the best degradation performance of OTC near to 100% under neutral conditions, along with satisfactory reusability and stability. Additionally, it exhibited a high anti-interference capacity for inorganic anions and natural organic matter s in the different water qualities. XPS spectrum revealed that the electron cycle of ≡Co 2+ -O-C/H and ≡Co 3+ -O-C/H played a vital effect on the formation of 1 O 2 . Quenching experiments and EPR testing further verified that 1 O 2 converted from ·O 2 – was the dominant oxidative species, and no hydroxyl radical (·OH) appeared in this reaction. Moreover, the results of the Fukui function and T.E.S.T (Toxicity Estimation Software Tool) analysis provided significant assistance in the exploration of degradation pathways and ecological risks of OTC and its intermediates.
研究领域:
环境科学
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材料科学
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污染控制
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DOI
高影响因子
Biomedicines
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2021
·Vol. 9
·期 3
·271
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IF 6.081
Qingjun Kong,Qingzhi Zeng,Jia Yu,Hongxi Xiao,Jun Lu,Xueyan Ren
Resveratrol dimers have been extensively reported on due to their antioxidative activity. Previous studies revealed that resveratrol dimer has been shown to selectively quench singlet oxygen (1O2), and could protect DNA from oxidative damage. The mechanism of resveratrol dimers protecting DNA against oxidative damage is still not clear. Therefore, in this project, the reactants and products of resveratrol dimers protecting guanine from oxidative damage were qualitatively monitored and quantitatively analyzed by UHPLC-QTOF-MS2and UHPLC-QQQ-MS2. Results showed that when guanine and resveratrol dimers were attacked by1O2, mostly resveratrol dimers were oxidized, which protected guanine from oxidation. Resveratrol dimers’ oxidation products were identified and quantified atm/z467.1134 [M-H]−and 467.1118 [M-H]−, respectively. The resorcinol of resveratrol dimers reacted with singlet oxygen to produce p-benzoquinone, protecting guanine from1O2damage. Therefore, it is hereby reported for the first time that the resorcinol ring is the characteristic structure in stilbenes inhibiting1O2induced-DNA damage, which provides a theoretical basis for preventing and treating DNA damage-mediated diseases.Keywords:resveratrol dimers;antioxidative activity;singlet oxygen quenching;DNA damage
研究领域:
生物化学
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分子生物学
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药理学
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DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
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2026
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IF 8.2
Yaru Li,Heming Wang,Rong Qiao,Dongxu Zhou,Fuyun Deng,Gaoyang Chen,Peixin Mao,Chaolin Yang,Xiaodong Zhang
The coexistence of antibiotics and hexavalent chromium (Cr(VI)) in aquatic environments complicates remediation due to their incompatible transformation pathways. Herein, a Co/N-doped carbon catalyst (CoNC) was prepared to activate peroxymonosulfate (PMS) for co-removal of norfloxacin (NOR) and Cr(VI), achieving 91.69% NOR degradation (k obs = 0.3135 min −1 ) within 60 min and near-complete Cr(VI) reduction (k obs = 0.5098 min −1 ) within 20 min. Mechanistic analysis revealed that NOR degradation was mainly governed by singlet oxygen ( 1 O 2 ) and electron transfer mediated non-radical pathways, while Cr(VI) reduction was facilitated through interfacial electron transfer. Electrons released during NOR oxidation enhanced Cr(VI) reduction and promoted the Co(II)/Co(III) cycle, maintaining PMS activation and 1 O 2 generation. Co–N coordination sites promoted 1 O 2 formation, and the N-doped carbon matrix mediates interfacial electron transfer. This work highlights the potential of CoNC/PMS system for efficient treatment of wastewater co-contaminated with antibiotics and Cr(VI), providing insights into coupled oxidative-reductive mechanisms.
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DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2024
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IF 6.3
Zhihao Zhang,Jing Wang,Huidi Zhang,Yao Deng,Binbin Tan,Jiang Wang,Ting Yang,Wenlei Wang
The strategy of constructing edge sulfur vacancies at cellulose surface interfaces has attracted widespread interest in fields such as electronics, photonics, optoelectronics, electrocatalysis, environmental remediation, and biosensing. In this study, NiCo 2 S 4 (NCS) was modified onto cellulose sulfide nanocrystals (SCNC) with chiral helical structures. Utilizing high energy β Particle bombardment on the surface of photocatalysts induces the generation of edge S vacancies in SCNC, while promoting the formation of heterometallic single-atom clusters (Co n , Ni n ) in NCS. The edge sulfur vacancies on the surface of SCNC exhibit high reactivity and adsorption capacity. The aggregation of Co and Ni at this position can transfer photo generated electrons to the edge sulfur vacancies, thereby protecting the edge sulfur vacancies and prolonging the carrier lifetime. Electrons enriched in edge S vacancies can activate the O–O bond of PMS, thereby achieving efficient degradation of ciprofloxacin (CIP). The degradation kinetics constant of Co n -Ni n /NCS/SCNC-S v /PMS is 1.69 times higher than that of NCS/SCNC/PMS. In addition, electron paramagnetic resonance (EPR) shows that the sample produces a large amount of 1 O 2 during photocatalysis This article constructs a new approach for protecting edge S vacancies with heterogeneous single atom clusters, providing a new perspective for achieving efficient photocatalytic degradation of CIP.
研究领域:
环境科学
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材料科学
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光催化
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Zhiming Sun,Rui Zhu,Tianle Ding,Xiangwei Zhang,Chunquan Li
Persulfate activation technology based on sulfate radicals is currently a hot spot in the field of environmental governance. In our work, α-FeOOH was successful in situ loaded on kaolinite surface through a simple one-step hydrothermal process. The prepared composites were systematically characterized, and the relationship between the structural properties and peroxymonosulfate activation properties was explored. Interestingly, compared to bare α-FeOOH, the introduction of kaolinite in composite induced the transformation of α-FeOOH crystal and affected the morphology, where uniformly dispersed nanoparticles rather than rod-like agglomerated crystals appeared. The received FeOOH/kaolinite composite exhibited admirable adsorption and degradation of ciprofloxacin performance with the removal efficiency of 86.1%, and the degradation rate constant was up to 5.2 times higher than that of bare α-FeOOH. In addition, the main active species in the catalytic oxidation system are surface-bound SO 4 •− , • OH and free 1 O 2 . This work would give a deep insight into the role of natural minerals in composite catalytic materials and the construction of high-efficient mineral-based composite materials.
研究领域:
环境科学
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催化
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材料科学
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DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）