Catalysts
·
2026
·Vol. 16
·期 5
·448
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IF 4.5
Shaomeng Huang,Jiawen Sheng,Yiqing Xu,Liping Wang,Feijian Jing,Qiongqiong He
1O2has significant advantages over free radicals in Fenton-like reactions, but the induction of a single1O2reaction pathway is challenging and is often accompanied by free radical reactions and direct electron transfer pathways. In this study, Zn-O-C/N and Zn-S/O-C/N catalysts were synthesized by controlling the doping of the S element, and the single1O2reaction pathway was successfully induced. Furthermore, Zn-O-C/N performed better than the Zn-S/O-C/N system, with higher phenanthrene (PHE) degradation rates of 76.14% compared to 62.86%. And Zn-O-C/N can achieve a maximum degradation rate of 85.62% under the developed optimization condition. The characterization results revealed that the ZnO active sites are located on the surface of the Zn-O-C/N catalyst and participate in electron mediation together with C-N. ZnS was generated with the doping of S, speculating that a large amount of ZnS with low catalytic activity is generated and occupies the active sites, thereby inhibiting the catalytic activity. Additionally, only1O2was generated in the two systems, without the formation of free radicals and the occurrence of direct electron transfer reaction. However, the Zn-O-C/N catalyst has been proven to have strong stability and a low amount of dissolution, demonstrating environmental safety. This study confirmed the inhibitory effect of S on the activity of the Zn-O-C/N system and provided a synthesis strategy for the catalyst design, which can only induce the1O2reaction pathway.
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Antioxidants
·
2026
·Vol. 15
·期 5
·625
·
IF 8.2
Dongkun Zhao,Xin Wang,Lijuan Wang,Qing Ma,Jingwen Li,Baocheng Xu,Xinjing Dou,Lili Liu
Furfuryl alcohol (FFA), a methanol-soluble and highly specific compound for singlet oxygen (1O2), was used as a1O2trapping agent to reevaluate physical and chemical1O2quenching efficiency of five antioxidants, namely α-tocopherol, butylated hydroxyanisole (BHA), tert-butylhydroquinone (TBHQ), epigallocatechin gallate (EGCG), and quercetin. The total1O2quenching rate constants of α-tocopherol, BHA, TBHQ, EGCG, and quercetin were 2.0 (±0.1) × 109, 1.1 (±0.1) × 108, 5.6 (±0.3) × 108, 4.1 (±0.1) × 108, and 2.2 (±0.1) × 108M−1s−1, respectively. The chemical quenching rate constants of α-tocopherol, BHA, TBHQ, EGCG, and quercetin were 1.4 × 107, 2.0 × 106, 7.7 × 106, 2.0 × 107, and 7.9 × 106M−1s−1, respectively. The percentages of chemical quenching in total1O2quenching were 0.7%, 1.8%, 1.4%, 4.8%, and 3.6% for α-tocopherol, BHA, TBHQ, EGCG, and quercetin, respectively, indicating that the five antioxidants quenched1O2almost exclusively by a physical quenching mechanism. This is the first report on the1O2quenching mechanism of quercetin in methanol solvent. The results of this study will provide theoretical guidance for the application of antioxidants to inhibit edible oil or fat-containing food from photooxidation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Xianglong Yang,Xing Ding,Shengyao Wang,Jin Mao,Ling Cheng,Peiwu Li,Hao Chen
Establishing an ideal photocatalytic system with efficient reactive oxygen species (ROS) generation has been regarded as the linchpin for realizing efficient nitric oxide (NO) removal and unveiling the ROS-mediated mechanism. In this work, a novel oxygen-deficient 0D/1D Bi 3.64 Mo 0.36 O 6.55 /Bi 2 MoO 6 heterojunctions (BMO-12-H) were successfully synthesized under the enlightenment of clarified crystal growth mechanism of bismuth molybdates . Because of the synergies between defect-engineering and heterojunction-construction, BMO-12-H demonstrated improved photoelectrochemical properties and O 2 adsorption capacity, which in turn facilitated the ROS generation and conversion. The enhancement of •O 2 – and 1 O 2 endowed BMO-12-H with strengthened NO removal efficiency (59%) with a rate constant of 12.6*10 -2 min −1 . A conceivable NO removal mechanism dominated by •O 2 – and 1 O 2 was proposed and verified based on the theoretical calculations and in-situ infrared spectroscopy tests, where hazardous NO was oxidized following two different exothermic pathways: the •O 2 – -induced NO → NO 3 – process and the 1 O 2 -induced NO → NO 2 → NO 3 – process. This work offers a basic guideline for accelerating ROS generation by integrating defect-engineering and heterojunction-construction, and provides new insights into the mechanism of efficient NO removal dominated by •O 2 – and 1 O 2 .
研究领域:
环境科学
·
材料科学
·
催化化学
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ENVIRONMENTAL RESEARCH
·
2026
·
IF 8.2
Shuai Xia,Dandi Cai,Qiyuan Zhang,Wei Lu,Donglei Zou,Haiyang Yu,Shuang Zhong
This study aims to enhance singlet oxygen ( 1 O 2 ) generation in visible-light-driven photocatalytic systems through photosensitizer structural regulation and heterojunction engineering. Polyazene zinc phthalocyanine (ZnPPc) was synthesized and coupled with bismuth oxychloride (BiOCl) to construct a BiOCl/ZnPPc composite photocatalyst with a proposed Z-scheme charge transfer pathway. BiOCl/ZnPPc exhibited excellent photocatalytic degradation performance toward the electron-rich antibiotic chlorotetracycline (CTC), with an apparent degradation rate constant of 0.108 min −1 , which was nearly one order of magnitude higher than that of pristine BiOCl (0.011 min −1 ). Reactive species trapping experiments and EPR analysis confirmed that 1 O 2 was the dominant reactive species, contributing up to 72% to CTC degradation. Photoelectrochemical measurements, PL/phosphorescence analysis, and DFT calculations further revealed that BiOCl/ZnPPc promotes 1 O 2 generation through the synergistic contribution of energy transfer and Z-scheme interfacial charge transfer pathways. The porous polymeric structure of ZnPPc alleviates the π–π stacking of monomeric ZnPc and facilitates singlet/triplet exciton generation, thereby enhancing 1 O 2 production via the energy transfer pathway. Meanwhile, the interfacial electronic coupling, built-in electric field, and charge redistribution between BiOCl and ZnPPc promote charge separation and migration, supporting 1 O 2 generation through the electron transfer pathway. In addition, BiOCl/ZnPPc showed good environmental adaptability and cycling stability, while degradation pathway identification, and toxicity assessment indicated that CTC was mainly transformed into less toxic intermediates with partial mineralization under the present reaction conditions. This work provides a feasible strategy for constructing photosensitizer-based heterojunction photocatalysts capable of efficient 1 O 2 generation for antibiotic pollutant degradation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Zhiyuan Feng,Qingling Tian,Qianqian Yang,Yanbo Zhou,Hongying Zhao,Guohua Zhao
The fine-tuning of generating hydroxyl radical ( OH) and singlet oxygen ( 1 O 2 ) was firstly proposed via the selectively photoelectrochemical (PE) reduction of oxygen with Cu-coordinated carbon-nitride-electrode (CuCN). Complete removal efficiency and trace Cu leaching (<0.01 ppm) were achieved during treatment of dimethyl phthalate and atrazine, which were mainly oxidized by OH and 1 O 2 , respectively. Besides, no toxic intermediates was detected in the whole degradation process. The overall oxygen reduction pathway in PE system was demonstrated by electron paramagnetic resonance measurements and quenching tests. The valence band position of CuCN was designed to be more negative (−1.5 V SHE ) for favoring the photocatalytic oxygen reduction. Specifically, Cu-N 2 -C as active sites optimized the Gibbs free energy of intermediate *OOH (ΔG *OOH = 3.99 eV) to improve the reactivity of two-electron oxygen reduction. The CuCN/photoelectrochemical system is applied for treatment of coal water slurry gasification (CWS) wastewater with high concentration of salt. The TOC of CWS was successfully decreased from 127 to 1.9 mg·L −1 in 3 h with a low specific energy consumption of 0.024−0.05 kW·h·g −1 ·TOC −1 . The treated CWS wastewater can be used for recovery and utilization of salt as chemical raw materials. This work highlights the important role of synergistic photo-electro-catalytic effect in regulating the generation of active oxygen species via oxygen reduction pathway, which can be a promising way especially for salinity coal wastewater remediation.
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Jingfeng Li,Zhaoyi An,Junyang Sun,Chunyan Tan,Dan Gao,Ying Tan,Yuyang Jiang
A cationic conjugated polyelectrolyte PPET3-N2 was used as a photosensitizer for photocatalytic oxidation of organic sulfides, including thioanisole, ethyl phenyl sulfide, 4-methylphenyl methyl sulfide, etc., to form sulfoxides with good yields and high selectivity. Oxidation reactions were performed in both batch and microfluidic reactors, where the microfluidic reactor can significantly promote the conversion of photocatalytic oxidation reaction to over 98% in about 8 min. Further studies of the photocatalytic oxidation of the antitumor drug ricobendazole in the microfluidic reactor demonstrate the potential application of the polymer material in organic reactions given its high selectivity, good efficiency, and operation convenience.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Lehui Ren,Mei Chen,Jinxing Ma,Yang Li,Zhiwei Wang
In this study, a novel reactive electrochemical membrane (REM) made of Pd-loaded porous Ti was prepared to achieve ultrafast and efficient oxidation of trace antibiotics sulfamethoxazole (SMX) under anodic polarization. At a current density of 0.5 mA/cm 2 , the percentage removal of SMX by the REM was 96.3% in flow-through mode, with the energy cost ( i.e. , the electrical energy per order of removal, 1.34 Wh/m 3 ) being much lower than the flow-by mode (125.76 Wh/m 3 ) under the same operating condition. Quenching experiments and electron spin resonance spectra demonstrated that singlet oxygen ( 1 O 2 ) was the main reactive oxygen species in the REM system, playing a vital role in SMX degradation. Results of this study indicated that 1 O 2 was mainly generated on the anode via Pd–O 2 interaction that directly activated oxygen, rather than the evolution of 1 O 2 precursors ( e.g ., O 2 − and H 2 O 2 ). The constantly high electrochemical removal of SMX (88.5–91.9%) from actual surface water demonstrated that the matrix effect on the process performance was minimal in realistic applications, highlighting this novel REM to be a viable way to remove trace organic contaminants from surface water.
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ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Juanjuan Li,Xuan Meng,Jian Deng,Di Lu,Xin Zhang,Yanrui Chen,Jundong Zhu,Aiping Fan,Dan Ding,Deling Kong,Zheng Wang,Yanjun Zhao
Nanoparticulate antitumor photodynamic therapy (PDT) has been suffering from the limited dose accumulation in tumor. Herein, we report dually hypoxia- and singlet oxygen-responsive polymeric micelles to efficiently utilize the photosensitizer deposited in the disease site and hence facilely improve PDT’s antitumor efficacy. Tailored methoxy poly(ethylene glycol)-azobenzene-poly(aspartic acid) copolymer conjugate with imidazole as the side chains was synthesized. The conjugate micelles (189 ± 19 nm) obtained by self-assembly could efficiently load a model photosensitizer, chlorin e6 (Ce6) with a loading of 4.1 ± 0.5% (w/w). The facilitated cellular uptake of micelles was achieved by the triggered azobenzene collapse that provoked poly(ethylene glycol) shedding; rapid Ce6 release was enabled by imidazole oxidation that induced micelle disassembly. In addition, the singlet oxygen-mediated cargo release not only addressed the limited diffusion range and short half-life of singlet oxygen but also decreased the oxygen level, which could in turn enhance internalization and increase the intracellular Ce6 concentration. The hypoxia-induced dePEGylation and singlet oxygen-triggered Ce6 release was demonstrated both in aqueous buffer and in Lewis lung carcinoma (LLC) cells. The cellular uptake study demonstrated that the dually responsive micelles could deliver significantly more Ce6 to the cells, which resulted in a substantially improved cytotoxicity. This concurred well with the superior in vivo antitumor ability of micelles in a LLC tumor-bearing mouse model. This study presented an intriguing nanoplatform to realize interactively triggered photosensitizer delivery and improved antitumor PDT efficacy.
研究领域:
药学
·
生物医学工程
·
肿瘤学
·
材料科学
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NEW JOURNAL OF CHEMISTRY
·
2017
·Vol. 41
·期 24
·15187-15194
·
IF 3.269
Jing Wu,Yue Xing,Huan Wang,Hongjing Liu,Mei Yang,Jingli Yuan
Although molecular luminescent probes capable of detecting target analytes in an organelle of interest are especially appreciated, lanthanide complex-based organelle-targetable luminescent probes have rarely been developed. Herein, by using an anthryl-substituted terpyridine derivative, 4′-(9-anthryl)-2,2′:6′,2′′-terpyridine (ATPY), as a singlet oxygen (1O2)-recognition ligand, and a diphenyl-containing β-diketone coligand, 6-(1′,1′′-diphenyl-4′-yl)-1,1,1,2,2,3,3-heptafluoro-4,6-hexanedione (DHH), a new β-diketonate–Eu3+ complex-based luminescent probe, Eu(DHH)3(ATPY), has been designed and synthesized for the time-gated luminescence imaging detection of 1O2 in the mitochondria of living cells. The probe showed only weak luminescence due to the quenching effect of the 9-anthryl group. After the specific reaction of the 9-anthryl group with 1O2, the corresponding endoperoxide derivative that exhibited great quantum yield (Φ = 53%), Eu(DHH)3(EP-ATPY), was formed, accompanied by a remarkable luminescence enhancement. The luminescence response behaviors of Eu(DHH)3(ATPY) to 1O2 were investigated using two different 1O2 reaction systems in aqueous media. In addition, the time-gated luminescence imaging study has demonstrated the applicability of the probe for monitoring the 1O2 generation in 5-aminolevulinic acid (a drug for photodynamic therapy) loaded HepG2 cells with high sensitivity and selectivity. Furthermore, by coloading the probe and a mitochondrial indicator, Mito-Tracker Green, into HepG2 cells, the mitochondria-targetable feature of the probe has also been confirmed by confocal luminescence imaging measurements.
研究领域:
生物化学
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医学影像
·
细胞生物学
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Chen Yang,Xuefeng Hu,Yao Huang,Baiyu Liu,Junhan Yang
We report a rational and scalable synthetic approach to prepare Fe-decorated carbon nitride materials assisted by carbonized polyamine (C-Fe@PDA-CN). The material exhibited extremely high activity and stability for the degradation of 2-mercaptobenzothiazole (MBT) and other organic pollutants (phenol, BPA , MB , and RhB) under visible light irradiation. Furthermore, escape from CN to C-Fe@PDA provides an electron transfer channel to facilitate carrier separation and accelerate the generation of active species, as confirmed by photoluminescence , photoelectrochemical, and electron paramagnetic resonance (EPR). Fe exists in the material coordinated with the pyrrole nitrogen of polydopamine. This coordination structure is conducive to the generation of singlet oxygen ( 1 O 2 ). It is confirmed by steady-state phosphorescence spectroscopy (PH) that 1 O 2 originates from electron transfer. Superoxide radicals are generated by electron transfer and then oxidized into 1 O 2 by holes. The main intermediates of MBT degradation were identified by the LC-MS method, and a possible photocatalytic mechanism based on quenching experiments and EPR tests was proposed.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Han-Qing Zhao,Jun-Sheng Song,Peili Lu,Yang Mu
Singlet oxygen ( 1 O 2 ) is an excellent active species generated in advanced oxidation processes (AOPs) that exhibits high selectivity, long life and wide pH tolerance. Therefore, catalysts for highly efficient and selective generation of 1 O 2 in AOPs would be highly desirable. This study developed a single atom Co-anchored nitrogen‑doped graphene (Co SAC -NG), which showed excellent catalytic performance for peroxymonosulfate (PMS) activation and bisphenol A degradation, with the pseudofirst-order reaction rate constant improved from 8.13 × 10 −4 min −1 without catalyst to 4.42 × 10 −2 min −1 with 5 mg L −1 Co SAC -NG. Mechanism studies indicated that Co SAC -NG selectively enhanced 1 O 2 generation, which was the dominant active specie for pollutant degradation. Moreover, the Co SAC -NG/PMS system effectively reduced the acute toxicity of pollutant, and Co SAC -NG exhibited remarkable cycling stability and negligible leaching. This study develops a new catalyst with high selectivity for 1 O 2 generation and provides a reference for application of single atom catalyst in PMS-based AOPs.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Wei Zhang,Mu Li,Wentao Shang,Mingming Wang,Jianjun Zhang,Feiyun Sun,Mei Li,Xiaoyan Li
Peroxymonosulfate-based advanced oxidation processes (PMS–based AOPs) catalyzed by cobalt nanoparticles have attracted increasing attention due to their special valence electron structure. In this study, nitrogen-doped carbon-encapsulated Co nanoparticle catalysts with core–shell structure were prepared using a simple pyrolysis method at different pyrolysis temperatures (Co@NC-T, T = 650 °C, 750 °C, 850 °C, and 950 °C). Co@NC-750 exhibited excellent activity and high stability for PMS–based removal of methylene blue (MB). More than 99.9 % of MB was degraded with 20 mg/L Co@NC-750 and 100 mg/L PMS within 10 min, displaying good catalytic performance under a wide pH range (3.0–9.0). The quenching tests and electron spin resonance examination results indicated that nonradical, singlet oxygen ( 1 O 2 ), was the major reactive oxygen species in the Co@NC-750/PMS system, other than the radicals. Density functional theory analysis verified that the Co nanoparticles contained heteroatoms N in the carbon layers and provided outstanding activity in activating PMS, as well as good stability, reusability, and versatile adaptability. The analysis of intermediates also revealed that the MB degradation pathway. The results obtained in this study may help to elucidate the application of cobalt species in nonradical–dominated AOPs and stimulate the development of efficient and stable cobalt-based catalysts.
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