Nature Communications
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2019
·Vol. 10
·期 1
·1-14
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IF 11.878
Wu Qing,He Zhigang,Wang Xia,Zhang Qi,Wei Qingcong,Ma Sunqiang,Ma Cheng,Li Jiyu,Wang Qigang
As the first line of innate immune cells to migrate towards tumour tissue, neutrophils, can immediately kill abnormal cells and activate long-term specific adaptive immune responses. Therefore, the enzymes mediated elevation of reactive oxygen species (ROS) bioinspired by neutrophils can be a promising strategy in cancer immunotherapy. Here, we design a core-shell supramolecular hybrid nanogel via the surface phosphatase triggered self-assembly of oligopeptides around iron oxide nanoparticles to simulate productive neutrophil lysosomes. The cascade reaction of superoxide dismutase (SOD) and chloroperoxidase (CPO) within the bioinspired nanogel can convert ROS in tumour tissue to hypochlorous acid (HOCl) and the subsequent singlet oxygen ( 1 O 2 ) species. Studies on both cells and animals demonstrate successful 1 O 2 -mediated cell/tumour proliferation inhibition, making this enzyme therapy capable for treating tumours without external energy activation.
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ANALYTICA CHIMICA ACTA
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2018
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IF 5.123
Ying Ding,Qingyan Jia,Yongmei Wen,Weimin Liu,Jiechao Ge,Jiasheng Wu,Hongyan Zhang,Pengfei Wang
The distance-dependent based sensing mechanism, such as fluorescence resonance energy transfer (FRET) and surface plasmon resonance (SPR) absorption of gold nanoparticles , has been used widely in visual detection. In this work, we report another distance-dependent detection method for nucleoside triphosphates (NTPs) based on carbon dots (CDs) ( 1 O 2 donor) and 9, 10-diphenylanthracene-2-boronic acid (DABA, 1 O 2 acceptor). The CDs can generate singlet oxygen ( 1 O 2 ) which allows diffusion within 200 nm. Thus, the distance between CDs and DABA decreased through binding of NTPs (<200 nm), leading to absorption changes of DABA under light irradiation due to 1 O 2 trapping. This sensing system ( [email protected] ) has high selectivity for the detection of NTPs due to the double molecular recognition and a linear response in the 0–80 μM concentration range was accomplished with the detection limit as low as 4.35 μM.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Yulong Yuan,Minghua Nie,Caixia Yan,Leliang Wu,Wenbo Dong,Mingjun Ding,Peng Wang
This study investigated for the first time the potential of the novel combination of peroxymonosulfate (PMS) and carbonate (CO 3 2− ) toward bisphenol S (BPS) under solar light irradiation. Compared with the Na 2 CO 3 /PMS and solar/PMS system, the solar/Na 2 CO 3 /PMS system significantly reduces the time required for the degradation of BPS. The excellent removal performance is possible due to the synergistic effect between enhanced light absorption and PMS activation, which accelerated the decomposition of PMS to generate more reactive oxygen species. Scavenging tests and electron paramagnetic resonance analysis revealed that the singlet oxygen ( 1 O 2 ) was the dominant oxidant formed and contributed to BPS elimination with a small proportion of superoxide anion radical (O 2 •– ), rather than sulfate radical (SO 4 •− ) and hydroxyl radical (HO•). The addition of Cl − could promote the degradation of BPS, but the addition of HA and a higher HCO 3 − concentration inhibited this process. The presence of SO 4 2− and NO 3 − slightly promote the degradation of BPS. Besides, the solar/Na 2 CO 3 /PMS system represented significant degradation efficiency in a wide initial pH range (5.02–10.96). Such a system is favorable for the application in actual water matrices such as domestic wastewater, river water, lake water, and tap water. Meanwhile, based on the intermediates identified, the possible degradation pathways of BPS were proposed. In addition, most of the degradation intermediates of BPS were less toxic to different organisms than the parent compound. Moreover, the highly efficient degradation of several typical organic contaminants was also achieved using the solar/Na 2 CO 3 /PMS system under simulated and natural solar light irradiation. This study provides a novel idea and demonstrates the great potential for the elimination of organic pollutants in water.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
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IF 11.357
Lan Tang,Sining Zhou,Fan Li,Lianpeng Sun,Hui Lu
The efficient and selective removal of refractory antibiotics from high-strength antibiotic production wastewater is crucial but remains a substantial challenge. In this study, a novel ozone micronano-bubble (MNB)-enhanced treatment system was constructed for antibiotic production wastewater treatment. Compared with conventional ozone, ozone MNBs exhibit excellent treatment efficiency for oxytetracycline (OTC) degradation and toxicity decrease. Notably, this study identifies the overlooked singlet oxygen (1O2) for the first time as a crucial active species in the ozone MNB system through probe and electron paramagnetic resonance methods. Subsequently, the oxidation mechanisms of OTC by ozone MNBs are systematically investigated. Owing to the high reactivity of OTC toward 1O2, ozone MNBs enhance the selective and anti-interference performance of OTC degradation in raw OTC production wastewater with complex matrixes. This study provides insights into the mechanism of ozone MNB-enhanced pollutant degradation and a new perspective for the efficient treatment of high-concentration industrial wastewater using ozone MNBs. In addition, this study presents a promising technology with scientific guidance for the treatment of antibiotic production wastewater.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2022
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IF 5.876
Shan Xue,Zhilin Xie,Xiaoyu Ma,Yinqi Xu,Shiyu Zhang,Qina Jia,Rui Wan,Haisheng Tao
Carbon-based catalyst-activated persulfate-driven advanced oxidation processes (AOPs) have received great attention for wastewater treatment . Herein, a magnetic Fe-doped activated carbon (FeC 2 O 4 /AC) was successfully prepared via a conventional method using FeC 2 O 4 as an iron source and Zoysia sinica as biomass. FeC 2 O 4 /AC was characterized and used to activate peroxymonosulfate (PMS) for Rhodamine B (RhB) degradation. The influence of various factors on RhB removal was evaluated, including initial pH, temperature, coexisting ions, RhB concentration, PMS concentration and catalyst dosage. Under the optimized condition, the removal efficiency of FeC 2 O 4 /AC for RhB (300 mg/L) reached up to 97% within 150 min. Radical scavenging results and EPR experiments confirm that singlet-oxygen ( 1 O 2 ) was confirmed as the main active species in the degradation of RhB in the FeC 2 O 4 /AC/PMS system. More importantly, the possible route of 1 O 2 generation was revealed: the synergistic effect of Fe species and the activated carbon acts as a crucial part in promoting the PMS activation and contributing to the generation of 1 O 2 . The reaction rate constant ( k obs ) of FeC 2 O 4 /AC is about 7.4 times that of pure AC, and the excellent leaching rate of Fe 2+ (<0.09%) proves that this material is an excellent catalyst. This research on the development of Fe-doped activated carbon with high activity and high stability has profound implications for the effective treatment of organic wastewater.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Hengyu Cai,Jing Zou,Jinbin Lin,Jiawen Li,Yixin Huang,Shuyin Zhang,Baoling Yuan,Jun Ma
Owing to the high peroxide bond dissociation energy (377 kJ mol −1 ), peroxymonosulfate (PMS) is rather difficult to be activated by heat for degrading organic pollutants. This work is the first to add sodium hydroxide (NaOH) to enhance the elimination of acetaminophen in heat/PMS system. Heat/PMS system even possessed a better Performance than heat/peroxydisulfate (PDS) system with the addition of NaOH. Quenching experiments and electron paramagnetic resonance tests demonstrated that singlet oxygen and hydroxyl radical were the primary reactive oxygen species responsible for acetaminophen elimination in NaOH-enhanced heat/PMS system. Singlet oxygen mainly came from the alkaline activation of PMS, while hydroxyl radical was generated from the thermolysis of peroxide bond. Increasing PMS concentration and reaction temperature favored the production of reactive oxygen species and the elimination of acetaminophen. Nine degradation intermediates of acetaminophen were identified by LC/TOF/MS and the corresponding degradation pathways were proposed. Chloride ion significantly accelerated the elimination of acetaminophen, while humic acid and carbonate ion slightly retarded acetaminophen removal. NaOH-enhanced heat/PMS system was highly efficient in eliminating many organic pollutants and more prone to degrading electron-rich organics. This study developed a simple and efficient approach to strengthening the oxidation capacity of heat-activated PMS and highlighted the superiority of PMS to PDS in thermolysis under alkaline conditions.
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Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Xiurong Zhu,Yue Zhang,Wei Yan,Shengjiong Yang,Kun Wu,Gen Wang,Pengkang Jin,Jing Wei
Cupric oxide (CuO) is reported to be an effective catalyst for peroxymonosulfate (PMS) based advanced oxidation process for degrading refractory organic pollutants . In this work, mesoporous CuO nanocage was prepared via calcination of metal-phenolic coordination polymer (Cu-TA). The CuO nanocage exhibited high catalytic activity for PMS activation to degrade bisphenol A (BPA) with a high kinetic rate constant (0.17 min −1 ). The high catalytic activity was attributed to the unique hollow mesoporous structure which renders high specific surface area, high-level exposure of active sites and efficient mass diffusion of pollutants and PMS. Systematic evaluation on BPA removal under different experimental conditions indicated that the mesoporous CuO nanocage was highly active in a wide pH range and resistant to inorganic ions and background organic constituents. Electron paramagnetic resonance tests and chemical scavenging experiments implied that the degradation of BPA was mainly ascribed to singlet oxygen ( 1 O 2 ) with a small contribution from hydroxyl radicals (OH • ). A redox cycle of surface Cu(II)-Cu(I)-Cu(II) was responsible for the production of reactive oxygen species (i.e., 1 O 2 and OH • ). The possible degradation pathway of BPA was proposed according to the intermediates (such as hydroxylated BPA, quinones , phenol, etc.) identified by ultra-performance liquid chromatography-Quadrupole-time of flight mass spectrometer . This work provides a new prospect for engineering the nanostructure of CuO catalyst to maximize its catalytic activity for water purification .
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
·
IF 7.963
Fuwei Sun,Tianhu Chen,Haibo Liu,Xuehua Zou,Peixun Zhai,Ziyang Chu,Daobing Shu,Hanlin Wang,Dong Chen
Occurring naturally siderite (FeCO 3 ) was used as the heterogeneous catalyst to activate peroxodisulfate (PDS) for the degradation of sulfadiazine under different initial pH values. The findings of this system exhibited various ROS (e.g. 1 O 2 , SO 4 − and OH) present during a wide range of pH values. Among them, 1 O 2 could significantly facilitate the initial degradation rate, and the increased pH enhanced the role of 1 O 2 . The factors including initial pH values, siderite dosage, PDS concentration, initial contaminants concentration, and water matrix were discussed. The role of each ROS was investigated through quenching test and electron paramagnetic resonance (EPR). Furthermore, the comprehensive degradation process was proposed based on the LC-MS results. And the cycle test demonstrates the reusability of siderite at a pH of 3. Accordingly, this study is of great significance for understanding the degradation of such sulfonamide pollutants in the siderite/PDS system.
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INORGANIC CHEMISTRY
·
2015
·
IF 4.762
Jingyan Sun,Bo Song,Zhiqiang Ye,Jingli Yuan
Singlet oxygen (1O2) plays a key role in the photodynamic therapy (PDT) technique of neoplastic diseases. In this work, by using a 9,10-dimethyl-2-anthryl-containing β-diketone, 1,1,1,2,2-pentafluoro-5-(9′,10′-dimethyl-2′-anthryl)-3,5-pentanedione (Hpfdap), as a 1O2-recognition ligand, a novel β-diketonate–europium(III) complex that can act as a luminescence probe for 1O2, [Eu(pfdap)3(tpy)] (tpy = 2,2′,2″-terpyridine), has been designed and synthesized for the time-gated luminescence detection of 1O2 in living cells. The complex is weakly luminescent due to the quenching effect of 9,10-dimethyl-2-anthryl groups. After reaction with 1O2, accompanied by the formation of endoperoxides of 9,10-dimethyl-2-anthryl groups, the luminescence quenching disappears, so that the long-lived luminescence of the europium(III) complex is switched on. The complex showed highly selective luminescence response to 1O2 with a remarkable luminescence enhancement. Combined with the time-gated luminescence imaging technique, the complex was successfully used as a luminescent probe for the monitoring of the time-dependent generation of 1O2 in 5-aminolevulinic acid (a PDT drug) loaded HepG2 cells during the photodynamic process. In addition, by coloading the complex and a mitochondrial indicator, Mito-Tracker Green, into HepG2 cells, the specific localization of [Eu(pfdap)3(tpy)] molecules in mitochondria of HepG2 cells was demonstrated by confocal fluorescence imaging measurements.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Guanhan Chen,Wenhui Ding,Wenyi Dong,Hongjie Wang,Shuting Zhu,Tianzhe Liang,Cheng Luo,Yuxiong Huang
The wide occurrence of pharmaceutically active contaminants (PhACs) in aquatic environments has received more and more concern owing to the associated high risks to ecosystems. Even worse, conventional wastewater treatment techniques fail to provide effective decontamination for these emerging contaminants . Herein, we designed and constructed mAg 3 PO 4 @g-C 3 N 4 heterojunction for a persulfate-assisted photocatalytic system (mAg 3 PO 4 @g-C 3 N 4 /PDS/Vis) for the rapid and effective degradation of PhACs. Superior mineralization of CBZ (87.15 %) was achieved within 30-minute treatment with mAg 3 PO 4 @g-C 3 N 4 /PDS/Vis, exhibiting 11-fold enhancement compared to mAg 3 PO 4 /Vis system. Integrating experimental investigations with theoretical calculations, singlet oxygen ( 1 O 2 ) was identified as the key reactive species, while the 1 O 2 -dominated ring-opening pathway contributed significantly to the high mineralization of CBZ. Moreover, mAg 3 PO 4 @g-C 3 N 4 /PDS/Vis showed robust degradation performance of multiple PhACs across various water matrices. Multiple PhACs could be simultaneously degraded with high mineralization efficiency in the wastewater effluent, demonstrating the promising application of mAg 3 PO 4 @g-C 3 N 4 /PDS/Vis for decontaminating emerging contaminants in wastewater treatment .
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Journal of Environmental Chemical Engineering
·
2025
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IF 7.2
Weihao Cong,Lin Zang,Mengting Pan,Liyuan Zhang,Yan Zhao,Weiheng Kong
Singlet oxygen ( 1 O 2 ), a highly reactive oxygen species, possesses significant utility in the domains of chemistry and materials science, with applications encompassing wastewater treatment, advanced battery fabrication and the degradation of organic pollutants. The generation of 1 O 2 is typically facilitated through specific processes such as photocatalytic reactions involving photosensitizers, electron transfer reactions, or enzymatic catalysis. The production of 1 O 2 is challenging and its reactivity is constrained, thereby limiting its generation and applications. This study aims to surmount these limitations by investigating the exceptional capacity of a nanomorphic copper phosphate (Cu 3 (PO 4 ) 2 ) to generate 1 O 2 in no need of light activation. A comprehensive characterization of the micromorphology, physical, and chemical properties of Cu 3 (PO 4 ) 2 was conducted to analyze and evaluate its structural and intrinsic characteristics. Systematic research on the kinetic simulation properties of Cu 3 (PO 4 ) 2 was undertaken to acquire experimental data pertaining to the efficiency and mechanism of the catalytic process, providing a scientific foundation for further optimizing its performance as a catalyst for 1 O 2 generation. This research may pave the way for the development of novel and efficient systems for the generation of effective 1 O 2 .
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ChemPhotoChem
·
2024
·
IF 3
Zhenyan Zhou,Lei Wang,ShouCai Yan,Ziang Liu,Rensong Sun,Yuan Qiao,Engin Umut Akkaya
Cancer cells change their glucose metabolism towards lactic acid production for various defensive and proliferative advantages. Dichloroacetate (DCA) is an inhibitor of a key enzyme and thus, changes back the OX-PHOS to glycolysis ratio. We designed and synthesized a singlet oxygen triggered source of dichloroacetate which releases this inhibitor during photodynamic singlet oxygen generation. Synergistic action of DCA and singlet oxygen results in significant enhancement of photocytotoxicity. The results suggest that this approach could offer significant improvement in the therapeutic outcome of PDT.
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