CHEMOSPHERE
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2023
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IF 8.8
Gangya Cheng,Chen Yuan,Wansheng Ruan,Ben Ma,Xinyu Zhang,Xinjing Yuan,Zhihui Li,Dan Wang,Fei Teng
In this work, Fe-based metal-organic frameworks (Fe-MOFs) are prepared by a simple solvothermal method, in which acetic acid/N, N-dimethylformamide (HAc/DMF) mixture solvents are employed to regulate the particle morphology, exposed facets and ligand defects. At HAc/DMF = 0/50, 5/45 and 8/42 (volume ratio), the irregular particles (MIL-53(Fe)), elongated icosahedrons (5H-MIL-101(Fe)) and icosahedrons (8H-MIL-101(Fe)) are obtained, respectively. Under visible light irradiation (λ > 420 nm) and the addition of sodium persulfate (PS), 5H-MIL-101(Fe) shows the highest degradation activity for tetracycline (TC). Specifically, 80% of TC has been removed by 5H-MIL-101(Fe) within 25 min, and the degradation kinetics rate is 3.03 times higher than that over MIL-53(Fe). The improvement of catalytic activity is mainly attributed to the active facets exposed and ligand defects of 5H-MIL-101(Fe). Density functional theory (DFT) calculation further confirms that the active facets exposed and ligand defects of 5H-MIL-101(Fe) favor the adsorption and activation of PS, benefiting the generation of •SO 4 − . Besides, a probable degradation pathway of TC is proposed based on trapping experiments and liquid chromatography-mass spectrometry (LC-MS) test. Furthermore, the toxicities of intermediates are predicted by the quantitative structure-activity relationship (QSAR) mathematical model. This work demonstrates that visible light enhanced PS activation (Vis-PSA) can more effectively degrade organic pollutants, and this work also provides a simple strategy to precisely regulate ligand defects and actively exposed facets of Fe-MOFs to enhance the adsorption and activation of PS.
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Nature Communications
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2023
·Vol. 14
·期 1
·1-15
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IF 16.6
Gao Wenhui,He Jiuyang,Chen Lei,Meng Xiangqin,Ma Yana,Cheng Liangliang,Tu Kangsheng,Gao Xingfa,Liu Cui,Zhang Mingzhen,Fan Kelong,Pang Dai-Wen,Yan Xiyun
Nanozymes with superoxide dismutase (SOD)-like activity have attracted increasing interest due to their ability to scavenge superoxide anion, the origin of most reactive oxygen species in vivo. However, SOD nanozymes reported thus far have yet to approach the activity of natural enzymes. Here, we report a carbon dot (C-dot) SOD nanozyme with a catalytic activity of over 10,000 U/mg, comparable to that of natural enzymes. Through selected chemical modifications and theoretical calculations, we show that the SOD-like activity of C-dots relies on the hydroxyl and carboxyl groups for binding superoxide anions and the carbonyl groups conjugated with the π-system for electron transfer. Moreover, C-dot SOD nanozymes exhibit intrinsic targeting ability to oxidation-damaged cells and effectively protect neuron cells in the ischemic stroke male mice model. Together, our study sheds light on the structure-activity relationship of C-dot SOD nanozymes, and demonstrates their potential for treating of oxidation stress related diseases.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Zitong Yang,Yunkai Sun,Zexi Hou,Haiyan Yu,Mingxue Li,Yanwei Li,Yude Li,Baoyu Gao,Shiping Xu
Although the effect of Cu 2+ on antibiotic removal during photocatalytic reaction has been studied in depth, there is less known about the effect of antibiotics on Cu 2+ removal. In this study, we report for the first time that, during the photocatalytic purification of sulfamerazine (SMZ) and Cu 2+ combined pollution, Cu 2+ concentration showed an obvious five-stage fluctuation, which was completely different from the simple promotion or inhibition reported in previous studies. By employing HPLC-MS analysis and density functional theory (DFT) calculation, the repeated fluctuation of Cu 2+ concentration was found to be closely related to the SMZ degradation process, mainly resulting from solution pH drop and formation of Cu-containing intermediates which acted as sacrificial agents for Cu 2+ reduction. In addition, compared with the SMZ-free system, the presence of SMZ can greatly enhance the deep removal of Cu 2+ (minimum Cu 2+ concentration was only 0.17 mg/L vs. 1.28 mg/L without SMZ), and there was a wide time interval to ensure the efficient recovery of Cu metal. More interestingly, the in-situ obtained Cu-decorated TiO 2 photocatalyst performed well in water splitting, nitrogen fixation and bacterial sterilization. Results of this study confirmed the great potential of photocatalytic technology in purifying antibiotic-heavy metal combined pollution.
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APPLIED CATALYSIS A-GENERAL
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2023
·
IF 5.5
Yajing Huang,Dingren Ma,Jing Cao,Zhuoyun Tang,Lingling Hu,Yexing Zhang,Huinan Zhao,Dehua Xia,Chun He,Po Keung Wong
A simple hydrothermal method was applied to synthesize a 2D/2D g-C 3 N 4 /Bi 2 WO 6 (CN/BWO) composite photocatalyst for the photocatalytic removal of gaseous methyl mercaptan (CH 3 SH). The layered structure of CN/BWO and the C-O-Bi bonds at the interlayer interface were confirmed by thorough characterization techniques. The C-O-Bi bonds were demonstrated to reduce interlayer charge transfer resistance and inhibit photogenerated electron/hole pairs recombination. Therefore, 0.1-CN/BWO exhibited the highest photocatalytic efficiency for CH 3 SH removal, which was 1.4 times higher than 0.1-CN/BWONF with nanoflower structure, and 5.1 and 1.9 times higher than that of pure g-C 3 N 4 and Bi 2 WO 6 . The photocatalytic oxidation pathway and mechanism for CH 3 SH removal were revealed based on reactive species trapping, electron spin resonance (ESR), and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) tests. This work provides new insights into the design of photocatalysts with high photocatalytic performance and stability for the removal of volatile organic compounds (VOCs).
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Fangmin Wu,Jun Nan,Tianzuo Wang,Zhencheng Ge,Bohan Liu,Meng Chen,Xuesong Ye
The activity and selectivity of the cathode towards electrosynthesis of H 2 O 2 are critical for electro-Fenton process. Herein, nickel-foam modified with N, O co-doped graphite nanosheets (NO-GNSs/Ni-F) was developed as a cathode for highly efficient and selective electrosynthesis of H 2 O 2 . Expectedly, the accumulation of H 2 O 2 at pH= 3 reached 494.2 mg L −1 h −1 , with the selectivity toward H 2 O 2 generation reaching 93.0%. The synergistic effect of different oxygen-containing functional groups and N species on the performance and selectivity of H 2 O 2 electrosynthesis was investigated by density functional theory calculations, and the combination of epoxy and graphitic N (EP + N) was identified as the most favorable configuration with the lowest theoretical overpotential for H 2 O 2 generation. Moreover, NO-GNSs/Ni-F was applied in the electro-Fenton process for p-nitrophenol degradation, resulting in 100% removal within 15 min with the kinetic rate constant of 0.446 min −1 and 97.6% mineralization within 6 h. The efficient removal was mainly attributed to the generation of bulk ·OH. Furthermore, NO-GNSs/Ni-F exhibited excellent stability. This work provides a workable option for the enhancement of H 2 O 2 accumulation and the efficient degradation of pollutants in electro-Fenton system.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Yuancai Lv,Shiyu He,Shuting Liu,Zhendong Yu,Yanting Jiang,Yihui Hu,Yifan Liu,Chunxiang Lin,Xiaoxia Ye,Guifang Yang,Minghua Liu
Doping polymetals on Fe-based catalysts is proved to be an effective way to improve the performance on activating persulfate. In this paper, a highly efficient persulfate activation catalyst (FeCo@MoS 2 ) was successfully synthesized by introducing MoS 2 onto the surface of FeCo nanoboxes. During the activation of PMS the introduced of MoS 2 effectively promoted the formation of free radicals (∙OH, SO 4 · - ), 1 O 2 and Fe(IV). Due to the synergistic effects between Mo and Fe, FeCo@MoS 2 has better catalytic activity (2.01 times larger of defluorination efficiency and 3.91 times larger of the apparent rate constant ( k obs )) than FeCo. Under the optimal conditions (catalyst dosage of 0.2 g L −1 , PMS dosage of 1.0 g L −1 and initial pH 4.0), the perfluorooctanoic acid (PFOA, 10 mg L −1 ) could be degraded in 60 min, with 90.26 ± 2.64% of the defluorination efficiency. The LC- MS results showed that under the attack of free radicals (∙OH, SO 4 · - ), 1 O 2 and Fe(IV), the PFOA underwent step-by-step defluorination process. In addition, the ECOSAR results showed that during the whole degradation of PFOA in FeCo@MoS 2 /PMS system, no highly toxic intermediates was accumulated, suggesting a green degradation process. This work showed new ideas and strategies for studying the influence of polymetallic doping on the catalytic process of PMS multiphase catalytic system.
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ENVIRONMENTAL POLLUTION
·
2023
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IF 8.9
Jyunhong Shen,Antong Shi,Jiahui Lu,Xiangtao Lu,Hongyu Zhang,Zhuwu Jiang
A novel magnetically separable Cu/ZnO/CoFe‒CLDH composite, whose synthesis was optimized using the Taguchi approach, was optimally synthesized by hydrothermally coupling Cu-doped ZnO and calcined CoFe–LDH. The synthesized Cu/ZnO/CoFe‒CLDH was applied to construct a synergistic process of integrating visible-light photocatalysis (VPC) with persulfate activation (PSA) and to degrade bisphenol A (BPA). Various characterizations proved that Cu/ZnO/CoFe‒CLDH possessed excellent physicochemical, optoelectronic and magnetic properties, thereby enhancing the catalytic performance. The Cu/ZnO/CoFe‒CLDH composite achieved highly efficient BPA degradation during the synergistic VPC‒PSA process, and its reaction rate constant (0.74 h −1 ) was 6.17-, 4.11-, and 2.85-fold higher than that of Cu/ZnO, CoFe‒CLDH, and Cu/ZnO/CoFe‒CLDH (VPC only), respectively. Moreover, the effects of the catalyst dosage, initial pollutant concentration , solution pH, persulfate dosage and coexisting ions on BPA degradation were comprehensively investigated. Radical-trapping experiments revealed that the contributions of ·OH, SO 4 · ‒ , ·O 2 − , and 1 O 2 involved in BPA degradation. Based on the intermediates identified by LC/MS, the main BPA degradation pathways were determined, the overall trend of which reflects a decreasing ecotoxicity. This study verified the effectiveness of the synergistic VPC‒PSA process with Cu/ZnO/CoFe‒CLDH, which could be used as a new reference for removing organic micropollutants from water.
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APPLIED SURFACE SCIENCE
·
2023
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IF 6.7
Lixin Wang,Jiahao Sun,Ji'an Sun,Yuchen Yang,Yuge Wang,Ziwei Zhang,Xiyang Jin,Weiyang Lv
Layered double oxides (LDOs)-based materials have received widespread interests in advanced oxidation processes (AOPs) due to their adjustable layered structure and superior stability, while the evolution of LDOs as high-efficiency catalysts is hindered by their easy aggregation and weak conductivity. Here, we report a novel strategy to simultaneously overcome the agglomeration and poor conductivity of LDOs via calcining the mixture of polystyrene microsphere supported MgFeAl-LDH and urea, in which the introduction of hollow structure and nitrogen-doped carbon composition can not only significantly increase the specific surface area to expose more active sites, but also remarkably improve conductivity to accelerate electron transfer, giving rise to the outstanding performance of the final catalyst (HC@LDH-CN) in peroxymonosulfate (PMS) activation. Systematic characterizations and experiments further confirm that O 2 •− radicals play the dominant role in HC@LDO-CN/PMS system, which can altogether remove the model pollutant bisphenol A (BPA) in 10 min with k obs to be 0.403 min −1 . Particularly, the HC@LDO-CN still maintains extraordinary catalytic activity for BPA degradation in an extremely high-salt wastewater (100 mM). Our strategy thereby provides an innovative notion to synthesize efficient PMS-based catalysts for organic pollutant degradation in high saline water.
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Materials
·
2023
·Vol. 16
·期 3
·1169
·
IF 3.4
Qian Wei,Beibei Lu,Qing Yang,Can Shi,Yulan Wei,Minmin Xu,Chenjie Zhang,Yaxian Yuan
Fenton technology is one of advanced oxidation process (AOP) methods to treat wastewater through chemical oxidation. Due to the limitations of classical iron-based catalysts, it is still challenging to find suitable catalysts for Fenton-like reactions. Here, MoS2/Au heterojunctions were successfully synthesized by reduction of chloroauric acid in the solution of layered MoS2prepared by hydrothermal method. As a model molecule, methylene blue (MB) was used as the species to be degraded to evaluate the performance of the catalyst. It was determined by UV–visible spectra that the optimal catalyst can be obtained when MoS2(mg): HAuCl4(wt. % mL) is 2:2. The Fenton-like reaction process was monitored by introducing highly sensitive surface enhanced Raman spectroscopy (SERS). The results show that MB can be degraded by 83% in the first 10 min of the reaction, indicating that MoS2/Au has good catalytic performance. In addition, as a fingerprint spectrum, SERS was used to preliminarily analyze the molecular structure changes during the degradation process. The result showed that C-N-C bond was easier to break than the C-S-C bond. NH2group and the fused ring were destroyed at the comparable speed at the first 30 min. In terms of application applicability, it was showed that MB degradation had exceeded 95% at all the three pH values of 1.4, 5.0, and 11.1 after the reaction was carried out for 20 min. The test and analysis of the light environment showed that the catalytic efficiency was significantly improved in the natural light of the laboratory compared to dark conditions. The possible mechanism based on ·OH and ·O2−from ESR data was proposed. In addition, it was demonstrated to be a first-order reaction from the perspective of kinetics. This study made a positive contribution to broaden of the applicable conditions and scope of Fenton-like reaction catalysts. It is expected to be used as a non-iron catalyst in practical industrial applications. From the perspective of detection method, we expect to develop SERS as a powerful tool for the in situ monitoring of Fenton-like reactions, and to further deepen our understanding of the mechanism.Keywords:MoS2/Au heterojunctions;Fenton-like reaction;methylene blue;surface enhanced Raman spectroscopy
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COLLOIDS AND SURFACES B-BIOINTERFACES
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2023
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IF 5.8
Xinyu Cui,Minghui Li,Lei Tong,Miaojing Li,Xuefeng Tang,Xiaojun Han
Chemodynamic therapy (CDT) is based on the endogenous generation of cytotoxic hydroxyl free radicals (·OH) with high specificity and selectivity between cancer and normal cells. However, its efficacy is often limited by the relatively deficient catalytic activity of nanozymes in the tumor microenvironment (TME). Therefore, the combination of CDT with other strategy to realize synergistic therapy is necessary. Herein, a versatile plasmonic Au/Ag nanorods (abbreviated as Au/Ag NRs) via anisotropic Ag overgrowth on Au nanobipyramids was rationally devised to achieve synergistic nanozyme catalytic therapy and near infrared II (NIR-II) light induced photothermal therapy (PTT) with the guidance of computed tomography (CT) imaging. As TME contains high concentrations of H + and H 2 O 2 , Au/Ag NRs exhibited peroxidase (POD) activity to catalyze H 2 O 2 to produce ·OH, inducing cancer cell death. Meanwhile, Au/Ag NRs showed a preeminent NIR-II photothermal effect. More importantly, the enhanced ·OH generation by in-situ heating up resulting from PTT could conversely inhibit the expression of heat shock proteins (HSPs) to abate their resistance to PTT, realizing self-augmented synergistic effect. The NIR-II photothermally enhanced nanozyme catalytic cancer therapy validly inhibited the cancer proliferation, as demonstrated via both cell and animal assays. Moreover, ideal high-contrast CT imaging was realized, owing to the X-ray attenuation capability of elemental Au. The multifunctional Au/Ag NRs hold potential in oncotherapy with imaging capability, high efficiency and low side effects.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Chengyu Zhang,Zhisheng Yu,Xiangyang Wang,Bobo Wang
In this study, a novel γ-Fe 2 O 3 /biochar (BF γ ) composite by a plant in-situ enrichment and one-step pyrolysis strategy was prepared, which was applied as a photocatalyst to activate peroxymonosulfate (PMS) for the degradation of p-chlorophenol (4-CP) under visible light irradiation (BF γ /PMS/Vis) system. The characterization results exhibited that γ-Fe 2 O 3 with localized carbon doping was evenly embedded in biochar during the pyrolysis. BF γ exhibited better photoresponse properties than biochar (BC) and γ-Fe 2 O 3 . The removal efficiency of this system for 4-CP reached 96.41% under optimal conditions. This system showed high removal efficiency with a wide pH range (3.0–13.0) and under conditions of different organic pollutants . It also showed strong resistance to interference with co-existing inorganic ions and humic acid (HA). Electron paramagnetic resonance (EPR) and radical scavenging experiments revealed that the reactive oxygen species (ROS) in this system included SO 4 - ·, ·OH, ·O 2 - and 1 O 2 . The density functional theoretical (DFT) calculations further revealed the promotion of localized carbon doping in γ-Fe 2 O 3 on electron transfer and photoresponse, including C-O bond (d=1.29 Å), C-Fe bond (d=1.80 Å) and band gap value (E gap < 0.72 eV). This study provides new insights into constructing environmentally-friendly catalysts and the possibility of the solid waste recycling for other wetland plants.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Yanyan Chen,Manlin Zhang,Tiantian Chen,Ganbing Zhang,Hui Xu,Hongwei Sun,Lizhi Zhang
The application of powdered nanoscale zero-valent iron (nZVI) in conventional reactors for water treatment is limited by insufficient mass-transfer and difficult post-separation of catalysts. Herein, a novel microreactor was constructed by anchoring nZVI on the reduced graphene oxide/polypyrrole nanocomposite (rGO/PPy) substrate within the microchannel of a stainless-steel tube through two-step electrodeposition , which catalyzed the Fenton-like reaction to remove > 99% p-nitrophenol (PNP) within 50 s, outperforming traditional batch reactors. The rGO/PPy composite substrate consolidated the adhesion on steel surface, stabilized the nZVI by forming electron-transfer complex, facilitated the decomposition of H 2 O 2 to free •OH, and promoted the redox cycle of Fe(III)/Fe(II) via the electron donating capacity of rGO/PPy. Besides, the significant convection and highly-effective mass transfer within the microreactor also contributed to the ultrafast PNP removal. With acceptable durability, easy re-generation, and scalability, the rGO/PPy/nZVI microreactor is promising for the ultrafast removal of pollutants from water.
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