ACS Applied Nano Materials
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2023
·
IF 5.9
Shanyi Wang,Weihao Jin,Yujia Wu,Wanzhen Li,Yugui Tao,Jun Wang,Kai Yang,Weiwei Zhang,Lin Gui,Fei Ge
Drug-resistant bacterial infections pose a significant threat to global public health. Furthermore, the formation of biofilms makes traditional antibiotic treatments significantly less effective in killing multidrug-resistant (MDR) bacteria. In this work, we prepared a molybdenum disulfide (MoS2) nanosphere-based nanocomposite that utilized both photothermal therapy (PTT) and chemodynamic therapy (CDT) for effectively eradicating biofilms. A layer of manganese dioxide (MnO2) was adsorbed onto the surface of the MoS2 nanospheres by redox and electrostatic adsorption methods, and the resulting MoS2/MnO2 were loaded with 2,2′-azobis[2-(2-imidazolin-2-yl)propane]-dihydrochloride (AIPH) to form the MoS2/MnO2-AIPH nanocomposite (MMA). The microenvironment of biofilms is slightly acidic, lacks oxygen, and has a high concentration of glutathione (GSH). The MnO2 was capable of reacting with GSH to deplete it while also generating •OH radicals for CDT. In the presence of NIR light (808 nm), the temperature increase brought about by PTT further enhanced the CDT efficacy synergistically. The results showed that the photothermal conversion efficiency of the MMA was 40.5% at a concentration of 100 μg/mL, and the biofilm eradication rate of both MDR Escherichia coli and MDR Staphylococcus aureus was above 90%. The high bacterial inhibition rate (above 96%), as well as the excellent biosafety and biocompatibility of the MMA nanocomposite enabled it to effectively promote wound healing, which has significant implications in treating bacterial infections and promoting wound healing in clinical settings.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Cong Pan,Wenyu Wang,Yihui Zhang,Jong Chol Nam,Feng Wu,Zhixiong You,Jing Xu,Jinjun Li
Wet scrubbing coupled with adsorption-enhanced heterogeneous advanced oxidation processes (AOPs) are promising approaches to the treatment of chlorinated volatile organic compounds (CVOCs). However, microporous activated carbon-based adsorbents and catalyst supports have the disadvantage of difficult molecule diffusion. Herein, we have demonstrated that porous graphitized carbon (PGC) allowed faster intra-particle diffusion of organic molecules due to its well-developed mesoporous structure. Therefore, a wet scrubbing system containing H 2 O 2 and a PGC-supported FeOCl catalyst has been developed to effectively remove gaseous dichloroethane, trichloroethylene, dichloromethane and chlorobenzene. The scrubber performed well at pH 3.0 using a FeOCl/PGC dosage of 0.2 g/L and initial H 2 O 2 concentration of 40 mM. Its good long-term performance was achieved by replenishing H 2 O 2 to maintain a suitable concentration. The degradation pathways of dichloroethane have been proposed using a combination of intermediate analysis and density functional theory calculations. PGC-supported catalysts may be desirable bifunctional adsorbent-catalyst materials for wet scrubbing of CVOCs.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
·
IF 13.6
Xiupeng Yue,Yongping Shan,Wentao Jiao,Kai Shen,Yaping Zhang
Electrokinetic (EK) delivery followed by thermal activated peroxydisulfate (PS) has turned out to be a potential in situ chemical oxidation technology for soil remediation , but the activation behavior of PS in an electrical coupled thermal environment and the effect of direct current (DC) intervention on PS in heating soil has not been explored. In this paper, a DC coupled thermal activated PS (DC-heat/PS) system was constructed to degrade Phenanthrene (Phe) in soil. The results indicated that DC could force PS to migrate in soil, changing the degradation rate-limiting step in heat/PS system from PS diffusion to PS decomposition, which greatly accelerated the degradation rate. In DC/PS system, 1 O 2 was the only reactive species directly detected at platinum (Pt)-anode, confirming that S 2 O 8 2- could not directly obtain electrons at the Pt-cathode to decompose into SO 4 •- . By comparing DC/PS and DC-heat/PS system, it was found that DC could significantly promote the conversion of SO 4 •- and •OH generated by thermal activation of PS to 1 O 2 , which was attributed to the hydrogen evolution caused by DC that destroys the reaction balance in system. It was also the fundamental reason that DC leaded to the reduction of oxidation capacity of DC-heat/PS system. Finally, the possible degradation pathways of phenanthrene were proposed on the basis of seven detected intermediates.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jingyi Xu,Xianjun Tan,Wenhui Ding,Arturo A. Keller,Yuxiong Huang
To overcome the obstacles of adding oxidants for the decontamination of antibiotics in natural aqueous environment, an external oxidant-free system was developed to in-situ generate reactive oxygen species (ROS) through the activation of dissolved oxygen molecules (O 2 ). Guided by density functional theory (DFT) calculation, cobalt-doped Fe 3 S 4 (Co-Fe 3 S 4 ) nanoflowers were designed and synthesized, which exhibited superior O 2 adsorption and activation ability. Co-Fe 3 S 4 triggered a long-lasting generation of •OH with a high yield of 16.63 μM •OH, which was 3 times higher than that of Fe 3 S 4 . Furthermore, use of Co-Fe 3 S 4 resulted in a 7.33-fold improvement in sulfamethoxazole’s degradation rate and boosted the degradation efficiency from 43% to over 90% in the long-run experiments compared to Fe 3 S 4 . With 18 O 2 isotopic investigations, we quantitatively revealed that •OH was generated via O 2 ′s one-step dissociative adsorption process and the directional electron transfer contributed by structural S(-II). Without the addition of external oxidants (e.g., H 2 O 2 , O 3 ), we have reported an efficient one-step activation of O 2 to generate ROS for effective degradation of antibiotics. Hence, we have provided a new strategy for the control of emerging organics in natural water systems, as well as shed light on the mechanisms of in-situ •OH generation.
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DIAMOND AND RELATED MATERIALS
·
2023
·
IF 4.1
Lin Chai,Yequn Liu,Wenjun Yan,Na Teng,Hongyan Li,Yongqin Qi,Haoliang Huang,Xiaojing Cui,Xianglin Hou,Tiansheng Deng
It is of fundamental and industrial interest to develop a facile method to modify the graphene sheets with heteroatoms such as oxygen (O) and nitrogen (N). Herein, the O and N atoms were discovered to be grafted onto the edges of graphene sheets during the simple grinding process with solvent in air or N 2 atmosphere. By combining X-ray photoelectron spectroscopy (XPS), high resolution transmission electron microscope (HRTEM), energy dispersive X-ray spectrometer (EDS), electron spin resonance spectroscopy (ESR) and H 2 O 2 experiments, we show where the O and N atoms were grafted and how the modification of graphene with O and N atoms occurred. The results showed that the O atoms of air and N atoms of solvent molecules could be bonded to the edges of graphene sheets during the grinding process, which followed the radical reaction mechanism.
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CATALYSIS COMMUNICATIONS
·
2023
·
IF 3.7
Hua Jin,Lin Zhu,Xinyuan Xu,Xiaoyang Yu,Xiaoshu Qu,Zhigang Liu,Yanyan Yang,Yan Gao,Qingling Wei
Herein, we investigated the synergistic degradation of p -chlorophenol by a Ag 3 PO 4 /Fe 3 O 4 /graphene oxide visible light – peroxydisulfate coupled system, probed the effects of catalyst and peroxydisulfate dosage, pH, operating mode, and coexisting substances, identified decomposition intermediates, and proposed plausible degradation pathways. The advantages of the coupled system, namely reduced agent dosage and efficient and thorough degradation, justified the involvement of a precious metal (Ag), while mechanistic investigations suggested the importance of the peroxydisulfate peroxo bond and electron transfer between multivalent metal catalyst components for degradation performance enhancement. Thus, this work facilitates the development of high-efficiency and low-cost combinations of advanced oxidation processes.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Yuxuan He,Jin Qian,Peifang Wang,Taiping Xie,Dionysios D. Dionysiou,Bianhe Lu,Sijing Tang
Advanced strategies for enhancing catalytic performance of catalysts include multi-metal active site exposure, vacancy growth and electronic structure optimization. Here, carbon nanotube-loaded CoSe 2 /FeSe 2 catalysts (Co/Fe-CNT) with multiphase boundaries and embedded selenium vacancies (V Se ) were prepared using a one-step hydrothermal method. The catalysts feature unique electronic structures and abundant active sites, and were found to exhibit unexpectedly high activity and stability in photocatalytic mediated sulphate radical (SR-photo) system, with impressive oxidation capacity for complex matrix polluted water. The spontaneously formed internal electric field strongly promoted charge transport and significantly enhanced the photocatalytic property. The V Se formed at the heterogeneous interface could modulate the surface electronic structure and accelerate the redox cycling of transition metals, thereby accelerating the production of reactive oxygen species and boosting the efficiency of contaminant degradation. This work provides guidance for the design of high-performance catalysts for V Se engineering and expands their potential for application in wastewater purification.
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WATER RESEARCH
·
2023
·
IF 12.8
Peng Xu,Rui Wei,Peng Wang,Xiang Li,Chunyan Yang,Tianyao Shen,Tong Zheng,Guangshan Zhang
Peroxymonosulfate (PMS) activation is a promising technology for water purification, but the removal performance of multiple pollutant matrices and the mechanism for reactive species transformation in the heterogeneous catalytic system remain ambiguous. Herein, a novel CuFe 2 O 4 /diatomite was fabricated for PMS activation to achieve efficient removal of typical pesticides. Uniform distribution of CuFe 2 O 4 on diatomite efficiently alleviated the agglomeration of CuFe 2 O 4 and increased specific surface area (57.20 m 2 g − 1 , 3.8-fold larger than CuFe 2 O 4 ). CuFe 2 O 4 /5% diatomite (5-CFD)/PMS system showed nearly 100% removal efficiency for mixed pesticide solution within 10 min (0.10 g L − 1 5-CFD and 0.40 g L − 1 PMS) and excellent anti-interference performance towards various coexisting substances (≥90% removal efficiency). The electrochemical measurements confirmed that the lower charge transfer resistance of 5-CFD significantly enhanced the electron-transfer capacity between 5-CFD and PMS, accelerating the reactions among Fe(III)/ Fe(II), Cu(II)/ Cu(I), and PMS, further generating •OH (261.3 μM), 1 O 2 (138.8 μM), SO 4 •– (11.8 μM), and O 2 •– . The O in reactive oxygen species didn't originate from dissolved oxygen (DO) but PMS, independent of the low solubility of DO and slow diffusion rate of O 2 in water. Furthermore, the production of 1 O 2 went through the process: PMS → O 2 •– → 1 O 2 , and SO 4 •– could rapidly convert into •OH. The degradation pathways and the evolution of intermediates were proposed by HPLC-QTOF-MS/MS and DFT calculations. QSAR analysis illustrated that the toxicity became lower with the reaction process. This study provides novel insights into the mechanism for pesticide degradation and active species transformation and the anti-interference capability of systems.
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Chem
·
2023
·
IF 23.5
Jie Ding,Zhenyuan Teng,Xiaozhi Su,Kosaku Kato,Yuhang Liu,Ting Xiao,Wei Liu,Lingyue Liu,Qiao Zhang,Xinyi Ren,Jincheng Zhang,Zhaoyang Chen,Ohno Teruhisa,Akira Yamakata,Hongbin Yang,Yanqiang Huang,Bin Liu,Yueming Zhai
By breaking structural symmetry of the single atomic active site, the photocatalytic water oxidation pathway is tuned for highly selective oxidation of CH 4 to CH 3 OH in an aqueous solution. The water oxidation ability and its influence on photocatalytic oxidation of CH 4 over symmetrically coordinated cobalt single atom (Co-4N) on carbon nitride (SC-Co 1 /PCN) and asymmetrically coordinated cobalt single atom (Co-C2N2) on carbon nitride (AC-Co 1 /PCN KOH ) photocatalysts are systematically investigated. A super selectivity of 87.22% for photocatalytic oxidation of CH 4 to CH 3 OH is realized on AC-Co 1 /PCN KOH , which is only 45% on SC-Co 1 /PCN. Moreover, a CH 4 conversion of 2.42% and a CH 3 OH yield of 2.11% are achieved over AC-Co 1 /PCN KOH (200 mg). Combining multiple in-situ characterizations and time-dependent density functional theory calculations, it is revealed that AC-Co 1 /PCN KOH possesses a desired electronic configuration for single-electron transfer water oxidation reaction during photocatalysis, leading to a notably promoted selectivity for CH 4 oxidation to CH 3 OH under illumination.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Lixue Yang,Xiuyan Wang,Shengyan Yin,Xinjian Shi,Li Wang,Ping She,Yudong Song,Zhenning Liu,Hang Sun
Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) have great potential for water treatment. Herein, a 3D nitrogen-doped porous carbon (3D-NPC) aerogel has been prepared by direct ink writing of a hydrogel containing agarose, urea, sodium chloride and hydroxypropyl methylcellulose, and subsequent freeze-drying and pyrolysis. The obtained 3D-printed aerogel exhibits multiple desirable properties including self-supportability, hierarchical porous structure, and good structural stability, and thus can be used as a monolithic catalytic filter in flow-through experiments. The 3D-NPC catalysts have demonstrated excellent PMS-based performances toward degradation of organic dyes and disinfection of bacterial culture. The degradation efficiency of Rhodamine B by 3D-NPC is as high as 97.2% within 5 min and the high degradation efficiency can be sustained for 5 h. Moreover, 100% inactivation of bacteria by 3D-NPC can also be maintained for at least 5 h, which far exceeds those of traditional catalysts. The key reactive species of the 3D-NPC + PMS system is found to be singlet oxygen in both Rhodamine B degradation and antibacterial disinfection, where the non-radical pathway contributes to the majority of the catalytic activity. Our work has innovatively presented a 3D-printed monolithic catalyst for efficient flow-through degradation and disinfection.
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Polymers
·
2023
·Vol. 15
·期 10
·2347
·
IF 5
Shengyun Jiang,Mingshan Yin,Huixue Ren,Yaping Qin,Weiliang Wang,Quanyong Wang,Xuemei Li
Microplastics (MPs) in the water system could easily enter the human body and pose a potential threat, so finding a green and effective solution remains a great challenge. At present, the advanced oxidation technology represented by photocatalysis has been proven to be effective in the removal of organic pollutants, making it a feasible method to solve the problem of MP pollution. In this study, the photocatalytic degradation of typical MP polystyrene (PS) and polyethylene (PE) by a new quaternary layered double hydroxide composite photomaterial CuMgAlTi-R400 was tested under visible light irradiation. After 300 h of visible light irradiation, the average particle size of PS decreased by 54.2% compared with the initial average particle size. The smaller the particle size, the higher the degradation efficiency. The degradation pathway and mechanism of MPs were also studied by GC–MS, which showed that PS and PE produced hydroxyl and carbonyl intermediates in the process of photodegradation. This study demonstrated a green, economical, and effective strategy for the control of MPs in water.Keywords:microplastics;photocatalysis;polystyrene;polyethylene;layered double hydroxide
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 27
·71088-71102
·
IF 5.8
Fan Xinfei,Liu Na,Yang Jia,Yu Yueling,Xu Yuanlu,Song Chengwen,Liu Yanming
Persulfate activation is emerged as an alternative applied in environment remediation, but it is still a great challenge to develop highly active catalysts for efficient degradation of organic pollutants. Herein, a heterogeneous iron-based catalyst with dual-active sites was synthesized by embedding Fe nanoparticles (FeNPs) onto the nitrogen-doped carbon, which was used to activate peroxymonosulfate (PMS) for antibiotics decomposition. The systematic investigation indicated the optimal catalyst exhibited a significant and stable degradation efficiency of sulfamethoxazole (SMX), in which the SMX can be completely removed in 30 min even after 5 cycle tests. Such satisfactory performance was mainly attributed to the successful construction of electron-deficient C centers and electron-rich Fe centers via the short C-Fe bonds. These short C-Fe bonds accelerated electrons to shuttle from SMX molecules to electron-rich Fe centers with a low transmission resistance and short transmission distance, enabling Fe (III) to receive electrons to promote the regeneration of Fe (II) for durable and efficient PMS activation during SMX degradation. Meanwhile, the N-doped defects in the carbon also provided reactive bridges that accelerated the electron transfer between FeNPs and PMS, ensuring the synergistic effects toward Fe (II)/Fe (III) cycle to some extent. The quenching tests and electron paramagnetic resonance (EPR) indicated O 2 ·− and 1 O 2 were the dominant active species during the SMX decomposition. As a result, this work provides an innovative method to construct a high-performance catalyst to active sulfate for organic contaminant degradation.
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