Journal of Materials Chemistry B
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2022
·Vol. 10
·期 42
·8760-8770
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IF 7.571
Zhimin Mo,Xinyuan Pan,Xiaoli Pan,Lin Ye,Han Hu,Qi Xu,Xiaoxi Hu,Zushun Xu,Jie Xiong,Guangfu Liao,Shengli Yang
Fe-based metal–organic frameworks (MOFs) can be used for chemodynamic therapy (CDT) for tumors due to their unique Fenton-like effects and porous and biodegradable nature. The adsorption and transport of small molecule drugs by their structure has attracted much attention. Herein, MnO2@NH2-MIL101(Fe)@Ce6-F127 nanoparticles (MNMCF NPs) were synthesized using a facile solvothermal strategy. The small molecule photosensitizer Ce6 was adsorbed by MOFs to improve the biocompatibility of Ce6 and give it high bioavailability when injected intravenously. When the MNMCF NPs reached the tumor site, Fe-based MOFs exhibited Fenton-like properties, producing ˙OH and showing CDT effects. MnO2 could specifically respond to produce O2 in a tumor microenvironment, thereby improving the tumor hypoxia state and enhancing the efficacy of photodynamic therapy (PDT) by Ce6. Both the in vitro and in vivo experiments showed that the MNMCF-guided CDT/PDT combination therapy could effectively ablate tumors without the drawbacks of poor tolerability and potential long-term side effects. Therefore, the prepared MNMCF NPs can be used as promising candidates for synergistic CDT/PDT tumor therapy.
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Advanced Science
·
2022
·Vol. 9
·期 22
·2201594
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IF 17.521
Rui Yang,Xiaozhong Zheng,Minkai Qin,Binbin Lin,Xiaoyun Shi,Yong Wang
Recently, extensive research efforts have been devoted to drive electrocatalytic water-splitting for hydrogen generation by electricity or solar cells. However, electricity from power grid and the intermittent property of sunlight inevitably brings about environmental pollution and energy loss. Thus, a novelty energy system for simultaneous generating H 2 from solar energy and overcoming the intermittence of sunlight is highly desirable. Herein, a self-powered energy system with solar energy as the sole input energy is successfully assembled by integrated Zn–air batteries with stable output voltage, solar cells, and water splitting electrolyzer to efficient H 2 production. Specially, the Zn–air batteries are charged by the solar cell to store intermitted solar energy as electricity during light reaction. Under unassisted light reaction, the batteries could release electric energy to drive H 2 production. Therefore, the aim for simultaneous generating H 2 and eliminating the restrictions of intermittent sunlight are realized. The solar-to-hydrogen efficiency and solar-to-water splitting device efficiency of the self-powered energy system are up to 4.6% and 5.9%, respectively. This work provides the novel design systems for H 2 production and the usage of renewable energy.
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Asian Journal of Pharmaceutical Sciences
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2022
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IF 9.273
Qiongzhe Ren,Xuefeng Tang,Yi Lu,Qing Li,Zhiqian Liao,Shinan Jiang,Haoli Zhang,Zhigang Xu,Lei Luo
The use of nanocrystal technology to manufacture drug delivery systems intended to enhance therapeutic efficacy has attracted the attention of the pharmaceutical industry. However, the clinical application of nanocrystal drugs for injection is restricted by Ostwald ripening and the large-scale use of stabilizers such as polysorbate and lecithin, which have potential toxicity risks including hemolysis and allergies. Here, we designed an amorphous nanocrystal drug complex (IHNC), which is stabilizer-free and composed of indocyanine green (ICG) framework loading with a chemotherapeutic agent of 10-hydroxycamptothecin (HCPT). Considering the possibility of industrial manufacturing, IHNC was simply prepared with the assistance of ferric ion (III) via supramolecular assembly strategy. The theoretical result of Materials Studio simulation indicated that the prepared ICG-Fe(III) framework showed a stable spherical structure with the appropriate cavity for encapsulating the two drugs of HCPT and ICG with equal mass ratio. The IHNC was stable at physiological pH, with excellent PTT/PDT efficacy, and in vivo probing characteristics. The nanoscale size and reductive stimuli-responsiveness can be conducive to drug accumulation into the tumor site and rapid unloading of cargo. Moreover, such combination therapy showed synergistic photo/chemotherapy effect against 4T1 breast cancer and its tumor inhibition rate even up to 79.4%. These findings demonstrated that the nanocrystal drug delivery strategy could avoid the use of stabilizers and provide a new strategy for drug delivery for combination therapy.
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COLLOIDS AND SURFACES B-BIOINTERFACES
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2022
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IF 5.999
Ruigeng Yang,Yueru Wei,Mengyang Zhao,Mengxiao Shi,Yongxing Zhao,Pengchao Sun
The abuse of antibiotics has led to the emergence of multidrug-resistant bacterial strains worldwide, which greatly threatens human health. In the present work, we developed single-atom catalysts (SACs) with atomically dispersed Fe as catalytic sites (Fe-SACs) to combat multidrug-resistant bacteria by elevating cellular reactive oxygen species (ROS). Our intensive studies confirmed that Fe-SACs were successfully prepared and exhibited excellent catalase (CAT)-, oxidase (OXD)-, and peroxidase (POD)-like activities. To enhance water dispersibility, biosafety and the interactions between the nanodrugs and gram-positive bacteria, phenylboronic acid group-functionalized carboxylated chitosan (CCS-PBA) was coated on the surface of Fe-SACs to yield [email protected] for in vitro and in vivo studies. The synergistic catalytic activity and photothermal activity of [email protected] effectively overcame multidrug-resistant bacterial strains ( MRSA) in vitro and significantly accelerated wound healing in vivo , suggesting the great potential of SACs to overcome infectious disease caused by multidrug-resistant bacteria.
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JOURNAL OF THE ENERGY INSTITUTE
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2022
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IF 6.47
Xinbo Zhu,Haiping Xiong,Jin Liu,Yuting Gan,Zitan Xu,Chunlin Zhou,Yaolin Wang,Ye Jiang,Xin Tu
In this work, Fe–Mn based ternary catalysts (Fe–Mn-X, X = Ce, Co and Cu) were evaluated in the plasma-catalytic oxidation of ethylene oxide (EO) using a cylindrical dielectric barrier discharge (DBD) reactor. The addition of transition metal dopants to the Fe–Mn catalyst significantly improved the performance of plasma-catalyzed EO oxidation compared to the reaction using plasma only and the Fe–Mn catalyst. The highest EO conversion (91.9%) and CO 2 selectivity (78.9%) were obtained over the Fe–Mn–Co catalyst at a specific energy input (SEI) of 730.2 J l −1 . Moreover, the presence of water vapor improved EO conversion and CO 2 selectivity in the relative humidity (RH) range of 0–60%, while further increasing the RH to 80% reduced EO conversion. The interactions between Fe, Mn and dopants increased the specific surface area and pore volume of the Fe–Mn-X catalyst, while maintaining the crystalline structure of the catalysts. The presence of the dopants enhanced the reducibility of the Fe–Mn-X catalysts and produced more surface adsorbed oxygen (O ads ) on the catalyst surfaces. Moreover, the interactive effects among the Fe, Mn and dopants facilitated the plasma-catalytic oxidation reactions via enhanced surface reactions. The coupling of plasma with the Fe–Mn–Co catalyst reduced the formation of organic by-products in the plasma-catalyzed oxidation of EO.
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ACS Applied Materials & Interfaces
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2022
·
IF 10.383
Wenjie Feng,Wanrui Shi,Ze Wang,Yanqi Cui,Xinxin Shao,Shuwei Liu,Li Rong,Yi Liu,Hao Zhang
Ferroptosis has been considered as a promising pathway to overcome apoptosis-induced tumor chemoresistance. However, the antitumor efficacy of ferroptosis-inducing agents is still limited because of the complexity and diversity of tumor microenvironments. Herein, we demonstrate a triple ferroptosis amplification strategy for tumor therapy by associating iron-based nanocarriers, ferroptosis molecular drugs, and H2O2-producing enzymes. Fe(III)-Shikonin (FeShik) metal-polyphenol-coordinated networks are employed to load a ferroptosis inducer of sorafenib (SRF) inside and glucose oxidase (GOx) outside, thus producing SRF@FeShik-GOx supramolecular nanomedicines (SNs). After delivering into glutathione (GSH)-overexpressed tumor cells, FeShik will disassemble and release Fe2+ to induce cell death via ferroptosis. At the same time, GOx executes its catalytic activity to produce an acid environment and plenty of H2O2 for stimulating •OH generation via the Fenton reaction. Moreover, SRF will suppress the biosynthesis of GSH by inhibiting system Xc–, further deactivating the enzymatic activity of glutathione peroxidase 4 (GPX4). Up-regulation of the oxidative stress level and down-regulation of GPX4 expression can dramatically accelerate the accumulation of lethal lipid peroxides, leading to ferroptosis amplification of tumor cells. The current strategy that utilizes ferroptosis-inducing agents as both nanocarriers and cargoes provides a pathway to enhance the efficacy of ferroptosis-based tumor therapy.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Anlin Xu,Siyan Fan,Tong Meng,Ren Zhang,Yunhai Zhang,Shunlong Pan,Yongjun Zhang
Metal oxides, as a popular group of ozonation catalyst, are usually synthesized with physiochemical protocols involving hazardous materials and extreme conditions. In this study, a biological method was studied with manganese oxidizing bacteria Pseudomonas sp. to synthesize multi-metal oxides consisting of iron, manganese, and cobalt (Bio-FeMnCoOx) to catalyze ozonation for the first time. It was found that the dosage of cobalt, the cultivation time, and the polishing methods could significantly impact the catalytic activities of degrading benzotriazole as a model. The second-order degrading kinetic constant with optimized Bio-FeMnCoOx was 4.8 times that with the physiochemically synthesized peer. The activity of Bio-FeMnCoOx was compared with other reported catalysts in terms of Rct value. The quenching tests and EPR spectra indicated the participation of hydroxyl radicals, superoxide radicals, and singlet oxygen. The study demonstrates the great potential of biosynthesis as a green protocol for preparing metal oxides to efficiently catalyze ozonation.
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ENVIRONMENTAL RESEARCH
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2022
·
IF 8.431
Xuelian Xia,Yanguo Teng,Yuanzheng Zhai
Riverbank filtration (RBF) constitutes an important part of the water cycle , which involves active natural filtration leading to pollution of river water being intercepted and retained. The RBF has the function of water purification , but retention of exogenous pollutants in the RBF system complicates biogeochemical processes due to the presence of primary active components. In this study, we verified the essential role of microbial mediation during the interactions between primary Fe minerals in the RBF system and dissolved organic matter (DOM) in river water based on lab-scale experiments. The results demonstrated that DOM from infiltration of river water increased the amount of iron (Fe) released from the sediment in RBF, leading to an increase in Fe concentration in groundwater by higher than one order of magnitude. In particular, the existence of Fe bacteria even made this effect more thorough and more complex. Abiotic reduction was shown to play a more significant role in increasing Fe release than microbe-mediated reduction. Increasing the amount of Fe released could change the distribution of Fe minerals at the sediment surface, thereby affecting the structure of the microbial community in the RBF system and decreasing the DOM concentration in the groundwater. Moreover, As and Mn were found to behave in a similar manner as Fe due to their close biochemical properties when interacting with primary minerals in sediment. This study not only provides mechanistic insight into the higher Fe concentrations encountered in the groundwater of nearby rivers but also has important practical implications for developing nature-based technologies for water pollution control and environmental remediation.
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Sustainability
·
2022
·Vol. 14
·期 19
·12097
·
IF 3.889
Yuchen Zhang,Xigai Jia,Ziyang Kang,Xiaoxuan Kang,Ming Ge,Dongbin Zhang,Jilun Wei,Chongqing Wang,Zhangxing He
Tetracycline (TC) is a broad-spectrum antibiotic commonly, made use of in aquaculture and animal husbandry. After entering water bodies, it will represent a major threat to human health. In this study, sterculia foetida biochar (SFC) was readied by the combined hydrothermal pyrolysis (co-HTP) method with sterculia foetida as raw materials. Fen-SFC (Fe2-SFC, Fe3-SFC, and Fe4-SFC) was obtained by doping SFH with different concentrations of FeCl3. Finally, activation of peroxodisulfate (PDS) was achieved, using Fe3-SFC to degrade TC. The degradation of TC obeyed pseudo-second-order kinetics, and the constant of the reaction rate was 0.491 L mg−1min−1. Radical trapping experiments, EPR test and electrochemical tests evidenced that the high catalytic performance of the Fe3-SFC/PDS system was ascribed to free radical pathway (•OH and SO4•−) and non-radical pathway (1O2and electron transfer), in which the latter plays a dominant role. This research not only demonstrates a new kind of biochar as an effective catalyst for PS activation, but also offers an avenue for the value-added reuse of sterculia foetida.Keywords:peroxydisulfate activation;biochar;sterculia foetida;tetracycline wastewater;degradation
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Cong Pan,Libin Fu,Fenna Lide,Yaobin Ding,Chengjun Wang,Jia Huang,Shaobin Wang
Reduction of bromate (BrO 3 − ) by various technologies has been extensively investigated, while the fate of oxygen and bromine atoms in BrO 3 − in these processes has been largely ignored. In this study, reduction of BrO 3 − by Fe(II) ions was investigated under various conditions via electron spin resonance (ESR), laser flash photolysis (LFP), probe of phenol and quenching experiments. It was found that reduction of BrO 3 − by Fe(II) ions produced HO•, O 2 • − and reactive bromine species (eg., Br• and Br 2 • − ). HO• and O 2 • − were generated from release of one/two oxygen atoms in BrO 3 − and its reduction intermediates (BrO 2 − and BrO − ) at one time, while Br• and Br 2 • − were generated from activation of hypobromous acid by Fe(II) and reactions of HO• with formed Br − . Due to the formation of these reactive species, the tested ten organic pollutants with diverse structures can be efficiently degraded, which including carbamazepine (CBZ), ibuprofen, phenol, benzoic acid, paracetamol, bisphenol a, 4-chlorophenol, oxcarbazepine, diclofenac and sulfamethoxazole. CBZ degradation intermediates by BrO 3 − /Fe(II) system were specially identified by liquid chromatography (LC)-mass spectrometry (MS), and three pathways of hydroxylation/nitrosylation, ring contraction-amine cleavage and bromination for CBZ degradation were proposed accordingly. This study might shed new fundamental insights to bromate reduction and its implication for transformation of co-existed organic pollutants.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Jiangya Ma,Rui Zhang,Wei Xia,Yanli Kong,Yong Nie,Yahua Zhou,Chi Zhang
A novel covalently bonded composite coagulant CAFM was synthesized by using inorganic PAFC and organic CPAM through UV initiation. The algae and turbidity removal efficiency were investigated by using CAFM in algae-laden water coagulation process. The Al/Fe residual and algae flocs size were also examined. Results showed that 96% chlorophyll a and 87% turbidity were removed by using CAFM at dosage of 40 mg/L. The removal efficiency was larger than that by using PAFC or CPAM at their optimal dosage. The minimum Al residual of 12.47 μg/L, Fe residual of 9.64 μg/L together with the most compact algae flocs were achieved by using CAFM 0.6 , which was great favorable and essential for drinking water treatment . Finally, the charge neutralization of PAFC and bridging of CPAM synergetic contributed to algae harvesting.
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Journal of Physical Chemistry C
·
2021
·
IF 4.126
Yao Li,Le Xin Song,Wei Ping Wang,Yue Teng,Juan Xia,Nan Ning Liu
In this work, we prepared a series of Fe-MOF polyhedra [metal organic framework (MOF)-1 ∼ −13] by introducing β-cyclodextrin (CD) as a morphology modifier using an interaction between ferric chloride and terephthalic acid in dimethylformamide. A novel structural evolution from a hexagonal bipyramid to a bipyramidal hexagonal prism was clearly observed. This evolution was gradual and could be well reflected by the height ratio of the prism and pyramid in these polyhedral structures. It is the relative concentration of β-CD that drives this structural evolution. Although the reaction temperature and time can also affect the height ratio to some extent, their influence can only be realized in the presence of β-CD. In the absence of β-CD, only hexagonal bipyramid structures were obtained. It is worth noting that Fe-MOF-1 with a bipyramidal hexagonal prism structure (prism height, ∼130 nm) showed typical paramagnetic characteristics, and its saturation magnetization was determined to be 23.1 emu·g–1. Furthermore, we found that Fe-MOF-1 exhibited good photocatalytic performance for different types of dyes (crystal violet with positives and methyl orange with negative charges). At the same time, a possible photocatalytic mechanism was proposed to explain the difference of degradation efficiency between the two dyes. Also, we use the combination of specific surface area and zeta potential to explain the differences in the catalytic properties of a series of Fe-MOF materials. In addition, MOF-1 shows the same electrocatalytic oxygen evolution reaction performance as some bimetallic MOFs such as Fe-Co-MOF. For example, the overpotential of MOF-1 is 398 mV at 10 mA·cm–2 current density, while that of Fe-Co-MOF is 410 mV. We believe that the current work can contribute to the adjustment, modification, and application of MOF nanostructures.
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