ANALYTICAL SCIENCES
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2023
·
IF 1.6
Yang Yu Meng,Yan Yuan,Zhou Jia Ying,Huang Cheng Zhi,Zhen Shu Jun,Zhan Lei
Real-time monitoring of hypochlorous acid (HClO) in biological systems is of great significance for exploring and regulating its pathological functions because abnormal production of HClO is closely related with many diseases, such as atherosclerosis, rheumatoid arthritis, and cancer. Herein, we developed a reliable fluorescent Fe-doped carbon dots (Fe-CDs) for the sensitive and selective detection of biological HClO using ferrocenecarboxylic acid and m -phenylenediamine as precursors through a one-step solvothermal procedure. The Fe-CDs exhibited excellent a wide HClO detection range from 20 nmol/L to 1000 nmol/L with corresponding limits of detection at 7.8 nmol/L. The sensing mechanism is based on the chemical oxidation of the hydroxyl groups on the surface of Fe-CDs by HClO. In addition, Fe-CDs also displayed high photoluminescence yield, excitation-independence emission, as well as good biocompatibility, enabling the successful imaging of endogenous and exogenous HClO in HeLa cells. These results revealed that Fe-CDs holds great promise as a robust fluorescent probe for investigating HClO-mediated biological events. Graphical abstract
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Naiyun Liu,Ruqiang Wu,Yixian Liu,Yunliang Liu,Peiji Deng,Yaxi Li,Yongchao Du,Yuanyuan Cheng,Zechao Zhuang,Zhenhui Kang,Haitao Li
Electrochemical nitrogen reduction reaction (NRR) is a promising method for ammonia synthesis under ambient conditions. However, the NRR performance is limited to an extremely strong N≡N bond in N2 and the competing hydrogen evolution reaction. Introducing oxygen vacancies (OVs) has been considered as a forceful means to accelerate the sluggish NRR reaction kinetics. Herein, we reported the design of Fe-doped NiMoO4 catalysts for NRR. Fe doping can increase the amount of OVs in the catalyst and contribute to lattice strain enhancement, thereby leading to the improvement of the electron transport rate and catalytic active for NRR. In 0.1 M Na2SO4 solution, the 5% Fe-NiMoO4 catalyst achieves a NH3 yield rate of 15.36 μg h–1 mgcat.–1 and a Faradaic efficiency of 26.85% under −0.5 V versus RHE. Furthermore, the 5% Fe-NiMoO4 catalyst exhibits excellent stability (up to 13 h) during the reaction.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Ying Wang,Gareth R. Williams,Yilu Zheng,Honghua Guo,Shiyan Chen,Rong Ren,Tong Wang,Jindong Xia,Li-Min Zhu
One of the major challenges in effective cancer therapy arises because of the hypoxic microenvironment in the tumor. This compromises the efficacy of both chemo- and radiotherapy , and thus hinders patient outcomes. To solve this problem, we constructed polydopamine (PDA)-cloaked Fe-based metal organic frameworks (MOFs) loaded with d -arginine ( d -Arg), glucose oxidase (GOX), and the chemotherapeutic drug tirapazamine (TPZ). These offer simultaneous multifaceted therapy combining chemodynamic therapy (CDT)/radiotherapy (RT)/starvation therapy (ST)/gas therapy (GT) and chemotherapy. The particles further can act as contrast agents in magnetic resonance imaging. GOX catalyses the conversion of endogenous glucose and O 2 to hydrogen peroxide and gluconic acid , blocking the cells’ energy supply and providing ST. With the resultant acidification of the local environment, the breakdown of the MOF releases TPZ (for chemotherapy) and Fe 3+ , which reacts with H 2 O 2 to produce reactive oxygen species and thus stimulates the conversion of d -Arg to NO for GT and RT sensitization. The PDA coating not only seals the pores and chelates Fe 3+ to enhance the T 1 -weighted magnetic resonance imaging (MRI) properties, but also is used to graft folate bovine serum albumin (FA-BSA) and thereby target the tumor site. The combined administration of low doses of X-ray irradiation and nanoparticles reduces the side effects on healthy tissue and can prevent lung metastases in mice. This work highlights the synergistic treatment of osteosarcoma via ST/GT/CDT/RT/MRI/ chemotherapy using a PDA-cloaked MOF system.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Xukai Li,Weirui Chen,Dongpo Liu,Gaozu Liao,Jing Wang,Yiming Tang,Laisheng Li
Due to its low interfacial electron migration ability and highly hydrophilic, Fe-MCM-41 (FeM) had poor activity and stability during catalytic ozonation . To this end, the secondary metal Zn and Si-F group were introduced into the framework of FeM to create surface potential difference and hydrophobic sites. Comparative characterizations showed that there existed rich acid sites with great potential difference on F-Fe-Zn-MCM-41 (FFeZnM). Additionally, because of the existence of hydrophobic and electron-withdrawing Si-F unit, the electron migration ability, hydrophobicity and acidity of FFeZnM were enhanced. The greater O 3 mass transfer was induced by Si-F group and O 3 was directly activated at Fe and Zn Lewis acid sites into •OH, •O 2 - and 1 O 2 . With •OH acting as main species, FFeZnM/O 3 achieved the superior IBP removal (93.4%, 30 min) and TOC removal (46.6%, 120 min) over those of sole O 3 and F-FeM/O 3 processes, respectively. HCO 3 - , Cl - , NO 3 - and SO 4 2- hindered IBP degradation by FFeZnM/O 3 , but high concentration humic acid (HA) exhibited promotion by forming HA-IBP complex. IBP degradation by FFeZnM/O 3 was enhanced with tap water , river water, and effluent from the secondary sedimentation tank of the sewage plant acting as medium. This study proposed an innovative approach to catalyst design for catalytic ozonation.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 37
·87830-87850
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IF 5.8
Liu Gen,Lin Yingzi,Li Siwen,Shi Chunyan,Zhang Dongyan,Chen Lei
Fe-BOC-X
photocatalyst was successfully prepared by solvothermal method. The photocatalytic activity of Fe-BOC-X was determined by ciprofloxacin (CIP), a typical fluoroquinolone antibiotic. Under sunlight irradiation, all Fe-BOC-X showed better CIP removal performance than original BiOCl. In comparison, the photocatalyst with iron content of 50 wt% (Fe-BOC-3) has excellent structural stability and the best adsorption photodegradation efficiency. The removal rate of CIP (10 mg/L) by Fe-BOC-3 (0.6 g/L) reached 81.4% within 90 min. At the same time, the effects of photocatalyst dosage, pH, persulfate, persulfate concentration, and combinations of different systems (PS, Fe-BOC-3, Vis/PS, Vis/Fe-BOC-3, Fe-BOC-3/PS, and Vis/Fe-BOC-3/PS) on the reaction were systematically discussed. In reactive species trapping experiments, electron spin resonance (ESR) signals revealed that the photogenerated holes (h + ), hydroxyl radical (•OH), sulfate radical (•SO 4 − ), and superoxide radical (•O 2 − ) played an important role in CIP degradation; hydroxyl radicals (•OH) and sulfate radicals (•SO 4 − ) play a major role. Various characterization methods have demonstrated that Fe-BOC-X has larger specific surface area and pore volume than original BiOCl. UV–vis DRS indicate that Fe-BOC-X has wider visible light absorption and faster photocarrier transfer and provides abundant surface oxygen absorption sites for effective molecular oxygen activation. Accordingly, a large number of active species were produced and participated in the photocatalytic process, thus effectively promoting the degradation of ciprofloxacin. Based on HPLC–MS analysis, two possible decomposition pathways of CIP were finally proposed. The main degradation pathways of CIP are mainly due to the high electron density of piperazine ring in CIP molecule, which is mainly attacked by various free radicals. The main reactions include piperazine ring opening, decarbonylation, decarboxylation, and fluorine substitution. This study can better open up a new way for the design of visible light driven photocatalyst and provide more ideas for the removal of CIP in water environment.
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DIAMOND AND RELATED MATERIALS
·
2023
·
IF 4.1
Yi Chen,Rong Qiang,Yulong Shao,Xiao Yang,Qian Ma,Rui Xue,Bowen Chen,Shijiang Feng,Fangjie Ren,Yuancheng Ding,Lijuan Sun,Zheng Guo,Zishuo Ma,Zihan Liu,Xinyu Chen
Porous carbon materials typically exhibit excellent microwave absorption performance and lightweight characteristics, providing a positive significance for controlling the composites weight. This work employed a one-step method, and in situ growth techniques to fabricate a foam-structure Fe 3 C/Fe/C with a density of only 0.142 g/cm 3 . The carbon skeleton encapsulates Fe 3 C/Fe nanoparticles to slow down its oxidation in the natural environment. Remarkably, the Fe 3 C/Fe/C composite achieves an impressive effective bandwidth of 5.73 GHz with a 2.2 mm thickness and only 10 wt% filling ratio. The outstanding performance can be ascribed to the enhanced interfacial polarization caused by high porosity. Additional nitrogen doping provides active sites to enhance dipole polarization. Additionally, after in-depth analysis of the various magnetic loss mechanisms present in Fe 3 C/Fe/C, we have revealed the promotion of introducing magnetic nanoparticles on the microwave absorption performance of foam-like carbon. This work provides an effective reference for reducing the weight of microwave absorbers, simplifying preparation methods, and understanding the mechanisms of magnetic nanoparticles in foam-like carbon.
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ACS Applied Nano Materials
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2023
·
IF 5.9
Kang Ji,Junpeng Wang,Ping Yang
Modulation of oxygen intermediates in the oxygen evolution reaction (OER) tends to be an effective method for intensifying OER activity. In this paper, NiCo nanolayered double hydroxide (NC-LDH)-decorated FeNi bimetallic metal–organic framework (FN-MIL) heterostructures were constructed for enhanced OER performance. Various characteristics including Raman and Fourier-transform infrared spectra, X-ray diffraction patterns, scanning and transmission electron microscopy images, and X-ray photoelectron spectroscopy spectra help to explore the composition and microstructure. The band gap of samples was discussed using Mott–Schottky curves and Tauc plots to analyze the interfacial electron transfer driven by the energy level difference, resulting in the formation of electron-rich and electron-deficient regions at the interface and realizing the directed modulation of oxygen intermediates. The as-prepared composite catalyst revealed excellent OER performance, long-term stability, a high faradic efficiency of 97.8%, and a low potential of 244 mV at 10 mA cm–2 (without iR-compensation). Interestingly, the catalyst maintained high OER activity in seawater containing 1 M KOH due to its favorable resistance to chloride ions, suggesting an appealing prospect in practical application.
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 27
·14900-14910
·
IF 11.9
Mengdi Liu,Sai Zhang,Min Chen,Shuxue Zhou,Limin Wu
Electrochemical nitrogen reduction reaction (NRR) is considered a promising alternative for green and sustainable ammonia (NH3) synthesis, which has, however, long suffered from low efficiency and poor selectivity. In this study, an isolated bimetallic Fe–Ru single atom catalyst was synthesized via anchoring the metal single atoms on nitrogen-doped carbon nanorod spheres. The catalyst exhibits an optimized faradaic efficiency of 29.3% along with an NH3 yield rate of 43.9 μg h−1 mg−1 for the NRR under −0.2 V vs. RHE. Control experiments and isotopic labelling test confirm that the generated NH3 originates from the nitrogen (N2) feeding gas. Computational analysis indicates that Fe acts as the active sites for nitrogen reduction. Impressively, an obvious synergistic effect exists between spatially isolated single atoms, which could be overlooked previously. The electronic structure of Fe sites is effectively influenced by Ru atoms, which results in the d-band center shift and stronger N2 adsorption, further improving NRR performance.
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MOLECULES
·
2023
·Vol. 28
·期 11
·4366
·
IF 4.6
Dan Wang,Fuhe Le,Jing Lv,Xue Yang,Xianhao Chen,Haibin Yao,Wei Jia
Developing cost-effective and high-efficiency catalysts for electrocatalytic oxygen evolution reaction (OER) is crucial for energy conversions. Herein, a series of bimetallic NiFe metal–organic frameworks (NiFe-BDC) were prepared by a simple solvothermal method for alkaline OER. The synergistic effect between Ni and Fe as well as the large specific surface area lead to a high exposure of Ni active sites during the OER. The optimized NiFe-BDC-0.5 exhibits superior OER performances with a small overpotential of 256 mV at a current density of 10 mA cm−2and a low Tafel slope of 45.4 mV dec−1, which outperforms commercial RuO2and most of the reported MOF-based catalysts reported in the literature. This work provides a new insight into the design of bimetallic MOFs in the applications of electrolysis.Keywords:metal–organic frameworks;NiFe-BDC;electrocatalytic oxygen evolution;synergistic effect
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 18
·53355-53369
·
IF 5.8
Ding Chunsheng,Lei Jia,Cai Zhiyue,Gao Mengying,Zou Zhaozheng,Li Yuanfeng,Deng Jing
In this research, FeCo 2 O 4 nanomaterial was successfully synthesized by a typical sol–gel method and conducted as an effective agent for peroxymonosulfate (PMS) activation to eliminate antibiotics flurbiprofen (FLU), a strong nonsteroidal drug. FeCo 2 O 4 nanomaterial was characterized by XRD, TEM, SEM, and XPS. Various characterization results proved that FeCo 2 O 4 held stable spinel structure. The interfering factors including initial pH, PMS concentration, catalyst dosage, inorganic anions, and humic acid on FLU removal were also discussed. The conclusion was that the removal efficiency of FLU reached 98.2% within 120 min after adding FeCo 2 O 4 (0.4 g L −1 ) and PMS (3 mM). The optimal pH for FLU degradation was the initial pH of 6.5; too acidic or alkaline was not conductive to the degradation. The existence of HA and Cl − restrained the degradation of FLU, and HCO 3 − promoted the removal, while the influence of NO 3 − and SO 4 2− could not be considered. The radical scavenging experiment confirmed that • OH, O 2 •− , and SO 4 •− participated in FLU removal and SO 4 •− functioned a leading role. FeCo 2 O 4 showed high efficiency for PMS activation in pH range of 3.0 to 10.0. After the fourth cycle operation, the FLU removal rate exceeded 76.9%, and the Co leaching rate was low during the catalytic reaction. This study shows that FeCo 2 O 4 nanomaterial is an efficient and environment-friendly catalyst, which can be applied for PMS activation to remove organic pollutants in water.
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CATALYSIS LETTERS
·
2023
·
IF 2.8
Zhao Liping,Wang Changzhen,Bai Juan,Wu Ruifang,Li Haitao,Zhao Yongxiang
2-Hydroxytetrahydrofuran (HTHF) is the main by-product of hydrogenation of 1,4-butynediol (BYD) to 1,4-butanediol (BDO) in industry, which is difficult to be effectively removed in the subsequent distillation process and seriously affects the product quality. Here, a series of silica-supported bimetallic Ni–Fe catalysts with different Fe/Ni weight ratios were prepared by using incipient wetness impregnation method and investigated the effect of Fe on the catalyst performance in the hydrogenation of HTHF to BDO. In comparison with monometallic Ni and Fe catalysts, bimetallic Ni–Fe catalysts exhibited better performance for HTHF hydrogenation due to the formation of Ni–Fe alloy phase identified by XRD, TEM, STEM-EDS, H 2 -TPR, NH 3 /H 2 -TPD, Pyridine FTIR and XPS, etc. A mechanism is proposed to explain the promoting effect of Fe, which can be assigned to the synergism between nickel sites with high ability to activate/overflow hydrogen and Fe-containing sites with strong oxophilicity for the activation of the O-C-O bond over the tetrahydrofuran ring. Graphical Abstract
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Frontiers in Bioengineering and Biotechnology
·
2023
·
IF 5.7
Liang Zixing,Li Xiaofeng,Chen Xiaofang,Zhou Jiawei,Li Yanan,Peng Jianhui,Lin Zhousheng,Liu Gai,Zeng Xiancheng,Li Cheng,Hang Lifeng,Li Hailiang
Introduction: Photodynamic therapy (PDT) and photothermal therapy (PTT) are widely used in the treatment of tumors. However, their application in the treatment of clinical tumors is limited by the complexity and irreversible hypoxia environment generated by tumor tissues. To overcome this limitation, a nanoparticle composed of indocyanine green (ICG) and Fe-MOF-5 was developed.Methods: We prepared F-I@FM5 and measured its morphology, particle size, and stability. Its enzyme like ability and optical effect was verified. Then we used MTT, staining and flow cytometry to evaluated the anti-tumor effect on EMT-6 cells in vitro. Finally, the anti-tumor effect in vivo has been studied on EMT-6 tumor bearing mice.Results: For the composite nanoparticle, we confirmed that Fe-MOF-5 has the best nanozyme activity. In addition, it has excellent photothermal conversion efficiency and generates reactive oxygen species (ROS) under near-infrared light irradiation (808 nm). The composite nanoparticle showed good tumor inhibition effect in vitro and in vivo, which was superior to the free ICG or Fe-MOF-5 alone. Besides, there was no obvious cytotoxicity in major organs within the effective therapeutic concentration.Discussion: Fe-MOF-5 has the function of simulating catalase, which can promote the decomposition of excessive H2O2 in the tumor microenvironment and produce oxygen to improve the hypoxic environment. The improvement of tumor hypoxia can enhance the efficacy of PDT and PTT. This research not only provides an efficient and stable anti-tumor nano platform, but also has broad application prospects in the field of tumor therapy, and provides a new idea for the application of MOF as an important carrier material in the field of photodynamic therapy.
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