NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 5
·2102-2110
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IF 3.288
Shuangyan Meng,Wei Zeng,Mingming Wang,Litong Niu,Shaoping Hu,Bitao Su,Yaoxia Yang,Zhiwang Yang,Qunji Xue
Polydopamine/MIL-53(Fe) (PDA/MIL-53(Fe)) nanocomposite photocatalysts were synthesized with PDA (PDA = polydopamine) and MIL-53(Fe) using a nature-mimicking method. The structures, morphologies, optical properties and thermal stabilities of all the synthesized materials were characterized using a series of methods. In particular, the separation efficiency of photogenerated charge significantly increased after the incorporation of PDA into MIL-53(Fe), which resulted in an elevated photocatalytic activity of PDA/MIL-53(Fe) compared with the control groups. The PDA/MIL-53(Fe) nanocomposite could accelerate the conversion of primary or secondary alcohols into the corresponding aldehydes or ketones with a high specificity by direct hole-involving oxidation under visible-light irradiation and room temperature. The catalysts could be cycled at least three times without a significant decrease in the catalytic activity and this result showed the excellent recyclability and stability of the catalysts.
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JOURNAL OF HAZARDOUS MATERIALS
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2019
·
IF 7.65
Qin Zhu,Jiaorong Yan,Qiguang Dai,Qingqing Wu,Yuanpu Cai,Jinyan Wu,Xingyi Wang,Wangcheng Zhan
A unique zeolite catalyst, Fe doped ZSM-5 microsphere assembled by uniform nanorod-like crystals with hierarchical pore structure, was successfully synthesized and applied for the adsorption and degradation of trace chlorobenzene (CB) in the presence of H 2 O 2 . The organic ferric salts as the precursors, ethylene glycol as a chelating/reducing agent and the dynamic two-stage temperature-varied hydrothermal technique, together made the synthesized hierarchical Fe-ZSM-5 nanorods assembled microspheres (FZ-CA-5EG) to be characterized by abundant highly dispersed and valency-controlled framework Fe 3+/2+ species. As a result of these features, the FZ-CA-5EG showed excellent ability of adsorption and degradation efficiency of CB, and enhanced durability due to negligible leaching of framework Fe species. Moreover, the hydroxyl radicals were determined as the main the reactive oxygen species of CB oxidation degradation, and a possible adsorption-oxidation degradation pathway was proposed.
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Molecular Catalysis
·
2019
·
IF 2.938
Qi Song,Rui Ran,Jiancai Ding,Xiaodong Wu,Zichun Si,Duan Weng
Porous ceria nanorods modified with Fe or Co were prepared via a hydrothermal method. The structural properties, catalytic activities for the total oxidation of propane, and catalytic mechanisms of these materials were systematically investigated by X-ray diffraction, Raman spectroscopy, N 2 adsorption–desorption, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, catalytic activity measurements and in situ Fourier transform infrared spectroscopy. Co-modified ceria exhibited the best catalytic activity during propane oxidation as well as enhanced reducibility due to the synergistic interactions between the Co and the CeO 2 support. Variations in the activating ability and reducibility of the catalysts resulted in the formation of distinctive intermediates during the catalytic process, and this explained the observed differences in catalytic performance.
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Biomaterials Science
·
2019
·Vol. 7
·期 9
·3683-3692
·
IF 5.251
Zongjun Liu,Tuo Li,Fang Han,You Wang,Yang Gan,Junhui Shi,Tianran Wang,Muhammad Luqman Akhtar,Yu Li
Synergistic cancer starvation/ROS-mediated/chemo-therapy is developed through a cascade reaction with enzyme glucose oxidase (GOX) modified on the surface of an Fe-based metal organic framework (MOF(Fe)) and drug camptothecin (CPT) loaded into the cavities of MOF(Fe). Once internalized by tumor cells, GOX catalyzes endogenous glucose into hydrogen peroxide (H2O2) and gluconic acid (H+) enabling starvation therapy through choking off energy (glucose) supply. Meanwhile, the acidic micro-environment of tumor enhanced by the generated H+ degrades the MOF(Fe) simultaneously releasing CPT for chemotherapy and Fe3+, catalyzing H2O2 into one of the strongest reactive oxygen species (ROS) ˙OH enabling ROS-mediated therapy. Both in vitro and in vivo results show remarkable tri-modal synergistic anticancer effects. This work may shed some light on the development of novel multi-modal cancer therapies without any external intervention.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2019
·
IF 2.931
Zheng Fu,Jiantong He,Fengchun Jia,Mengjiao Wang,Fengling Cui
Since thiosemicarbazide contains numerous nitrogen and sulfur atoms in its structural formula that enhance its strong coordinating abilities with metal ions , it is always selected as the mother molecule for the design of metal-ion sensors. In this report, a thiosemicarbazide derivative (4-naphthalenyl-3-thiosemicarbazide (NTSC)) was synthesized via a single step process and covalently conjugated onto the surfaces of carbon dots (CDs). The modified CDs demonstrated excellent monodispersity, good photostability, and tunable luminescence properties. More importantly, the CDs retained a highly specific Fe 3+ recognition capacity in contrast to other competing metal ions . Fe 3+ can efficiently quench the fluorescence of CDs even at fairly low concentration (30 μM) with a detection limit as low as 1.68 nM. The fluorescence quenching kinetics are likely to involve static quenching, which is caused by specific interactions between NTSC-CDs and Fe 3+ toward the formation of a ground state complex. Due to their excellent optical performance, low toxicity, and good biocompatibility the NTSC-CDs may be applied to the imaging and monitoring of Fe 3+ in bacillus subtilis. In effect we successfully fabricated an effective fluorescent nanosensor for both the quantitative detection of Fe 3+ in aqueous solutions, and its real-time imaging in vivo.
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JOURNAL OF POWER SOURCES
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2018
·
IF 6.945
Xiaogeng Feng,Xiangjie Bo,Liping Guo
Rational synthesis and development of earth-abundant materials with efficient electrocatalytic activity and stability for water splitting is a critical but challenging step for sustainable energy application . Herein, a family of bimetal (CoFe, CoCu, CoNi) embedded nitrogen-doped carbon frameworks is developed through a facile and simple thermal conversion strategy of metal-doped zeolitic imidazolate frameworks. Thanks to collaborative superiorities of abundant M-N-C species, modulation action of secondary metal, cobalt-based electroactive phases, template effect of MOFs and unique porous structure , bimetal embedded nitrogen-doped carbon frameworks materials manifest good oxygen and hydrogen evolution catalytic activity . Especially, after modulating the species and molar ratio of metal sources, optimal Co 0.75 Fe 0.25 nitrogen-doped carbon framework catalyst just requires a low overpotential of 303 mV to achieve 10 mA cm −2 with a low Tafel slope (39.49 mV dec −1 ) for oxygen evolution reaction , which even surpasses that of commercial RuO 2 . In addition, the optimal catalyst can function as an efficient bifunctional electrocatalyst for overall water splitting with satisfying activity and stability. This development offers an attractive direction for the rational design and fabrication of porous carbon materials for electrochemical energy applications.
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ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Ping Zhang,Deyi Hou,David O’Connor,Xuanru Li,Simo Pehkonen,Rajender S. Varma,Xun Wang
Many challenges remain for the mass production of nanoparticles for the removal of contaminants from water, primarily due to the complexity of the synthetic protocols involved and the use of hazardous reagents. Although the development of phytosynthetic methods for the green fabrication of nanomaterials have seen keen interest, there remains much scope for improvement in terms of maximizing adsorption capacity and controlling the size of the nanoparticles produced. A green and sustainable pathway is described using Virginia creeper (Parthenocissus quinquefolia) leaf extract in the presence of oxalic acid for the synthesis of earth abundant Fe,Cu-based nanoparticle adsorbents. This optimized green method could produce Fe,Cu-based nanoparticles with a remarkably high maximum adsorptive capacity (1399 mg g–1) for aqueous Malachite Green (MG) removal. Furthermore, various particle sizes (between 160 and 1000 nm) were attained by simply varying the amount of oxalic acid. The synthesized adsorbent displayed other excellent characteristics, including (i) maintaining a high adsorption capacity over a wide range of pH conditions, (ii) remaining chemically stable under an ambient storage environment, and (iii) having good recycling potential, with consistent removal efficiency observed over four adsorption/desorption cycles. This work not only promotes the use of natural, earth-abundant, and renewable resources in synthesizing novel and efficient absorbents but also provides a simple, convenient, and cost-effective strategy for the purification of dye-laden wastewater.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2018
·Vol. 25
·期 31
·31358-31367
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IF 2.8
Wan Zhong,Wang Jianlong
The advanced treatment of municipal secondary effluent by heterogeneous and homogeneous Fenton processes using Fe/Ce-RGO (reduced graphene oxide) and Fe 2+ as catalysts was studied and compared. Sulfamethazine (SMT) was spiked in the effluent to examine the effectiveness of the emerging contaminant removal. The Fe/Ce-RGO catalyst was characterized using a scanning electron microscope (SEM) and cycle voltammetry curves. The removal of dissolved organic carbon (DOC), soluble chemical oxygen demand (SCOD), SMT, and ultraviolet-visible spectroscopy in 254 nm (UV 254 ) of municipal secondary effluents was examined. The DOC removal efficiency of secondary effluent (without addition of SMT) was 36.30% and 11.74% using Fe/Ce-RGO and Fe 2+ as catalysts, respectively. The removal efficiency of DOC, SCOD, and SMT in heterogeneous Fenton process was higher than that in homogeneous Fenton process. The changes of three-dimensional excitation-emission matrix (3DEEM) fluorescence, soluble microbial products (SMPs), humic acids, and UV 254 were determined, and the results indicated that UV 254, aromatic proteins, and humic acids decreased rapidly in both processes; however, polysaccharides and protein-like substances were difficult to degrade. Although some toxic substances produced after Fenton-like treatment, the biodegradability of the treated effluent was enhanced.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2018
·Vol. 25
·期 31
·31705-31717
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IF 2.8
Zheng Xiang,Wang Jinlin,Xue Xiaolong,Liu Wanxia,Kong Yadong,Cheng Rong,Yuan Donghai
In this research, the adsorptive removal of diclofenac sodium, one of the representative pharmaceuticals and personal care products, from aqueous solution using Fe 3 O 4 @MOF-100(Fe) magnetic microspheres was studied for the first time. The Fe 3 O 4 @MOF-100(Fe) microspheres exhibit strong magnetism and stability, which were observed as a core-shell structure. The maximum adsorption capacity of Fe 3 O 4 @MOF-100(Fe) for diclofenac sodium can reach 377.36 mg L −1 , which was higher than most of the adsorbents reported. The adsorption kinetics follows the pseudo-second-order kinetic equation. And the adsorption equilibrium of DCF can be described with Langmuir isotherm. In the cycle experiment, Fe 3 O 4 @MOF-100(Fe) material performed high adsorption efficiency for low-concentration diclofenac sodium solution, and the removal rate can still reach 80% after 5 cycles of adsorption without desorption. The mechanisms including electrostatic interaction, H-bond interaction, and π-π interaction that coexisted in the adsorption processes would be of benefit to enhance the adsorption capacity. The Fe 3 O 4 @MOF-100(Fe) magnetic microspheres offer exciting opportunities for further application.
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MACROMOLECULAR CHEMISTRY AND PHYSICS
·
2018
·Vol. 219
·期 24
·1800403
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IF 2.492
Chunyan Zhang,Jianxin Luo,Wenjun Li,Lijuan Ou,Guipeng Yu,Chunyue Pan
An environment-friendly synthesis of a covalently bonded terbium(Tb)-complex-containing monodispersed fluorescent porous copolymer microspheres, and their highly selective detection of Fe 3+ are described. The as-made copolymer microspheres exhibit intense green fluorescence originating from Tb ions and high photostability in water. Encouragingly, the fluorescence of the copolymer microspheres can be selectively quenched by trace Fe 3+ due to the interaction between Fe 3+ and the ligands, which disturbs the coordination structure of Tb-complexes and inhibits the energy transfer from ligands to Tb ions. The intense fluorescence intensity, high fluorescence stability, together with the nanoscale and porous nature of the copolymer microsphere endows them with wide detection range (0–1500 µ m ) and low detection limit (2.1 µ m ) for selective recognition of Fe 3+ in aqueous environment. This study paves a new pathway for the function of porous copolymer microspheres being used as targeting for biological detection and environmental issues.
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CHEMOSPHERE
·
2018
·
IF 4.427
Zhe Li,Shunqin Luo,Yang Yang,Jiawei Chen
Advanced oxidation processes (AOPs) are promising environmental remediation technologies for in-situ groundwater treatment . In this study, a bentonite supported Fe/Ni bimetallic nanoparticle (BNF) was fabricated for peroxymonosulfate (PMS) activation. The resultant BNF exhibited high catalytic activity for trichloroethylene (TCE) degradation in weak alkaline conditions. The conditions optimal for this activity were assessed in terms of peroxygen type and BNF/PMS dosage ratios. Complete degradation of 0.1 mM TCE was achieved in 25 min at pH = 8.2 when BNF was present at 1 g/L and PMS at 5 mM concentrations. Analysis of the underlying mechanisms indicated that SO 4 − has a dominant role whereas OH was rather trivial. The enhancement of catalytic activity was attributed to the strong oxidization of SO 4 − , dispersion of Fe/Ni nanoparticles and synergistic effects between Fe and Ni. The effects of inorganic anions, pH and temperature on the BNF/PMS activity were also investigated. Cl − and NO 3 − has little effect on TCE degradation, while PO 4 3− and HPO 4 2− were inhibitory. Higher temperatures favored PMS activation and BNF/PMS exhibited good catalytic activity across a wide range of solution pH. The results indicate that a novel BNF/PMS system holds promise as a superior AOP to remediate emerging organic pollutants in groundwater.
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APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Xiu-Xiu Fang,Wen-Min Liao,Jian-Dong Song,Wen-Zhi Jia,Yun Wang,Ji-Qing Lu,Meng-Fei Luo
A series of 3V-xFe/MgF 2 catalysts with different V/Fe molar ratios were prepared by a sol-gel method, and the effect of Fe promotion on the catalytic performance of gas-phase dehydrofluorination of 1,1,1,3,3-pentafluoropropane (HFC-245fa) was investigated. It was found that proper V/Fe ratio was helpful to improve the activity. The 3V-0.5Fe/MgF 2 catalyst (with a V/Fe ratio of 6/1) gave a HFC-245fa conversion of 76.6% at 320 °C, which was 13.4% higher than that on the 3V/MgF 2 (63.2%). The synergy between V and Fe species resulted in enhanced surface acidity which accounts for the enhanced activity. The VO x and FeO x species in the fresh catalyst could be transformed to VOF x and FeF 3 species during the reaction, which were regarded as the active sites. However, higher content of Fe in the catalyst resulted in the partial coverage of V species, which led to decline of surface acidity and thus the suppressed activity. Also, surface carbon deposition was responsible for the slight catalyst deactivation .
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