ACS Applied Nano Materials
·
2021
·
IF 5.097
Mingqi Xu,Dingzhou Liu,Jinghua Yang,Qian Zhu,Yunliang Wang,Jingquan Sha
Study and application of MIL-100(Fe)-based two-dimensional graphene oxide (GO) nanocomposite was limited because the nucleation of the spherical structure of MIL-100(Fe) on GO along different directions hindered the formation of MOF-100(Fe). To address this issue, MIL-100(Fe)/three-dimensional graphene (3DG) nanocomposites (abbreviated as MIL-3DG-n, n = 25, 50, 75, and 100) were successfully fabricated via in situ growth of MIL-100(Fe) on 3DG matrixes in this work because the unique structure of 3DG can avoid the attachment with MIL-100(Fe) on nucleation sites along multiple directions, resulting in their ideal combination. The prepared MIL-3DG nanocomposites exhibited higher peroxidase-like catalytic activities than pure MIL-100(Fe), and MIL-3DG-75 exhibited the best peroxidase-like activities for detecting xanthine with the detection limit of 0.0014 μM in the linear range of 0–200 μM to date, to the best of our knowledge, which is attributed to the higher affinity of MIL-3DG-75 nanocomposite to peroxidase substrates o-phenylenediamine (OPD) and H2O2, confirmed by the Michaelis–Menten kinetics (Vm: 49.5 × 10–8 M s–1 for H2O2, 18 × 10–8 M s–1 for OPD, Km: 0.029 mM for H2O2, 0.011 mM for OPD). Owing to the high catalytic efficiency of the MIL-3DG-75 nanocomposite, a rapid and efficient strategy for the sensitive colorimetric detection of xanthine was established.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Lizhu Chen,Xueting Xie,Xianliang Song,Shucan Luo,Shengying Ye,Wenbei Situ
To maintain the quality of harvested fruits and vegetables in a closed refrigerated environment, a novel nanocomposite photocatalyst MIL101(Fe)-TiO 2 -rGO (MTR) for ethylene degradation was synthesized. The characterization of MTR was analyzed by X-ray Diffraction (XRD), Fourier Transform Infrared Spectroscopy (FTIR), Raman spectroscopy, X-ray Photoelectron Spectroscopy (XPS) and High-resolution transmission electron microscope (HRTEM). Moreover, with the good conductivity of rGO, MTR had the smallest band gaps according to ultraviolet–visible solid diffuse reflection (UV–Vis DRS) analysis; this small band gap size improved the utilization of light. According to the results of the photoluminescence spectra and electrochemical impedance spectra, the charge transfer resistance and transient photocurrent of MTR were improved. The redox process of Ti 4+ /Ti 3+ from TiO 2 and Fe 3+ /Fe 2+ from MIL101(Fe) efficiently prevented the recombination of e - -h + pairs. In this cycle, oxidative active substances ( • O 2 − ) were provided, which played a key role in the ethylene degradation of MTR. Additionally, MTR has excellent gas adsorption capacity, and the photocatalytic degradation rate of C 2 H 4 by MTR was 2.07 × 10 -4 min −1 , which is better than that of other photocatalysts. Furthermore, the photocatalytic activity of MTR was still stable after 4 times of recycling, indicating the potential to maintain the quality of horticultural products after harvesting.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 23
·13678-13687
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IF 12.732
Dan Wang,Hao Xu,Peixia Yang,Xiangyu Lu,Jingyuan Ma,Ruopeng Li,Lihui Xiao,Jinqiu Zhang,Maozhong An
Compared to individual metal sites, e.g. Fe–N4 sites, the synergistic effect of dual-metal sites can further adjust the interaction of reactants or intermediates with active sites, which is beneficial for boosting the oxygen reduction reaction (ORR) in Zn–air batteries. However, developing a simple and direct method instead of complicated procedures and post-treatment to realize well-defined dual-metal sites is still a grand challenge. Herein, a facile one-step impregnation-pyrolysis route without any post-treatment is developed to controllably synthesize Fe and Co dual-metal sites embedded in hierarchical N-doped carbon from metal–organic frameworks. X-ray absorption spectra coupled with density functional theory calculations demonstrate that the Fe–N4 and Co–N4 dual sites can synergistically enhance the ORR activity. Impressively, the well-controlled FeCo–N–C catalyst exhibits excellent ORR performance, with half-wave potentials (E1/2) of 0.807 and 0.904 V in 0.1 M HClO4 and 0.1 M KOH, respectively. Benefiting from the highly active dual-metal sites and desired porous structure, FeCo–N–C serving as a cathode catalyst achieves an uplifting peak power density of 196.3 mW cm−2 and a remarkable specific capacity of 728.6 mA h gZn−1 at a discharge current density of 20 mA cm−2 in a practical liquid Zn–air battery. Besides this, such superb battery performance is demonstrated in an all-solid-state Zn–air battery.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
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IF 10.588
Tingting Liu,Jian Luo,Shangke Liu,Tongtong Li,Haolin Li,Lingyan Zhang,Wei Mu,Nan Zou
Neonicotinoid insecticides have been widely used due to their excellent systemic activity and high insecticidal activity, but the problems of low utilization rate and environmental risk have attracted widespread attention. Controlled-release technology is an approach to realize the efficient utilization of pesticides and reduce environmental pressure. In this study, clothianidin (CLO) controlled-release granules ( [email protected] TA (tannic acid)/Fe (III)) were prepared with TA/Fe (III) coordination chelate as the coating material. These granules exhibited the core-shell structure with 500–1200 µm of particle size, and had obvious release performance and hydrolysis behavior of coating materials. Pot experiments by root application showed that the [email protected] /Fe (III) showed balanced and lasting control efficacy to broad bean aphids. The plants have a stronger capacity for absorption and enrichment and a higher utilization rate of CLO for [email protected] /Fe (III), than those for 10% suspension concentrate (SC). One of the hydrolysates of coating materials, TA, a polyphenolic antioxidant, could improve the bioaccumulation amount and alleviating the oxidative stress response of CLO in plants. Our study illustrates that the controlled-release granules base on TA have efficient controlled-release properties and free radical scavenging performance that may eventually be used as pesticide carriers and antioxidants in the field of plant protection.
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高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2021
·Vol. 56
·期 28
·15782-15797
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IF 4.22
Jiang Danni,Zhou Yu,Wang Ping,Huang Chao,Zhu Jian,Liu Zhiming
In the MOFs-based composites, the co-catalyst nanoparticles loads tend to agglomerate. In the self-assembly process of MOFs-based composites, the use of acid modulators solved the accumulation of AgI nanoparticles cocatalyst. The active sites of carboxyl groups and mesoporous structure brought by acid modulator provide more loading sites for AgI nanoparticles. The novel AgI/D-MIL-53(Fe) showed good adsorption and photocatalytic performance in the process of removing tetracycline pollutants. Compared to the degradation efficiency of the MIL-53(Fe) with 50.8%, it of AgI/MIL-53(Fe) increased to 85.1% and which further increased to 96.2% by AgI/D-MIL-53(Fe) based on the HCl modulator. On the one hand, it is beneficial for the mesoporous D-MIL-53(Fe) modulated by HCl modulator to disperse the AgI nanoparticles co-catalyst. On the other hand, AgI nanoparticles, as a photosensitive agent, adsorb visible light to generate photogenerated electrons and holes, and electrons rapidly transferred to the heterojunction bridge Ag 0 and then captured by the holes from the D-MIL-53(Fe). The construction of AgI/D-MIL-53(Fe) Z-scheme heterojunction provided favorable conditions for the rapid separation and photogenerated electrons and holes. Finally, ·O 2 − , ·OH and h + as the main active free radicals were driving forces. This study provided more possibilities and opportunities for the construction of mesoporous MOFs-based composites.
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Journal of Materials Chemistry B
·
2021
·Vol. 9
·期 22
·4555-4566
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IF 6.331
Wenhui Chen,Qiu Han,Yang Liu,Yiwen Wang,Fu Liu
Hyperphosphatemia, a common complication of chronic renal failure patients, is described as an excess amount of serum phosphate >4.5 mg dL−1. Current therapy for hyperphosphatemia is limited by low removal efficiency, secondary hyperparathyroidism, uremic bone disease, and the promotion of vascular and visceral calcifications. Metal organic frameworks (MOFs) have aroused great interest in the field of blood purification because of their strong specific adsorption. Herein, we prepared mixed matrix microspheres (MMMs) encapsulated NH2-MIL-101(Fe) with specific adsorption to blood phosphate. Simultaneously, a heparinoid copolymer poly (acrylic acid-sodium 4-vinylbenzenssulfonate) (P(AA-SSNa)) was incorporated to improve the hemocompatibility. The proposed MMMs exhibited excellent phosphate adsorption capacity both in aqueous and human plasma environments. They also showed comprehensive hemocompatibility e.g. low tendency of protein adsorption, low hemolysis rate and extended blood coagulation time. In general, we envision that the MMMs are potentially suitable as highly efficient hemoperfusion adsorbents for hyperphosphatemia treatment.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 6
·3120-3127
·
IF 3.591
Yixuan Huang,Liyan Xie,Kangji Zhuo,Hao Zhou,Yanhui Zhang
MIL-101(Fe)-based composite materials and their application for the generation of H2 by the catalytic reduction of nitro organics are reported in this study. NaBH4 and water contribute hydrogen for the catalytic reduction of nitro organics, but the possibility of nitro organics as a potential hydrogen source is often overlooked due to the simplicity of the reaction. However, experiments have revealed that the reaction process is accompanied by the production of H2, which is affected by the concentration of nitro organics. Moreover, the reaction is more conducive to the generation of H2 compared to NaBH4 hydrolysis under the same conditions. Unlike specially catalyzing the expensive NaBH4 hydrolysis, hydrogen is a by-product of the reduction of pollutants by inexpensive catalysts (NaBH4 acted as an electron donor for the catalyst). Accordingly, the reaction mechanism of p-nitrophenol hydride reduction was optimized. This work provides a new perspective on the application of this reaction.
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Catalysts
·
2020
·Vol. 10
·期 9
·1096
·
IF 3.52
Ligang Luo,Xiao Han,Qin Zeng
A series of Ni-Fe/SBA-15 catalysts was prepared and tested for the catalytic hydrogenation of levulinic acid to γ-valerolactone, adopting methanol as the only hydrogen donor, and investigating the synergism between Fe and Ni, both supported on SBA-15, towards this reaction. The characterization of the synthesized catalysts was carried out by XRD (X-ray powder diffraction), TEM (transmission electron microscopy), H2-TPD (hydrogen temperature-programmed desorption), XPS (X-ray photoelectron spectroscopy), and in situ FT-IR (Fourier transform–infrared spectroscopy) techniques. H2-TPD and XPS results have shown that electron transfer occurs from Fe to Ni, which is helpful both for the activation of the C=O bond and for the dissociative activation of H2molecules, also in agreement with the results of the in situ FT-IR spectroscopy. The effect of temperature and reaction time on γ-valerolactone production was also investigated, identifying the best reaction conditions at 200 °C and 180 min, allowing for the complete conversion of levulinic acid and the complete selectivity to γ-valerolactone. Moreover, methanol was identified as an efficient hydrogen donor, if used in combination with the Ni-Fe/SBA-15 catalyst. The obtained results are promising, especially if compared with those obtained with the traditional and more expensive molecular hydrogen and noble-based catalysts.Keywords:biomass ester derivatives;solvothermal processing;levulinic acid;γ-valerolactone;Ni-Fe bimetallic catalysts
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MINERALS ENGINEERING
·
2020
·
IF 3.795
Yang Cao,Xian Xie,Xiong Tong,Dongxia Feng,Jinfang Lv,Yumeng Chen,Qiang Song
This paper systematically analyzed the effects of Fe(II) ions on the cassiterite surface to promote the adsorption of salicylhydroxamic acid (SHA). The interaction behavior and mechanisms re investigated using micro-flotation experiments, adsorption experiments, zeta potential measurements, Fourier transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS). The micro-flotation tests revealed that the Fe(II) ions had a strong activation effect on the cassiterite, and the recovery reached the maximum at pH values of 7–8. The results of the adsorption experiment showed that the adsorption capacity of SHA on the mineral surface significantly improved after Fe (II) ion activation; this result was confirmed by the zeta potential test. In addition, the zeta potential results indicated that the positively charged Fe species absorbed on the cassiterite surface led to positive changes in the mineral surface potential and an increase in the number of active sites, thereby increasing the SHA adsorption. The XPS and FTIR results demonstrated that the Fe(II) ions activated the cassiterite through the interaction of terminal oxygen atoms with Fe species on the cassiterite surfaces, and redox reactions and displacement reactions occurred between Fe 2+ and Sn 4+ . SHA was chemisorbed on the cassiterite surface, allowing the anions to react readily with the Fe species to form Fe-SHA complexes. Therefore, the Fe(II) ion-activated cassiterite surfaces enhanced the strength and stability of the SHA chemisorption. Based on the results, an adsorption model of the Fe(II) ion-activated cassiterite surface in the SHA system was established.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Jing Wu,Mei Lin,Xiulan Weng,Gary Owens,Zuliang Chen
Emerging contaminants such as Mitoxantrone (MTX) are a major environmental concern because they have potential genotoxicity and mutagenesis to both aquatic organisms and humans. In this study, a pre-adsorption/Fenton-like oxidation system was developed which used a reduced graphene oxide/iron nanoparticles hybrid (rGO/Fe NPs) as both the adsorbent and the Fenton catalyst to remove MTX from solution. While the addition of H 2 O 2 alone removed only 11.3% of MTX, the rGO/Fe NPs/H 2 O 2 system was significantly more efficient removing 99.8% of MTX in the same period. This indicated that rGO/Fe NPs had excellent catalytic activity even at pH 7. This efficient removal was attributed to significant production of ·OH mainly by heterogeneous catalysis but supplemented by a homogeneous Fenton reaction, where ·OH had a higher affinity for MTX than SO 4 − ·. The sequential Fenton-like oxidation process best fits a pseudo-second-order kinetic model (R 2 ≥ 0.974). Characterizations of rGO/Fe NPs before and after the reaction, together with the identification of specific MTX degradation products , allowed possible degradation pathways to be proposed together with insights into the underlying mechanisms of MTX degradation when using rGO/Fe NPs in a pre-adsorption/Fenton-like oxidation system. Finally, the rGO/Fe NPs developed was successfully applied for the removal of MTX from spiked wastewater with 93.6% removal efficiency, which indicated that the proposed system had significant potential for wastewater treatment applications.
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ANALYST
·
2020
·Vol. 146
·期 1
·207-212
·
IF 3.978
Wenjie Jing,Xiangkun Cui,Fanbo Kong,Wei Wei,Yunchao Li,Louzhen Fan,Xiaohong Li
Identifying the species and concentrations of antioxidants is really important because antioxidants play important roles in various biological processes and numerous diseases. Compared with an individual sensor detecting a single antioxidant with limited specificity, a sensor array could simultaneously identify various antioxidants, in which 3–5 types of nanomaterials with peroxidase-like activity are absolutely necessary. Herein, as a single-atom nanozyme, Fe–N/C with oxidase-mimicking activity was applied to construct a triple-channel colorimetric sensor array: (1) Fe–N/C catalytically oxidized three substrates 3,3′,5,5′-tetramethylbenzidine (TMB), 2,2′-azino-bis(3-ethylbenzthiazoline-6-sulfonic acid) (ABTS) and o-phenylenediamine (OPD) to produce blue oxidized TMB (oxTMB), green oxidized ABTS (oxABTS) and yellow oxidized OPD (oxOPD), respectively; (2) with oxTMB, oxABTS and oxOPD as three sensing channels, a colorimetric sensor array was constructed for simultaneously discriminating glutathione (GSH), L-cysteine (L-Cys), ascorbic acid (AA), uric acid (UA), and melatonin (MT), even quantifying concentrations (with GSH as a model analyst). The performance of the sensor array was validated through accurately identifying 15 blind samples containing GSH, L-Cys, AA, UA and MT in buffer solution and human serum samples, and also in binary and ternary mixtures. This work proved that fabricating a single nanozyme-based sensor array was a simplified and reliable strategy for simultaneously probing multiple antioxidants.
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Scientific Reports
·
2020
·Vol. 10
·期 1
·1-11
·
IF 3.998
Dong Zijun,Chen Guanhan,Li Mu,Sun Feiyun,Jiang Chengchun,Bharti Bandna
Iodinated contrast media (ICM), which was widely used in medical imaging and was difficult to remove by conventional wastewater treatment methods, attained much attention due to its potential environmental impacts. Herein, iopamidol (IPM), one typical compound of ICM, was found to be rapidly degraded by ferrous activated persulfate oxidation (Fe(II)/PS) as compared with PS or Fe(II) alone. With a persulfate concentration of 1 mmol L −1 , n(Fe(II))/n(PS) of 1:10, and a pH of 3.0, 78% IPM was degraded within 60 min, with a degradation rate of 0.1266 min −1 . It was demonstrated that IPM degradation and deiodination were favored by a high temperature, while affected positively by acidic and neutral conditions. Radical quenching experiments and Electron Paramagnetic Resonace (EPR) spectra showed that the combined effects of SO 4 − · and · OH contributed dominantly to degrade IPM, while the · OH played an essential role during the degradation reaction. Through the Discrete Fourier Transform quantum chemical calculation, the possible reaction pathways for the oxidation of IPM by · OH are as follows: IPM-TP651-TP667-TP541-TP557, IPM-TP651-TP525-TP557, IPM-TP705-TP631-TP661, and IPM-TP705-TP735. The obtained results showed that IPM could be degraded effectively by Fe(II)/PS system, giving a promising technique for IPM removal from water.
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