JOURNAL OF FLUORINE CHEMISTRY
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2020
·
IF 2.332
Yongyang Chen,Dan Guo,Xiaochun Dong,Yahui Li,Yixuan Huang,Hao Chen,Shanping Li
Perfluorooctanoic acid (PFOA), as a refractory organic pollutant, seriously harms the environment and damages human health. Here, the electrocatalytic method was selected to degrade PFOA. In this work, perovskite catalysts doped with different elements, and corresponding gas diffusion electrodes (GDE) were prepared by the gel-sol method and citric acid complexation method. The crystal structure, microscopic morphology, and electrochemical properties of the LaNi x Y 1-x O 3 (Y = Fe, Cu, Co, Sr) perovskite catalyst electrode were analyzed by XRD, TEM, and CV. Moreover, the electrocatalytic performances of the as-prepared electrodes were assessed by the degradation of PFOA, and the Sr-doped GDE exhibited the highest degradation rate of PFOA. The optimum degradation conditions, such as the current density, pH, and initial concentration were also investigated. It was observed that when the current density was 20 mA/cm 2 , pH was 5, and initial concentration was 0.25 mmol/L, the Sr-doped GDE had the best degradation and defluorination efficiency of PFOA reached 90.0 % and 75.1 %, respectively. High performance liquid chromatography-mass spectrometry (HPLC-MS) was used to analyze the intermediate products of PFOA degradation and obtain the degradation pathway. With the combined action of OH and O 2 , PFOA was degraded by stepwise removal of CF 2 groups, which were ultimately degraded into F − and CO 2 .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Hailong Tian,Mengzhu Zhang,Guoxia Jin,Yue Jiang,Yuxia Luan
Chemodynamic therapy (CDT) utilizes Fenton catalysts to convert intracellular hydrogen peroxide (H 2 O 2 ) into cytotoxic hydroxyl radical (OH∙) for tumor therapy, but endogenous H 2 O 2 is usually insufficient to achieve satisfactory tumor therapy effect. Engineering an efficient CDT nanoplatform for satisfactory cancer therapy remains a challenge. Herein, we rationally designed a Cu-based metal-organic framework-199 (MOF-199) nanoplatform integrating vitamin k3 (Vk3) for amplified CDT-mediated cancer therapy, which could accumulate efficiently in tumor tissues through enhanced permeability and retention (EPR) effect. The MOF-199 nanoparticles (MOF-199 NPs) were dissociated by glutathione (GSH) into MOF-199 fragments, which triggered Fenton-like reaction for CDT. On the one hand, Vk3 was catalyzed by NAD(P)H quinone oxidoreductase-1 (NQO1) to produce sufficient H 2 O 2 to activate Fenton-like reaction. On the other hand, GSH was largely consumed in the tumor microenvironment. Thus, this nanoplatform enabled sufficient cytotoxic reactive oxygen species (ROS) for amplified CDT effect, demonstrating effective tumor growth inhibition with minimal side-effect in vivo. Our work provides an innovative strategy to modulate GSH and H 2 O 2 levels for amplified CDT.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Xiang-Dong Xue,Cheng-Ran Fang,Hai-Feng Zhuang
In this work, the hypothesis that thermoplastic polyurethane (TPU) microplastics (MPs) could form complex toxic pollution by absorbing both antibiotics and heavy metals simultaneously was proposed. The unique features of the adsorption of Cu(II) and oxytetracycline (OTC) on the pristine TPU and photo-aged (aged) TPU MPs in single and coexisting system were investigated, which included the kinetics, isothermal equilibrium and thermodynamics. The possibly synergistic or competitive effects between Cu(II) and OTC were also evaluated. The results showed that the adsorption process of Cu(II) and OTC could be described well by pseudo-second-order kinetic equation . The entire process could be divided into two stages: internal diffusion and external diffusion. The Sips model could give good fitting for the isothermal adsorption equilibrium. The thermodynamic parameters depicted the endothermic nature of adsorptions and the process was spontaneous. In the coexisting system, synergistic or competitive effects depended critically on the ratio of concentrations (Cu(II) vs OTC). When the ratio was 1:1, Cu(II) significantly enhanced the adsorption of OTC, while OTC showed a weak effect on Cu(II) adsorption. The synergies could be attributed to the formation of Cu(II)-OTC complex and the bridging effect of Cu(II). Overall, the adsorption capacity of aged TPU was higher than that of pristine TPU, which was due to the differences in morphological characteristics and functional groups. FTIR studies revealed that ester carbonyl and acylamino groups in the TPU may be involved in the adsorption of Cu(II) and OTC.
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Polymers
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2020
·Vol. 12
·期 10
·2419
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IF 3.426
Fang Wang,Sheng Hu,Fengna Shi,Kexin Huang,Jiarui Li
Herein, a composite structure, consisting of Cu nanoparticles (NPs) deposited onto carbon nanotubes and modified with ferrocene-branched chitosan, was prepared in order to develop a nonenzymatic electrochemical glucose biosensor ferrocene-chitosan/carbon nanotube@ Cu (Fc-CHIT/CNT@Cu). The elemental composition of the carbon nanohybrids, morphology and structure were characterized by various techniques. Electrochemical impedance spectroscopy (EIS) was used to study the interfacial properties of the electrodes. Cyclic voltammetry (CV) and chronoamperometry methods in alkaline solution were used to determine glucose biosensing properties. The synergy effect of Cu NPs and Fc on current responses of the developed electrode resulted in good glucose sensitivity, including broad linear detection between 0.2 mM and 22 mM, a low detection limit of 13.52 μM and sensitivity of 1.256 μA mM−1cm−2. Moreover, the modified electrode possessed long-term stability and good selectivity in the presence of ascorbic acid, dopamine and uric acid. The results indicated that this inexpensive electrode had potential application for non-enzymatic electrochemical glucose detection.Keywords:carbon nanotube;chitosan;copper nanoparticles;ferrocene;electrochemical sensor;glucose;non-enzymatic
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JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Dazhong Yang,Zheting Chu,Renji Zheng,Wenfei Wei,Xuezhen Feng,Juan Zhang,Chunyan Li,Zuotai Zhang,Hong Chen
Due to the large output and potential ecological risks, disposal of engineering abandoned soils (EAS) has become an enormous challenge for human society. Herein, EAS has been transformed into microporous analcime (ANA) zeolite material through a fast, energy-efficient, and straightforward conversion process. The as-synthesized ANA has been employed to remediate Cu-polluted soil, which shows a significant ecological restoration function in a vegetable pot experiment. With 25 g/kg ANA into Cu contaminated soil (total Cu concentration: 200 ppm), the Cu accumulation concentration in vegetables has been decreased from 5.60 down to 1.80 mg/kg (approaching the background Cu level 1.70 mg/kg in vegetables). Detailed mechanism study combining with DFT calculations reveals that the Cu 2+ in soil has been captured both inside the ANA pore channels and on the surface via ion-exchange and surface adsorption mechanism. The whole process, including ANA synthesis and Cu polluted soil remediation , has been optimized to show a valuable conceptual model to recycle EAS resource and in-situ remediate Cu polluted soil.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
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IF 4.939
Ying-Hua Zhou,Xingyun Cao,Jingzhu Ning,Changchun Ji,Yong Cheng,Jing Gu
To exploit the low-cost and efficient catalyst for the hydrolytic dehydrogenation of ammonia borane , trace amount of palladium-doped transition metal (Cu, Ni, Co, Fe and Zn) nanoparticles have been incorporated into the interior of metal-organic frameworks named ZIF-8, ZIF-67, ZIF-67/ZIF-8 and core-shell ZIF-67@ZIF-8 by a double-solvent approach. The optimized catalyst of CuPd 0.01 @ZIF-67@ZIF-8 composite exhibited an excellent activity with a turnover frequency (TOF) value of 30.15 mol H 2 (mol metal ) −1 min −1 at 298 K and a relatively low activation energy of 38.78 kJ mol −1 . It might attributed to both ultrafine size of metal nanoparticles (~3 nm) induced by the confinement of core-shell ZIF-67@ZIF-8 and the synergistic effect between Pd and Cu. Moreover, the detailed kinetic study has manifested that this catalytic reaction is first-order in regards to the catalyst amount while zero-order as for the concentration of ammonia borane. In addition, the durability and recyclability of CuPd 0.01 @ZIF-67@ZIF-8 have been demonstrated to be great.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Huiyuan Cheng,Xuemei Wu,Xiangcun Li,Xiaowa Nie,Shuai Fan,Manman Feng,Zihao Fan,Mingqian Tan,Yonggang Chen,Gaohong He
Although considerable progress has been achieved by Cu nanoparticles for catalyzing CO 2 reduction reaction (CO2RR), Cu single atom catalysts (Cu SACs) are generally suffered from inferior performance to that of widely investigated Fe, Co, Ni SACs. This phenomenon mainly ascribes to the lack of effective geometry and electronic engineering of copper active center from an atomic level. Herein, highly exposed atomically dispersed Cu-N x ( x denotes Cu–N coordination number) sites anchored on 3D porous carbon matrix are successfully synthesized through facile one step thermal activation, and Cu-N 4 sites exhibit boosted activity and selectivity compared to its nearly inert Cu-N 3 counterparts. Aided by density functional theory (DFT) calculations, the edge-hosted Cu-N 4 moieties are revealed as key active sites for efficient CO generation via optimized local coordination environment and electronic properties, which strongly interact with *COOH intermediate and facilitate the desorption of *CO. As a result, Cu-N 4 catalyst achieves high CO Faradaic efficiency (FE CO ) of over 90% from −0.6 to −1.1 V vs . RHE with a maximum value of 98%, surpassing the previously reported Cu SACs for CO 2 -to-CO conversion. This work provides new insight into proper Cu SACs design and fundamental mechanism understanding to boost CO2RR.
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Journal of Central South University
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2020
·Vol. 27
·期 4
·1176-1185
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IF 1.249
Jin Lin-feng,Chai Li-yuan,Song Ting-ting,Yang Wei-chun,Wang Hai-ying
Magnetic Fe 3 O 4 @Cu/Ce microspheres were successfully prepared by one-step solvothermal approach and further utilized to remediate toxic arsenic (As(III)) pollution. The effects of Cu/Ce elements co-doping on the crystal structure, catalytic oxidation and adsorption behaviors of magnetic microspheres were researched systematically. The results showed that with the aid of Cu/Ce elements, the grain size reduced, lattice defects increased, and the oxygen vacancies and surface hydroxyl groups were improved. Therefore, Cu/Ce elements endowed magnetic Fe 3 O 4 @Cu/Ce microspheres with excellent As(III) removal performance, whose maximum adsorption capacity reached 139.19 mg/g. The adsorption mechanism mainly involved catalytic oxidant co-adsorption. This research developed a feasible strategy for the preparation of high efficiency magnetic adsorbent to enhance the removal of As(III).
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
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IF 3.573
Tengjiao He,Yonghou Xiao,Qidong Zhao,Mengxue Zhou,Gaohong He
Separation of carbon dioxide (CO2) from a CO2/ethylene (C2H4) mixture represents an important and challenging field in industrial applications. Selective adsorption has become an attractive option as an energy-saving and environmentally friendly CO2 capture technology. In this work, an ultramicroporous metal–organic framework (MOF) Qc-5-Cu was prepared by solution method and applied for the highly selective separation of CO2 from an C2H4 stream. The performance of Qc-5-Cu was evaluated by static and dynamic adsorption experiments. It was found that the single-component adsorption capacities of CO2 and C2H4 on Qc-5-Cu at 298 K and 1 bar were 2.48 and 0.74 mmol/g, respectively. The measured breakthrough curves further illustrate that Qc-5-Cu could effectively separate CO2 from the C2H4 stream for more than 10 cycles. The pore size of the obtained Qc-5-Cu was ∼3.3 Å, as characterized by nitrogen adsorption. The ultramicroporous structure of Qc-5-Cu benefits the separation of CO2, as evidenced by the selectivity values of the CO2/C2H4 binary mixture (1:99, v/v) based on the ideal adsorbed solution theory (SIAST ≈ 39.95 avg.), which are larger than some MOFs with open metal sites, owing to the weak interaction between organic ligands with high aromaticity and C2H4, as well as the porous screening effect of Qc-5-Cu on ethylene. The observed high selectivity, excellent stability, and regeneration performance demonstrate that Qc-5-Cu is a promising adsorbent for the separation of the CO2/C2H4 mixture.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2020
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IF 7.864
Yi Ren,Mengqi Shi,Weiming Zhang,Dionysios D. Dionysiou,Junhe Lu,Chao Shan,Yanyang Zhang,Lu Lv,Bingcai Pan
A novel Fenton-like catalyst was synthesized by immobilizing nano-Fe2O3 (nFe2O3) on MIL-53(Cu). The pseudo-first-order rate constant of bisphenol A degradation in the nFe2O3/MIL-53(Cu)/H2O2 system reached 0.0123 min–1, while the values in MIL-53(Cu)/H2O2 and nFe2O3/H2O2 systems were only 0.0026 and 0.0040 min–1, respectively. The characterization of nFe2O3/MIL-53(Cu) reveals that the supreme catalytic activity of this material could be ascribed to iron–copper synergy, smaller size, and better dispersion of nFe2O3 particles. Moreover, a method of trapping Cu(I) by neocuproine was developed, which could shield Cu(I) from interacting with iron and H2O2, and thus allow quantitative differentiation of the contribution to the enhanced catalytic activity by each of the factors. Using this method, 19% of the enhancement was determined to be contributed by synergistic effect, while 24% of the enhancement was due to the smaller size and better dispersion of the nFe2O3 particles on MIL-53(Cu) support. In addition, the performance of nFe2O3/MIL-53(Cu) only dropped 10.7% after five treatment cycles in real wastewater, showing good potential in practical application. We believe this study sheds light on the tailored design of Fenton-like catalysts and elucidates the catalytic mechanisms of supported bimetallic catalysts.
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Arabian Journal of Chemistry
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2020
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IF 4.762
Shuailong Cheng,Qintie Lin,Yupeng Wang,Haoyu Luo,Zhuofan Huang,Hengyi Fu,Hengrui Chen,Rongbo Xiao
In order to improve the heavy metal removal ability of traditional single washing agents and explore the removal mechanism of heavy metals. Then, the washing reagents that mixed by low-molecular weight organic acids (citric acid, oxalic acid, and tartaric acid) and artificial chelating compound ethylenediaminetetraacetic acid disodium (EDTA) were selected. Furthermore, the effect of soil washing parameters, the variation of leaching toxicity, mobility, stability and speciation of heavy metals were also considered. The results of soil washing experiments showed that mixing an equal volume of 0.05 M EDTA and 0.2 M organic acids (citric acid, oxalic acid, and tartaric acid) could remove more than about 80% heavy metals from soil under the optimal conditions. In addition, the soil leaching toxicity was decreased and the stability of remaining heavy metals was increased, indicating that EDTA-organic acid washing reagents could effectively reduce the ecological risk of contaminated soil. EDTA had a stronger chelating ability with heavy metals than the organic acids, and the organic acids could not only chelate heavy metals but also decrease the pH of the mixture for promoting the desorption of heavy metals. Thus, mixing EDTA and organic acids was advisable method to improve soil washing technology.
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CATALYSIS TODAY
·
2020
·
IF 5.825
Jianzhe Shi,Yan He,Kui Ma,Siyang Tang,Changjun Liu,Hairong Yue,Bin Liang
The dimethyl oxalate (DMO) hydrogenation reaction is the key step of indirect synthesis of C 2 -C 4 oxygenates (e.g., ethanol) from syngas. Copper-based catalysts have been extensively explored for DMO hydrogenation. However, the unstable copper active sites induced by metal-particle growth at high rection temperatures (e.g., > 553 K) is an impediment to the stable performance. Herein, we report a facile co-precipitation method to confine Cu active sites in the layered double hydroxide for the hydrogenation of DMO to ethanol. The effects of Mg/Al molar ratio on the catalytic performance were systematically investigated to get insights into the structure-activity relationship. The results indicate that the CuMgAl-LDH-1.25 catalyst possesses regular lamellar structures, highly dispersed Cu active sites, and moderate acidic sites, which synergistically achieves a stable performance with a DMO conversion of ca. 100 % and ethanol selectivity exceeding 83 % at 553 K, 3 MPa.
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