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POLYMERS FOR ADVANCED TECHNOLOGIES · 2020 ·Vol. 32 ·期 2 ·690-702 · IF 2.578

Graphene oxide/multi-walled carbon nanotubes nanocompsite polyamide nanofiltration membrane for dyeing-printing wastewater treatment

Xiuzhen Wei,Shiyu Cao,Jiayao Hu,Yi Chen,Ruiyuan Yang,Jiahao Huang,Ze Wang,Qinghua Zhou,Jinyuan Chen

Graphene oxide (GO)/multi-walled carbon nanotubes (MWCNTs) modified nanofiltration (NF) membranes were successfully fabricated by interfacial polymerization of piperazine (PIP) and 1,3,5-benzenetricarbonyl trichloride (TMC). Compared with the pristine polyamide (PA) membrane and GO membrane, the typical structure of the granular protrusions on the surface of the GO/MWCNTs membrane gradually disappeared, and a regular ordered morphology appeared. The membrane thickness and surface roughness were increased according to the results of field emission scanning electron microscopy (FE-SEM) and atomic force microscopy (AFM). The contact angle of GO/MWCNTs NF membranes progressively decreased from 57° to 23°, indicating the enhancement of surface hydrophilicity. The best NF performance was achieved when the ratio of GO to MWCNTs was 6:3 (G-M-3). The water flux was 55.6 L/m 2 .h, which was 33.7% higher than that of the GO membrane, and the rejection rate for Na 2 SO 4 was maintained at approximately 94%. Both modified NF membranes could treat actual dyeing-printing wastewater effectively. The anti-fouling performance of G-M-3 was better than that of G3. Therefore, GO/MWCNTs-modified NF membranes have a good application prospects in the field of wastewater treatment and water purification.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2020 · IF 7.489

Thermal removal of partial nitrogen atoms in N-doped graphene for enhanced catalytic oxidation

Yang Zhao,Di Wu,Ying Chen,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Wenchao Peng

Carbon materials are effective catalysts to activate peroxymonosulfate (PMS) for organic pollutant degradation. Both nitrogen doping and structural defects could enhance their catalytic performance for PMS activation. In this study, nitrogen-doped graphene (NG) is first synthesized by the calcination of graphene oxide (GO) with ammonium nitrate (NH 4 NO 3 ). The obtained NG is then annealed further at a higher temperature under a N 2 atmosphere to remove partially doped N atoms and create new structural defects. The obtained defective nitrogen-doped graphene (D-NG) can activate PMS for bisphenol A (BPA) degradation more effectively. Different annealing temperatures from 850 to 1150 °C are investigated, and D-NG synthesized at 1050 °C exhibits the highest activity. The enhanced catalytic performance is proposed to originate from the synergistic effect between doped N atoms and created structural defects. According to radical quenching, electron paramagnetic resonance (EPR), and electrochemical results, both radical and nonradical pathways are present during PMS activation, and the nonradical pathway plays the dominant role. This study provides a facile method for metal-free catalyst synthesis, which also enriches the synergistic mechanism between doped N and structural defects and thus should have great potential in wastewater remediation.

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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2020 · IF 3.99

Difference between ammonia and urea on nitrogen doping of graphene quantum dots

Yanyun Zhu,Luting Yan,Mingyuan Xu,Yuting Li,Xiaodong Song,Lan Yin

Nitrogen-doped graphene quantum dots (N-GQDs) with prime fluorescence properties were synthesized through a simple one-pot hydrothermal method by using citric acid as carbon source and ammonia (A-GQDs) or urea (U-GQDs) as nitrogen source. Both A-GQDs and U-GQDs exhibited a graphene-like structure, but their average particle size is about ten times different. A-GQDs exhibited an evident excitation-dependent photoluminescence (PL) behavior. By contrast, the emission of U-GQDs can be divided into two regions with the development of excitation wavelength: a wavelength-independent emission peak at approximately 540 nm (green) with the excitation wavelength from 400 nm to 500 nm and an excitation-dependent emission peak with the excitation wavelength below 400 nm. Ammonia was introduced into citric acid polycondensator in the form of five membered ring and urea in the form of seven membered ring, respectively, which further affected the subsequent crystallization and surface functionalization. At this time, the structural instability of the nitrogen-containing doped ring itself, coupled with the progress of carbonization, mostly forms a stable nitrogen-containing ring structure, which is likely to be pyrrolic nitrogen or graphitized nitrogen. Therefore, the differences in particle size and nitrogen-containing doped rings partially between A-GQDs and U-GQDs lead to the differences in optical properties. Finally, U-GQDs with high quantum yield (QY) of 54 % were obtained at the molar ratio of 9:10 (citric acid/urea) by optimizing the reaction conditions.

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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Flexible, Strong, Multifunctional Graphene Oxide/Silica-Based Composite Aerogels via a Double-Cross-Linked Network Approach

Zheng Zheng,Yongliang Zhao,Jianhua Hu,Haitao Wang

Multifunctional silica-based aerogels are an emerging material due to their unique properties and wide applications. However, their large-scale production and application are limited due to the high cost and cumbersome preparation process. Herein, we prepare graphene oxide (GO)/silica-based composite aerogels via a simple in situ sol–gel reaction. GO nanosheets (GOs) are functionalized with polyethylenimine (PEI) and 3-glycidyloxypropyltrimethoxysilane (GPTMS) successively. After a cohydrolysis and condensation of trimethoxymethylsilane (MTMS) and dimethoxydimethylsilane (DMDMS) in the presence of GOs and a convenient ambient-pressure drying process, the composite aerogels are obtained. In addition to the normal cross-linking of MTMS and DMDMS, the GOs also behave as cross-linking points to significantly enhance the mechanical properties and thermal stability of the network of the composite aerogels. The pore structure of the aerogels is tailored by varying the GO loads as well as its surface modification. The Young’s modulus of a composite aerogel with a GO load of 0.5 wt % is about 5 times that for a neat polysiloxane aerogel, and the maximum degradation rate temperature is increased to over 90 °C. Compared with pure polysiloxane aerogel, the thermal insulation and flame resistance are also improved by a small addition of GOs. Moreover, GO/silica-based composite aerogels show stable piezo-resistive behavior. With the excellent mechanical properties, thermal stability, and multifunctionality, GO/silica-based composite aerogels show promising applications under some harsh and extreme conditions.

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Journal of Materials Chemistry A · 2021 ·Vol. 9 ·期 12 ·7791-7806 · IF 12.732

Modulating a 2D heterointerface with g-C3N4 mesh layers: a suitable hetero-layered architecture for high-power and long-life energy storage

Yunping Wu,Wei Wei,Tianyi Ding,Sheng Chen,Rui Zhai,Caihe Bai

Two-dimensional (2D) heterostructures combine the advantageous features of different 2D materials and represent advanced electrode architectures for the development of efficient energy storage devices. However, common 2D heterostructures made by stacking different 2D sheets in van der Waals (vdW) contact impose obvious limitations in light of the energy storage performance. Here, we shed light on how heterointerface conditions exert a great influence on the electrochemical properties of the heterostructured electrode and provide an example to modulate the interface contact mode via sandwiching unique g-C3N4 mesh (m-g-C3N4). We find that such m-g-C3N4 bonded heterointerfaces can greatly increase the electrochemical activity, redox conversion kinetics and structural integrity of the constituent component (NiS2), manifesting excellent electrochemical performance with respect to vdW heterostructures. Experimental characterization along with theoretical simulations demonstrates that the synergistic effects of the mesh-bonded interfacial contact and plenty of in-between porous channels contribute to superior electrochemical performance. This study directs attention to elaborate interface engineering toward high-performance energy storage and paves the way for designing and manufacturing of advanced heterostructured electrodes for supercapacitors, batteries and other hybrid devices.

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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2021 · IF 5.816

Hydrogen adsorption performance of Cu-BTC/graphene aerogel composite: A combined experimental and computational study

Wen Ren,Xudong Zhuang,Zhilu Liu,Song Li

Metal-organic frameworks (MOFs) are reported as potential hydrogen storage materials due to ultrahigh surface area and pore volume . However, most top-performing MOFs for hydrogen storage require strict synthesis conditions and high cost, which limits their wide applications. In this work, Cu-BTC/graphene aerogel (GA) composite is prepared at room temperature with improved hydrogen uptake at 100 bar compared with pristine Cu-BTC. To understand the mechanism of the enhanced hydrogen uptakes in the composite, grand canonical Monte Carlo (GCMC) simulation is executed for Cu-BTC/GA composites with different numbers of graphene oxide (GO) layers. It is demonstrated that the increased hydrogen uptake in Cu-BTC/GA composites is mainly ascribed to the hydrogen uptake in the interface region between Cu-BTC and GA. Additionally, the hydrogen uptake of the Cu-BTC/GA composites decreases as the number of GO layers increases, implicating that fewer GO layers or thinner GA is favorable for hydrogen adsorption of Cu-BTC/GA composites.

CAS / MDL: 7782-42-5 554-95-0
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NEW JOURNAL OF CHEMISTRY · 2021 ·Vol. 45 ·期 7 ·3630-3639 · IF 3.591

Study of the removal of ciprofloxacin by Zn–GO@SA aerogel microspheres

Kaijia Li,Hongxiang Ou,Dongsheng Zhou,Chenxia Gong,Honglai Xue,Yuyan Li

Graphene oxide (GO) has the advantages of a high specific surface area and great mechanical properties, which make it useful in the field of adsorption; however, it is difficult to obtain and utilize nano-size GO for adsorption and separation. In this study, zinc ion crosslinked GO and sodium alginate aerogel microspheres (Zn–GO@SA) were prepared using the ion–gel method and used for ciprofloxacin (CIP) adsorption, and this was easy to separate and collect from solutions. Methods such as SEM, EDX, FT-IR, and TGA were used for physical and chemical characterization. The adsorption properties and mechanisms were examined via static and dynamic adsorption experiments. The results indicated that the Zn–GO@SA aerogel microspheres had abundant and ordered cavities. The adsorption isotherm and kinetic data fitting results showed that the adsorption process was consistent with the Freundlich model and a quasi-second-order kinetics model. The adsorption of CIP was a multi-layer adsorption process dominated by chemical adsorption. At 308 K, the maximum adsorption capacity was 134.85 mg g−1, while increasing the adsorption temperature had an adverse effect on CIP adsorption. The results of regeneration and dynamic adsorption experiments showed that Zn–GO@SA aerogel microspheres maintained good adsorption performance after repeated use, which means they have potential for practical applications.

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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Self-Assembly of Hollow Graphene Oxide Microcapsules Directed by Cavitation for Loading Hydrophobic Drugs

Luyao Wei,Zhiquan Lu,Xiang Ji,Yike Jiang,Lan Ma

Hollow graphene oxide microcapsules (GOMs) have been widely used in energy, electronics, catalysis, sensing, tissue engineering, and drug loading due to their unique properties. However, it is still a great challenge to prepare GOMs with high quality and in large quantity using a simple method. In this work, we obtained single-component GOMs using the liquid nitrogen cavitation effect, which directed the self-assembly of graphene oxide (GO) debris at the gas–liquid interface. This method avoids the introduction of additional components and removal of templates. The morphology of GOM with wrinkles on its surface was characterized by transmission electron microscopy and scanning electron microscopy. The abundant polar groups of GO microcapsules enabled them to easily disperse in water. Based on this, GOMs have good potential for loading hydrophobic drugs. Subsequently, we used GOMs as carriers to deliver a hydrophobic drug paclitaxel (PTX), which exhibited a good loading capacity. Moreover, PTX loaded GOMs showed excellent cytotoxicity to A549 and MDA-MB-231 cells. The GOMs also showed a pH-dependent drug release performance. Therefore, GOMs can be regarded as potential carriers for biomedical applications.

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NEW JOURNAL OF CHEMISTRY · 2020 ·Vol. 45 ·期 4 ·1822-1833 · IF 3.288

One-step carbonization of a nickel-containing nitrogen-doped porous carbon material for electrochemical supercapacitors

Xufeng Song,Tianen Shui,Wanying Zhang,Keru Song,Xuesong Shan,Dongyu Zhao

In this study, we report a nickel-containing nitrogen-doped porous carbon material. Before this material is composited using a simple high-temperature treatment, it uses polystyrene microspheres as templates to prepare polyaniline microspheres and nickel ion-containing graphene oxide materials. This preparation method is efficient and convenient. We observed that polystyrene microspheres disappeared during high-temperature treatment, and the formation of a porous structure increased the specific surface area of this material. The prepared polyaniline provides N atoms and adds additional capacitance to the material. Besides, during the high-temperature treatment of graphene oxide containing nickel ions, the electrical properties of the material is further increased due to nickel-metal formation after reducing nickel ions. Hence, the Ni-containing N-doped porous carbon material samples showed good specific capacitance (351 F g−1). After 5000 cycles of charge and discharge, the capacitance remained at 92.1%. The calculated energy and power density of the assembled symmetrical supercapacitor were 6.16 W h kg−1 and 5994 W kg−1, respectively. Therefore, in the field of supercapacitors, the Ni-containing N-doped porous carbon materials prepared in this paper have a broad application prospect.

CAS / MDL: 1321-74-0 7782-42-5
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Analytical Methods · 2020 ·Vol. 13 ·期 5 ·672-684 · IF 2.596

Facile synthesis of magnetic molybdenum disulfide@graphene nanocomposite with amphiphilic properties and its application in solid-phase extraction for a wide polarity of insecticides in wolfberry samples

Xiao-Chun Ma,Zong-Qin Ma,Meng-Xin Zhao,Ying-Hui Wang,Yuan Peng,Xin Guo,Fang-Huan Wang,Zhe Meng,Hao-Bo Zheng

A novel magnetic molybdenum disulfide@graphene (Fe3O4/MoS2@G) nanocomposite with amphiphilic properties was prepared via a co-mixing solvothermal method. To demonstrate the feasibility of Fe3O4/MoS2@G as a sorbent during sample preparation, it was employed for the magnetic solid phase extraction (MSPE) of ten pyrethroids, three triazoles and two acaricide pyridaben and picoxystrobin in an emulsified aqueous solution. Dichloromethane was used as the extractant to form an emulsified aqueous solution. Subsequently, the Fe3O4/MoS2@G sorbent with amphiphilic properties was used to retrieve 15 wide polarity insecticides from dichloromethane via MSPE. The proposed method has the advantage of being applicable to different polar pesticides, strengthening the capacity of enrichment and purification of target analytes. The π–π interaction between the hydrophilic and hydrophobic moieties of Fe3O4/MoS2@G and the aromatic rings of target analytes were responsible for the efficient sorption. Thus, a reliable, convenient, and efficient method for the analysis of 15 insecticides with wide polarity in wolfberry samples was established by coupling Fe3O4/MoS2@G nanocomposite MSPE with gas chromatography-mass spectrometry (GC-MS) analysis. The obtained linearity of this method was in the range from 1 to 5000 ng mL−1 for 15 analytes, with determination coefficients (R2) ≥0.9907. The limit of detection (LOD) for 15 insecticides was in the range from 0.1 to 5.0 ng g−1. The recoveries of 15 insecticides from spiked wolfberry samples were in the range from 71.41% to 110.53%, and RSD was less than 14.8%.

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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Constructing a charged-state Na-NiCl2 battery with NiCl2/graphene aerogel composite as cathode

Yanpei Li,Lei Shi,Xingpeng Gao,Jingyi Wang,Yingying Hu,Xiangwei Wu,Zhaoyin Wen

The hierarchical nickel chloride/reduced graphene oxide (NiCl 2 -rGO) aerogels are synthesized via a facile hydrothermal and freeze-drying methods using low-cost nickel chloride hexahydrate (NiCl 2 ·6H 2 O) as raw material. The NiCl 2 -rGO hybrid aerogel structure enables the uniform distribution of lamellar NiCl 2 on the three-dimensional (3D) cross-linked conductive graphene sheets. When employed as cathode for sodium-nickel chloride (Na-NiCl 2 ) batteries, the as-obtained NiCl 2 -rGO aerogels exhibit excellent electrochemical performance with high reversible capacities (116 mAh g −1 after 50 cycles, 128 mAh g −1 in a fixed capacity window (20%–80% state of charge (SOC)) after 50 cycles), and a ultra-low polarization (0.05 V in the fixed capacity window). The outstanding performance of NiCl 2 -rGO aerogels can be attributed to the excellent conductivity of graphene. Moreover, the strong contact between NiCl 2 and graphene sheets can effectively promote the transfer of electrons. Compared with traditional tubular Na-NiCl 2 batteries, the molar ratio of Ni/NaCl of NiCl 2 -rGO aerogels can be decreased from 1.8 to the stoichiometric ratio (0.5). To the best of our knowledge, this work paves a perspective way for the first time to develop charged-state NiCl 2 -based cathodes with splendid performance for Na-NiCl 2 batteries.

CAS / MDL: 7647-14-5 7782-42-5
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CHEMOSPHERE · 2020 · IF 5.778

Reduced graphene oxide/Bi4O5Br2 nanocomposite with synergetic effects on improving adsorption and photocatalytic activity for the degradation of antibiotics

Mengwen Xu,Yanying Wang,Enna Ha,Huijuan Zhang,Chunya Li

A photocatalyst based on the integration of reduced graphene oxide (rGO) with Bi 4 O 5 Br 2 nanosheets was facilely prepared and was confirmed by transmission electron microscope , scanning electron microscope, X-ray diffraction and Raman spectroscopy . The integration of rGO can effectively improve the adsorption and the photocatalytic properties of Bi 4 O 5 Br 2 nanosheets towards the target antibiotics under visible light irradiation. rGO/Bi 4 O 5 Br 2 nanocomposite containing 1.0 wt% of rGO exhibits the optimal adsorption and photocatalytic activity towards ciprofloxacin (CIP), norfloxacin (NOR) and tetracycline (TC). The removal efficiencies of CIP, NOR and TC are 97.6%, 80.7% and 98.7%, which are higher than that obtained with Bi 4 O 5 Br 2 nanosheets. The capture experiments and ESR data show that ·O 2 − , OH· and h + are the main active species that participated in the photodegradation system. This work provides a simple strategy to integrate rGO with Bi x O y X z (X = Cl, Br, I) nanosheets to construct effective photocatalysts for the degradation of antibiotics.

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