Journal of Materials Chemistry B
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2020
·Vol. 8
·期 37
·8671-8683
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IF 5.344
Zhen Xiang,Yiyao Qi,Yusheng Lu,Zhenrong Hu,Xiao Wang,Wenwen Jia,Jingzhou Hu,Jiansong Ji,Wei Lu
Multifunctional nanomedical platforms have broad prospects in imaging-guided combination therapy in cancer precision medicine. In this work, metal–organic framework (MOF)-derived novel porous Fe3O4@C nanocomposites were developed as an intelligent cancer nanomedical platform for combined cancer therapy with MRI-guided magnetic-triggered hyperthermia and chemotherapy functions. The magnetic behavior, porous character and good surface modification endowed this smart nanoplatform with favorable biocompatibility, high-efficiency MRI imaging, magnetic-triggered on-demand DOX release function, and synergistic therapy of magnetic hyperthermia and chemotherapy, which proposed an all-in-one platform for cancer therapy. Additionally, in vivo animal experiments verified the significant suppression of malignant tumor growth with negligible side effects, which were attributed to the consecutive 13 day synergistic therapy of magnetic hyperthermia and chemotherapy in one. To be specific, Fe3O4@C-PVP@DOX significantly decreases the volume (2.5 to 0.44 of tumor volume ratio) and weight (0.49 g to 0.10 g) of tumors after magnetic-triggered hyperthermia and chemotherapy treatments. Moreover, no big difference of body weight and associated damage was observed among all major organs. Therefore, owing to its high-efficiency combined therapy of magnetic-triggered hyperthermia and chemotherapy, this smart nanoplatform holds great potential application in the precise treatments of clinical cancer.
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高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
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2020
·Vol. 26
·期 56
·12882-12890
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IF 4.857
Qiongguang Li,Yanhong Wang,Qiangqiang Tan,Ziyi Zhong,Fabing Su
Graphical Hollow core–shell anode : An SnO 2 @C@Co-NC anode material with hollow core–shell structure was structurally designed and synthesized by a heteroatom-doping and multiconfinement approach. This material can efficiently alleviate the volume expansion of the SnO 2 -based anode materials and exhibits much-enhanced electrochemical performance, including high rate performance and cycle stability, as well as superior capacity. To overcome the drawbacks of the structural instability and poor conductivity of SnO 2 -based anode materials, a hollow core–shell-structured SnO 2 @C@Co-NC (NC=N-doped carbon) composite was designed and synthesized by employing the heteroatom-doping and multiconfinement strategies. This composite material showed a much-reduced resistance to charge transfer and excellent cycling performance compared to the bare SnO 2 nanoparticles and SnO 2 @C composites. The doped heteroatoms and heterostructure boost the charge transfer, and the porous structure shortens the Li-ion diffusion pathway. Also, the volume expansion of SnO 2 NPs is accommodated by the hollow space and restricted by the multishell heteroatom-doped carbon framework. As a result, this structured anode material delivered a high initial capacity of 1559.1 mA h g −1 at 50 mA g −1 and an initial charge capacity of 627.2 mA h g −1 at 500 mA g −1 . Moreover, the discharge capacity could be maintained at 410.8 mA h g −1 after 500 cycles with an attenuation rate of only 0.069 % per cycle. This multiconfined SnO 2 @C@Co-NC structure with superior energy density and durable lifespan is highly promising for the next-generation lithium-ion batteries.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
·
IF 3.573
Yinan Gu,Guixiang Teng,Xiaodong Jin,Liping Wang,Zengwei Qiang,Weigang Ma,Chun Zhang
A coral-like ZnO/C-ZnFe2O4 (Z/C-ZFO) photocatalyst was synthesized by simulating the structural characteristics of coral since its structure is conducive to the capture and absorption of light. The synthesis process involves a two-step process. First, flowerlike hierarchical precursors were synthesized through a hydrothermal self-assembled route. Next, the precursors were thermally annealed in a nitrogen atmosphere after doping with a zinc source. In addition to forming heterojunctions that enhance its photocatalytic properties, the coral-like nanostructures endowed Z/C-ZFO with significant light-harvesting efficiency. Finally, the photocatalyst was used for antibacterial applications against Escherichia coli and Staphylococcus aureus bacteria. The results showed that the optimized sterilization efficiencies toward E. coli and S. aureus bacteria were 99.4 and 98.0%, respectively, combined with excellent cycling stability. The method of designing and synthesizing coral-like structures in this study may also be extended to the synthesis of other photocatalytic and optical materials.
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CARBON
·
2020
·
IF 8.821
Shuqi Hu,Wenpeng Ni,Daihui Yang,Chao Ma,Jiaheng Zhang,Junfei Duan,Yang Gao,Shiguo Zhang
Atomically dispersed Fe–N–C catalysts with additional Fe-containing nanoparticles including metal, carbides or oxides have shown great potentials towards oxygen reduction reaction (ORR) catalysis. However, the formation of these synergistically active nanoparticles and the effect of the porous carbon structures remain unclear. In this work, a novel single-atom-involved electrochemical catalyst, i.e. , Fe 3 O 4 nanoparticles encapsulated in atomically dispersed Fe–N–C (Fe 3 O 4 @FeNC) was reported. The optimized Fe 3 O 4 @FeNC exhibits excellent ORR activity with a half-wave potential of 0.890 V and a Tafel slope of 58.8 mV dec −1 , comparable with recently reported ORR catalysts and superior to these of commercial Pt/C. More importantly, the porous architectures not only affect the mass transfer and active sites, but casts huge influence on the nucleation of Fe 3 O 4 nanoparticles, the graphitization degree of the carbon support, the chemical environments of the elements, and the ORR catalytic pathways. Density functional theory calculations show stronger O 2 adsorption on Fe–N–C when supported on Fe 3 O 4 moieties, which may increase the reactant concentration for ORR and promote the overall activity. These findings will provide important references for the future understanding and design of single-atom-involved catalysts with enhanced electrochemical properties .
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MOLECULAR PHARMACEUTICS
·
2020
·
IF 4.321
Zhengzhong Wu,Bin Chen,Ziying Gan,Fan Chen,Xianglin Luo
The effective accumulation at tumor sites and endocytosis by tumor cells for anticancer agents in carriers are essential in successful cancer therapy, and both of the processes are affected by the surface charge of drug carriers. In this study, vitamin C (VC) was employed as an “exogenous switch” to trigger the surface charge conversion of DOX-loaded micelles to obtain a better antitumor effect. T micelles formed by poly(ε-caprolactone)-b-poly(N,N-diethylaminoethyl methacrylate)-ss-b-poly(2-methacryloyloxyethyl phosphorylcholine) (PCL–PDEA-ss-PMPC) turned their ζ potentials from +1 mV to +18 mV under treatment of 20 mM VC, while the ζ potentials of control R micelles formed by PCL-ss-P(DEA-r-MPC) almost remained unchanged under the same condition. DOX-loaded T@DOX and R@DOX had high DLCs of 12% and 13.8%, respectively, and both showed an accelerated drug release in a reductive environment (10 mM GSH or 20 mM VC) at pH 5.0. Notably, due to the surface charge conversion and fast drug release triggered by VC, T@DOX/VC (T@DOX was pretreated by VC) showed an enhanced cytotoxicity and cellular uptake superior to T@DOX, R@DOX, and R@DOX/VC. T@DOX/VC also displayed the in vivo antitumor effect well, which was comparable to DOX·HCl but with less toxic side effects than DOX·HCl. In summary, VC as an exogenous trigger can induce a better antitumor effect of drug-loaded micelles with a suitable polymer structure by charge conversion, and T@DOX/VC has shown to be as a promising approach to achieve potent treatment of tumors.
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APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Yuan Zhuang,Jiemin Liu,Siyi Yuan,Ben Ge,Hao Du,Chen Qu,Haiying Chen,Chuandong Wu,Wenhui Li,Yan Zhang
Volatile organic compound (VOC) elimination technologies have been investigated to alleviate health damage and to reduce serious environmental risks. The degradation of hydrophobic and refractory VOCs calls for advanced oxidation processes with high degradation efficiency and low-level toxic byproduct generation. In this study, core-shell Fe 3 O 4 @C was employed as an advanced oxidation microreactor for hydrophobic and refractory VOC removal during the Fenton process, and octane was chosen as a typical target pollutant. The average octane removal efficiency increased by 41.6%, while the main byproduct concentrations decreased by 65.8% in the initial 60 min compared with Fe 3 O 4 . Density functional theory (DFT) calculations revealed the key role of Fe O C bond during the regeneration of Fe(II) species, and the enhanced octane adsorption process by the carbonyl sites. Calculation of mass transfer enhancement factor proved that the carbon shell was critical during mass transfer process. The advanced oxidation mechanism was investigated by detection and measurement of byproducts and hydroxyl radicals and XPS analysis. The synergism and the octane degradation pathway was proposed based on the two main types of reactions. This core-shell Fenton system suggests a promising approach for catalyst and microreactor design in advanced oxidation technologies for refractory VOCs removal.
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JOURNAL OF CATALYSIS
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2020
·
IF 7.888
Yingchun Guo,Lei Feng,Changcheng Wu,Xiaomei Wang,Xu Zhang
Rational design and fabrication of metal–organic framework (MOF)-derived ordered hierarchical macro-/meso-/microporous N-doped carbon materials featured with the atomically dispersed metal atoms can effectively enhance their catalytic performance. Herein we develop a template-assisted strategy, namely the confined growth and pyrolysis of single-crystalline zeolite imidazolate framework-8 (ZIF-8) in three-dimensional ordered template voids, to create hierarchical porosity in MOFs-derived N-doped carbon materials. The as-synthesized single-atom Zn on N-doped hierarchically ordered porous carbon polyhedrons (Zn-N-HOPCPs) show integrated Lewis acid (single-atom Zn) and base sites (pyridinic N), high surface area (1128 m 2 ·g −1 ), large pore volume (0.90 cm 3 ·g −1 ), periodically interconnected open windows (~55 nm), highly accessible micro/mesopore channels (0.55, 0.8, 1.2, and 4 nm), and abundant Zn content (5.8 wt%). The hierarchical nanoarchitecture (macro-/meso-/micropores) significantly facilitates mass transfer for bulky-molecule-involved reactions and exposes inside active sites, resulting in satisfactory CO 2 photoconversion under mild conditions. The strategy presented here sheds light on the design and fabrication of various hierarchically ordered porous carbon decorated with atomically dispersed metal atoms for other important applications.
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Nanomaterials
·
2020
·Vol. 10
·期 9
·1629
·
IF 4.324
Ranran Jiao,Li Zhao,Shuli Zhou,Yanjun Zhai,Denghu Wei,Suyuan Zeng,Xianxi Zhang
In this study, a simple method was adopted for the synthesis of MnO@C nanocomposites by combining in-situ reduction and carbonization of the Mn3O4precursor. The carbon content, which was controlled by altering the annealing time in the C2H2/Ar atmosphere, was proved to have great influences on the electrochemical performances of the samples. The relationships between the carbon contents and electrochemical performances of the samples were systematically investigated using the cyclic voltammetry (CV) as well as the electrochemical impedance spectroscopy (EIS) method. The results clearly indicated that the carbon content could influence the electrochemical performances of the samples by altering the Li+diffusion rate, electrical conductivity, polarization, and the electrochemical mechanism. When being used as the anode materials in lithium-ion batteries, the capacity retention rate of the resulting MnO@C after 300 cycles could reach 94% (593 mAh g−1, the specific energy of 182 mWh g−1) under a current density of 1.0 A g−1(1.32 C charge/discharge rate). Meanwhile, this method could be easily scaled up, making the rational design and large-scale application of MnO@C possible.Keywords:MnO@C nanocomposites;carbon content;current density;lithium-ion battery;transition metal oxide anode
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CARBON
·
2020
·
IF 8.821
Xueliang Fan,Hongbin Zhang,Boxu Gao,Haiyang Lu,Luyao Zheng,Xue Yang,Yahong Zhang,Qingsheng Gao,Yi Tang
To explore high-performance carbide catalysts for hydrogen evolution reaction (HER), the rational design of hierarchically porous catalyst benefitting active-site exposure and fast mass transport is extremely demanded. Herein, Chinese ink (CI), used for writing and drawing for thousands of years, is adopted to promote the formation of co-assembly of carbon nanoparticles and Mo-based lamellar organic-inorganic hybrids, which, after pyrolysis in Ar atmosphere , is further converted to 3D hierarchically structured and porous MoC x /C nanocomposites (HSP-MoC x /C) for high-efficient HER. Their skeleton structure, porosity, carbon amounts, phase composition and active species dispersity are well modulated by simply tuning the CI dosage in starting mixture, and its mechanism is monitored via a series of physicochemical characterization techniques. The optimal composite exhibits remarkable HER activity with low overpotentials of 112 and 86 mV at current density of 10 mA cm −2 , and the small Tafel slopes of 52 and 50 mV dec −1 in 0.5 M H 2 SO 4 and 1 M KOH solution, respectively. Such performance stems from the combined effects of enhanced ion/mass transport, abundant exposed active sites and high conductivity due to the 3D hierarchically skeleton architecture of catalysts. This work paves a new strategy to design hierarchically porous materials for chemical conversion and energy storage .
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CELLULOSE
·
2019
·Vol. 27
·期 2
·799-823
·
IF 3.917
Lv Wei,Liao Yuhe,Zhu Yuting,Liu Jing,Zhu Changhui,Wang Chenguang,Xu Ying,Zhang Qi,Chen Guanyi,Ma Longlong
The cleavage of linkages of lignocellulose is important for its valorization. The linkage cleavage of cornstalk hydrolysis residue was investigated over catalysts (Ru/C + MgCl 2 ) in EtOAc/H 2 O solvents. The results show that almost hydrogen bonds, C–C bonds, ether and ester bonds in the matrix of lignin and cellulose were broken, accompanying 80.6% of lignin and 98.5% of cellulose conversion, and obtaining 37.5% of aromatic monomers and 28.8% of lignin oligomers. In the reaction system, biphasic EtOAc/H 2 O solvents exhibited an effect on cleaving the intermolecular linkages between lignin and cellulose. MgCl 2 showed limited abilities of breaking the α-O-4 and β-O-4 linkages in lignin and limited β-1, 4-glycosidic and hydrogen bonds in cellulose were cleaved over Ru/C catalyst. The cleavage of C–O linkages (α-O-4, β-O-4, 4-O-5) and C–C bonds (α-β, β-5) in lignin were mainly dependent on Ru/C catalyst. Much C–O and the stubborn C–C linkages of β-5, β-1 and 5-5 were significantly disrupted by the synergistic effect between MgCl 2 and Ru/C. However, MgCl 2 exhibited great contribution to breakage of β-1, 4-glycosidic linkage, hydrogen bonds and sugar ring of cellulose. The linkage of β-1, 4-glycosidic, hydrogen bonds and C–C in C5/C6 sugars were significantly broken. The increased yield of products was evidently due to the synergistic effect of Ru/C combined with MgCl 2 .
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RSC Advances
·
2019
·Vol. 9
·期 68
·39561-39571
·
IF 3.049
Fahim A. Qaraah,Samah A. Mahyoub,Mahmoud Elsayed Hafez,Guangli Xiu
Herein, we fabricated a C and N co-modified Nb2O5 nanonet structure (C–N/Nb2O5NNs) from niobium oxalate using 2-methylimidazole (Hmim) as a source for C and N via a simple hydrothermal route. The obtained nanonets are robust and cost-effective with excellent recycling stability. Compared with N-doped TiO2 (N-TiO2) and a Nb2O5 control sample (Nb2O5-CS), the resulting nanonets exhibited the highest performance toward the photocatalytic degradation of Rhodamine B (RhB) upon visible light irradiation (λ > 420 nm). Through this study, we revealed that the synergetic effects of C and N on the nanonet surface, which were effectively incorporated into the surface of the Nb2O5 nanonet structure, not only remarkably enhanced the visible light response by decreasing the bandgap to 2.9 eV but also improved the light utilization efficiency and photo-induced electron–hole pair separation efficiency of our nanonet structure. We also proposed that the presence of carbonate species (COx) and nitrogen species (NOx) increased the population of generated holes (h+) that had the key role in the photodegradation mechanism of RhB, suggesting reasonable importance for the modification of Nb2O5 with C and N. This synergism offers a new view to reveal the origin of photodegradation processes, introducing h+ as a key intermediate. Our approach provides a new insight to design 2D nanostructures with potential applications in catalysis, solar energy conversion, and environmental protection.
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高影响因子
CARBON
·
2019
·
IF 7.466
Shakiaz Ahmad,Chao Yang,Wenyu Xie,Zhibo Deng,Heng Zhang,Yunlong Zhao,Xintai Su
The integration of two transition metals with carbon materials provides a great potential to boost the catalytic and electrochemical properties of supercapacitor . However, a scalable fabrication of such composite materials remains a challenge. Here, ternary composites of NiS–NiCo 2 O 4 @C nanosheets were derived from nickel and cobalt oleate using Na 2 SO 4 as both hard template and sulfur source. The NiS–NiCo 2 O 4 @C composites were then tested as catalysts toward rapid reduction of 4-nitrophenol (4-NP) and as electrode materials for supercapacitors. It was found that the catalytic and electrochemical properties of the composites were tuned by adjusting the ratios of Co to Ni and annealing temperature. The optimized composite showed the highest reduction rate constant for 4-NP reduction (1.78 min −1 ). In addition, this composite has also shown high specific capacitance of 1411 F g −1 at 1 A g −1 and 99.5% capacity retention after 2000 continuous charge-discharge cycles at a current density of 3 A g −1 , which is much higher than their respective monometallic Co and Ni composites. Furthermore, the ASC device (CN14//AC) achieved a high energy density of 37.2 W h kg −1 at a power density of 799.9 W kg −1 , and a good cycling performance of retention(89%) after 5000 cycles.
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