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JOURNAL OF CATALYSIS · 2018 · IF 6.759

A study of FeNx/C catalysts for the selective oxidation of unsaturated alcohols by molecular oxygen

Jinping Zhang,Shinichi Nagamatsu,Junmou Du,Chaoli Tong,Huihuang Fang,Dehui Deng,Xi Liu,Kiyotaka Asakura,Youzhu Yuan

Transition-metal nitrides can exhibit catalytic performance comparable to that of noble metal catalysts in many reactions. However, investigations on the correlation of catalyst structure, performance, and stability are still highly demanded. Here, a series of metal nitrides were prepared and evaluated for the selective oxidation of alcohols by molecular oxygen. Among them, FeN x /C- T catalysts ( T represents the pyrolysis temperature) display above 95% selectivity to the corresponding aldehydes in the selective oxidation of unsaturated alcohols. The optimized FeN x /C-900 catalyst gives the highest TOF of 7.0 h −1 for the conversion of 5-hydroxymethylfurfural to 2,5-diformylfuran. A combination of characterizations and experiments suggests that Fe N 4 species are the main active sites. In addition, we investigate the reasons for the catalyst deactivation and provide an effective approach to regenerating the catalysts. The results indicate that the deactivated catalysts can be regenerated by heat treatment under NH 3 /N 2 after each run. Based on these studies, a plausible reaction mechanism over the FeN x /C catalysts is proposed.

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JOURNAL OF MAGNETISM AND MAGNETIC MATERIALS · 2018 · IF 3.046

Catalytic synthesis and enhanced Curie temperature of ε-Fe3N@C nanostructure synthesized in a tetraethylenepentamine solution

Yong Li,Desheng Pan,Da Li,Yang Feng,C.J. Choi,Wei Liu,Zhidong Zhang

ε-Fe 3 N@C nanocrystals without oxidation are one-pot synthesized by using the iron(II) acetylacetonate and tetraethylenepentamine (TEPA) as Fe and N precursors under a low temperature (533 K) in the presence of a small quantity of Pt atoms as the co-catalyst. The ε-Fe 3 N@C nanoparticles with a core-shell structure are nearly spherical and have a wide particle size distribution of 100–500 nm in diameter. Fe nanoparticles obtained by reduction of Fe 2+ with TEPA are an effective catalyzer for decomposing TEPA to produce N and C atoms at a temperature much lower than the boiling point of TEPA. The diffusion of N atoms into Fe nanoparticles for the formation of ε-Fe 3 N@C is proposed, based on the results obtained by kinetically controlling the synthetic temperature and surfactants. The ε-Fe 3 N@C nanoparticles have an excellent saturation magnetization of 135.5 emu/g at room temperature. A significantly enhanced Curie temperature (T C ) of 614 K is reached in the present ε-Fe 3 N@C nanoparticles, which is much higher than the T C values in the previously reported ε-Fe 3 N x .

CAS / MDL: 112-90-3
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Nanoscale · 2018 ·Vol. 10 ·期 24 ·11418-11429 · IF 7.233

An autonomous tumor-targeted nanoprodrug for reactive oxygen species-activatable dual-cytochrome c/doxorubicin antitumor therapy

Yuxia Pei,Menghuan Li,Yanhua Hou,Yan Hu,Guangyu Chu,Liangliang Dai,Ke Li,Yuxin Xing,Bailong Tao,Yonglin Yu,Chencheng Xue,Ye He,Zhong Luo,Kaiyong Cai

The precise tumor cell-specific delivery of therapeutic proteins and the elimination of side effects associated with routine chemotherapeutic agents are two current critical considerations for tumor therapy. In this study, we report a reactive oxygen species (ROS)-activated yolk–shell nanoplatform for the tumor-specific co-delivery of cytochrome c (Cyt c) prodrug and doxorubicin, in which the bioactivity of Cyt c could be restored by the intracellular ROS-trigger and readily initiate the sequential doxorubicin release. The DOX-loaded lactobionic acid-modified yolk–shell mesoporous silica nanoparticles were first encapsulated with 4-nitrophenyl 4-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl)benzyl carbonate (NBC)-modified Cyt c via boronic ester linkages, and functionalized again with lactobionic acid to further shield Cyt c and confer the selective tumor targeting against liver cancer cells. The key feature in this design is that by taking advantage of the boronic ester linkage, the cytotoxicity of Cyt c capped on the nanoparticle could be temporarily deactivated during blood transportation and rapidly restored upon exposure to the ROS-rich microenvironment within liver cancer cells, thereby simultaneously achieving the protein therapy and stimuli-responsive doxorubicin release. This study presents a novel strategy for the development of tumor-sensitive co-delivery nanoplatforms.

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Journal of Materials Chemistry A · 2018 ·Vol. 6 ·期 32 ·15755-15761 · IF 9.931

Molecular self-assembly of a nanorod N-Li4Ti5O12/TiO2/C anode for superior lithium ion storage

Sainan Luo,Pengcheng Zhang,Tao Yuan,Jiafeng Ruan,Chengxin Peng,Yuepeng Pang,Hao Sun,Junhe Yang,Shiyou Zheng

Spinel lithium titanate (Li4Ti5O12, LTO) is one of the most appealing anode materials for lithium-ion batteries (LIBs) due to its long cycle life and high safety performance. However, its low intrinsic electronic conductivity limits its high rate capability. Herein, we develop a novel one-pot in situ molecular self-assembly approach to prepare a dual N- and anatase-TiO2- modified Li4Ti5O12/C nanorod material (NT-LTO/C). Polypyrrole (PPy), as a pivotal carbon and nitrogen source, is introduced to confine the morphology and particle size of the NT-LTO/C anode. Due to the synergistic effects of the multilevel particle structure, uniform carbon coating, N doping, anatase TiO2 pseudopotential effect and such benefits, the NT-LTO/C electrode delivers a high reversible capacity of 196.3 mA h g−1 at 0.5C, and it maintains 105.5 mA h g−1 even at an ultrahigh rate of 100C with progressive cycling of more than 3000 cycles. In addition, the three electrode pouch full-cell shows much smaller polarization than the pristine one. This novel and facile molecular self-assembly method has broad advanced functional material applications including for ceramics, polymer/carbon-based metal alloys and inorganic non-metallic materials.

CAS / MDL: 13463-67-7
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SYNTHESIS-STUTTGART · 2019 ·Vol. 51 ·期 16 ·3085-3090 · IF 2.867

Iron-Promoted Construction of Indoles via Intramolecular Oxidative C–N Coupling of 2-Alkenylanilines Using Persulfate

Menglan Wang,Yudong Li,Qing-An Wu,Shuping Luo,Yuehui Li

Indole scaffold synthesis relies primarily on oxidative C–H amination of N-protected alkenylanilines for C–N intramolecular cyclization reactions. Herein, for the first time, without N-protection, various readily prepared 2-alkenylanilines were transformed into the desired indole products in good yields by using K2S2O8 as oxidant in the presence of catalytic amounts of FeF2. The K2S2O8/FeF2 system offers a direct and benign synthetic route to 3-arylindoles and it is applicable to a wide range of substituted indoles including drug intermediates.

CAS / MDL: 10026-22-9
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Frontiers in Chemistry · 2018 · IF 4.155

Photocatalytic Activation of Saturated C–H Bond Over the CdS Mixed-Phase Under Visible Light Irradiation

She Houde,Li Liangshan,Zhou Hua,Wang Lei,Huang Jingwei,Wang Qizhao

Selective activation of saturated C–H bond in hydrocarbons to produce high-value-added chemicals is of great significance for chemical synthesis and transformation. Herein, we present a facile procedure to achieve Ni-doped CdS nanoparticles with mixed (cubic and hexagonal) phases, as well as its application to the photocatalytic activation of saturated primary C–H bond of toluene and its derivatives. The photocatalytic oxidation rate of toluene into benzaldehyde of formation reached up to 216.7 μmolh−1g−1 under visible light irradiation. The excellent photocatalytic performance of Ni(II)-doped CdS [Ni(II)/CdS] can be attributed to its unique structural assembly with cubic and hexagonal phases and also the addition of Ni ions, together taking effect in promoting the separation of photogenerated charge carriers. The possible reaction mechanism for the photocatalytic selective oxidation is illustrated in this work. The band width of the as-prepared mixed phase CdS is reduced, which can effectively expand the response range and improve photocatalytic performance.

CAS / MDL: 98-08-8
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DRUG DEVELOPMENT AND INDUSTRIAL PHARMACY · 2018 · IF 1.883

Targeted thrombolysis by using c-RGD-modified N,N,N-Trimethyl Chitosan nanoparticles loaded with lumbrokinase

Jie Liao,Xiaoting Ren,Bowen Yang,Hou Li,Yuexin Zhang,Zongning Yin

Lumbrokinase (LK) has strong fibrinolytic and thrombolytic activities, but it has a short half-life, can be easily inactivated, and may cause hemorrhage as a side effect. This study develops a potential thrombolytic therapy by fabricating N,N,N-Trimethyl Chitosan (TMC) nanoparticles modified with the cyclic Arg-Gly-Asp-Phe-Lys peptide (c-RGD) and loaded with LK (i.e. c-RGD-LK-NPs). The binding of c-RGD to platelet membrane GPIIb/IIIa receptors is expected to enable targeted delivery of the c-RGD-conjugated TMC to the thrombus. The synthesized c-RGD-LK-NPs had a mean particle size of 232.0 nm, zeta potential of 19.8 mV, entrapment efficiency of 52.7% ± 2.5%, and loading efficiency of 17.4% ± 0.65%. Transmission electron microscopy showed that they were generally spherical. The c-RGD-LK-NPs gave a cumulative in vitro LK release of 80.6% over 8 h, and the activity of LK was close to 80%, indicating that the nanoparticles protected the activity of LK. In vitro blood clot lysis assays were carried out and in vivo thrombolysis effect was tested in Sprague-Dawley rats carotid artery thrombus model. In all cases, the c-RGD-LK-NPs showed superior performance compared with the free LK and the unmodified TMC nanoparticles loaded with LK. The c-RGD-LK-NPs reagent is expected to be potentially useful in treating thromboembolic diseases.

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ELECTROCHIMICA ACTA · 2018 · IF 5.116

Cryo-treatment in enhancing the electrochemical properties of SnSb/C nanofiber anodes for lithium ion batteries

Yao Sun,Zhehang Yu,Tianyu Li,Yu Chen,Xin Xia

Aiming at improving the cycling stability of SnSb/C nanofibers prepared by electrospinning followed by carbonization , cryo-treatment was used as a thermal compensation method to adjust the internal stress and obtain different structures. Inspired by cryogenic treatment , we first raised the temperature of cryo-treatment (−50 °C, −150 °C) and discussed the effect that cryo-treatment temperature on the structure and electrochemical performance. The morphology structure and microstructure of SnSb/C nanofibers were investigated. It was shown that properly cryo-treated temperature could increase the degree of graphitization and effectively offset the internal stress gained from carbonization, which made the metal dispersed more evenly in the nanofibers. Benefiting from the structural advantage, SnSb/C nanofibers obtained at −50 °C for 1 h manifested the best capacity retention of 133.1 % for 500 cycles. This work proved temperature is one of the key factors for the production of cryo-treated anodes and −50 °C is the most suitable cryo-treatment temperature for the as-derived SnSb/C nanofibers. Carbonization results in volume change and creates internal stress. Properly cryo-treatment can release residual stress and adjust the structure, which can explain the increase of the graphitization. The findings may help to promote the application of cryo-treatment in the field of electrode production.

CAS / MDL: 25014-41-9
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Journal of Chemistry · 2018 · IF 1.726

Alkaline Ionic Liquid Modified Pd/C Catalyst as an Efficient Catalyst for Oxidation of 5-Hydroxymethylfurfural

Zou Bin,Chen Xueshan,Xia Jiaojiao,Zhou Cunshan

Conversion of HMF into FDCA was carried out by a simple and green process based on alkaline ionic liquid (IL) modified Pd/C catalyst (Pd/C-OH−). Alkaline ionic liquids were chosen to optimize Pd/C catalyst for special hydrophilicity and hydrophobicity, redox stability, and unique dissolving abilities for polar compounds. The Pd/C-OH− catalyst was successfully prepared and characterized by SEM, XRD, TG, FT-IR, and CO2-TPD technologies. Loading of alkaline ionic liquid on the surface of Pd/C was 2.54 mmol·g−1. The catalyst showed excellent catalytic activity in the HMF oxidation after optimization of reaction temperature, reaction time, catalyst amount, and solvent. Supported alkaline ionic liquid (IL) could be a substitute and promotion for homogeneous base (NaOH). Under optimal reaction conditions, high HMF conversion of 100% and FDCA yield of 82.39% were achieved over Pd/C-OH− catalyst in water at 373 K for 24 h.

CAS / MDL: 7647-10-1
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ELECTROCHIMICA ACTA · 2013 · IF 3.777

A novel bi-protein bio-interphase of cytochrome c and glucose oxidase: Electron transfer and electrocatalysis

Yonghai Song,Hongyu Liu,Yu Wang,Li Wang

Glucose oxidase (GOD) and cytochrome c (Cyt c ) were co-entrapped in the poly(diallyldimethylammonium chloride)–graphene nanosheets–gold nanoparticles (PDDA–Gp–AuNPs) hybrid nanocomposites modified glassy carbon electrode to prepare a novel bi-protein bio-interphase. Electron transfer and electrocatalysis of the bi-protein bio-interphase were investigated in detail. The results showed that the PDDA–Gp–AuNPs nanocomposites accelerated the electron transfer between proteins and electrode. The bi-protein exhibited effective direct electron transfer (DET) reaction with an apparent rate constant ( k s ) of 2.36   s −1 . The optimal molar ratio and total amount of Cyt c and GOD in the bio-interphase for DET of GOD was estimated to be about 3:1 and 1.40   nmol, respectively. The bi-protein bio-interphase could be used to detect glucose based on the consumption of O 2 with the oxidation of glucose catalyzed by GOD. The resulted biosensor exhibits wide linear range from 2.0 to 18.0   mM. Thus, this study not only successfully achieved DET of GOD, but also constructed a novel biosensor for glucose detection.

CAS / MDL: 7782-42-5
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2014 · IF 2.235

One-Pot Transformation of Cellulose to Sugar Alcohols over Acidic Metal Phosphates Combined with Ru/C

Qi-Ying Liu,Yu-He Liao,Tie-Jun Wang,Chi-Liu Cai,Qi Zhang,Noritatsu Tsubaki,Long-Long Ma

ZrP with large surface, mesoporous volume, and size was prepared. Its catalytic performance was evaluated in hydrolytic hydrogenation of cellulose to sorbitol/mannitol combined with commercial Ru/C. A significantly enhanced sorbitol/mannitol yield was obtained as compared with that of the water-soluble acidic phosphates and buffer solution of potassium acid phthalate combined with the same Ru/C. The enhanced yield was attributed to the Lewis and Brönsted acid on ZrP surface improving the surface’s absorption and activation for cellulose and accelerating the rate-determined hydrolysis step. The maximal sorbitol/mannitol yield of 63% and 81% could be obtained by using microcrystalline and ball milling cellulose as the feedstock, respectively. The ZrP combined with Ru/C was adaptable to the high concentrated cellulose and obtained 5.8 wt % of sorbitol/mannitol concentration. The remarkably enhanced cellulose hydrolysis by ZrP sharply decreased the use of Ru/C, which is significant for the essential application.

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RSC Advances · 2015 ·Vol. 5 ·期 85 ·69479-69486 · IF 3.84

Highly effective oxygen reduction activity and durability of antimony-doped tin oxide modified PtPd/C electrocatalysts

Yuan Gao,Ming Hou,Zhigang Shao,Changkun Zhang,Xiaoping Qin,Baolian Yi

Antimony-doped tin oxide (ATO) nanoparticles are synthesized by a simple one-step hydrothermal method. The oxygen reduction reaction (ORR) activity of the PtPd/C catalyst is promoted by the presence of ATO. Moreover, after accelerated durability testing, the PtPd/C-ATO catalyst reserves most of its electrochemically active surface area (ESA) and ORR activity compared to the PtPd/C catalyst. The improved electrochemical stability and activity of PtPd/C-ATO is attributed to the high stability of ATO support and the strong interaction between Pt and ATO.

CAS / MDL: 10025-97-5 10025-99-7
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