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RSC Advances · 2019 ·Vol. 9 ·期 60 ·34912-34925 · IF 3.049

Combined inorganic base promoted N-addition/[2,3]-sigmatropic rearrangement to construct homoallyl sulfur-containing pyrazolones

Shou-Jie Shen,Xiao-Li Du,Xiao-Li Xu,Yue-Hua Wu,Ming-gang Zhao,Jin-Yan Liang

The first sequentially combined inorganic base promoted N-addition/[2,3]-sigmatropic rearrangement reaction of α-alkylidene pyrazolinones and propargyl sulfonium salts has been reported to construct homoallyl sulfur-containing pyrazolones with moderate to excellent yields. α-Alkylidene pyrazolinones function as N-nucleophilic agents distinguished from the reported C-addition reactions. Propargyl sulfonium salts were first involved in the [2,3]-sigmatropic rearrangement protocol differentiated from the well-established annulation reactions. The excellent regioselectivity, the broad scope of substrates, gram-scale synthesis and convenient transformation embody the synthetic superiority of this cascade process.

CAS / MDL: 112926-00-8
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ANALYTICAL CHEMISTRY · 2019 · IF 6.35

Stable Isotope Sequential Derivatization for Linkage-Specific Analysis of Sialylated N-Glycan Isomers by MS

Ye Peng,Limeng Wang,Ying Zhang,Huimin Bao,Haojie Lu

Sialylated N-glycans play pivotal role in several important biological and pathological processes. Their sialyl-linkage isomers, mostly α-2,3- and α-2,6-linked, act differently during the cellular events and several diseases. While mass spectrometry (MS) technology is a powerful tool in N-glycome analysis, it still suffers from an inability to distinguish linkage isomers of native N-glycans. Herein, we described a sequential selective derivatization method, by which α-2,6- and α-2,3-linked sialic acids are sequentially labeled with methylamide incorporated with a different stable isotope. Isobaric labeling avoids inducing bias in ionization efficiency and chromatographic behavior. In optimized reaction conditions, high derivatization selectivity (∼99%) was achieved for both α-2,3- and α-2,6-linked sialic acid. High accuracy of quantitation within a dynamic range of 2 orders of magnitude and high reproducibility (CV < 20%, n = 3) were demonstrated using standard glycans and multisialylated N-glycans. Finally, this method was applied in profiling the N-glycome of serum from CRC patients, where a level of six sialyl-linkage isomers were found to be altered significantly compared with that from healthy individuals.

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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2019 · IF 3.218

New application of p-n junction in electrochemical detection: The detection of heavy metal ions

Jinghua Shang,Minggang Zhao,Huiyan Qu,Hui Li,Rongjie Gao,Shougang Chen

The 3D Ni/NiO/MoO 3 /chitosan foam was fabricated and the interfacial barrier of p-n junction was proposed as a driving factor for electrochemical detection of Cu 2+ . The electrochemical response resulted from the decreased barrier height caused by the absorbed Cu 2+ . The liner range (0–25 μM) and the lower detection limit (5.69 nM) were obtained. The direct electrochemical detection of Cu 2+ in real water sample with excellent stability and recovery was achieved. It affords a new approach to achieve the direct electrochemical detection of metal ions with depressed interference by employing the interfacial effects of p-n junction.

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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2019 · IF 4.084

Non-noble-metal Ni nanoparticles modified N-doped g-C3N4 for efficient photocatalytic hydrogen evolution

Puhui Deng,Mengxiang Gan,Xue Zhang,Zhuzhu Li,Yu Hou

The use of non-noble-metal to replace precious metal as co-catalyst in solar-driven hydrogen evolution reaction (HER) is important for lowering hydrogen production cost. In this work, nickel metal nanoparticles loaded nitrogen-doped graphite carbon nitride (NiNCN3) was prepared, which significantly enhanced the HER activity of nitrogen-doped graphite carbon nitride. The hydrogen evolution rate of NiNCN3 can reach to 1507 μmol g −1  h −1 , much higher than that of 3 wt % Pt/NCN (1055 μmol g −1  h −1 ). The distinguished photocatalytic performance is due to the accelerated electron transfer efficiency and inhibited photogenerated electron-hole recombination. Our study offers an alternative method to achieve the low-cost and effective noble-metal-free photocatalyst for HER.

CAS / MDL: 102-71-6
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RSC Advances · 2019 ·Vol. 9 ·期 69 ·40222-40227 · IF 3.049

Synthesis of N-doped carbon dots and application in vanillin detection based on collisional quenching

Yongping Wang,Qiaoli Yue,Yingying Hu,Chen Liu,Lixia Tao,Cong Zhang

N-doped carbon dots (NCDs) exhibit bright blue emissions and have been used as viable fluorescent probes in the turn-off fluorometric assay for vanillin detection. NCDs were prepared from glucose and tyrosine using a facile and green synthesis process. The one-pot hydrothermal treatment was used without any strong acid or oxidant. The fluorescence of NCDs (with excitation/emission peaks at 323/416 nm, respectively) can be quenched by vanillin. The quenching mechanism belongs to the dynamic quenching mode due to the molecular collisions of the ground state of vanillin and the excited state of NCDs. This turn-off system could be utilized to quantify vanillin within a linear range of 0.43–264 μM. The limit of detection was 0.10 μM. Moreover, this approach was successfully applied toward the determination of vanillin in food samples.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2019 · IF 6.361

Self-assembled N-doped carbon with a tube-in-tube nanostructure for lithium-sulfur batteries

Xinxin Zhu,Yabo Li,Rong Li,Keke Tu,Junsheng Li,Zhizhong Xie,Jiaheng Lei,Dan Liu,Deyu Qu

Lithium-sulfur batteries hold broad prospects as the low-cost and high-energy storage system. However, the practical application is limited by the intrinsic insulating nature of sulfur and severe shuttle effect of soluble polysulfide intermediates. Herein, we demonstrate a convenient self-assembly strategy for encapsulating carbon nanotubes in nitrogen-doped hollow carbon shells, to construct a nitrogen-doped tube-in-tube carbon nanostructure (NTTC) as a host material of sulfur. In this peculiar structure, the highly conductive carbon nanotube cores facilitate the electron transfer while the hollow porous structure is capable of accommodating high sulfur content of 70 wt% in the composites. Moreover, the nitrogen doping helps to alleviate the shuttle effect owing to enhanced chemisorption towards polysulfides. Benefiting from these merits, the NTTC/S composite with the high areal mass loading of ~2.5 mg cm −2 presents a high reversible capacity (1346.9 mAh g −1 at 0.05 C) and excellent rate capability (533.5 mAh g −1 at 3C). More impressively, NTTC/S electrode exhibits good cycling stability at a high rate of 2 C corresponding to slight capacity decay of 0.055% per cycle over 500 discharge/charge cycles.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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JOURNAL OF CATALYSIS · 2019 · IF 7.723

Fabrication of Ni3N nanorods anchored on N-doped carbon for selective semi-hydrogenation of alkynes

Xiaozhen Shi,Xin Wen,Shilin Nie,Jie Dong,Jingde Li,Yongqing Shi,Huiling Zhang,Guoyi Bai

Nickel is a highly active catalyst for the semi-hydrogenation of alkynes. However, the low selectivity of the alkene product caused by the over-hydrogenation reaction on Ni has hindered its practical applications. In this work, we report a new nickel nitride (Ni 3 N)-catalyzed semi-hydrogenation of alkynes to the corresponding alkenes. The Ni 3 N nanorods were facilely fabricated via a direct pyrolysis of the solid mixture of nickel acetate tetrahydrate and melamine (Mlm). The Ni 3 N phase in the optimum catalyst (Ni 3 N/NC-6/5-550) is shown to be effective and stable in the semi-hydrogenation of alkynes, with a high yield and good selectivity for alkenes ( Z / E ratios up to >99/1). Both terminal and internal alkynes bearing a broad scope of functional groups are readily converted into alkenes with good chemo- and stereoselectivity. Notably, it was found that the over-hydrogenation can be markedly suppressed even at high conversion of alkyne. Density functional theory (DFT) calculations reveal that the low interaction between the alkene product and the Ni 3 N might plays a critical role in the selectivity enhancement.

CAS / MDL: 13478-00-7 6018-89-9
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2019 · IF 3.375

Strong Synergy between Ti3C2 and N-Doped Co Nanoparticles Boosts the Selective Hydrogenation of Propyne

Jianian Chen,Mingyu Chu,Fenglei Lyu,Jin Gong,Linzhong Wu,Lijia Liu,Yong Xu,Qiao Zhang

Two-dimensional (2D) metal carbides, carbonitrides, and nitrides (MXenes) have recently emerged as promising candidates in catalysis due to their unique properties. In this work, we composited Ti3C2 with Co-embedded N-doped carbon nanotubes (CNTs) via the pyrolysis of zeolitic imidazolate frameworks (ZIF-67) for propyne selective hydrogenation. Detailed characterizations show that strong synergistic effects are observed between the Ti3C2 and Co-embedded N-doped CNTs in the composite catalysts. This work provides an efficient strategy to achieve N-doping on Co nanoparticles, which play a vital role in the propyne selective hydrogenation. The optimized catalyst gives a high propyne conversion (∼99%) and high propene selectivity (∼96%) on propyne selective hydrogenation at 150 °C, which surpasses the reported non-noble metal catalysts in literature works. This work may not only open an avenue for obtaining active and selective catalysts for propyne selective hydrogenation but also promote research on the role of MXenes in catalysis.

CAS / MDL: 693-98-1
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ANALYTICA CHIMICA ACTA · 2019 · IF 5.256

Carbon dots as fluorescent nanoprobe for the determination of N-acetyl-β-d-glucosaminidase activity

Jimei Ma,Heng Zhang,Fangfang Peng,Xiaoqing Yang,Zi-Long Li,Linhao Sun,Hong Jiang

Carbon dots (CDs) were synthesized from p -aminophenol and ethylenediamine via one-step under mild condition and used as a sensitive fluorescent nanoprobe for the activity determination of N -acetyl-β- d -glucosaminidase (NAG). In this assay, p -nitrophenol was in situ produced from p -nitrophenyl-β-D- N -acetyl-glucosaminide, which was exclusively hydrolyzed by NAG. The UV absorption peak of p -nitrophenol (maximum at 400 nm) overlapped the excitation peak of CDs with maximum wavelength at 415 nm, which caused the fluorescence decline of CDs based on inner filter effect. The activity of NAG was determined by the fluorescence changes. The assay is highly sensitive to NAG with a low detection limit of 0.75 U L −1  (K = 3) and showed a good linear relationship in the range from 1 to 45 U L −1 . This CDs nanoprobe was successfully applied for the determination of NAG activity in human serum and urine samples.

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RSC Advances · 2019 ·Vol. 9 ·期 58 ·33997-34003 · IF 3.049

Boosting the hydrogen evolution activity of a Co–N–C electrocatalyst by codoping with Al

Xiao Zhou,Haoran Yu,Yang Liu,Yong Kong,Yongxin Tao,Yong Qin

Co, Al and N tri-doped graphene (CANG) was successfully fabricated via annealing N-doped graphene with Co and Al precursors. The material was characterized by scaning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), Raman spectroscopy, physical adsorption, and X-ray photoelectron spectroscopy (XPS). It was found that the as-prepared CANG features a robust three-dimensional hierarchically porous structure. The contents of Co and Al can achieve the maximum value of 2.18 at% and 0.51 at% at the annealing temperature of 950 °C. Upon using the electrocatalyst for the hydrogen evolution reaction (HER), the CANG exhibited remarkable electrocatalytic performance in both acidic (η10 = 105 mV) and alkaline media (η10 = 270 mV), and outperforms Co,N-codoped graphene and Al,N-codoped graphene, respectively. In combination with the density functional theory (DFT) calculations, it was revealed that the introduction of the Al heteroatom can decrease the absolute value of hydrogen adsorption free energy (ΔG(H*)) of Co–N–C catalysts, thus greatly enhancing the HER activity. This discovery will provide new guidance to the design of advanced and inexpensive carbon materials for fuel cell, water-splitting and other electrochemical devices.

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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2023 · IF 4.2

Integration of Hydrogenation and Dehydrogenation Based on N-Ethylcarbazole as a Liquid Organic Hydrogen Carrier

Yuanchao Huang,Yuxi Si,Ying Xiang,Siyu Yao,Youwei Cheng

N-Ethylcarbazole (NEC), as a novel liquid organic hydrogen carrier (LOHC), has presented superiority to lower hydrogen storage cycle temperature and acceptable hydrogen storage capacity compared to benzene/toluene, etc. However, there is a lack of optimization of reaction conditions and cyclic testing for further commercial applications. Herein, we optimized the hydrogenation and dehydrogenation reaction conditions to obtain higher hydrogen storage capacity based on NEC/12H-NEC. The results revealed that 99.0% hydrogenation percentage and 91.7% dehydrogenation percentage could be available over Pd-based catalysts under optimal conditions. The cycling tests of the NEC-based hydrogenation and dehydrogenation reactions exhibited the desired stability after six cycles. Process simulation had been performed for the integration of NEC’s hydrogen storage unit in hydrogen vehicles, demonstrating that the actual hydrogen storage capacity of 5.3% and the energy output efficiency of 66% can be achieved. This work demonstrated the potential of the NEC/12H-NEC system for commercial applications.

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DIAMOND AND RELATED MATERIALS · 2023 · IF 4.1

Self-supporting Co-MoOx@N-doped carbon/expanded graphite paper for efficient water splitting catalyst

Huajun Zhou,Haifeng Cao,Yongping Qu,Yanzhong Wang

Molybdenum oxides are widely used as electrocatalysts due to their polymetallic oxidation state, abundant reactive sites and low production cost. However, the low electrical conductivity and easy agglomeration has limited their practical application. Here, MoO 3 nanowires encapsulated with ZIF-67 polyhedra were grown in situ on expanded graphite paper (EGP) by a simple hydrothermal synthesis method, and then the precursors were pyrolyzed to obtain self-supported Co-MoO x @N-doped carbon/EGP composites. Thanks to the three-dimensional porous structure and the synergistic effect of Co and multi-valance MoO x , the as-prepared Co-MoO x @N-doped carbon/EGP exhibits the excellent performances of OER (η 10  = 256 mV) and HER (η 10  = 138 mV), and a small Tafel slope and good durability. Furthermore, the assembled water splitting device achieved a current density of 10 mA cm −2 at a low voltage of 1.62 V and the excellent stability after 24 h continuous water splitting.

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