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EUROPEAN JOURNAL OF MEDICINAL CHEMISTRY · 2018 · IF 4.816

Novel nicotinoyl pyrazoline derivates bearing N-methyl indole moiety as antitumor agents: Design, synthesis and evaluation

Kun Chen,Ya-Liang Zhang,Jing Fan,Xiang Ma,Ya-Juan Qin,Hai-Liang Zhu

In the present work, twenty-five nicotinoyl pyrazoline derivates bearing N-methyl indole moiety have been designed and synthesized. The biological evaluation of these compounds as tubulin assembly inhibitors revealed that most of them were potential antitumor agents . Among them, compound 28 exhibited most potency against cancer cell line panels (GI 50  = 29–90 nM for HeLa, HepG2 and MCF-7 cells) without toxicity to non-tumor cells (CC 50  > 300 μM for 293  T cell), bound to the colchicine site of tubulin and displayed excellent inhibitory activity in tubulin assembly assay (IC 50  = 1.6 μM, better than CA-4). Molecular dynamics simulation was carried out to validate the docking pose of compound 28 with tubulin crystalline. Further investigation on HepG2 and HeLa cells demonstrated that compound 28 could cause mitosis arrest to G2/M phase, and subsequently induced cell apoptosis . The efficiency in vivo of compound 28 was also evaluated on HeLa-Xenograft nude mice , and the relative tumor inhibition ration was up to 61.52% without noticeable weight loss and tissue damage (examined by H&E staining), which was comparable to CA-4 (inhibited 59.92%). In brief, compound 28 is a promising candidate for tumor therapy as tubulin assembly inhibitor.

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APPLIED CATALYSIS B-ENVIRONMENTAL · 2023 · IF 22.1

Unravelling the role of hydrogen peroxide in pH-dependent ORR performance of Mn-N-C catalysts

Yuan Li,Miao-Ying Chen,Bang-An Lu,Hao-Ran Wu,Jia-Nan Zhang

Although the Mn-N-C catalyst has low toxicity and high durability, its intense pH-dependent ORR activity is perplexing and prevents its commercial use in PEMFCs. Herein, we have developed a novel understanding of the role of hydrogen peroxide in the pH-dependent activity and stability of Mn-N-C catalysts. Instead of nitrogen protonation, the strong pH effects of ORR activity are caused by the much faster kinetics of the H 2 O 2 reduction reaction in alkaline medium than in acid, due to the lower dissociation energy of the HO-OH bond in alkaline environment. Regarding durability, the deactivation induced by H 2 O 2 demonstrates a strong pH dependence, primarily due to the differing intensities of reactive oxygen species at different pH values. Correspondingly, isopropanol effectively reduces Fenton reagents and increases the acid resistance of Mn-N-C sites. The present research provides a mechanistic understanding of pH effects and paves the way for the creation of more efficient catalysts.

CAS / MDL: 7722-64-7
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SENSORS AND ACTUATORS B-CHEMICAL · 2023 · IF 8.4

Epitaxial growth of Co3O4/In2O3 p-n heterostructure with rich oxygen vacancies for ultrahigh triethylamine sensing

Jianwang He,Zhijin Cheng,Zhuo Liu,Meijuan Yin,Yuchi Zhang,Le Han,Yan Xu

Although metal oxides based gas sensors have been researched extensively in previous works, there are enormous challenges on improving the deficiencies in poor selectivity, sensitivity, humidity resistance and so on. Hence, we developed an epitaxial growth method to prepare dendritic Co 3 O 4 /In 2 O 3 -(1−3) heterostructures of distinct Co/In mass ratios through perfect lattice matching between the two crystal domains at the interface, along with introducing large amounts of oxygen vacancies . As a result, the Co 3 O 4 /In 2 O 3 -2 heterostructure based gas sensor showed enhanced sensing properties towards triethylamine (TEA, 100 ppm) with a high response value of Ra/Rg = 576.1 at an optimal working temperature of 200 °C, which is 93 times higher than that of pristine In 2 O 3 . Moreover, the Co 3 O 4 /In 2 O 3 -2 sensor exhibited excellent gas selectivity, quick recovery time, repeatable cycling, long-term stability, as well as outstanding humidity resistance. The improved TEA gas sensing performance can be attributed to the integration of interfacial synergies in Co 3 O 4 /In 2 O 3 p-n heterostructure and generation of rich oxygen vacancies, exposing more active sites to facilitate the adsorption/desorption of gas molecules. This work provides a feasible pathway to regulate TEA sensing performance of metal oxide semiconductor (MOS) gas sensors by capitalizing on self-sacrificial template strategy and reconstruction of novel metal oxide heterostructure.

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Water · 2023 ·Vol. 15 ·期 20 ·3670 · IF 3.4

Reductive Degradation of N-Nitrosodimethylamine via UV/Sulfite Advanced Reduction Process: Efficiency, Influencing Factors and Mechanism

Xiaosong Zha,Shuren Wang,Deyu Zhang

N-nitrosodimethylamine (NDMA), as an emerging nitrogenous disinfection byproduct, is strictly controlled by multiple countries due to its high toxicity in drinking water. Advanced reduction processes (ARPs) are a new type of water treatment technology that can generate highly reactive reducing radicals and make environmental contaminants degrade rapidly and innocuously. In this study, a systematic investigation on the kinetics of the NDMA degradation via the chosen UV/sulfite ARP and the impacts of some key parameters of reaction system was conducted. The results indicated that the UV/sulfite ARP was an efficient and energy saving method for the reductive degradation of NDMA. A total of 94.40% of NDMA was removed using the UV/sulfite ARP, while only 45.48% of NDMA was removed via direct UV photolysis under the same reaction conditions. The degradation of NDMA via the UV/sulfite ARP followed pseudo-first-order kinetics. Increasing both the UV light intensity and sulfite dosage led to a proportional increase in the NDMA removal efficiency. The alkaline condition favored the degradation of NDMA, with the removal efficiency increasing from 21.57% to 66.79% within the initial 5 min of the reaction when the pH increased from 3 to 11. The presence of dissolved oxygen substantially decreased the removal efficiency of NDMA due to the formation of oxidizing superoxide radicals, which competed with NDMA by capturing the reducing active radicals during the reaction. An analysis of the degradation products indicated that several refractory intermediates such as dimethylamine, methylamine and nitrite were completely decomposed via the UV/sulfite ARP, and the final degradation products were formate, ammonia and nitrogen.Keywords:N-nitrosodimethylamine;UV/sulfite ARP;reductive degradation;influencing factors;mechanism

CAS / MDL: 75-05-8 67-56-1
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IONICS · 2023 ·Vol. 29 ·期 12 ·5183-5193 · IF 2.8

Facile synthesis of MoS2/N-doped carbon as an anode for enhanced sodium-ion storage performance

Du Fang-Xiao,Liu Song-Li,Li Yang,Wang Jian-Kang,Zhang Peng

The scalable synthesis of MoS 2 /N-doped carbon (MoS 2 /NC) nanosheets was accomplished using a facile salt template–assisted synthesis method. The MoS 2 nanosheets were uniformly encapsulated in nitrogen-doped carbon frameworks. As an anode for sodium-ion batteries (SIBs), the electrochemical performance of the MoS 2 /NC electrode was significantly improved compared to pure MoS 2 , which demonstrated a reversible capacity of 334.6 mAh g −1 after 100 cycles at 0.2 A g −1 ; even after 250 cycles of 1 A g −1 , the capacity could still be maintained at 252.9 mAh g −1 . This excellent sodium storage performance was mainly due to the coupling of nitrogen-doped carbon with MoS 2 and the uniform distribution of the nanosheets, which improved the reaction kinetics. Besides, the electrochemical reconstruction ensured the integrity of the electrode. This work was of great significance for the large-scale synthesis of MoS 2 anode material with enhanced stability SIBs.

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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Photovoltaic–Pyroelectric coupled effect enhanced photo-responsivity of a p-n heterojunction Self-Powered ultraviolet photodetector

Xinsheng Tang,Tursun Abdiryim,Ruxangul Jamal,Xiong Liu,Fangfei Liu,Feng Xu,Abdukeyum Abdurexit,Qian Cheng,Nawrzhan Serkjan,Shuyue Xie,Yiming Liu

TiO 2 -based ultraviolet (UV) photodetectors (PDs) with broadband optical detection range are widely used in commercial and military applications. Nevertheless, the self-powered UV PDs of TiO 2 nanoarrays (NRs) have relatively low response rates and slow response times. Here, a high responsivity self-powered p-n heterojunction UV PD based on TiO 2 NRs: CQDs/FTO and PEDOS/FTO is fabricated by a simple face-to-face assembly process. The pyroelectric effect of TiO 2 NRs is enhanced by sensitizing TiO 2 NRs with CQDs, which would reduce the bandgap value of TiO 2 NR, broaden the range of photoresponse, and reduce recombination of electron-hole. Furthermore, the pyro-phototronic effect of CQDs, the energy level matching from CQDs to PEDOS and the interaction between –OH in CQDs and ethylene oxide groups in PEDOS enhance the performance of the prepared UV PDs. The TiO 2 NRs: CQDs//PEDOS UV PDs achieve a high photo-responsivity and photo-detectivity of 150.95 mA/W and 3.73 × 10 11 Jones at 0 bias (365 nm), respectively, which are better than those at wavelengths of 380 nm. We also found that the photocurrent induced via the pyro-phototronic effect increases with the light power intensity. This work points the way for photovoltaic and photo-induced pyro-phototronic effects to improve the performance of TiO 2 NRs-based UV PDs.

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MICROPOROUS AND MESOPOROUS MATERIALS · 2023 · IF 5.2

Synthesis of copper-based nanoparticles confined in a pyridine N-containing COF and their catalytic applications

Yuyang Liu,Qiong He,Yarong Li,Yongqiang Li,Chiyang He

The main challenge of using non-noble metal copper nanoparticles (Cu NPs) as catalysts is to find or prepare suitable support platforms to anchor Cu NPs, thereby avoiding the aggregation tendency owing to their high surface energy. In this study, a novel pyridine N-containing covalent organic framework (COF) was designed and used as a template for the confined growth of Cu NPs. The prepared imine-connected TAPB-PCBA had abundant one-dimensional ordered channels, moderate specific surface area and good stability. The skeleton structure of TAPB-PCBA contained a large number of evenly distributed pyridine N, which can act as the nucleation site for Cu NPs. The well-defined pore structure confines the growth of Cu NPs and makes them controllable in size. The pores in TAPB-PCBA are completely independent and isolated from each other, minimizing the accumulation of Cu NPs. With the help of these factors, ultrafine Cu/Cu 2 O composite NPs (2.5 nm) with narrow size distribution anchored inside the cavity of the TAPB-PCBA were successfully prepared. The as-prepared Cu-containing COF, Cu@TAPB-PCBA, showed excellent catalytic capacity for dye degradation and nitrophenol reduction under mild conditions and low catalyst loads, respectively. In addition, Cu@TAPB-PCBA also has a good recyclability, multiple use without significant loss of catalytic activity. We expect this COF-supported growth-confined preparation of metal NPs to further facilitate the design and preparation of non-noble metal NPs@ COF composites, replacing noble metals in certain catalytic applications.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Tuning N coordination environment in AgNC single atom catalysts for efficient electrochemical CO2-to-Ethanol conversion

Haiqiang Mu,Yu-An Li,Xiuli Wang,Feng Li,Xin Du,Jing Li

The rational modulation of the coordination environment of the active center of single-atom catalysts (SACs) is a potential strategy to improve the activity and selectivity of electrocatalytic CO 2 reduction. We developed a series of single-atom Ag-anchored on N -doped carbon catalysts with different N -coordination environments by regulating the carbon source (glucose/graphene oxide, GO). Results demonstrated that the CO 2 -to-CO/C 2 H 5 OH pathway can be converted through reasonable regulation of the content of pyrrolic N and pyridine N. At a highly dominant pyrrolic N content of 40.0 %, the electrocatalyst of Ag-N-rGO 0.025 M facilitates the formation of CO with a Faradaic efficiency (FE) of 69.7 %. By contrast, when the pyridine N content is 70.5 %, the best Ag-N-C 0.05 M catalyst in the H-cell shows an FE of 42 % for C 2 H 5 OH at −0.97 V vs. RHE; moreover, the FE is stable at 40 % within 31 h. Density functional theory calculations further confirm that the pyrrolic N site is conducive to the conversion of CO 2 to intermediate *CO, whereas pyridine N exhibits the highest binding energy (ΔG = -4.73 eV) to hold *CO intermediates for dimerization, consequently steering the pathway to the formation of C 2 H 5 OH. The results of this study provide novel insights into the rational design of carbon-based SACs based on efficient electrochemical CO 2 reduction reaction and the regulation of CO 2 selectivity and activity for C 2 H 5 OH production.

CAS / MDL: 9003-11-6 143-19-1
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JOURNAL OF ALLOYS AND COMPOUNDS · 2023 · IF 6.2

Construction of 3D N-doped Ti3C2/TiO2 hollow sphere structure with superior electrochemical performance for supercapacitor

Yanhua Li,Guolong Ni,Kuo Zhang,Dongjia Wang,Qun Li,Shuhuan Wang

Herein, the 3D N-doped Ti 3 C 2 /TiO 2 sphere structure is constructed via an innovative three-step method including the preparation of 3D Ti 3 C 2 microspheres with PMMA as templates, the situ-growth of TiO 2 nanoparticles on Ti 3 C 2 and the subsequent annealing treatment in NH 3 . N element is doped in composite after annealing in NH 3 to improve the transfer rate of ions and electrons, and N-doped Ti 3 C 2 /TiO 2 hollow composite provides an abundant active surface for the sufficient contact between electrodes and electrolytes to enhance charge transport and electrolyte diffusion. Benefiting the unique structure feature and the synergistic effects of active materials, the N-doped Ti 3 C 2 /TiO 2 electrode exhibits a high specific capacitance of 572 F g −1 at a current density of 1 A g −1 and a superior cyclic stability of 99.6% of its initial value for 9500 cycles at 10 A g −1 . Based on this, a symmetric supercapacitor (SSC) based on N-doped Ti 3 C 2 /TiO 2 electrode is further assembled. The SSC shows a competitive capacitance of 157 F g −1 at 1 A g −1 . More importantly, the comparable energy density of 17.7 Wh kg −1 is achieved at the power density of 450 W kg −1 . This work will give promising guidance for designing and fabricating the durable electrodes with excellent electrochemical behavior for practical application in future.

CAS / MDL: 1333-86-4 24937-79-9
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NEW JOURNAL OF CHEMISTRY · 2023 ·Vol. 47 ·期 44 ·20298-20305 · IF 3.3

In situ-engineered coral-like multiphase NC@NiCoCu–N/NCF nanoarrays for enhanced hydrogen evolution reaction

Yaoxia Yang,Lan Zhang,Fengyao Guo,Dangxia Wang,Xingwei Guo,Wei Zeng,Dongfei Sun

It is necessary to explore new energy sources to alleviate the excessive demand for fossil energy. Water electrolysis is a promising means of sustainable hydrogen evolution. Herein, a Cu/NCF precursor was nitrized to prepare a nitrogen-doped carbon-coated multi-component NC@NiCoCu-N/NCF composite material. The good synergistic interactions among the three nitride phases, Cu3N, Ni4N, and Co2N, make H2O decomposition and H2 release more balanced during the reaction. The content and temperature were adjusted to explore the changes in the catalyst morphology and the trapezoidal nanosheets were transformed into a disordered rough coral-like nanostructure that facilitates better electrolyte penetration and provides more accessible active sites during the nitriding process. Nitrogen-doped carbon can enhance the conductivity of the catalyst, protecting the internal active structure from the erosion of the electrolyte and improving the structural stability. The NC@NiCoCu-N/NCF composite exhibited excellent hydrogen evolution performance and the overpotentials reached 89 mV and 131 mV under the current density of 10 mA cm−2 in 1.0 M KOH and 0.5 M H2SO4, respectively. Chronopotentiometry results indicated that the catalyst could operate continuously for at least 48 h and still maintain excellent structural stability. This study has great significance for the development of polymetallic or multicomponent catalysts designed to accelerate the field of hydrogen energy.

CAS / MDL: 12125-01-8 461-58-5
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SENSORS AND ACTUATORS B-CHEMICAL · 2023 · IF 8.4

High performance porous LaFeO3 gas sensor with embedded p-n junctions enabling ppb-level formaldehyde detection

Changlin Xiao,Zihuan Tang,Zhuangzhuang Ma,Xiaotong Gao,Hongqiang Wang,Lichao Jia

Metal oxides based semiconductors promise high performance gas sensing owing to their robustness and low cost, but are limited by their unsatisfied adsorption ability and intrinsic low carriers' mobility. We herein demonstrate an efficient strategy of reducing the adsorption energy and improving the carrier mobility via bulk implanted TiO 2 nanocrystals (NCs) in LaFeO 3 porous structure . By implanting laser generated sub-3 nm TiO 2 NCs in LaFeO 3 samples, the response value (221.8 for 100 ppm formaldehyde) increases about 4 times comparing with that of pristine. Additionally, the sample exhibits high sensitivity and fast response/recovery speed toward formaldehyde steam. The detailed analyses and theoretical calculation proves that the TiO 2 NCs could cause the increase of adsorbed oxygen levels as well as the carrier mobility through forming the heterojunction with LaFeO 3 . This work verifies that TiO 2 NCs implanted LaFeO 3 is a promising formaldehyde sensing material, which provides a new approach to improve sensing ability of metal oxide semiconductor (MOS) based gas sensors.

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JOURNAL OF MOLECULAR LIQUIDS · 2023 · IF 6

Excess properties, spectral analyses, and CO2 capture performance of N-methyldiethanolamine + polyethylene glycol 300 binary system

Yuting Wang,Xiaoyu Wang,Liming Chai,Enna Wang,Xionghui Wei,Zhaojun Wu,Jianbin Zhang

Density ( ρ ) and viscosity ( η ) data of polyethylene glycol 300 (PEG300) + N-methyldiethanolamine (MDEA) binary system at T = (298.15–318.15) K with a step of 5 K were measured at P  = 1005 hPa. After that, the experimental ρ and η values were correlated and predicted by several semi-empirical models. Meanwhile, the Jouyban-Acree model presented a better fitting for the density, and the McAllister four-body equation presented a better fitting for the kinematic viscosity. Based on the ρ and η values, excess molar volume ( V m E VmE ), partial molar volume ( V 1 ¯ V1¯ and V 2 ¯ V2¯ ), viscosity deviation ( Δη ), and excess Gibbs energy of activation of viscous flow ( Δ G ∗ E ΔG∗E ) of PEG300 (1) + MDEA (2) binary system were systematically calculated and analyzed. These excess properties showed the predominance of intermolecular self-conjugation in PEG300 (1) + MDEA (2) binary system, and it was further demonstrated by various spectral characterizations. Importantly, the PEG300 + MDEA aqueous system was used for 5 CO 2 absorption (room temperature)-desorption (371.15 K) cycles at a CO 2 flow rate of 200 mL/min, with the average CO 2 capture performance of 0.65 mol CO 2 /mol MDEA of per cycle, demonstrating excellent absorption capability, and remained stable throughout the entire cycle.

CAS / MDL: 105-59-9
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