JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Jiawei Gu,Hongfei Wang,Sha Li,Muhammad Sohail Riaz,Jiqiang Ning,Xiong Pu,Yong Hu
Doping engineering in nanostructured carbon materials is an effective approach to modify heteroatom species and surface electronic structures. Herein, an advanced electrode material based on a honeycomb-like porous carbon matrix with tunable N-doped configurations is prepared via 4,4′-bipyridine (4,4′-bpy)-assisted pyrolysis of SiO 2 @ZIF-8 templates and subsequent etching treatment. Interestingly, the amounts of pyridinic-N and graphitic-N can be controlled by rationally varying the content of 4,4 ′ -bpy which acts as the N source in the pyrolysis process. Both experimental results and density functional theory calculations have revealed that synergistically with 3D interconnected porous architecture, pyridinic-N and graphitic-N have different effects on the electrochemical performances in aqueous and ionic liquid gel electrolytes for symmetric supercapacitors. Highly exposed pyridinic-N endows the carbon electrode with a strengthened pseudocapacitance contribution manifested as a high specific capacitance of 436.1 F g −1 and exceptional stability of almost 100% capacitance retention after 5000 cycles at 10 A g −1 in the KOH/polyvinyl alcohol (PVA) electrolyte. By contrast, graphitic-N is propitious for reinforced electrical double-layer capacitance contribution, reflected by a maximum energy density of 125.4 Wh kg −1 in the 1-ethyl-3-methylimidazolium tetrafluoroborate/poly(vinylidene fluoride- co -hexafluoropropylene) (EMIMBF 4 /PVDF-HFP) electrolyte. This work offers an in-depth insight into the understanding of the energy storage mechanism of N-rich carbon electrodes in different electrolyte media.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
OPTICAL MATERIALS
·
2021
·
IF 3.08
Xin Li Wang,Jin Li,Wei Meng Liu
The disadvantage of bismuth vanadate (BiVO 4 ), a metal oxide semiconductor photocatalytic material, can be overcome by constructing nitrogen-doped graphene-based nanocomposites. Here we state to synthesis pyridinic-N doped graphene/BiVO 4 nanocomposite (N-rGO/BiVO 4 ). Because of many defects were existed pyridinic N-rGO, more tiny particle size and interaction from abundant interfacial, between BiVO 4 and N-rGO sheets, can produce synergistic effects and enhance photocatalytic performance. N-rGO/BiVO 4 composite has a large light absorption range and high photocatalytic activity compared with BiVO 4 and rGO/BiVO 4 . XPS, PXRD , HRTEM , FESEM, UV–vis, PL . etc analytical methods are used to characterize samples and the change of bandgap of samples is verified through theoretical analysis and simulation. After photocatalytic testing, the decomposition of methylene blue dye just required only 80 min under visible light and photocatalytic degradation efficiency of 99.3%. N-rGO/BiVO 4 has great potential for the removal of refractory pollutants from wastewater.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
ACS Catalysis
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2022
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IF 13.7
Qing Lu,Chen Chen,Qian Di,Wanli Liu,Xiaohui Sun,Yongxiao Tuo,Yan Zhou,Yuan Pan,Xiang Feng,Lina Li,De Chen,Jun Zhang
Developing efficient and stable electrocatalysts within a wide potential range is vital for the mature applications of the electrocatalytic CO2 reduction reaction (CO2RR) into value-added chemical products. Herein, we engineered a NC@Ni/C nano-composite featuring a core–shell structure of a pyridinic-N-rich carbon layer encapsulating Ni nanoparticles (NPs) as a highly effective electrocatalyst for CO2RR to CO over a wide potential range. The catalyst demonstrates a high CO Faradaic efficiency (FECO) of >90% in a wide potential range from −0.65 to −1.45 V [vs reversible hydrogen electrode (RHE)] with the maximum FECO of 97% at −1.05 V (vs RHE). Strikingly, it exhibits an excellent stability with a constant current density and a FECO > 95% for 92 h at −1.05 V (vs RHE). Structural studies and DFT calculations further reveal that pyridinic-N doping in the carbon shell of Ni NPs plays a dual role in promoting the CO2RR activity. It not only alleviates the mass transfer limitation of CO2 by enhancing the CO2 adsorption capacity, but it also lowers the reaction energy barrier of the *COOH formation rate-determining step with the electronic structure modulation by Ni. This work may shed more light on the seeking of practical catalysts for high-efficiency electrochemical CO2 reduction over a broad potential window.
研究领域:
材料科学
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电催化
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能源转换
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DOI
高影响因子
JOURNAL OF POWER SOURCES
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2024
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IF 8.1
Yangkai Sun,Zijian He,Huiyang Fan,Shurong Wang
Carbon nanosheets with layer-stacked porous structures and surface functionalized groups are beneficial for efficient ion storage in supercapacitor electrode materials, but achieving high cost-effectiveness and controllable surface groups remains a significant challenge. Herein, the biomass-derived chitosan and sodium alginate are selected as raw materials for self-assembly reaction with phytic acid as a cross-linking agent. The protonated chitosan and sodium alginate form a cross-linked network structure through hydrogen bonding and electrostatic adsorption, which is subsequently carbonized and activated to synthesize porous graphitic carbon nanosheets (PNPCN-X). PNPCN-X realizes an efficient distribution of porous and graphitic structures. It's noteworthy that phytic acid facilitates the fixation of N atoms, and various N configurations can be adjusted by altering the content of phytic acid. Optimized PNPCN-1.5 exhibits a high content of structurally stable pyridinic-N and graphitic-N configurations, which are confirmed to serve as active sites substantially augmenting the ion adsorption capacity through Density Functional Theory (DFT) calculations. Benefiting from its exceptional physicochemical properties, PNPCN-1.5 achieves 322 F g −1 as electrode materials in the three-electrode system, while the symmetrical supercapacitor assembled with EMIMBF 4 electrolyte attains 56.29 W h kg −1 . Furthermore, various kinetic analyses extensively elucidate its capacitance distribution characteristics and ion diffusion rates.
研究领域:
材料科学
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能源存储
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化学工程
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产品关联
DOI
高影响因子
SYNLETT
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2011
·Vol. 2012
·期 01
·145-149
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IF 2.447
Wenpeng Mai,Jinwei Yuan,Zhicheng Li,Gangchun Sun,Lingbo Qu
All articles of this category A novel direct arylation of pyridine N -oxideswith arylboronic acids through C-H functionalization hasbeen developed. This new reaction is performed at room temperatureusing catalytic silver(I) nitrate in the presence of potassium persulfateand give 2-pyridyl arylation derivatives of pyridine N -oxides.
研究领域:
有机化学
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催化反应
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产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2025
·
IF 4.7
Zehong Zhu,Qingxin Wu,Xueying Wang,Haiyang Zhang,Jian Li,Yanzhao Dong,Yongsheng Xu,Yunsheng Dai,Jinli Zhang
Here, the spiral mesoporous hydrothermal carbonaceous nanospheres (SMHNs) were designed and fabricated from pentose precursors to enhance gas diffusion in acetylene hydrochlorination. Through the optimization of hydrothermal conditions, the optimized SMCNs-800 material showcased the highest catalytic activity with an acetylene conversion of 77 % under the condition of GHSV (C 2 H 2 ) = 30 h −1 . The structural analysis indicated that the material with helical structure could provide larger pore sizes and abundant defect sites, exposing more active sites. The structure-activity relationship among acid-base properties of the catalyst surface, the adsorption-desorption capacity for the reactants and the catalytic activity jointly demonstrated that pyridine-N and -C=O could provide abundant basic sites for the adsorption and activation of H-Cl, thus accelerating the process of acetylene hydrochlorination reaction.
研究领域:
化学工程
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材料科学
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催化反应
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2024
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IF 10.8
Ying Chen,Lei Tian,Wen Liu,Yi Mei,Qiu-Ju Xing,Yi Mu,Ling-Ling Zheng,Qian Fu,Jian-Ping Zou,Daishe Wu
Dechlorination of chloropyridines can eliminate their detrimental environmental effects. However, traditional dechlorination technology cannot efficiently break the C–Cl bond of chloropyridines, which is restricted by the uncontrollable nonselective species. Hence, we propose the carbonate species-activated hydrogen peroxide (carbonate species/H2O2) process wherein the selective oxidant (peroxymonocarbonate ion, HCO4–) and selective reductant (hydroperoxide anion, HO2–) controllably coexist by manipulation of reaction pH. Taking 2-chloropyridine (Cl–Py) as an example, HCO4– first induces Cl–Py into pyridine N-oxidation intermediates, which then suffer from the nucleophilic dechlorination by HO2–. The obtained dechlorination efficiencies in the carbonate species/H2O2 process (32.5–84.5%) based on the cooperation of HCO4– and HO2– are significantly higher than those in the HO2–-mediated sodium hydroxide/hydrogen peroxide process (0–43.8%). Theoretical calculations confirm that pyridine N-oxidation of Cl–Py can effectively lower the energy barrier of the dechlorination process. Moreover, the carbonate species/H2O2 process exhibits superior anti-interference performance and low electric energy consumption. Furthermore, Cl–Py is completely detoxified via the carbonate species/H2O2 process. More importantly, the carbonate species/H2O2 process is applicable for efficient dehalogenation of halogenated pyridines and pyrazines. This work offers a simple and useful strategy to enhance the dehalogenation efficiency of halogenated organics and sheds new insights into the application of the carbonate species/H2O2 process in practical environmental remediation.
研究领域:
环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
CRYSTAL GROWTH & DESIGN
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2022
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IF 4.01
Xirui Zhang,Yunfei Xu,Denghui Yang,Yue Gong,Wei Du,Na Tang,Jianwei Jiang
Dry grinding and solvent-drop grinding to prepare the cocrystals of 4-nitropyridine N-oxide (NPNO) and p-aminobenzoic acid (PABA) were investigated in this study. Seven solvents were used during the solvent-drop grinding to accelerate the formation of the cocrystal, and the corresponding implicit solvent models were applied to compute the binding energy between NPNO and PABA via Gaussian 09 to determine the effect of the solvent on solvent-drop grinding. With a combination of Raman spectroscopy and powder X-ray diffraction (PXRD), the ternary phase diagrams of the NPNO–PABA–acetonitrile system at different temperatures were experimentally determined. It was found that the formation of the cocrystal is mainly due to the involvement of an O···H–O hydrogen bond between the −NO group of NPNO and the −OH group of PABA, and the stronger the binding energy of O···H–O in solvents, the faster the formation of the cocrystal. The crystallization region of the cocrystal of NPNO and PABA becomes larger with an increase in temperature. From an analysis of Ksp and K11, the equation KSPK11≪ [B]T is satisfied when the experimental temperature is 308.15 K, and a 1:1 complex solution model was used to describe the NPNO–PABA–acetonitrile system at 308.15 K. While the equation was not satisfied at 298.15 K, a solution-free complexation model was applied to describe the system at 298.15 K. The solution crystallization of the cocrystal of NPNO and PABA was successfully monitored by in situ Raman, PXRD, and a polarizing microscope, which collaboratively indicate that the nucleation of the cocrystal occurred almost immediately as soon as the two components were mixed in acetonitrile, and the dissolution processes of NPNO and PABA are the rate-determining steps during the solution crystallization of the cocrystals of NPNO and PABA.
研究领域:
化学
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物理化学
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材料科学
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产品关联
DOI
高影响因子
PROCESS SAFETY PROGRESS
·
2017
·Vol. 37
·期 3
·355-361
·
IF 0.812
Min Hua,Min Qi,Xuhai Pan,Wendi Yu,Lu Zhang,Juncheng Jiang
Alkyl pyridine-N-oxide can decompose to pyridine which readily leads to explosion accident in air. Therefore, risk analysis and inherently safer design are necessary for this process. This article aims to study the thermal hazards of the process of 3-methylpyridine oxidized by hydrogen peroxide, and then the corresponding Inherently Safer Designs (ISDs) were proposed. The inherent hazards during the process were first qualitatively evaluated by Qualitative Assessment for Inherently Safer Design. Then, the reaction calorimeter was employed to analyze the thermal hazards of the target reaction. Meanwhile, the Integrated Inherent Safety Index methods were simplified to quantitatively estimate the level of inherent safety of the process. The results show that the potential risk of the process is 87.2% which is at the high risk level. Based on the hazard identification and assessment results, three ISDs, namely adding catalyst (ISD I), improving reaction condition (ISD II), and using a tubular (ISD III), were proposed to enhance the safety. Finally, combining comparative experiments with ISI methods, an effect evaluation model for ISD was established to verify the rationality of the ISDs. The results indicate that the reaction hazards are diminished when three ISDs are utilized in production process. The inherent safety level of the reaction is increased by 22.2%, 50.7%, and 31.8%, respectively. © 2017 American Institute of Chemical Engineers Process Process Saf Prog 37:355–361, 2018
研究领域:
化学工程
·
安全科学
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产品关联
DOI
高影响因子
Asian Journal of Organic Chemistry
·
2018
·Vol. 7
·期 12
·2527-2533
·
IF 2.496
Wei-Ze Li,Zhong-Xia Wang
Graphical Reaction of quinoline N -oxides and pyridine N -oxides with arylzinc reagents under transition-metal-free conditions was studied. The reaction was carried out in toluene (for quinoline N -oxides) or THF (for pyridine N -oxides) at 100 °C and required 2 equiv. of arylzinc loadings and the presence of 2.5 equiv. of TFAA, affording 2-arylquinolines and 2-arylpyridines, respectively, in 24% to 95% yields. Reaction of quinoline N -oxides and pyridine N -oxides with arylzinc reagents under transition-metal-free conditions was studied. The reaction was carried out in toluene (for quinoline N -oxides) or THF (for pyridine N -oxides) at 100 °C and required 2 equiv. of arylzinc loadings and the presence of 2.5 equiv. of TFAA, affording 2-arylquinolines and 2-arylpyridines, respectively, in 24% to 95% yields. Functional groups OMe, F, Cl, Br, CF 3 , C(O)NH 2 , COOR and NO 2 were tolerated. Mechanistic studies showed that the reaction of quinoline N -oxides proceeded via a 2-arylquinolin-1(2 H )-olate intermediate, and the reaction of pyridine N -oxides via a 5-arylpenta-2,4-dienal oxime intermediate.
研究领域:
有机化学
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合成化学
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2013
·Vol. 15
·期 5
·1274-1279
·
IF 6.828
Ran Ma,An-Hua Liu,Cheng-Bin Huang,Xue-Dong Li,Liang-Nian He
A green process was developed for efficient reduction of sulfoxides and pyridine-N-oxides using the iron powder in the presence of H2O–CO2 to sulfides and pyridines, respectively. Notably, H2O is employed as the terminal hydrogen source, and CO2 could enhance hydrogen generation through in situ formation of carbonic acid. Thus carbonic acid offers simple neutralization by depressurizing CO2 and the system can eliminate unwanted byproducts. The high generality and chemo-selectivity of this protocol were demonstrated by the scope of substrates, in which chlorine, vinyl group and benzene ring can be tolerated.
研究领域:
有机化学
·
绿色化学
·
药物化学
·
催化化学
·
合成方法学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Qinghua Gu,Zheng Yan,Xin Ke
To evaluate the potential of aerogel materials for selectively recovering Cu 2+ from highly acidic wastewater, the adsorption behavior of Cu 2+ by bis-pyridine N-functionalized cellulose (PEIPD/CMC) aerogel was systematically investigated. Characterization of structural and chemical properties of the absorbent revealed that the bis-pyridine N plays a crucial role in the adsorption process. The PEIPD/CMC aerogel exhibited excellent adsorption capacity and selectivity for Cu 2+ in multi-component acidic solutions (Cu 2+ /Zn 2+ /Pb 2+ ), achieving a maximum adsorption capacity of 1.19 mmol/g at pH = 2. The adsorption process was well-described by the pseudo-second-order model and the Langmuir model, indicating monolayer chemisorption. Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS) analyses confirmed the involvement of bis-pyridine N groups in the adsorption of heavy metals. To further elucidate the interaction mechanisms between PEIPD/CMC and heavy metals at the microscopic level, Molecular dynamics (MD) simulations and Density functional theory (DFT) were conducted. MD simulations revealed that the adsorption process is predominantly governed by chemisorption, with the binding strength of the adsorbent to heavy metals following the order Cu 2+ > Zn 2+ > Pb 2+ . DFT calculations provided direct evidence of the chelation mechanism, highlighting the role of energy and electron transfer in the selective adsorption of Cu 2+ . These findings conclusively demonstrate that bis-pyridine N is the key functional group responsible for the selective adsorption of Cu 2+ .
研究领域:
环境科学
·
材料科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）