RSC Advances
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2016
·Vol. 6
·期 89
·86034-86042
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IF 3.289
Lujiang Xu,Qian Yao,Ying Zhang,Yao Fu
In this study, nano-sized HZSM-5 catalysts with different Si/Al ratios were synthesized and employed for producing pyridines from glycerol via a thermo-catalytic conversion and ammonization (TCC-A) process. The catalytic performance of micro-sized HZSM-5 and nano-sized HZSM-5 was studied firstly. The nano-sized HZSM-5 showed better catalytic performance in pyridine production in the TCC-A process due to its smaller particle size. When the nano-sized HZSM-5 (Si/Al = 25) served as the catalyst, and the reaction temperature was about 550 °C with the weight hourly space velocity of glycerol to catalyst at 1 h−1 and the ammonia to glycerol ratio at 12 : 1, the highest yield of pyridines was up to 42.1%, which was much higher than that when using micro-sized HZSM-5 (35.6%) reported before. In addition, nano-sized HZSM-5 also showed a better catalytic performance than micro-sized HZSM-5 in the catalytic conversion of bio-derived furans to produce indoles. After five reaction/regeneration cycles, the catalytic performance of nano-sized HZSM-5 slightly decreased compared with the first run, but was still higher than that of micro-sized HZSM-5.
研究领域:
化学工程
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催化材料
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2016
·
IF 5.267
Lujiang Xu,Qian Yao,Zheng Han,Ying Zhang,Yao Fu
In this study, polylactic acid served as raw material to produce fine chemicals (pyridines) via a thermocatalytic conversion and ammonization (TCC-A) process. Ammonia was employed as not only carrier gas but also a reactant in this process. The thermal decomposition behavior of PLA under N2 or NH3 atmosphere was investigated. Different catalysts, including MCM-41, β-zeolite, ZSM-5 (Si/Al = 50) and HZSM-5 with different Si/Al ratios (Si/Al = 25, 50, 80) were also screened. Reaction temperature and residence time, which may affect the pyridines production, were investigated systematically. It was verified that all the investigated factors, including catalyst structure, catalyst acid amounts, reaction temperature, and residence time, influenced the PLA conversion and the pyridines production. The highest pyridines yield, 24.8%, was achieved by using HZSM-5 (Si/Al = 25) at around 500 °C. The catalyst regeneration tests were carried out. It demonstrated that the catalyst was stable after five regenerations and the catalytic activity did not change significantly. A possible reaction pathway from PLA to pyridines was also proposed. PLA initially thermally decomposed to form lactic acid and some byproducts such as acetaldehyde, acetone, etc., and then lactic acid, the mixture of acetaldehyde and acetone, or other byproducts reacted with ammonia to form imines and finally underwent complicated reactions to form pyridines.
研究领域:
化学工程
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环境科学
✓ 已验证
DOI
高影响因子
RARE METALS
·
2025
·
IF 11
Zhang Liang,He Zhi-Ling,Ning Hua,Luo Hui,Wei Qin-Qin,Qing Pei-Lin,Huang Xian-Tun,Wang Xin-Hua,Li Guang-Xu,Huang Cun-Ke,Lan Zhi-Qiang,Zhou Wen-Zheng,Guo Jin,Ismail Mohammad,Liu Hai-Zhen
As a hydrogen storage material, both AlH 3 and LiNH 2 possess a high hydrogen capacity. However, the dehydrogenated AlH 3 can hardly absorb hydrogen under normal conditions, while LiNH 2 will generate NH 3 rather than H 2 upon decomposition. In this work, we report that the combination of AlH 3 and LiNH 2 through simple ball milling leads to partial reversibility of the AlH 3 −LiNH 2 system and the suppression of NH 3 liberation. The negatively charged H δ − in AlH 3 will react with the positively charged H δ + in LiNH 2 through a redox reaction to form Li 2 NH, AlN, and H 2 at 120−170 °C. After dehydrogenation at above 270 °C, Li 3 AlN 2 is generated, which is crucial for the reversibility of this system. The more the Li 3 AlN 2 generated, the better the reversibility of this system. The dehydrogenation capacity of AlH 3 + 2LiNH 2 at the third cycle (3.0 wt%) is higher than that of AlH 3 + LiNH 2 (1.2 wt%) due to the generation of more Li 3 AlN 2 . The role of AlH 3 /Al in the AlH 3 −LiNH 2 system is to fix the nitrogen into the form of AlN and Li 3 AlN 2 and thus suppress the liberation of NH 3 . Therefore, the synergy of AlH 3 and LiNH 2 leads to the reversibility of the Li–Al–N–H system and the suppression of NH 3 . Graphical abstract
研究领域:
材料科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2015
·
IF 4.321
Qian Yao,Lujiang Xu,Zheng Han,Ying Zhang
Furfural, an abundant biomass derived compound, was converted into indoles via thermo-catalytic conversion and ammonization with zeolites. The effect of reaction temperature, catalyst, weight hourly space velocity (WHSV) and ammonia to furfural molar ratio on the product distribution was investigated systematically. They all played important roles on indoles production. The maximal carbon yield of indoles (20.79%) was achieved by using HZSM-5 (Si/Al = 25) catalyst at 650 °C with WHSV as 1.0 h −1 and NH 3 to furfural molar ratio as 2. The HZSM-5 (Si/Al = 25) catalyst was recycled for five times and showed slight deactivation. Three possible aldehyde group of furfural conversion pathways were proposed and one possible reaction pathway from furfural to indoles was verified based on the experimental and quantum calculation results, that is, furfural firstly reacted with ammonia to form furfural-imine, and then furfural-imine underwent a cracking reaction to form furan. Thereafter, furan was converted to pyrrole and finally to indoles.
研究领域:
生物化学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2013
·
IF 4.814
Yongfeng Liu,Chao Li,Bo Li,Mingxia Gao,Hongge Pan
The hydrogen storage properties and mechanisms of the Mg(NH2)2–2LiH system with potassium halides (KF, KCl, KBr, and KI) were investigated and discussed. The results show that the KF-added sample exhibits superior hydrogen storage properties as ∼5.0 wt % of hydrogen can be reversibly stored in the 0.08KF-added sample via a two-stage reaction with an onset dehydrogenation temperature of 80 °C. However, hydrogen storage behaviors of the samples with KCl, KBr, and KI remain almost unchanged. The fact that KF can readily react with LiH to convert to KH and LiF due to the favorable thermodynamics during ball milling should be the primary reason for its significant effects, as the presence of KH provides a synergetic thermodynamic and kinetic destabilization in the hydrogen storage reaction of the Mg(NH2)2–2LiH system by declining the activation energy of the first-step dehydrogenation as a catalyst and reducing the desorption enthalpy change of the second step as a reactant. The understanding on the role played by KF sheds light on how to further decrease the operating temperature and enhance the hydrogen storage kinetics of the metal–N–H system.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2024
·
IF 11.2
Chouxuan Wang,Zhongguo Zhao,Shengtai Zhou,Lei Wang,Xinyue Liu,Rong Xue
The full arrival of 5G and advances in electronic integration make efficient heat dissipation crucial for stable operation and longer product lifespan. In this study, a vacuum-assisted filtration process was employed to fabricate ammoniated alumina/MXene/bacterial cellulose (Al 2 O 3 -NH 2 /MXene/BC) composite films that display a unique integration of properties, encompassing ultra-high thermal conductivity ( λ ), mechanical flexibility, and high photothermal conversion performance. By leveraging the bridging effect among spherical Al 2 O 3 -NH 2 and MXene nanosheets, a densely packed “point-surface” structure was constructed in BC by using a one-step preparation process. When the mass fraction of Al 2 O 3 -NH 2 /MXene (1:3, w/w) is 40 wt%, the O-BAl 1 M 3 exhibited an in-plane λ of 20.02 W m –1 K –1 , which was 436% and 94% higher than that of pure BC and T-BAl 1 M 3 (prepared by a two-step method), respectively. Furthermore, constructing an intact thermal conductive network within BC notably promoted photothermal and photoelectric conversion performance. The maximum surface temperature and voltage of the O-BAl 1 M 3 film reached 106.9°C and 48.34 mV when a sample with an area of 1.56 cm 2 was exposed under a light intensity of 200 mW cm –2 . By applying O-BAl 1 M 3 film, the temperature inside a self-built greenhouse model reached up to 64.8°C within 1200 s under a light intensity of 100 mW cm –2 , which validated the practical application of the composite films and offered a novel approach for creating flexible films with superior photothermal conversion capability. This work provided insights into preparing functional composite films for efficient thermal management and photothermal conversion applications.
研究领域:
材料科学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 12
·3982-3991
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IF 6.177
Guang-Rong Ding,Yao-Feng Wang,Guo-Yi Duan,Tao Guo,Xiao-Feng Xu,Chun-Shan Li,Bao-Hua Xu
Adiponitrile (ADN) is a key intermediate for the industrial production of polyamides represented by nylon 66. In this study, the chemoselective nitrilation of dimethyl adipate (DMA) with ammonia (NH3) under continuous flow conditions was studied on carbon encapsulated oxygen-deficient WOx<3 catalysts (WOx@C/C). A combination of dispersed anchor sites at a poly(ionic liquid) (PIL) template, the porosity of active carbon support, and the calcination procedure allows the formation of effective WOx@C-600-0.25-A1, persisting high BET specific surface area and WO2.83 active phase of appropriate size. It delivers ADN and methyl 5-cyanopentanoate (MCP) with an excellent selectivity of up to 95.8% at a weight hourly space velocity of DMA (WHSVDMA) of ∼0.64 gDMA gcat−1 h−1 and an NH3/DMA molar ratio of 13 : 1. A tandem reaction route from DMA to ADN via MCP was elucidated, wherein the second nitrilation of MCP to ADN proceeds very slowly. Besides, both CDMA and TONADN/TONMCP are significantly influenced by the physical dispersion and size of the active WO2.83 phase in WOx@C/C.
研究领域:
化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2020
·
IF 6.551
Xiaoqing Wang,Zizhang Guo,Zhen Hu,HuuHao Ngo,Shuang Liang,Jian Zhang
An innovative ammoniation-hydrothermal method of biochar production was developed for the adsorption of phenanthrene (PHE) from aqueous solutions in this paper. Phragmites australis (PA) was used to produce biochar in a hydrothermal kettle at 280 °C in muffle furnace using urea as an ammoniation reagent. Characterizations were executed by scanning electron microscope (SEM), N 2 adsorption/desorption isotherms, X-ray diffraction (XRD), elemental analysis, X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FT-IR) to explore its morphological, physical, and chemical properties. Batch experiments of PHE adsorption were carried out to study the adsorption isotherms and kinetics. Quantum chemistry computational simulations were employed based on density functional theory (DFT) to establish and optimize adsorption configurations and analyze the biochar's structural effects on adsorption performance. Results showed that the ammoniation-hydrothermal method produced biochar with a higher surface area and a maximum equilibrium adsorption capacity of 1.97 mg/g. The adsorption fitted well with Freundlich isotherm model (R 2 > 0.96) and Pseudo-second-order kinetic model (R 2 > 0.82). Adsorption energy calculation revealed that the N functionalities, especially pyridine N in the N-doped biochar structure, exhibited stronger binding ability with PHE, which contributed most to the favorable adsorption ability of the ammoniation-hydrothermal biochar.
研究领域:
环境科学
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化学
✓ 已验证
DOI
PubMed
高影响因子
ChemSusChem
·
2020
·Vol. 13
·期 21
·5683-5689
·
IF 7.962
Zhenbing Xie,Bingfeng Chen,Fangfang Peng,Mingyang Liu,Huizhen Liu,Guanying Yang,Buxing Han
Graphical A sustainable conversion : Developing highly efficient catalytic systems for amino acid productions from renewable bio-derived chemicals is very attractive for a sustainable future. N-doped carbon nanotube-supported Ru nanoparticles (Ru/N−CNTs) display excellent performance in the amination of bio-derived hydroxy acids into amino acids. The high-performance can be correlated with high dispersion of Ru nanoparticles and electronic effect resulting from the N-dopant. The amino acids have extensive applications, and their productions from biomass-derived feedstocks are very attractive. In this work, the synthesis of amino acids by amination of bio-derived hydroxy acids with ammonia over different metallic nano-catalysts supported on various supports is studied. It is found that Ru nano-catalysts on the nitrogen-doped carbon nanotubes (Ru/N−CNTs) have an outstanding performance for the reaction. Different hydroxy acids can be catalytically converted into the corresponding amino acids with yields up to 70.0 % under mild conditions, which is higher than those reported. The reasons for the high efficiency of the catalyst are investigated, and the reaction pathway is proposed on the basis of control experiments.
研究领域:
生物化学
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催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
KEY ENGINEERING MATERIALS
·
2019
·
IF 0
Yan Kai Huang,Qi Lin Mei,Zhi Xiong Huang,Yan Qin,Di Zhu
In this paper, the structure of the photosensitive diamines was designed and the method of synthesizing such diamines was investigated. The 1-(3-aminophenyl)-3-(4-aminophenyl)-2-propen-1-one analyzed by elemental analysis and infrared analysis was synthesized through two-step experiments with Aldol condensation and Nitroammoniation process. Through the experiment the optimum reaction conditions are raw material ratio of 1:1, anhydrous ethanol dosage of 60 ml, 10 % NaOH dosage of 10 ml and reaction temperature of 25°C for 4h. The yield was about 55.4 %.
研究领域:
有机化学
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材料科学
✓ 已验证
产品关联
DOI
GEOMICROBIOLOGY JOURNAL
·
2020
·
IF 1.989
Zijun Zhao,Chunli Zhao,Hoaithuong Do,Mingtang Li,Di Wu,Yuanhui Chen,Feng Zhang
Carbonate mineralization based on urea hydrolysis by bacteria has a significant implication in the remediation of heavy metals polluted environment, but a huge quantity of ammonium released due to the addition of urea may lead to non-point source pollution. In this study, a lead-resistant strain ZN5, identified as Brevibacillus laterosporus, which could induce different carbonate precipitations of Pb (II) through ammonification and nitrate assimilation processes without the addition of urea, was isolated. The maximum of pH values of bacterial fermentation suspensions were 9.07 and 9.22 during ammonification and nitrate assimilation processes, respectively. The minimum inhibitory concentrations of Pb (II) to strain ZN5 in two processes were 150 and 100 mg/L, respectively. Strain ZN5 could rapidly remove 94% and 70% of Pb (II) at an initial concentration of 15 mM through two processes, respectively. Furthermore, the induced carbonate precipitates of Pb (II) in ammonification and nitrate assimilation processes were dense spherical crystal of Pb3(CO3)2(OH)2 and loose irregular crystal of PbCO3, respectively, based on XRD and SEM-EDS. Besides, these two biominerals were relatively stable in dilute acid solution, especially the biomineral formed during nitrate assimilation process. These results showed that strain ZN5 had promising application in remediation of Pb-contaminated environment.
研究领域:
环境科学
·
微生物学
✓ 已验证
DOI
高影响因子
Chemical Engineering and Processing-Process Intensification
·
2022
·
IF 4.264
Kai Zhu,Wenjie Ye,Meng Hu,Yiping Huang,Jingjing Huang,Hanfei Liu,Hao Zhu,Zhenhao Wei,Feng Zhou
4-nitroaniline has been widely used in the production of antioxidants, dyes and pharmaceuticals. A continuous-flow strategy was exploited for the efficient synthesis of 4-nitroaniline through the noncatalytic amination of 4-chloronitrobenzene with aqueous ammonia in a highly controlled and safe manner, in which N-methyl-2-pyrrolidone was selected as the appropriate solvent. Various conditions (reaction temperature, residence time, 4-chloronitrobenzene concentration, molar ratio of ammonia to 4-chloronitrobenzene, presence of base catalyst) were investigated to improve the synthesis of 4-nitroaniline. The Box-Behnken design in response surface methodology was employed for the optimization of reaction conditions, and over 91% yield of 4-nitroaniline could be achieved. Furthermore, a kinetic model was proposed to guide the design and optimization of the synthesis of 4-nitroaniline.
研究领域:
有机合成
·
化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）