NEW JOURNAL OF CHEMISTRY
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2024
·Vol. 48
·期 26
·11802-11811
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IF 2.7
Chenxia Xu,Jianhua Lv,Jidong Liu,Bao Guo,Wensong Li
Ga2O3/MCM-41-x (x = 0.4, 0.5, 0.6) heterogeneous catalysts, each with varying levels of Br doping, were synthesized using mesoporous molecular sieves (MCM-41) as a carrier and employed in the synthesis of propylene carbonate (PC) from propylene oxide (PO) and carbon dioxide (CO2). The reaction was conducted under solvent-free and additive-free conditions. Various techniques were utilized to characterize the catalysts’ chemical composition, morphology, and structure. The effects of varied reaction conditions on PO conversion and PC selectivity using Ga2O3/MCM-41-0.5 catalysts were investigated. Under the reaction conditions of 120 °C, 3.5 MPa, 10 h and catalyst dosage of 2.6 wt%, the PO conversion and PC selectivity reached 99.7% and 99.1%, respectively. The catalytic impact correlates strongly with the doping amounts of Ga2O3 and Br, primarily due to the interaction of Ga2O3 with the surface of MCM-41, leading to the generation of more basic sites and, consequently, a greater abundance of alkali centers. As a nucleophilic reagent, Br functions synergistically with Ga2O3/MCM-41, augmenting the ring-opening rate of PO and improving the activation ability of CO2. The stability of the catalyst underwent evaluation, revealing a slight decrease in activity after repeated use. The reaction mechanism underlying PC synthesis catalyzed by Ga2O3/MCM-41-0.5 was speculated.
研究领域:
化学工程
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材料科学
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产品关联
DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 75
·70747-70755
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IF 3.289
Huijie Dong,Mingyu Wei,Jun Li,Jia Fang,Long Gao,Xiaoxia Li,Aihua Xu
A graphitic carbon nitride-containing MCM-41 catalyst (g-C3N4/MCM-41) was prepared through an in situ thermal approach and characterized by X-ray diffraction, Fourier transform infrared spectroscopy, transmission electron microscopy, N2 adsorption–desorption and X-ray photoelectron spectroscopy. It was found that Acid Orange 7 (AO7) and other five organic dyes can be completely degraded by the g-C3N4/MCM-41 catalyst within 30 min in the presence of peroxymonosulfate (PMS), while g-C3N4 + PMS and MCM-41 + PMS show nearly no activity. A non-radical pathway accompanied by radical generation in PMS activation and AO7 oxidation is proposed. The oxidized carbon species N–C–O on g-C3N4 with strong electron density plays a key role in the reaction, while the large surface area of the catalyst can also efficiently enhance the accessibility of catalytic active sites. Though the reusability of the g-C3N4/MCM-41 catalyst is not very good as that of metal oxide catalysts, its activity can be recovered by KOH treatment. The study can broaden the application of g-C3N4 in the area of wastewater treatment.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Yanxia Zhu,Ze Zhang,Jun Cheng,Hao Guo,Weijuan Yang
To improve catalytic performance of metal active sites in hydrodeoxygenation and hydrocracking conversion of methyl palmitate into high-quality jet biofuel, Ni-1,3,5-benzenetricarboxylate (Ni-BTC) metal-organic framework loaded on MCM-41(Mobil Composition of Matter No. 41) was prepared to enhance the accessibility of Ni active sites, facilitating hydrodeoxygenation to increase alkane yield with suitable arene content. The distance (0.98 nm) between Ni active sites within Ni-BTC structure, which was much larger than that (0.20 nm) within Ni nanoparticles , enabled methyl palmitate with maximum molecule width of 0.68 nm to go through Ni-BTC crystalline plane and get access to Ni active sites more easily. Ni-BTC nanosheets newly assembled in pore channels of MCM-41 were beneficial to effectively screen chain molecules of alkane products. With the largest BET surface area of 1014.2 m 2 /g, the Ni-BTC@MCM-41 catalyst with 2.5 wt% nickel (2.5Ni-BTC@MCM-41) reduced the nickel metal consumption by 75% comparing to nickel nanoparticle loading (10Ni@MCM-41), but achieved the best catalytic performances through hydrodeoxygenation on Ni active sites and hydrocracking on -SiOH acid sites. The alkane yield increased from 23.3% to 33.9%, while arene yield reduced from 22.4% to 6.5% in jet biofuel products. This resulted in an overall jet biofuel yield of 53.2% with uniform distribution along carbon numbers . The higher heating value of jet biofuel products thus increased to a peak of 45.90 MJ/kg.
研究领域:
催化材料
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能源化学
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纳米技术
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产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2013
·
IF 2.145
Anqiu Liu,Zehui Zhang,Zhongfeng Fang,Bing Liu,Kecheng Huang
In this study, we have developed a new method for the synthesis of EMF from HMF and fructose using mesoporous MCM-41 supported 12-tungstophosphoric acid (MCM-41-HPW) as the catalyst. The structure of 40 wt.% MCM-41-HPW was characterized by various techniques and its surface acidity was determined by potentiometric titration. A high EMF yield of 83.4% was obtained from HMF by the etherification reaction. Synthesis of EMF from fructose was also realized through one-pot reaction with a moderate yield of 42.9%. More importantly, the catalyst could be reused for several times without the loss of its catalytic activity.
研究领域:
化学工程
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催化科学
✓ 已验证
DOI
高影响因子
ChemSusChem
·
2019
·Vol. 12
·期 5
·978-982
·
IF 7.804
Yunchao Feng,Guihua Yan,Ting Wang,Wenlong Jia,Xianhai Zeng,Jonathan Sperry,Yong Sun,Xing Tang,Tingzhou Lei,Lu Lin
Graphical MCM's grand : A series of MCM-41 supported metal catalysts (denoted M/D41) were prepared by using the deep eutectic solvent (DES)-mediated ionothermal synthesis strategy. Al/D41 showed excellent performance in the conversion of carbohydrates into 5-hydroxymethylfurfural (HMF). Production of HMF from glucose could be performed at high concentrations in choline chloride aqueous solution. A series of MCM-41 supported metal catalysts (denoted M/D41) were prepared by using the deep eutectic solvent (DES)-mediated ionothermal synthesis strategy. Al/D41 was found to have excellent performance in the conversion of carbohydrates into 5-hydroxymethylfurfural (HMF). Furthermore, the production of HMF from glucose could be performed at high concentrations in choline chloride aqueous solution (CAS; 32 wt %, relative to the reaction phase) and as a result, CAS is a more promising solvent than water and DES for HMF production.
研究领域:
化学工程
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催化化学
✓ 已验证
DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2017
·
IF 3.615
Rong He,Zhihong Wang,Lei Tan,Yi Zhong,Weiming Li,Da Xing,Chaohai Wei,Youwen Tang
We developed two types of novel highly ordered Ni 2+ imprinted mesoporous organosilica materials (SBA-15 (NiIMS1) and MCM-41 (NiIMS2)) through co-condensation for selective adsorption of Ni 2+ from electroplating Ni 2+ effluents. FTIR and solid-state 13 C NMR spectra demonstrated the successful embedment of functionalized iminodiacetic acid and ethanediamine chelating groups in NiIMS1 and NiIMS2, respectively. X-ray photoelectron spectroscopy analysis confirmed that Ni 2+ was coordinated by N atom and carboxyl O atom of the functional groups. Furthermore, NiIMS1 and NiIMS2 displayed highly ordered periodic hexagonal P6mm meso-structure, large surface area, and highly specific recognition ability toward Ni 2+ . The adsorption experimental results proved that NiIMS1 was suitable for acidic wastewater treatment , whereas NiIMS2 was fit for alkaline wastewater. The saturated adsorption capacity of NiIMS2 was 20.8 mg/g at pH 6.0, and that of NiIMS1 reached up to 22.9 mg/g at pH 3.0. The values of selectivity coefficients of NiIMS1 and NiIMS2 for five competing metal ions ranged from 46.4 to 12.4 and 36.9 to 18.8, respectively. The adsorption efficiency of NiIMS1 was above 92.5% even after seven extraction-stripping cycles, while that for NiIMS2 was 90.9%. The real sample adsorption experiments demonstrated that these mesoporous organosilica materials have high potential for water treatment applications.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
RSC Advances
·
2014
·Vol. 4
·期 29
·15216-15224
·
IF 3.708
Chong-Wen Jiang,Xin Zhong,Zheng-Hong Luo
5-Hydroxymethylfurfural (5-HMF) which can be produced from cellulose is considered as one of the promising green platform chemicals. In this work, the conversion of cellulose to 5-HMF was carried out through hydrolysis in a batch reactor using the SO42−/Ti-MCM-41 catalyst at a temperature of 463–503 K. Two analytical techniques including the 3,5-dinitrosalicylic acid (DNS) method and high performance liquid chromatography (HPLC) were employed to track the time evolution of the main reagents, i.e., cellulose, 5-HMF and reducing sugar. Based on the typical kinetic experiments for the cellulose hydrolysis, a comprehensive hydrolysis mechanism was introduced to describe the heterogeneous hydrolysis of cellulose to 5-HMF. A corresponding kinetic model was proposed on the basis of the hydrolysis mechanism and the mass balance law. The results show that the predicted data obtained via the suggested model agree well with the experimental results. In addition, some data from the open reports were referred for further model verification in this work. The kinetic model suggested in this work is a mechanism model for the heterogeneous catalytic cellulose hydrolysis process, which is different from the previous first-order kinetic model.
研究领域:
化学工程
·
可再生化学
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Ping He,Huawei Geng,Lin Li,Qisong Yi,Lu Lin,Zhifeng Liu,Yuanshuai Liu,Valentin Valtchev
Solid acidic Al-MCM-41 materials are characterized by a high specific surface area and well-ordered hexagonally shaped mesopores. However, their relatively weak acidity compared to microporous zeolites significantly limits their practical applications in industrial catalytic reactions, particularly in upgrading biomass-derived organic feedstock that involves reactions with bulky molecules. Herein, we report a novel synthesis route for preparing acidity-enhanced Al-MCM-41 through the phase transformation of MWW-type zeolite precursors. The phase transformation approach markedly facilitates the incorporation of aluminum species into the MCM-41 framework, leading to strong Brønsted acidity of the resultant Al-MCM-41-T samples, as evidenced by comprehensive characterizations including 29 Si and 27 Al MAS NMR, NH 3 -TPD, and Py-IR. Owing to the enhanced acidity and its large pore structures, the as-prepared Al-MCM-41-T-15 sample (with Si/Al = 15) exhibited superior activity and selectivity toward C-alkylated products in both liquid-phase phenol-cyclohexanol and 4-cyclohexylphenol (4-CHP)-cyclohexene alkylation reactions compared the commercial Al-MCM-41-C with a similar Si/Al ratio. These findings afford an effective approach for preparing acidity-enhanced mesoporous solid acids, which hold significant potential for catalyzing lignin-derived bio-oils.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
TRANSACTIONS OF TIANJIN UNIVERSITY
·
2018
·Vol. 24
·期 4
·361-369
·
IF 0
Zhang Xubin,Dong Jianxin,Hao Zhencheng,Cai Wangfeng,Wang Fumin
Active Fe- and Mn-loaded MCM-41 (Fe–Mn/MCM-41), which was synthesized via a hydrothermal reaction followed by impregnation, is used in the heterogeneous Fenton reaction to degrade methyl orange (MO) in aqueous solution. The synthesized samples were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, N 2 adsorption–desorption isotherm analysis, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy. Compared with Fe/MCM-41 and Mn/MCM-41, Fe–Mn/MCM-41 showed higher activity for MO degradation and mineralization. Effects of various operating parameters, such as pH, Mn content, and H 2 O 2 dosage, on the degradation process were subsequently investigated. Results of experiments on the effect of radical scavengers revealed that the degradation of MO could be attributed to oxidation by HO·. The synergy of Fe and Mn species in the Fenton oxidation process was also explained.
研究领域:
环境科学
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催化材料
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水处理技术
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产品关联
DOI
RSC Advances
·
2019
·Vol. 9
·期 70
·40835-40844
·
IF 3.049
Jun Liu,Siqian Liu,Yaling Li,Jiayan Xue,Youyi He,Fuchi Liu,Li Yang,Junhui Hu,Zhengye Xiong,Lizhen Long
To research and develop potential multifunctional nanoprobes for biological application, lanthanide-doped MCM-41 (Ln-MCM-41, Ln = Gd/Eu) silica nanoparticles with excellent pore structure and optical–magnetic properties were synthesized via a facile and economical sol–gel method. The microstructure and pore distribution of Ln-MCM-41 nanoparticles were obviously affected by the Ln-doping. As the Ln/Si mole ratio increased, the specific surface area and total pore volume of Ln-MCM-41 nanoparticles rapidly decreased. However, the Ln-MCM-41 nanoparticles still retained the typical well-ordered mesoporous structure, and exhibited excellent drug release behavior. Moreover, the drug release rate of Ln-MCM-41 was remarkably pH-dependent and increased gradually upon decreasing pH. Additionally, these nanoparticles also exhibit considerable photoluminescence properties, living cells photoluminescence imaging in vitro, and paramagnetism behavior at room temperature due to the Ln3+-ions doping. Our research shows the possibility of our Ln-MCM-41 nanoparticles as multifunctional nanoprobes for application in bioseparation, bioimaging, and drug delivery.
研究领域:
材料科学
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生物医学工程
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纳米技术
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生物成像
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF POROUS MATERIALS
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2020
·Vol. 27
·期 6
·1639-1648
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IF 2.183
Zhang Tiantian,Li Bin,Zhang Xiaoli,Wang Jiao,Wei Longhui,Zhao Binxia,Li Binglin
N,N′-dimethyl-N-(4-pyridyl)-1,2-ethanediamine (DMPE) as a special N-alkylation precursor of 4-dimethylaminopyridine (DMAP) was grafted on the surface of γ-chloropropylated functionalized mesoporous silica MCM-41 to prepare immobilized DMAP. Characterization results of small angle X-ray diffraction, thermogravimetry and derivative thermogravimetry, Fourier transform infrared, scanning electron microscopy, energy-dispersive X-ray and transmission electron microscopy indicated that DMAP was successfully covalently bound to the surface of MCM-41. The highest loading of DMAP reached 0.9 mmol/g, which was 2.5 times higher than that of DMAP immobilized on the normal silica gel. The prepared immobilized DMAP as nucleophilic heterogeneous catalysts was successfully used for the acetylation reaction to produce α-tocopherol acetate. The highest yield reached 90.1% under the optimal condition which was summarized as follows: immobilized DMAP 100 mg, substrates mole ratio (acetic anhydride/α-tocopherol) 3:1, reaction temperature 50 ℃, stirring intensity 500 rpm, reaction in toluene for 12 h. The recyclability and stability of the DMAP grafted MCM-41 were excellent, as demonstrated by its use 20 times during batch operation without any loss of productivity.
研究领域:
化学工程
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xue-Yao Pang,Fan-Xiang Meng,Cheng Ma,Si-Yang Ni,Zi-Han Jia,Bo Li,Yu-Xiang Liu,Wei-Wei Gao
Gram-positive bacteria can cause a variety of infectious diseases. Selectively inhibiting Gram-positive bacteria will avoid the misuse of broad-spectrum antibiotics, achieve precise treatment, and delay the development of antibiotic resistance. In this work, we successfully developed an MCM-41 molecular sieve-supported copper-based nanozyme composites (MCM-41-Cu 2 O) for selectively combating Gram-positive bacteria. MCM-41, with its porous structure and excellent biocompatibility, not only serves as a carrier but also neutralizes the positive charges of the metal nanozyme, endowing MCM-41-Cu 2 O with negative zeta potentials. This allows it to interact electrostatically with Gram-positive bacteria, facilitating the penetration of free radicals into the bacterial cell membrane, thereby killing the bacteria. MCM-41-Cu 2 O continuously generates endogenous H 2 O 2 through its glutathione oxidase (GSHOx)-like activity·H 2 O 2 serves as the substrate for peroxidase (POD)-like catalytic reactions, producing •OH radicals, thereby enabling a self-cascade reaction. This approach avoids the toxic side effects associated with excessive exogenous H 2 O 2 and offers higher biosafety with potential for antibacterial applications. DFT calculations reveal that compared to Cu 2 O, MCM-41-Cu 2 O exhibits greater adsorption and decomposition capacity for H 2 O 2 , accelerating reaction rates and enhancing POD-like activity. MCM-41-Cu 2 O selectively targets Gram-positive bacteria, achieving a bactericidal rate of up to 99.6% against S. aureus and B. subtilis while leaving E. coli and P. aeruginosa colonies largely unaffected. Reactive oxygen species (ROS) generated by MCM-41-Cu 2 O-5% disrupt bacterial membranes, leading to depolarization, protein leakage, and bacterial death. Additionally, the MCM-41-Cu 2 O nanocomposites exhibit excellent biocompatibility and demonstrate superior in vivo antibacterial efficacy compared to antibiotics, effectively treating wound infections caused by S. aureus . These findings position MCM-41-Cu 2 O as a promising alternative for treating infections caused by Gram-positive bacteria and provide new insights into the antimicrobial applications of molecular sieves.
研究领域:
生物材料学
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抗菌研究
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纳米医学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）