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Catalytic oxidation of carbon monoxide, toluene, and ethyl acetate over the

Zhidan Fu, Lisha Liu, Yong Song, Qing Ye, Shuiyuan Cheng, Tianfang Kang, Hongxing Dai

《化学科学与工程前沿（英文）》 2017年 第11卷 第2期   页码 185-196 doi: 10.1007/s11705-017-1631-5

摘要： The Pd catalyst supported on cryptomelane-type manganese oxide octahedral molecular sieve (OMS-2) were prepared. The effect of Pd loading on the catalytic oxidation of carbon monoxide, toluene, and ethyl acetate over Pd/OMS-2 has been investigated. The results show that the Pd loading plays an important role on the physicochemical properties of the Pd/OMS-2 catalysts which outperform the Pd-free counterpart with the 0.5Pd/OMS-2 catalyst being the best. The temperature for 50% conversion was 25, 240 and 160 °C, and the temperature for 90% conversion was 55, 285 and 200 °C for oxidation of CO, toluene, and ethyl acetate, respectively. The low-temperature reducibility and high oxygen mobility of Pd/OMS-2 are the factors contributable to the excellent catalytic performance of 0.5Pd/OMS-2.

关键词： cryptomelane-type manganese oxide octahedral molecular sieve     oxygen mobility     reducibility     carbon monoxide oxidation     volatile organic compound combustion    

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Preparation of lithium ion-sieve and utilizing in recovery of lithium from seawater

Lu WANG, Changgong MENG, Wei MA

《化学科学与工程前沿（英文）》 2009年 第3卷 第1期   页码 65-67 doi: 10.1007/s11705-009-0105-9

摘要： Lithium is one of the most important light metals, which is widely used as raw materials for large-capacity rechargeable batteries, light aircraft alloys and nuclear fusion fuel. Seawater, which contains 250 billion tons of lithium in total, has thus recently been noticed as a possible resource of lithium. While, since the average concentration of lithium in seawater is quite low (0.17 mg·L ), enriching it to an adequate high density becomes the primary step for industrial applications. The adsorption method is the most prospective technology for increasing the concentration of lithium in liquid. Among the adsorbents for lithium, the ion-sieve is a kind of special absorbent which has high selectivity for Li , especially the spinel manganese oxides (SMO), which among the series of ion-sieves, has become the most promising adsorption material for lithium. In this study, the SMO ion-sieve was prepared by a coprecipitation method. The preparation conditions were discussed and the sample characters were analyzed. Recovery of Li from seawater were studied in batch experiments using prepared ion-sieve, and the effect of solution pH and the uptake rates were also investigated in different Li solutions.

关键词： lithium     ion-sieve     seawater     spinel manganese oxide    

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Chemical composition and formation mechanisms in the cathode-electrolyte interface layer of lithium manganeseoxide batteries from reactive force field (ReaxFF) based molecular dynamics

Sahithya REDDIVARI, Christian LASTOSKIE, Ruofei WU, Junliang ZHANG

《能源前沿（英文）》 2017年 第11卷 第3期   页码 365-373 doi: 10.1007/s11708-017-0500-8

摘要： Lithium manganese oxide (LiMn O ) is a principal cathode material for high power and high energy density electrochemical storage on account of its low cost, non-toxicity, and ease of preparation relative to other cathode materials. However, there are well-documented problems with capacity fade of lithium ion batteries containing LiMn O . Experimental observations indicate that the manganese content of the electrolyte increases as an electrochemical cell containing LiMn O ages, suggesting that active material loss by dissolution of divalent manganese from the LiMn O surface is the primary reason for reduced cell life in LiMn O batteries. To improve the retention of manganese in the active material, it is key to understand the reactions that occur at the cathode surface. Although a thin layer of electrolyte decomposition products is known to form at the cathode surface, the speciation and reaction mechanisms of Mn in this interface layer are not yet well understood. To bridge this knowledge gap, reactive force field (ReaxFF) based molecular dynamics was applied to investigate the reactions occurring at the LiMn O cathode surface and the mechanisms that lead to manganese dissolution. The ReaxFFMD simulations reveal that the cathode-electrolyte interface layer is composed of oxidation products of electrolyte solvent molecules including aldehydes, esters, alcohols, polycarbonates, and organic radicals. The oxidation reaction pathways for the electrolyte solvent molecules involve the formation of surface hydroxyl species that react with exposed manganese atoms on the cathode surface. The presence of hydrogen fluoride (HF) induces formation of inorganic metal fluorides and surface hydroxyl species. Reaction products predicted by ReaxFF-based MD are in agreement with experimentally identified cathode-electrolyte interface compounds. An overall cathode-electrolyte interface reaction scheme is proposed based on the molecular simulation results.

关键词： lithium manganese oxide batteries     reactive force field (ReaxFF)     cathode-electrolyte interface layer     molecular dynamics    

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Catalytic activity of manganese oxide supported on alumina in the synthesis of quinoxalines

Rekha M., H. Kathyayini, N. Nagaraju

《化学科学与工程前沿（英文）》 2013年 第7卷 第4期   页码 415-421 doi: 10.1007/s11705-013-1360-3

摘要： Two catalysts, alumina and manganese oxide supported on alumina, have been prepared by calcination and precipitation-impregnation methods, respectively. The catalysts are characterised by the following techniques: Brunner-Emmett-Teller-N adsorption-desorption for surface area, temperature programmed desorption of NH and -butyl amine back titration methods for surface acidity, powder X-ray diffraction for textural properties, and Fourier transform infrared spectroscopy for the anionic radicals. The catalytic activity has been determined under heterogeneous conditions in the condensation reaction between -phenylenediamine and benzil. The product purity is checked by thin-layer chromatography and melting point. The products are also analysed by LC-MS and H-NMR techniques. The yields of the products have been found to be good and catalysts exhibited excellent recyclability. The effect of changing the reaction parameters such as temperature, reaction time, amount of the catalyst, nature of solvent and molar ratio of reactants on the yield of the product has been studied. The surface acidity of the catalysts plays an important role in activating the reaction.

关键词： alumina     manganese oxide deposited on alumina     quinoxaline synthesis    

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Preparation and characterization of novel carbon molecular sieve membrane/PSSF composite by pyrolysis

Ying Yan, Peng Huang, Huiping Zhang

《化学科学与工程前沿（英文）》 2019年 第13卷 第4期   页码 772-783 doi: 10.1007/s11705-019-1827-y

摘要： Carbon molecular sieve membrane (CMSM)/paper-like stainless steel fibers (PSSF) has been manufactured by pyrolyzing poly (furfuryl alcohol) (PFA) coated on the metal fibers. PFA was synthesized using oxalic acid dihydrate as a catalyst and coated on microfibers by dip coating method. For the purpose of investigating the effects of final carbonization temperature, the composites were carbonized between 400°C and 800°C under flowing nitrogen. The morphology and microstructure were examined by X-ray diffraction, Fourier transforms infrared spectroscopy, scanning electron microscopy, thermogravimetric analysis, N adsorption and desorption, Raman spectra and X-ray photoelectron spectra. The consequences of characterization showed that the CMSM containing mesopores of 3.9 nm were manufactured. The specific surface area of the CMSM/PSSF fabricated in different pyrolysis temperature varies from 26.5 to 169.1 m ∙g and pore volume varies from 0.06 to 0.23 cm ∙g . When pyrolysis temperature exceeds 600°C, the specific surface, pore diameter and pore volume decreased as carbonization temperature increased. Besides, the degree of graphitization in carbon matrix increased with rising pyrolysis temperature. Toluene adsorption experiments on different structured fixed bed that was padded by CMSM/PSSF and granular activated carbon (GAC) were conducted. For the sake of comparison, adsorption test was also performed on fixed bed packed with GAC. The experimental results indicated that the rate constant ′ was dramatically increased as the proportion of CMCM/PSSF composites increased on the basis of Yoon-Nelson model, which suggested that structured fixed bed padded with CMSM/PSSF composite offered higher adsorption rate and mass transfer efficiency.

关键词： carbon molecular sieve membrane     stainless steel fibers     pyrolysis     structured fixed bed     toluene    

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Interlayer-confined two-dimensional manganese oxide-carbon nanotube catalytic ozonation membrane for

《化学科学与工程前沿（英文）》 2022年 第16卷 第5期   页码 731-744 doi: 10.1007/s11705-021-2110-6

摘要： Catalytic ozonation technology has attracted copious attention in water purification owing to its favorable oxidative degradation of pollutants and mitigation of membrane fouling capacity. However, its extensive industrial application has been restricted by the low ozone utilization and limited mass transfer of the short-lived radical species. Interlayer space-confined catalysis has been theoretically proven to be a viable strategy for achieving high catalytic efficiency. Here, a two-dimensional MnO2-incorporated ceramic membrane with tunable interspacing, which was obtained via the intercalation of a carbon nanotube, was designed as a catalytic ozonation membrane reactor for degrading methylene blue. Benefiting from the abundant catalytic active sites on the surface of two-dimensional MnO2 as well as the ultralow mass transfer resistance of fluids due to the nanolayer confinement, an excellent mineralization effect, i.e., 1.2 mg O3(aq) mg–1 TOC removal (a total organic carbon removal rate of 71.5%), was achieved within a hydraulic retention time of 0.045 s of pollutant degradation. Further, the effects of hydraulic retention time and interlayer spacing on methylene blue removal were investigated. Moreover, the mechanism of the catalytic ozonation employing catalytic ozonation membrane was proposed based on the contribution of the Mn(III/IV) redox pair to electron transfer to generate the reactive oxygen species. This innovative two-dimensional confinement catalytic ozonation membrane could act as a nanoreactor and separator to efficiently oxidize organic pollutants and enhance the control of membrane fouling during water purification.

关键词： catalytic membrane reactor     catalytic ozonation     nanoconfinement     two-dimensional manganese oxide    

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Thermal decomposition of poly(ethylene terephthalate)/mesoporous molecular sieve composites

RUN Mingtao, ZHANG Dayu, WU Sizhu, WU Gang

《化学科学与工程前沿（英文）》 2007年 第1卷 第1期   页码 50-54 doi: 10.1007/s11705-007-0010-z

摘要： The nonisothermal and isothermal degradation processes of poly (ethylene terephthalate)/mesoporous molecular sieve (PET/MMS) composites synthesized by in-situ polymerization were studied by using thermogravimetric analysis in nitrogen. The nonisothermal degradation of the composite is found to be the first-order reaction. An iso-conversional procedure developed by Ozawa is used to calculate the apparent activation energy (), which is an average value of about 260 kJ/mol with the weight conversion from 0% to 30%, and is higher than that of neat PET. Isothermal degradation results are confirmed with the nonisothermal process, in which PET/MMS showed higher thermal stability than neat PET. The polymer in mesoporous channels has more stability due to the protection of the inorganic pore-wall. These results indicate that mesoporous MMS in PET/MMS composites improve the stability of the polymer.

关键词： polymerization     isothermal degradation     conversion     nonisothermal degradation     activation    

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Simultaneous enhanced ammonia and nitrate removal from secondary effluent in constructed wetlands using a new manganese-containing

《环境科学与工程前沿（英文）》 2023年 第18卷 第4期 doi: 10.1007/s11783-024-1807-4

摘要：

● MnO2/PCL composite material (MPCM) enhances ammonia and nitrate removal in CWs.

关键词： Constructed wetland     Nitrogen removal     Manganese redox     Polycaprolactone     Nitrous oxide    

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Adsorptive behaviors of humic acid onto freshly prepared hydrous manganese dioxides

LIU Ruiping, LI Guibai, YANG Yanling, HE Wenjie, HAN Hongda

《环境科学与工程前沿（英文）》 2007年 第1卷 第2期   页码 240-245 doi: 10.1007/s11783-007-0041-1

摘要： This study focused on the adsorptive behaviors of humic acid onto freshly prepared hydrous MnO(s) (δMnO), and investigated the feasibility of employing δMnO for humic acid removal from drinking water. Effects of such parameters as molecular mass of humic acid, kinds of divalent cations on adsorptive behaviors and possible mechanisms involved were investigated. This study indicated that humic acid with higher molecular mass exhibited more tendency of adsorbing onto &MnO than that with lower molecular mass. Ca facilitated more humic acid adsorption than Mg; UV-Vis spectra analysis indicated higher capabilities of Ca coordinating with acidic functional groups of humic acid than that of Mg. Additionally, ζ potential characterization indicated that Ca showed higher potential of increasing ζ potential of &MnO than Mg. Ca of 1.0 mmol/L increased ζ potential of δMnO

关键词： Mg     molecular     functional     UV-Vis spectra     prepared hydrous    

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Ti incorporation in MCM-41 mesoporous molecular sieves using hydrothermal synthesis

Shengping WANG, Changqing MA, Yun SHI, Xinbin MA

《化学科学与工程前沿（英文）》 2014年 第8卷 第1期   页码 95-103 doi: 10.1007/s11705-014-1405-2

摘要： Titanium-containing mesoporous materials (Ti-MCM-41) were obtained by hydrothermal synthesis. Such materials are active catalysts for the transesterification of dimethyl oxalate and phenol to produce diphenyl oxalate. To understand the role of the Ti in the catalytic process, Ti-MCM-41 samples with different Si/Ti ratios (from 5 to 100) were prepared and the samples were analyzed by Fourier transform infrared spectroscopy, UV-visible spectroscopy, and ammonia temperature programmed desorption. It was concluded that the Ti is incorporated into the framework of the MCM-41 and formed weak Lewis acid sites. In addition, the number of Ti(IV) sites increased as the amount of titanium increased. X-ray powder diffraction, N adsorption-desorption and transmission electron microscopy results showed that the Ti-MCM-41 samples have a hexagonal arrangement of mono-dimensional pores. A large number of Ti(IV) sites coupled with the mesoporous structure and large pore diameters are favorable for the transesterification catalytic properties of Ti-MCM-41.

关键词： Ti-MCM-41     mesoporous molecular sieve     acid sites     transesterification     hydrothermal synthesis    

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Comparing the adsorption behaviors of Cd, Cu and Pb from water onto Fe-Mn binary oxide, MnO

Wei XU,Huachun LAN,Hongjie WANG,Hongming LIU,Jiuhui QU

《环境科学与工程前沿（英文）》 2015年 第9卷 第3期   页码 385-393 doi: 10.1007/s11783-014-0648-y

摘要： The adsorption potential of FMBO, FeOOH, MnO for the removal of Cd , Cu and Pb in aqueous systems was investigated in this study. Comparing to FMBO and FeOOH, MnO offered a much higher removal capacity towards the three metal ions. The maximal adsorption capacity of MnO for Cd , Cu and Pb were 1.23, 2.25 and 2.60 mmol·g , respectively. And that for FMBO were 0.37, 1.13, and 1.18 mmol·g and for FeOOH were 0.11, 0.86 and 0.48 mmol·g , respectively. The adsorption behaviors of the three metal ions on the three adsorbents were all significantly affected by pH values and heavy metal removal efficiency increased with pH increased. The Langmuir and Freundlich adsorption models were used to describe the adsorption equilibrium of the three metal ions onto the three adsorbents. Results showed that the adsorption equilibrium data fitted well to Langmuir isotherm and this indicated that adsorption of metal ions occurred on the three metal oxides adsorbents limited to the formation of a monolayer. More negative charged of MnO surface than that of FMBO and FeOOH could be ascribed by lower pH of MnO than that of FMBO and FeOOH and this could contribute to more binding sites on MnO surface than that of FMBO and FeOOH. The higher metal ions uptake by MnO than FMBO and FeOOH could be well explained by the surface charge mechanism.

关键词： heavy metals     Fe-Mn binary oxide     manganese dioxide     ferric hydroxide     adsorption    

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Synthesis and application of superparamagnetic iron oxide nanoparticles in targeted therapy and imaging

Liangqian Tong, Ming Zhao, Shu Zhu, Jing Chen

《医学前沿（英文）》 2011年 第5卷 第4期   页码 379-387 doi: 10.1007/s11684-011-0162-6

摘要： Superparamagnetic iron oxide (SPIO) nanoparticles have become a popular strategy of cancer treatment and molecular imaging because of their versatile properties and biocompatibility. A variety of studies have shown the exciting potential of functionalized SPIO nanoparticles, such as surface-coated, targeted ligand-conjugated, and/or drug-loaded SPIO nanoparticles, as powerful tools for targeted imaging and therapy. Moreover, the applications of SPIO nanoparticles that integrate diagnosis and therapy in SPIO nanoparticles facilitate the monitoring of therapeutic efficacy during treatment. In the present review, we primarily concentrate on the recent advancements in the field of SPIO nanoparticles in terms of synthesis, targeted therapy, and cancer imaging.

关键词： nanoparticles     superparamagnetic iron oxide     targeted therapy     molecular imaging     cancer    

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Efficient base-free oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid over copper-doped manganeseoxide nanorods with

Feng Cheng, Dongwen Guo, Jinhua Lai, Meihui Long, Wenguang Zhao, Xianxiang Liu, Dulin Yin

《化学科学与工程前沿（英文）》 2021年 第15卷 第4期   页码 960-968 doi: 10.1007/s11705-020-1999-5

摘要： 2,5-Furandicarboxylic acid (FDCA) is an important and renewable building block and can serve as an alternative to terephthalic acid in the production of bio-based degradable plastic. In this study, Cu-doped MnO  nanorods were prepared by a facile hydrothermal redox method and employed as catalysts for the selective oxidation of 5-hydroxymethylfurfural (HMF) to FDCA using -butyl hydroperoxide (TBHP) as an oxidant. The catalysts were characterized using X-ray diffraction analysis, Fourier transform infrared spectroscopy, thermogravimetric analysis, and transmission electron microscopy. The effects of oxidants, solvents, and reaction conditions on the oxidation of HMF were investigated, and a reaction mechanism was proposed. Experimental results demonstrated that 99.4% conversion of HMF and 96.3% selectivity of FDCA were obtained under suitable conditions, and -butanol was the most suitable solvent when TBHP was used as an oxidant. More importantly, the Cu-doped MnO catalyst can maintain durable catalytic activity after being recycled for more than ten times.

关键词： 5-hydroxymethylfurfural     25-furandicarboxylic acid     selective oxidation     Cu-doped MnO2     biomass transformation    

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Theoretical study on Janus graphene oxide membrane for water transport

Quan Liu, Mingqiang Chen, Yangyang Mao, Gongping Liu

《化学科学与工程前沿（英文）》 2021年 第15卷 第4期   页码 913-921 doi: 10.1007/s11705-020-1954-5

摘要： Graphene oxide (GO) membranes have received considerable attention owing to their outstanding water-permeation properties; however, the effect of the membrane’s microstructures (such as the distribution of oxidized and pristine regions) on the transport mechanism remains unclear. In this study, we performed molecular simulations to explore the permeation of a water–ethanol mixture using a new type of Janus GO membranes with different orientations of oxidized and pristine surfaces. The results indicate that the oxidized upper surface endows the GO membrane with considerable water-capture capability and the in-built oxidized interlayer promotes the effective vertical diffusion of water molecules. Consequently, using the optimized Janus GO membrane, infinite water selectivity and outstanding water flux (~40.9 kg⋅m ⋅h ) were achieved. This study contributes to explaining the role of oxidized regions in water permeation via GO membranes and suggests that Janus GO membranes could be used as potential candidates for water–ethanol separation.

关键词： graphene oxide membrane     molecular dynamics simulation     water permeation     water-ethanol separation     oxidized and pristine regions    

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Oxidation-extraction desulfurization of model oil over Zr-ZSM-5/SBA-15 and kinetic study

Chuanzhu LU,Hui FU,Huipeng LI,Hua ZHAO,Tianfeng CAI

《化学科学与工程前沿（英文）》 2014年 第8卷 第2期   页码 203-211 doi: 10.1007/s11705-014-1420-3

摘要： ZSM-5/SBA-15 composite molecular sieves were synthesized using post-synthesis method and characterized by X-ray diffraction and N adsorption-desorption. The oxidative-extration desulfurization of model oil was investigated by using hydrogen peroxide as the oxidant, tetrabutyl ammonium bromide as phase transfer catalyst, dimethyl sulfoxide as extractant, and Zr-ZSM-5/SBA-15, Ag-ZSM-5/SBA-15, Ce-ZSM-5/SBA-15 as catalyst. Under the optimal conditions, the desulfurization rate decreases in the order: Zr-ZSM-5/SBA-15>Ce-ZSM-5/SBA-15>Ag-ZSM-5/SBA-15. The highest desulfurization rate is 84.53% under the catalysis of Zr-ZSM-5/SBA-15. Kinetics analysis shows that the reaction is pseudo-first-order with the activation energy of 44.23 kJ/mol.

关键词： composite molecular sieve     oxidation desulfuration     extraction     kinetic    

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标题 作者 时间 类型 操作

Catalytic oxidation of carbon monoxide, toluene, and ethyl acetate over the

Zhidan Fu, Lisha Liu, Yong Song, Qing Ye, Shuiyuan Cheng, Tianfang Kang, Hongxing Dai

期刊论文

Preparation of lithium ion-sieve and utilizing in recovery of lithium from seawater

Lu WANG, Changgong MENG, Wei MA

期刊论文

Chemical composition and formation mechanisms in the cathode-electrolyte interface layer of lithium manganeseoxide batteries from reactive force field (ReaxFF) based molecular dynamics

Sahithya REDDIVARI, Christian LASTOSKIE, Ruofei WU, Junliang ZHANG

期刊论文

Catalytic activity of manganese oxide supported on alumina in the synthesis of quinoxalines

Rekha M., H. Kathyayini, N. Nagaraju

期刊论文

Preparation and characterization of novel carbon molecular sieve membrane/PSSF composite by pyrolysis

Ying Yan, Peng Huang, Huiping Zhang

期刊论文

Interlayer-confined two-dimensional manganese oxide-carbon nanotube catalytic ozonation membrane for

期刊论文

Thermal decomposition of poly(ethylene terephthalate)/mesoporous molecular sieve composites

RUN Mingtao, ZHANG Dayu, WU Sizhu, WU Gang

期刊论文

Simultaneous enhanced ammonia and nitrate removal from secondary effluent in constructed wetlands using a new manganese-containing

期刊论文

Adsorptive behaviors of humic acid onto freshly prepared hydrous manganese dioxides

LIU Ruiping, LI Guibai, YANG Yanling, HE Wenjie, HAN Hongda

期刊论文

Ti incorporation in MCM-41 mesoporous molecular sieves using hydrothermal synthesis

Shengping WANG, Changqing MA, Yun SHI, Xinbin MA

期刊论文

Comparing the adsorption behaviors of Cd, Cu and Pb from water onto Fe-Mn binary oxide, MnO

Wei XU,Huachun LAN,Hongjie WANG,Hongming LIU,Jiuhui QU

期刊论文

Synthesis and application of superparamagnetic iron oxide nanoparticles in targeted therapy and imaging

Liangqian Tong, Ming Zhao, Shu Zhu, Jing Chen

期刊论文

Efficient base-free oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid over copper-doped manganeseoxide nanorods with

Feng Cheng, Dongwen Guo, Jinhua Lai, Meihui Long, Wenguang Zhao, Xianxiang Liu, Dulin Yin

期刊论文

Theoretical study on Janus graphene oxide membrane for water transport

Quan Liu, Mingqiang Chen, Yangyang Mao, Gongping Liu

期刊论文

Oxidation-extraction desulfurization of model oil over Zr-ZSM-5/SBA-15 and kinetic study

Chuanzhu LU,Hui FU,Huipeng LI,Hua ZHAO,Tianfeng CAI

期刊论文