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Catalytic behavior of Mo-Bi-Fe-Co-K-M-O(M=Ce,Gd,CeGd)catalysts for selective oxidation of isobutene

Journal of Rare Earths 2024年第1期42卷 84-93,I0003页

作者： Qinghui Li Huahua Zhao Jian Yang Jun Zhao Liang Yan huanling song Lingjun Chou State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou730000China University of Chinese Academy of Sciences Beijing100049China

The further improvement of methacrolein(MAL)selectivity from isobutene(IB)oxidation is crucial and *** this study,based on the typical Mo-Bi-Fe-Co-K-O mixed metal oxide,the rare earth element Gd-doped,Ce-doped and CeGd co-doped catalysts were prepared by co-precipitation strategy to increase the selectivity of MAL from 47.9%to 49.8%,64.2% and 68.6%,*** order to elucidate in-depth the promoting effect of Ce and/or Gd,various characterizations were utilized including X-ray diffraction patterns(XRD),Raman,X-ray fluorescence spectrometry(XRF),X-ray photoelectron spectroscopy(XPS),O_(2)-temperature programmed desorption(O_(2)-TPD),H2-temperature programmed reduction(H2-TPR),CO_(2)-temperature programmed desorption(CO_(2)-TPD),IB-temperature programmed desorption(i-C4-TPD)and in-situ IB-Fourier transform infrared spectroscopy(IB-FTIR).Both Ce and Gd finely regulate the bulk and surface structure of the catalyst,thus altering the redox ability,oxygen mobility and storage ability and *** with Ce,Gd addition slightly regulates the variation of Co^(2+)/Co^(3+)redox couples,greatly enhances the interaction among the components on the catalyst,thus only increases the content of surface oxygen species and has little effect on their *** Cecontaining catalyst performs stronger oxygen storage and migration ability,thus leading to the overproduction of surface Odefectspecies,which are proposed to be the active sites for the production of MAL and *** CeGd co-doped catalyst possesses the proper content of surface Odefectspecies,thus exhibits much higher MAL ***,the promoting mechanism of Ce and/or Gd over IB oxidation is ***,this work is helpful for understanding the influence of rare earth elements on the structure of mixed metal oxides and the olefin selective oxidation reaction.

关键词： Mixed metal oxide catalyst Rare earth element Isobutene Selective oxidation Methacrolein

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Role of cerium dopants in MoVNbo multi-metal oxide catalysts for selective oxidation of ethane

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Journal of Rare Earths 2022年第5期40卷 753-762,I0003页

作者： Baohua Liu Liang Yan Huahua Zhao Jian Yang Jun Zhao huanling song Lingjun Chou State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical Physics(LICP)Chinese Academy of SciencesLanzhou 730000China University of Chinese Academy of Sciences Beijing 100049China Suzhou Research Institute of LICP Chinese Academy of SciencesSuzhou 215123China

The effect of Ce on the structure of MoVNbCeO multi-metal oxide catalysts and the performance of ethane selective oxidation was *** multi-metal oxide catalysts with superior oxidizability exhibit high catalytic activity,and vanadium acts as the active center for ethane oxidation *** improved catalytic activity is related to the increased V^(5+) content on the catalyst surface,which results from the enhanced transformation of the electrons between V and ***,Ce effectively promotes oxygen adsorption,activation,and *** the presence of Ce can also prevent MoO_(3) formation and stabilize the Mo_(5)O_(14)-like *** addition,the catalyst with a moderate amount of Ce exhibits outstanding catalytic ***,the MVN-Ce catalyst with a Ce/V ratio of 0.1 exhibits the best performance:the total selectivity of the catalyst toward C_(2)H_(4) and CH_(3) COOH is the highest(72%) at the ethane conversion of 31%.Therefore,MoVNbCeO multi-metal oxides are promising candidates for selective oxidation.

关键词： Ethane oxidation Redox Mo5O14 Ce Active oxygen Rare earths

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Characterization and performance of Cu/ZnO/Al_2O_3 catalysts prepared via decomposition of M(Cu,Zn)-ammonia complexes under sub-atmospheric pressure for methanol synthesis from H_2 and CO_2

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Journal of Natural Gas Chemistry 2011年第6期20卷 629-634页

作者： Danjun Wang Jun Zhao huanling song Lingjun Chou State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical Physics Chinese Academy of Sciences Lanzhou 730000 Gansu China Graduate School of Chinese Academy of Sciences Beijing 100049 China

Methanol synthesis from hydrogenation of CO2 is investigated over Cu/ZnO/Al2O3 catalysts prepared by decomposition of M（Cu,Zn）-ammonia complexes （DMAC） at various *** catalysts were characterized in detail,including X-ray diffraction,N2 adsorption-desorption,N2O chemisorption,temperature-programmed reduction and evolved gas *** influences of DMAC temperature,reaction temperature and specific Cu surface area on catalytic performance are *** is considered that the aurichalcite phase in the precursor plays a key role in improving the physiochemical properties and activities of the final *** catalyst from rich-aurichalcite precursor exhibits large specific Cu surface area and high space time yield of methanol （212 g/（Lcat·h）;T=513 K,p=3MPa,SV=12000 h-1）.

关键词： decomposition of M(Cu,Zn)-ammonia complexes Cu/ZnO/Al2O3 catalyst CO2 hydrogenation methanol synthesis

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Isobutane dehydrogenation over chromia alumina catalysts prepared from MIL-101: Insight into chromium species on activity and selectivity

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Journal of Energy Chemistry 2014年第6期23卷 708-716页

作者： Huahua Zhao huanling song Zhichao Miao Lingjun Chou State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of Sciences Institute of Nano-Tech and Nano-Bionics University of Chinese Academy of Sciences

Various mesoporous chromia alumina catalysts were prepared by five different methods based on a metal-organic framework MIL-101 and their catalytic performances over isobutane dehydrogenation were investigated. The highly dispersed chromium species were produced on catalyst KCrAI-I1 with largest specific surface area of 198 m2-g-1 prepared with aluminium isopropoxide （Al（i-OC3HT）3） by ultrasonic im- pregnation method. However, the catalyst KCrAI-I2 synthesized by stirring impregnation possessed crystalline a-Cr203 phase, which was poorly dispersed. Two types of Cr-rich and Al-rich CrzA12_zO3 solid solutions, designated as CrAI-I and CrAI-II phase, were formed over the catalysts KCrAI-I3 （prepared by Al（i-OC3HT）3 with nitric acid regulation）, KCrA1-C4 （prepared by aluminium chloride hexahydrate） and KCrA1-N5 （prepared by aluminium nitrate nonahydrate）. Catalytic evaluation results revealed that KCrAI-I1 exhibited the high isobutane con- version due to its highly dispersed chromium species. However, KCrAI-I3, KCrA1-C4 and KCrA1-N5 showed the higher isobutene selectivity （95.2%-96.4%） on account of the formation of chromia alumina solid solutions in the catalysts. Moreover, the solid solution over the chromia alumina catalysts could greatly suppress the coke formation.

关键词： isobutane dehydrogenation chromia alumina solid solution metal organic framework MIL-IO1

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Chemical equilibrium controlled synthesis of polyoxymethylene dimethyl ethers over sulfated titania

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Journal of Energy Chemistry 2015年第2期24卷 239-244页

作者： Huaju Li huanling song Feng Zhao Liwei Chen Chungu Xia Laboratory for Nano-Catalytic Material & Technology Division of Advanced Nano?materials Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of Sciences State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical Physics Chinese Academy of Sciences i-Lab Suzhou Institute of Nano-Tech and Nano-Bionics Chinese Academy of Sciences

The chemical equilibrium and reaction kinetic behavior in the synthesis of polyoxymethylene dimethyl ethers （DMMn） were investigated over sulfated titania in order to reveal the decisive factor controlling the reaction. The results showed that the molar ratio of adjacent DMMn products in equilibrium solution had the same value, which depended absolutely on the reaction temperature. Meanwhile, the reactions had the same DMMn products distributions under varied reaction conditions. The equilibrium constants of the related step-wise reactions for DMMn formation were equal, which were calculated based on the bulk compositions of the reaction solution. And thus, the selectivity to DMMn was mainly controlled by the chemical equilibrium, i.e., thermodynamic control. In brief, the present results provide some guidance for future synthesis of DMMn.

关键词： polyoxymethylene dimethyl ethers sulfated titania chemical equilibrium reaction kinetic molar ratio

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Effect of impregnation strategy on catalytic hydrogenation behavior of PtCo catalysts supported on La2O2CO3 nanorods

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Journal of Rare Earths 2018年第9期36卷 965-973页

作者： Fengjun Hou Huahua Zhao huanling song Lingjun Chou Jun Zhao Jian Yang Liang Yan State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical Physics Chinese Academy of Sciences Lanzhou 730000 China University of Chinese Academy of Sciences Beijing 100049 China Suzhou Research Institute of LICP Chinese Academy of Sciences Suzhou 215123 China

Small Pt and Pt-Co nanoparticles（NPs） stabilized on La2 O2 CO3 nanorods（LOC） were prepared by wet impregnation method,and probed in liquid-phase chemoselective hydrogenation of crotonaldehyde（CRAL） to crotyl alcohol（CROL）.It is found that incorporation of Co atoms into Pt catalyst significantly improves the hydrogenation activity and desired selectivity to CROL as it destroys the Pt-lanthanum interfaces and results into the formation of Pt-Co *** addition,a close examination of catalyst surface and reactive performance suggests that the impregnation sequence of Pt and Co exerts great influence on the physicochemical property and the catalytic hydrogenation behavior of PtCo/LOC *** a result of the interaction between Pt and Co species,high alloying degree of Pt-Co NPs is obtained in the co-impregnated catalyst（Pt-Co/LOC）,thus achieving the highest hydrogenation *** selective deposit of Co atoms onto the low-coordinated Pt sites leads to the smallest metal particle size and high dispersion of Pt-Co NPs over the Pt/Co/LOC,giving rise to the highest selectivity and yield to CROL.

关键词： La2O2CO3 nanorods Platinum-cobalt Metal-support interaction Crotonaldehyde hydrogenation Rare earths

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Enhancement of La2O3 to Li-Mn/WO3/TiO2 for oxidative coupling of methane

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Journal of Rare Earths 2020年第2期38卷 167-174页

作者： Fei Cheng Jian Yang Liang Yan Jun Zhao Huahua Zhao huanling song Ling Jun Chou State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China University of Chinese Academy of Sciences Beijing 100049China Suzhou Research Institute of LICP Chinese Academy of SciencesSuzhou 215123China

A series of La2O3-promoted Li-Mn/WO3/TiO2 catalysts were prepared by varying the concentration of La2O3 *** effect of La2O3 promoter on its properties and catalytic performance for OCM was characterized with XRD,FT-IR,O2-TPD,Raman,CO2-TPD,H2-TPR,XPS and CH4-TPSR,The results show that all the La2O3-promoted Li-Mn/WO3/TiO2 catalysts possess a larger amount of strong basic sites and more abundant chemisorbed oxygen species in comparison with Li-Mn/WO3/TiO2,which is beneficial to OCM ***,La2O3 promoter can enhance the mobility of the oxygen species and the Mn species redox ability,which can also be favorable for the improvement of the catalytic performance for OCM,Due to the optimal synergistic interaction of these factors,5 wt%La2O3-Li-Mn/WO3/TiO2 exhibits the best performance among all the catalysts,on which the highest C2 yield of 19.2% is achieved at 750℃.

关键词： OCM La2O3 Oxygen species CH4-TPSR Rare earths

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碳/金属氧化物复合材料的合成及催化应用研究进展

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复合材料学报 2022年第2期39卷 502-512页

作者：张通宋焕玲丑凌军中国科学院兰州化学物理研究所羰基合成与选择氧化国家重点实验室兰州730000 中国科学院大学北京100049 中国科学院兰州化学物理研究所苏州研究院苏州215123

碳材料和金属氧化物为常用的多相催化剂载体,其中碳材料具有巨大的比表面积、良好的吸附性能,但力学性能较差。金属氧化物载体则具有较高的机械强度和热稳定性,但常常会与活性金属作用太强使其催化活性降低。碳/金属氧化物复合材料作为... 详细信息

碳材料和金属氧化物为常用的多相催化剂载体,其中碳材料具有巨大的比表面积、良好的吸附性能,但力学性能较差。金属氧化物载体则具有较高的机械强度和热稳定性,但常常会与活性金属作用太强使其催化活性降低。碳/金属氧化物复合材料作为一类新型材料受到了科学家的广泛关注,由于碳与金属氧化物(如氧化钛、氧化铝等)之间的协同作用,该复合材料表现出不同于单一组分的独特物理化学性质,重点综述了该类复合材料的制备方法及其在催化领域近年来的研究进展。

关键词：碳/金属氧化物复合材料合成协同作用催化碳材料应用

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自修复光致变色聚氨酯复合织物的制备与性能

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复合材料学报 2024年第8期41卷 4189-4199页

作者：李含郭阳白松吴焕岭林玲冒海燕盐城工学院纺织服装学院

为提高光致变色涂层织物耐用性能，采用光致变色微胶囊(PM)与两性离子聚氨酯(ZPU)制备PM/ZPU薄膜，并热压到棉织物上得到自修复光致变色PM/ZPU复合织物。对PM/ZPU复合织物的结构和形貌进行表征，并详细探讨了PM/ZPU复合织物的光致变色... 详细信息

为提高光致变色涂层织物耐用性能，采用光致变色微胶囊(PM)与两性离子聚氨酯(ZPU)制备PM/ZPU薄膜，并热压到棉织物上得到自修复光致变色PM/ZPU复合织物。对PM/ZPU复合织物的结构和形貌进行表征，并详细探讨了PM/ZPU复合织物的光致变色性能、自修复及回收利用能力。结果表明：经紫外光照射后，PM/ZPU复合织物的最大吸收波长由470 nm转移到530 nm，颜色由黄橙色变为红褐色，且具有良好的耐疲劳性能；基于两性离子的动态可逆性，PM/ZPU复合织物划痕可以在80℃下完全修复，断裂的复合织物在60℃下的粘合强度达到1.47 MPa，展现了优异的自修复性能；通过简单的溶解法可将废弃织物上的涂层进行回收并再利用，重新制备PM/ZPU复合织物依然具有良好的光致变色性能。

关键词：聚氨酯光致变色自修复性能回收再利用复合织物

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金属对钛硅分子筛TS-1催化丁二烯环氧化性能的影响

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催化学报 2013年第4期34卷 789-797页

作者：吴妹丑凌军宋焕玲中国科学院兰州化学物理研究所羰基合成与选择氧化国家重点实验室甘肃兰州730000 中国科学院大学北京10049

制备了不同金属改性的钛硅分子筛样品M-TS-1(M=V,Cr,Mn,Fe,Co,Ni,Cu,Zn,Cd,La,负载量为1%),并研究了其催化丁二烯环氧化反应的性能.结果表明,V,Cr,Mn的加入导致H2O2无效分解,因而在丁二烯环氧化反应中表现出较高的H2O2转化率和较低有效... 详细信息

制备了不同金属改性的钛硅分子筛样品M-TS-1(M=V,Cr,Mn,Fe,Co,Ni,Cu,Zn,Cd,La,负载量为1%),并研究了其催化丁二烯环氧化反应的性能.结果表明,V,Cr,Mn的加入导致H2O2无效分解,因而在丁二烯环氧化反应中表现出较高的H2O2转化率和较低有效利用率;Fe,Co,Ni以及稀土金属La均在一定程度上促进了TS-1对H2O2的有效利用;Cu,Zn抑制了H2O2的转化,使得H2O2转化率和有效利用率都较低;Cd有效提高了TS-1的催化活性,H2O2转化率和有效利用率均接近100%.采用X射线衍射、N2吸附-脱附、X射线光电子能谱、傅里叶变换红外光谱等手段表征了上述各金属的改性对TS-1骨架结构以及Ti活性中心周围电子环境的影响.结果表明,各M-TS-1样品的骨架结构都仍保持原有的MFI构型,但是TS-1中Ti活性中心周围的电子环境受到来自各种金属的不同程度影响,关联催化活性时没有特定的规律性.

关键词：丁二烯环氧化乙烯基环氧乙烷金属钛硅分子筛

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