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2023 1

2022 2

2019 1

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氧化铈 2

乙烷干重整 1

二氧化碳 1

二氧化碳还原 1

催化剂活化 1

光热 1

原位谱学 1

反应机理 1

氧化钛 1

氧空位 1

甲烷化 1

结晶性 1

金属-载体强相互作用 1

镍 1

镍-氧化铈催化剂 1

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Enhanced activity of bimetallic Fe-Cu catalysts supported on ceria toward water gas shift reaction: synergistic

《化学科学与工程前沿（英文）》 2023年第17卷第12期页码 1962-1972 doi: 10.1007/s11705-023-2359-z

摘要： Within the “hydrogen chain”, the high-temperature water gas shift reaction represents a key step to improve the H₂ yield and adjust the H₂/CO_x ratio to fit the constraints of downstream processes. Despite the commercial application of the high-temperature water gas shift, novel catalysts characterized by higher intrinsic activity (especially at low temperatures), good thermal stability, and no chromium content are needed. In this work, we propose bimetallic iron-copper catalysts supported on ceria, characterized by low active phase content (iron oxide + copper oxide < 5 wt %). Fresh and used samples were characterized by inductively coupled plasma mass spectrometry, X-ray diffraction, nitrogen physisorption, scanning electron microscopy coupled with energy-dispersive X-ray spectroscopy, and temperature programmed reduction in hydrogen to relate physicochemical features and catalytic activity. The sample with iron/copper ≈ 1 and 4 wt % active phase content showed the best catalytic properties in terms of turnover frequency, no methane formation, and stability. Its unique properties were due to both strong iron-copper interaction and strong metal-support interaction, leading to outstanding redox behavior.

关键词： water gas shift iron copper bimetallic catalysts ceria hydrogen

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Preparation of ceria-zirconia solid solution with enhanced oxygen storage capacity and redox performance

Lijing MENG, Licheng LIU, Xuehong ZI, Hongxing DAI, Hong HE, Zhen ZHAO, Xinping WANG,

《环境科学与工程前沿（英文）》 2010年第4卷第2期页码 164-171 doi: 10.1007/s11783-010-0019-2

摘要： A new method called ultrasonic-assisted membrane reaction (UAMR) was reported for the fabrication of ceria-zirconia solid solution. A series of ceria-zirconia solid solutions with different Ce/Zr molar ratios were prepared by the UAMR method and characterized by X-ray diffraction (XRD), N adsorption, hydrogen temperature-programmed reduction (H-TPR), scanning electron microscope (SEM), and transmission electron microscopy (TEM) techniques. The UAMR method proved to be superior, especially when the Ce/Zr molar ratio was lower than 1, in fabricating ceria-zirconia solid solutions with large BET surface area, high oxygen storage capacity (OSC), and low reduction temperature.

关键词： membrane reaction ceria-zirconia Ce/Zr molar ratio solid solution hydrogen temperature-programmed reduction (H2-TPR)

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Methane partial oxidation over NiO-MgO/Ce

Piyawat PUE-ON, Vissanu MEEYOO, Thirasak RIRKSOMBOOON

《化学科学与工程前沿（英文）》 2013年第7卷第3期页码 289-296 doi: 10.1007/s11705-013-1345-2

摘要： Methane partial oxidation (MPO) is considered as an alternative method to produce hydrogen because it is an exothermic reaction to afford a suitable H /CO ratio of 2. However, carbon deposition on a catalyst is observed as a major cause of catalyst deactivation in MPO. In order to find suitable catalysts that prevent the carbon deposition, NiO-MgO/Ce Zr O (CZO) supported catalysts were prepared via the co-impregnation (C) and sequential incipient wetness impregnation (S) methods. The amount of Ni loading was fixed at 15 wt-% whereas the amount of MgO loading was varied from 5 to 15 wt-%. The results revealed that the addition of MgO shifted the light-off temperatures to higher temperatures. This is because the Ni surface was partially covered with MgO, and the strong interaction between NiO and NiMgO over CZO support led to the difficulty in reducing NiO to active Ni and thus less catalytic activity. However, among the catalysts tested, the 15Ni5Mg/CZO (S) catalyst exhibited the best catalytic stability for MPO after 18 h on stream at 750°C. Moreover, this catalyst had a better resistance to carbon deposition due to its high metallic Ni dispersion at high temperature.

关键词： methane partial oxidation NiO ceria-zirconia MgO mixed oxide solid solution

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复合镍基催化剂催化CO₂ 光热甲烷化反应中氧化铈和氧化钛的助催化作用 Article

Ee Teng Kho,Salina Jantarang,Zhaoke Zheng,Jason Scott,Rose Amal

《工程（英文）》 2017年第3卷第3期页码 393-401 doi: 10.1016/J.ENG.2017.03.016

摘要：

太阳能驱动二氧化碳(CO₂) 转化为燃料是解决CO₂ 减排和快速增长的世界能源需求的理想方案。本文利用光照辐射镍基负载催化剂床层引发加热效应以促进CO₂ 的转化，研究了不同组成的氧化铈-氧化钛复合氧化物载体及其对光热CO₂ 转化的影响。提高光热CO₂ 甲烷化活性的两个至关重要的因素分别是：①优化的镍颗粒负载对于高活性催化面积及用于加热催化床层的更高的光吸收能力是必需的；②载体上的缺陷位对于促进CO₂ 吸附及随后的活化是必需的。载体中的钛对维持掺杂氧化钛的氧化铈上的氧空位缺陷起着关键作用。当氧化铈和氧化钛混合比例理想时，再结合高光照吸收以及稳定的还原状态，有利于CO₂ 吸附及随后高效光热CO₂ 甲烷化反应的发生。

关键词：光热二氧化碳还原镍氧化铈氧化钛

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New insights into mercury removal mechanism on CeO

Ling Li, Yu He, Xia Lu

《环境科学与工程前沿（英文）》 2018年第12卷第2期 doi: 10.1007/s11783-018-1007-1

摘要： First-principles calculations were performed to investigate the mechanism of Hg adsorption and oxidation on CeO (111). Surface oxygen activated by the reduction of Ce to Ce was vital to Hg adsorption and oxidation processes. Hg was fully oxidized by the surface lattice oxygen on CeO (111), without using any other oxidizing agents. HCl could dissociate and react with the Hg adatom on CeO (111) to form adsorbed Hg–Cl or Cl–Hg–Cl groups, which promoted the desorption of oxidized Hg and prevented CeO catalyst deactivation. In contrast, O–H and H–O–H groups formed during HCl adsorption consumed the active surface oxygen and prohibited Hg oxidation. The consumed surface oxygen was replenished by adding O into the flue gas. We proposed that oxidized Hg desorption and maintenance of sufficient active surface oxygen were the rate-determining steps of Hg removal on CeO -based catalysts. We believe that our thorough understanding and new insights into the mechanism of the Hg removal process will help provide guidelines for developing novel CeO -based catalysts and enhance the Hg removal efficiency.

关键词： Elemental mercury removal Surface adsorption Ceria First-principles calculations

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Plasma-electrochemical synthesis of europium doped cerium oxide nanoparticles

Liangliang Lin, Xintong Ma, Sirui Li, Marly Wouters, Volker Hessel

《化学科学与工程前沿（英文）》 2019年第13卷第3期页码 501-510 doi: 10.1007/s11705-019-1810-7

摘要： In the present study, a plasma-electrochemical method was demonstrated for the synthesis of europium doped ceria nanoparticles. Ce(NO ) ·6H O and Eu(NO ) ·5H O were used as the starting materials and being dissolved in the distilled water as the electrolyte solution. The plasma-liquid interaction process was investigated by an optical emission spectroscopy, and the obtained products were characterized by complementary analytical methods. Results showed that crystalline cubic CeO :Eu nanoparticles were successfully obtained, with a particle size in the range from 30 to 60 nm. The crystal structure didn’t change during the calcination at a temperature from 400°C to 1000°C, with the average crystallite size being estimated to be 52 nm at 1000°C. Eu ions were shown to be effectively and uniformly doped into the CeO lattices. As a result, the obtained nanophosphors emit apparent red color under the UV irradiation, which can be easily observed by naked eye. The photoluminescence spectrum further proves the downshift behavior of the obtained products, where characteristic D → F transitions of Eu ions had been detected. Due to the simple, flexible and environmental friendly process, this plasma-electrochemical method should have great potential for the synthesis of a series of nanophosphors, especially for bio-application purpose.

关键词： plasma-electrochemical method europium doped ceria rare earth nanoparticles photoluminescence

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用于CO甲烷化的Ni/CeO₂催化剂还原过程重构行为调控研究 Article

曹昕宇, 浦天成, Bar Mosevitzky Lis, Israel E. Wachs, 彭冲, 朱明辉, 胡永康

《工程（英文）》 2022年第14卷第7期页码 94-99 doi: 10.1016/j.eng.2021.08.023

摘要：

还原预处理是活化负载型金属催化剂的重要步骤，但很少受到关注。本研究发现负载型镍催化剂的重构过程对预处理条件非常敏感。与使用氢气的传统活化方式相比，用合成气活化催化剂可以产生具有多晶结构的负载型镍纳米颗粒，其中包含丰富的晶界。独特的活化方式使得催化剂上CO吸附得到增强，提高了CO甲烷化率。通过操纵活化条件来调整催化剂结构的策略也可以被用于指导其他负载型金属催化剂的理性设计。

关键词：镍-氧化铈催化剂催化剂活化结晶性甲烷化原位谱学

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FeNi/Al-Ce-O催化剂上的乙烷干重整——组成诱导的金属-载体强相互作用 Article

张涛, 刘志成, 叶迎春, 王毓, 杨贺勤, 高焕新, 杨为民

《工程（英文）》 2022年第18卷第11期页码 173-185 doi: 10.1016/j.eng.2021.11.027

摘要：

在页岩气革命的背景下，乙烷干重整因在化学原料生产和碳减排方面的潜力而备受关注。本研究通过X射线光电子能谱、H₂程序升温还原和能量散射X射线谱等手段，揭示了一种组成诱导的金属-载体强相互作用。氧化铈中Al的引入增强了金属与载体之间的相互作用，显著影响了Al-Ce-O载体表面FeNi活性组分的分散度，从而提升了FeNi/Al-Ce-O催化剂的乙烷干重整反应性能。随着载体中Al含量的增加，负载FeNi催化剂的乙烷和二氧化碳的转化率与转换频率（TOF）以及一氧化碳选择性和产率都呈现先增大后减小的趋势，与载体的理论有效表面积（TESA）的变化趋势相同。其中，Al含量为50%的FeNi/Ce-Al_0.5催化剂在873 K下具有最好的乙烷干重整反应性能。结合原位傅里叶变换红外光谱（FTIR）分析观察到，Al的引入不仅增加了表面Ce³⁺和氧空位的含量，同时也促进了表面活性组分的分散，提升了负载FeNi催化剂的乙烷干重整性能。

关键词：乙烷干重整金属-载体强相互作用二氧化碳氧化铈氧空位反应机理