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Ni/MgO catalyst prepared via dielectric-barrier discharge plasma with improved catalytic performance

Yan LI,Zhehao WEI,Yong WANG

《化学科学与工程前沿（英文）》 2014年第8卷第2期页码 133-140 doi: 10.1007/s11705-014-1422-1

摘要： A Ni/MgO catalyst was prepared via novel dielectric-barrier discharge (DBD) plasma decomposition method. The combined characterization of Brunauer-Emmett-Teller measurement, X-ray diffraction, hydrogen temperature-programmed reduction and transmission electron microscopy shows that DBD plasma treatment enhances the support-metal interaction of Ni/MgO catalyst and facilitates the formation of smaller Ni particles. Sphere-like Ni particles form on plasma treated Ni/MgO catalysts. The plasma treated Ni/MgO catalyst shows a significantly improved low temperature activity and good stability for CO reforming of methane to syngas.

关键词： CO₂ reforming methane dielectric-barrier discharge (DBD) plasma Ni/MgO

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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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A density functional theory study of methane activation on MgO supported NiM cluster: role of M on C–H

《化学科学与工程前沿（英文）》 2022年第16卷第10期页码 1485-1492 doi: 10.1007/s11705-022-2169-8

摘要： Methane activation is a pivotal step in the application of natural gas converting into high-value added chemicals via methane steam/dry reforming reactions. Ni element was found to be the most widely used catalyst. In present work, methane activation on MgO supported Ni–M (M = Fe, Co, Cu, Pd, Pt) cluster was explored through detailed density functional theory calculations, compared to pure Ni cluster. CH₄ adsorption on Cu promoted Ni cluster requires overcoming an energy of 0.07 eV, indicating that it is slightly endothermic and unfavored to occur, while the adsorption energies of other promoters M (M = Fe, Co, Pd and Pt) are all higher than that of pure Ni cluster. The role of M on the first C–H bond cleavage of CH₄ was investigated. Doping elements of the same period in Ni cluster, such as Fe, Co and Cu, for C–H bond activation follows the trend of the decrease of metal atom radius. As a result, Ni–Fe shows the best ability for C–H bond cleavage. In addition, doping the elements of the same family, like Pd and Pt, for CH₄ activation is according to the increase of metal atom radius. Consequently, C–H bond activation demands a lower energy barrier on Ni–Pt cluster. To illustrate the adsorptive dissociation behaviors of CH₄ at different Ni–M clusters, the Mulliken atomic charge was analyzed. In general, the electron gain of CH₄ binding at different Ni–M clusters follows the sequence of Ni–Cu (–0.02 e) < Ni (–0.04 e) < Ni–Pd (–0.08 e) < Ni–Pt (–0.09 e) < Ni–Co (–0.10 e) < Ni–Fe (–0.12 e), and the binding strength between catalysts and CH ₄ raises with the CH₄ electron gain increasing. This work provides insights into understanding the role of promoter metal M on thermal-catalytic activation of CH₄ over Ni/MgO catalysts, and is useful to interpret the reaction at an atomic scale.

关键词： CH₄ dissociation Ni–M C–H bond activation charge transfer

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Development of solid base catalyst X/Y/MgO/-AlO for optimization of preparation of biodiesel from L.seed

WANG Rui, YANG Song, YIN Shitao, SONG Baoan, BHADURY Pinaki S., XUE Wei, TAO Shuwei, JIA Zhaohui, LIU Da, GAO Liang

《化学科学与工程前沿（英文）》 2008年第2卷第4期页码 468-472 doi: 10.1007/s11705-008-0074-4

摘要： The preparation and regeneration conditions of the identified catalyst X/Y/MgO/-AlO with high catalytic activity were studied and optimized. The biodiesel was prepared by transesterification of seed oil produced in Guizhou with methanol at its reflux temoerature in the presence of X/Y/MgO/-AlO The pilot plant tests were carried out in a 100 L reaction vessel. Both average yield and fatty acid methyl esters (FAME) content reached more than 96.50% under the optimum reaction conditions of the pilot plant tests designed with an oil/methanol molar ratio of 1 : 10, catalyst concentration of 1.00%, and reaction time of 3 h at reflux temperature. In addition, analysis shows that the quality of biodiesel meets the standard EN 14214.

关键词： temperature presence addition catalytic activity catalyst X/Y/MgO/-AlO

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Al₂O₃ and CeO₂-promoted MgO sorbents for CO₂ capture at moderate

Huimei Yu, Xiaoxing Wang, Zhu Shu, Mamoru Fujii, Chunshan Song

《化学科学与工程前沿（英文）》 2018年第12卷第1期页码 83-93 doi: 10.1007/s11705-017-1691-6

摘要： A series of Al O and CeO modified MgO sorbents was prepared and studied for CO sorption at moderate temperatures. The CO sorption capacity of MgO was enhanced with the addition of either Al O or CeO . Over Al O -MgO sorbents, the best capacity of 24.6 mg-CO /g-sorbent was attained at 100 °C, which was 61% higher than that of MgO (15.3 mg-CO /g-sorbent). The highest capacity of 35.3 mg-CO /g-sorbent was obtained over the CeO -MgO sorbents at the optimal temperature of 200 °C. Combining with the characterization results, we conclude that the promotion effect on CO sorption with the addition of Al O and CeO can be attributed to the increased surface area with reduced MgO crystallite size. Moreover, the addition of CeO increased the basicity of MgO phase, resulting in more increase in the CO capacity than Al O promoter. Both the Al O -MgO and CeO -MgO sorbents exhibited better cyclic stability than MgO over the course of fifteen CO sorption-desorption cycles. Compared to Al O , CeO is more effective for promoting the CO capacity of MgO. To enhance the CO capacity of MgO sorbent, increasing the basicity is more effective than the increase in the surface area.

关键词： CO₂ capture MgO sorbents Al₂O₃ CeO₂ flue gas

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Efficient MgO-doped CaO sorbent pellets for high temperature CO

Zhihong Xu, Tao Jiang, Hao Zhang, Yujun Zhao, Xinbin Ma, Shengping Wang

《化学科学与工程前沿（英文）》 2021年第15卷第3期页码 698-708 doi: 10.1007/s11705-020-1981-2

摘要： Novel MgO-doped CaO sorbent pellets were prepared by gel-casting and wet impregnation. The effect of Na and MgO on the structure and CO adsorption performance of CaO sorbent pellets was elucidated. MgO-doped CaO sorbent pellets with the diameter range of 0.5 1.5 mm exhibited an excellent capacity for CO adsorption and adsorption rate due to the homogeneous dispersion of MgO in the sorbent pellets and its effects on the physical structure of sorbents. The results show that MgO can effectively inhibit the sintering of CaO and retain the adsorption capacity of sorbents during multiple adsorption-desorption cycles. The presence of mesopores and macropores resulted in appreciable change of volume from CaO (16.7 cm ∙mol ) to CaCO (36.9 cm ∙mol ) over repeated operation cycles. Ca2Mg1 sorbent pellets exhibited favorable CO capture capacity (9.49 mmol∙g ), average adsorption rate (0.32 mmol∙g ∙min ) and conversion rate of CaO (74.83%) after 30 cycles.

关键词： MgO doping CaO sorbent pellets gel-casting technique CO₂ capture

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Effects of MgO promoter on properties of Ni/Al2O3 catalysts for partial oxidation of methane to syngas

QIU Yejun, CHEN Jixiang, ZHANG Jiyan

《化学科学与工程前沿（英文）》 2007年第1卷第2期页码 167-171 doi: 10.1007/s11705-007-0031-7

摘要： The effects of MgO promoter on the physico-chemical properties and catalytic performance of Ni/AlO catalysts for the partial oxidation of methane to syngas were studied by means of BET, XRD, H-TPR, TEM and performance evaluation. It was found that the MgO promoter benefited from the uniformity of nickel species in the catalysts, inhibited the formation of NiAlO spinel and improved the interaction between nickel species and support. These results were related to the formation of NiO MgO solid solution and MgAlO spinel. Moreover, for the catalysts with a proper amount of MgO promoter, the nickel dispersiveness was enhanced, therefore making their catalytic performance in methane partial oxidation improved. However, the excessive MgO promoter exerted a negative effect on the catalytic performance. Meanwhile, the basicity of MgO promoted the reversed water gas shift reaction, which led to an increase in CO selectivity and a decrease in H2 selectivity. The suitable content of MgO promoter in Ni/AlO catalyst was ?7 wt-%.

关键词： excessive selectivity decrease dispersiveness physico-chemical