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Comparison study on strategies to prepare nanocrystalline Li

Qiang XIAO, Xiaodan TANG, Yefeng LIU, Yijun ZHONG, Weidong ZHU

《化学科学与工程前沿（英文）》 2013年第7卷第3期页码 297-302 doi: 10.1007/s11705-013-1346-1

摘要： A comparison study has been conducted on the strategies for synthesizing nanocrystalline Li ZrO and K-doped Li ZrO absorbents for CO capture at high temperatures, including solid-state and liquid-phase methods, citrate route, and starch-assisted sol-gel method combined with freeze-drying technique. The absorption properties, including uptake rate and absorption capacity, of synthesized absorbents were investigated by thermogravimetric analysis (TGA) at different CO partial pressures. The nanosized Li ZrO crystals synthesized by the citrate route exhibit a faster uptake and a higher, nearly stoichiometric absorption capacity than those synthesized by the solid-state and liquid-phase methods. The doping of K into Li ZrO can significantly improve the uptake rate of CO , especially at low CO partial pressures. For the synthesis of K-doped Li ZrO , the citrate route has poor reproducibility and scalability, whereas the starch-assisted sol-gel method combined with freeze-drying technique is reproducible and easily scaled up, and the thus synthesized absorbents possess excellent CO capture properties.

关键词： CO₂ capture Li₂ZrO₃ K-doped Li₂ZrO₃ citrate starch freeze-drying technique

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Enhanced performance of oxygen vacancies on CO adsorption and activation over different phases of ZrO

《能源前沿（英文）》 2023年第17卷第4期页码 545-554 doi: 10.1007/s11708-023-0867-7

摘要： The effect of oxygen vacancies on the adsorption and activation of CO₂ on the surface of different phases of ZrO₂ is investigated by density functional theory (DFT) calculations. The calculations show that the oxygen vacancies contribute greatly to both the adsorption and activation of CO₂. The adsorption energy of CO₂ on the c-ZrO₂, t-ZrO₂ and, m-ZrO₂ surfaces is enhanced to 5, 4, and 3 folds with the help of oxygen vacancies, respectively. Moreover, the energy barrier of CO₂ dissociation on the defective surfaces of c-ZrO₂, t-ZrO₂, and m-ZrO₂ is reduced to 1/2, 1/4, and 1/5 of the perfect surface with the assistance of oxygen vacancies. Furthermore, the activation of CO₂ on the ZrO₂ surface where oxygen vacancies are present, and changes from an endothermic reaction to an exothermic reaction. This finding demonstrates that the presence of oxygen vacancies promotes the activation of CO₂ both kinetically and thermodynamically. These results could provide guidance for the high-efficient utilization of CO₂ at an atomic scale.

关键词： CO₂ activation oxygen vacancies ZrO₂ different phases

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Preparation of Cu/ZrO

Xinmei LIU, Shaofen BAI, Huidong ZHUANG, Zifeng YAN

《化学科学与工程前沿（英文）》 2012年第6卷第1期页码 47-52 doi: 10.1007/s11705-011-1170-4

摘要： Cu/ZrO catalysts for methanol synthesis from CO /H were respectively prepared by deposition coprecipitation (DP) and solid state reaction (SR) methods. There is an intimate interaction between copper and zirconia, which strongly affects the reduction property and catalytic performance of the catalysts. The stronger the interaction, the lower the reduction temperature and the better the performance of the catalysts. Surface area, pore structure and crystal structure of the catalysts are mainly controlled by preparation methods and alkalinity of synthesis system. The conversion of CO and selectivity of methanol are higher for DP catalysts than for SP catalysts.

关键词： Cu/ZrO₂ methanol synthesis deposition coprecipitation solid state reaction CO₂/H₂

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Stability of Ni/SiO

Bettina Stolze,Juliane Titus,Stephan A. Schunk,Andrian Milanov,Ekkehard Schwab,Roger Gläser

《化学科学与工程前沿（英文）》 2016年第10卷第2期页码 281-293 doi: 10.1007/s11705-016-1568-0

摘要： Ni/SiO -ZrO catalysts with Ni loadings of 1 to 13 wt-% were prepared, characterized by elemental analysis, X-ray diffraction, N sorption, temperature programmed oxidation, temperature programmed reduction, and tested for their activity and stability in the dry reforming of methane with carbon dioxide at 850 °C, gas hourly space velocity of 6000 and 1800 h and atmospheric pressure. The SiO -ZrO support as obtained through a simple and efficient sol-gel synthesis is highly porous ( = 90 m ·g , = 4.4 nm) with a homogeneously distributed Si-content of 3 wt-%. No loss of Si or formation of monoclinic ZrO , even after steaming at 850 °C for 160 h, was detectable. The catalyst with 5 wt-% Ni loading in its fully reduced state is stable over 15?h on-stream in the dry reforming reaction. If the catalyst was not fully reduced, a reduction during the early stages of dry reforming is accompanied by the deposition of up to 44 mg·g carbon as shown by experiments in a magnetic suspension balance. Rapid coking occurs for increased residence times and times-on-stream starting at 50 h. The Ni loading of 5 wt-% on SiO -ZrO was shown to provide an optimal balance between activity and coking tendency.

关键词： Ni/SiO₂-ZrO₂ synthesis gas dry reforming coking steaming

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Rh2sub>O3sub>/hexagonal CePO4sub> nanocatalysts for N2sub>O decomposition

Huan Liu, Zhen Ma

《化学科学与工程前沿（英文）》 2017年第11卷第4期页码 586-593 doi: 10.1007/s11705-017-1659-6

摘要： Hexagonal CePO nanorods were prepared by a precipitation method and hexagonal CePO nanowires were prepared by hydrothermal synthesis at 150 °C. Rh(NO ) was then used as a precursor for the impregnation of Rh O onto these CePO materials. The Rh O supported on the CePO nanowires was much more active for the catalytic decomposition of N O than the Rh O supported on CePO nanorods. The stability of both catalysts as a function of time on stream was studied and the influence of the co-feed (CO , O , H O or O /H O) on the N O decomposition was also investigated. The samples were characterized by N adsorption-desorption, inductively coupled plasma optical emission spectroscopy, X-ray diffraction, transmission electron microscopy, X-ray photoelectron microscopy, hydrogen temperature-programmed reduction, oxygen temperature-programmed desorption, and CO temperature-programmed desorption in order to correlate the physicochemical and catalytic properties.

关键词： Rh₂O₃ CePO₄ N₂O decomposition

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CO2sub> methanation and co-methanation of CO and CO2sub> over Mn-promoted Ni/Al2sub>O3sub> catalysts

Kechao Zhao,Zhenhua Li,Li Bian

《化学科学与工程前沿（英文）》 2016年第10卷第2期页码 273-280 doi: 10.1007/s11705-016-1563-5

摘要： A series of Mn-promoted 15 wt-% Ni/Al O catalysts were prepared by an incipient wetness impregnation method. The effect of the Mn content on the activity of the Ni/Al O catalysts for CO methanation and the co-methanation of CO and CO in a fixed-bed reactor was investigated. The catalysts were characterized by N physisorption, hydrogen temperature-programmed reduction and desorption, carbon dioxide temperature-programmed desorption, X-ray diffraction and high-resolution transmission electron microscopy. The presence of Mn increased the number of CO adsorption sites and inhibited Ni particle agglomeration due to improved Ni dispersion and weakened interactions between the nickel species and the support. The Mn-promoted 15 wt-% Ni/Al O catalysts had improved CO methanation activity especially at low temperatures (250 to 400 °C). The Mn content was varied from 0.86% to 2.54% and the best CO conversion was achieved with the 1.71Mn-Ni/Al O catalyst. The co-methanation tests on the 1.71Mn-Ni/Al O catalyst indicated that adding Mn markedly enhanced the CO methanation activity especially at low temperatures but it had little influence on the CO methanation performance. CO methanation was more sensitive to the reaction temperature and the space velocity than the CO methanation in the co-methanation process.

关键词： Mn promotion nickel catalysts CO₂ methanation co-methanation of CO and CO₂

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以净零排放为目标的封存驱动型CO2sub>提高采收率方法 Article

刘月亮, 芮振华

《工程（英文）》 2022年第18卷第11期页码 79-87 doi: 10.1016/j.eng.2022.02.010

摘要：可通过驱油过程将CO2sub>封存在油藏地质体中，因此，CO2sub>驱油与封存被视为降低CO2sub>排放的重要手段之一。本研究提出了一种新型的CO2sub>提高采收率（EOR）方法，即封存驱动型CO2sub>提高采收率，其主要目标是通过在油藏中封存尽可能多的CO2sub>来实现CO结果表明，DME可提高CO2sub>在原油中的溶解度，有利于CO2sub>的溶解封存；可抑制因CO2sub>的抽提作用造成的原油轻质组分“逃逸&rdquo封存驱动型CO2sub> EOR方法在提高波及效率方面优于传统的CO2sub> EOR，尤其是在采油后期更为明显；同时，封存驱动型CO2sub> EOR比传统的此外，通过封存驱动型CO2sub> EOR封存的CO2sub>量远超采出原油燃烧产生的碳排放总量。

关键词： CO2sub> EOR CO2sub>净排放量二甲醚封存驱动型CO2sub> EOR CO2sub>封存

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Al2sub>O3sub> and CeO2sub>-promoted MgO sorbents for CO2sub> 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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ZnFe2sub>O4sub> deposited on BiOCl with exposed (001) and (010) facets for photocatalyticreduction of CO2sub> in cyclohexanol

Guixian Song, Xionggang Wu, Feng Xin, Xiaohong Yin

《化学科学与工程前沿（英文）》 2017年第11卷第2期页码 197-204 doi: 10.1007/s11705-016-1606-y

摘要： ZnFe O -BiOCl composites were prepared by both hydrothermal and direct precipitation processes and the structures and properties of the samples were characterized by various instrumental techniques. The samples were then used as catalysts for the photocatalytic reduction of CO in cyclohexanol under ultraviolet irradiation to give cyclohexanone (CH) and cyclohexyl formate (CF). The photocatalytic CO reduction activities over the hydrothermally prepared ZnFe O -BiOCl composites were higher than those over the directly-precipitated composites. This is because compared to the direct-precipitation sample, the ZnFe O nanoparticles in the hydrothermal sample were smaller and more uniformly distributed on the surface of BiOCl and so more heterojunctions were formed. Higher CF and CH yields were obtained for the pure BiOCl and BiOCl composite samples with more exposed (001) facets than for the samples with more exposed (010) facets. This is due to the higher density of oxygen atoms in the exposed (001) facets, which creates more oxygen vacancies, and thereby improves the separation efficiency of the electron-hole pairs. More importantly, irradiation of the (001) facets with ultraviolet light produces photo-generated electrons which is helpful for the reduction of CO to ·CO . The mechanism for the photocatalytic reduction of CO in cyclohexanol over ZnFe O -BiOCl composites with exposed (001) facets involves electron transfer and carbon radical formation.

关键词： reduction of CO₂ cyclohexanol ZnFe₂O₄ deposited BiOCl facet composite photocatalyst

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The stabilization effect of Al2sub>O3sub> on unconventional Pb/SiO2sub> catalyst

《化学科学与工程前沿（英文）》 2023年第17卷第10期页码 1423-1429 doi: 10.1007/s11705-023-2315-y

摘要： Similar to Sn, Pb located at the same group (IVA) in the periodic table of elements, can also catalyze propane dehydrogenation to propene, while a fast deactivation can be observed. To enhance the stability, the traditional carrier Al₂O₃ with a small amount, was introduced into Pb/SiO₂ catalyst in this study. It has been proved that Al₂O₃ can inhibit the reduction of PbO, and weaken the agglomeration and loss of Pb species due to its enhanced interaction with Pb species. As a result, 3Al15Pb/SiO₂ catalyst exhibits a much higher stability up to more than 150 h. In addition, a simple schematic diagram of the change of surface species on the catalyst surface after Al₂O₃ addition was also proposed.

关键词： Pb/SiO₂ Al₂O₃ propane dehydrogenation propene stability

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Cu-doped Bi/Bi2sub>WO6sub> catalysts for efficient N2sub> fixation by photocatalysis

《化学科学与工程前沿（英文）》 2023年第17卷第10期页码 1412-1422 doi: 10.1007/s11705-023-2312-1

摘要： In this paper, Cu-doped Bi₂WO₆ was synthesized via a solvothermal method and applied it in photocatalytic N₂ immobilization. Characterization results showed the presence of a small amount of metallic Bi in the photocatalyst, indicating that the synthesized photocatalyst is actually Bi/Cu-Bi₂WO₆ composite. The doped Cu had a valence state of +2 and most likely substituted the position of Bi³⁺. The introduced Cu did not affect the metallic Bi content, but mainly influenced the energy band structure of Bi₂WO₆. The band gap was slightly narrowed, the conduction band was elevated, and the work function was reduced. The reduced work function improved the transfer and separation of charge carriers, which mainly caused the increased photoactivity. The optimized NH₃ generation rates of Bi/Cu-Bi₂WO₆ reached 624 and 243 μmol·L^–1·g^–1·h^–1 under simulated solar and visible light, and these values were approximately 2.8 and 5.9 times higher those of Bi/Bi₂WO₆, respectively. This research provides a method for improving the photocatalytic N₂ fixation and may provide more information on the design and preparation of heteroatom-doped semiconductor photocatalysts for N₂-to-NH₃ conversion.

关键词： Bi₂WO₆ Cu doping work function photocatalytic N₂ fixation charge separation

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固体氧化物电解池共电解H2sub>O/CO2sub>研究进展

范慧,宋世栋,韩敏芳

《中国工程科学》 2013年第15卷第2期页码 107-112

摘要：本文介绍了固体氧化物电解池的结构特点及其用于H2O/CO2的共电解制备H2和CO的工作原理，综述了固体氧化物电解池的组成形式，以及单片电解池和电解池堆用于H2O/CO2共电解反应的国内外研究进展，并阐述了提高固体氧化物电解池共电解效率所亟需解决的问题

关键词：固体氧化物电解池 H2sub>O/CO2sub>共电解合成气电解效率水电解

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含稀释剂的Al-Cr2sub>O3sub>体系燃烧合成反应热力学分析与反应模型

张衍诚,潘冶,张传

《中国工程科学》 2004年第6卷第6期页码 63-67

摘要：

对含稀释剂Al203和Cr203的Al-Cr203体系燃烧合成反应进行了热力学计算与分析，讨论了起始反应温度T0、稀释剂Al2O3和Cr2O3的含量对绝热反应温度7^的影响，并得出T0与Tad在特定温度段上的近似线性关系以及该关系在指导材料成分设计上的应用；揭示了反应驱动力—&mdash

关键词：金属陶瓷燃烧合成 Al-Cr203体系热力学反应模型

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Interfacial charge transfer and photocatalytic activity in a reverse designed BiO/TiO core-shell

《能源前沿（英文）》 2021年第15卷第3期页码 732-743 doi: 10.1007/s11708-021-0772-x

摘要： In this study, the electronic and photocatalytic properties of core-shell heterojunctions photocatalysts with reversible configuration of TiO₂ and Bi₂O₃ layers were studied. The core-shell nanostructure, obtained by efficient control of the sol-gel polymerization and impregnation method of variable precursors of semiconductors, makes it possible to study selectively the role of the interfacial charge transfer in each configuration. The morphological, optical, and chemical composition of the core-shell nanostructures were characterized by high-resolution transmission electron microscopy, UV-visible spectroscopy and X-ray photoelectron spectroscopy. The results show the formation of homogenous TiO₂ anatase and Bi₂O₃ layers with a thickness of around 10 and 8 nm, respectively. The interfacial charge carrier dynamic was tracked using time resolved microwave conductivity and transition photocurrent density. The charge transfer, their density, and lifetime were found to rely on the layout layers in the core-shell nanostructure. In optimal core-shell design, Bi₂O₃ collects holes from TiO₂, leaving electrons free to react and increase by 5 times the photocatalytic efficiency toward H₂ generation. This study provides new insight into the importance of the design and elaboration of optimal heterojunction based on the photocatalyst system to improve the photocatalytic activity.

关键词： photocatalysis core-shell heterojunction H₂ TiO₂ Bi₂O₃