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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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Formation of CaCO hollow microspheres in carbonated distiller waste from Solvay soda ash plants

《化学科学与工程前沿（英文）》页码 1659-1671 doi: 10.1007/s11705-022-2173-z

摘要： For decades, distiller waste and CO₂ were not the first choice for production of high valued products. Here, CaCO₃ hollow microspheres, a high-value product was synthesized from such a reaction system. The synthetic methods, the formation mechanism and operational cost were discussed. When 2.5 L·min^–1·L^–1 CO₂ was flowed into distiller waste (pH = 11.4), spheres with 4–13 μm diameters and about 2 μm shell thickness were obtained. It is found that there is a transformation of CaCO₃ particles from solid-cubic nuclei to hollow spheres. Firstly, the Ca(OH)₂ in the distiller waste stimulated the nucleation of calcite with a non-template effect and further maintained the calcite form and prevented the formation of vaterite. Therefore, in absence of auxiliaries, the formation of hollow structures mainly depended on the growth and aging of CaCO₃. Studies on the crystal morphology and its changes during the growth process point to the inside–out Ostwald effect in the formation of hollow spheres. Change in chemical properties of the bulk solution caused changes in interfacial tension and interfacial energy, which promoted the morphological transformation of CaCO₃ particles from cubic calcite to spherical clusters. Finally, the flow process for absorption of CO₂ by distiller waste was designed and found profitable.

关键词： distiller waste CO₂ hollow microsphere CaCO₃ Ca(OH)₂ inside−out Ostwald effect

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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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An investigation of the CHOH and CO selectivity of CO hydrogenation over Cu–Ce–Zr catalysts

《化学科学与工程前沿（英文）》 2022年第16卷第6期页码 950-962 doi: 10.1007/s11705-022-2162-2

摘要： A series of Cu–Ce–Zr catalysts with different Ce contents are applied to the hydrogenation of CO₂ to CO/CH₃OH products. The Cu–Ce–Zr catalyst with 2 wt% Ce loading shows higher CO selectivity (S_CO = 0.0%–87.8%) from 200–300 °C, while the Cu–Ce–Zr catalyst with 8 wt% Ce loading presents higher CO₂ conversion (

X C O 2

= 5.4%–15.6%) and CH₃OH selectivity (

S C H 3 O H

= 97.8%–40.6%). The number of hydroxyl groups and solid solution nature play a significant role in changing the reaction pathway. The solid solution enhances the CO₂ adsorption ability. At the CO₂ adsorption step, a larger number of hydroxyl groups over the Cu–Ce–Zr catalyst with 8 wt% Ce loading leads to the production of H-containing adsorption species. At the CO₂ hydrogenation step, a larger number of hydroxyl groups assists in encouraging the further hydrogenation of intermediate species to CH₃OH and improving the hydrogenation rate. Hence, the Cu–Ce–Zr catalyst with 8 wt% Ce loading favors CH₃OH selectivity and CO₂ activation, while CO is preferred on the Cu–Ce–Zr catalyst with 2 wt% Ce loading, a smaller number of hydroxyl groups and a solid solution nature. Additionally, high-pressure in situ diffuse reflectance infrared Fourier transform spectroscopy shows that CO is produced from formate decomposition and that both monodentate formate and bidentate formate are active intermediate species of CO₂ hydrogenation to CH₃OH.

关键词： CO₂ hydrogenation Cu–Ce–Zr hydroxyls CO/CH₃OH selectivity

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Catalytic hydrolysis of gaseous HCN over Cu–Ni/γ-Al

Linxia Yan, Senlin Tian, Jian Zhou, Xin Yuan

《环境科学与工程前沿（英文）》 2016年第10卷第6期 doi: 10.1007/s11783-016-0872-8

摘要： ? The Cu–Ni/γ-Al O catalyst was prepared to study HCN hydrolysis ? On catalyst calcined at 400°C, the HCN removal efficiency reaches a maximum. ? HCN removal is the highest at 480 min at a H O/HCN volume ratio of 150 ? The presence of CO facilitates HCN hydrolysis and increases NH production. ? O increases the HCN removal and NO production but decreases NH production GRAPHIC ABSTRACT To decompose efficiently hydrogen cyanide (HCN) in exhaust gas, g-Al O -supported bimetallic-based Cu–Ni catalyst was prepared by incipient-wetness impregnation method. The effects of the calcination temperature, H O/HCN volume ratio, reaction temperature, and the presence of CO or O on the HCN removal efficiency on the Cu–Ni/g-Al O catalyst were investigated. To examine further the efficiency of HCN hydrolysis, degradation products were analyzed. The results indicate that the HCN removal efficiency increases and then decreases with increasing calcination temperature and H O/HCN volume ratio. On catalyst calcined at 400°C, the efficiency reaches a maximum close to 99% at 480 min at a H O/HCN volume ratio of 150. The HCN removal efficiency increases with increasing reaction temperature within the range of 100°C–500°C and reaches a maximum at 500°C. This trend may be attributed to the endothermicity of HCN hydrolysis; increasing the temperature favors HCN hydrolysis. However, the removal efficiencies increases very few at 500°C compared with that at 400°C. To conserve energy in industrial operations, 400°C is deemed as the optimal reaction temperature. The presence of CO facilitates HCN hydrolysis andincreases NH production. O substantially increases the HCN removal efficiency and NO production but decreases NH production.

关键词： Hydrogen cyanide Cu–Ni/g-Al₂O₃ Catalytic hydrolysis

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Corrosion behavior of Fe–Cr–Ni based alloys exposed to molten MgCl2sub>–KCl–NaCl salt with over-added

《化学科学与工程前沿（英文）》 2023年第17卷第10期页码 1608-1619 doi: 10.1007/s11705-023-2349-1

摘要： MgCl₂–NaCl–KCl salts mixture shows great potential as a high-temperature (> 700 °C) thermal energy storage material in next-generation concentrated solar power plants. Adding Mg into molten MgCl₂–NaCl–KCl salt as a corrosion inhibitor is one of the most effective and cost-effective methods to mitigate the molten salt corrosion of commercial Fe–Cr–Ni alloys. However, it is found in this work that both stainless steel 310 and Incoloy 800H samples were severely corroded after 500 h immersion test at 700 °C when the alloy samples directly contacted with the over-added Mg in the liquid form. The corrosion attack is different from the classical impurity-driven corrosion in molten chloride salts found in previous work. Microscopic analysis indicates that Ni preferentially leaches out of alloy matrix due to the tendency to form MgNi₂/Mg₂Ni compounds. The Ni-depletion leads to the formation of a porous corrosion layer on both alloys, with the thickness around 204 µm (stainless steel 310) and 1300 µm (Incoloy 800H), respectively. These results suggest that direct contact of liquid Mg with Ni-containing alloys should be avoided during using Mg as a corrosion inhibitor for MgCl₂–NaCl–KCl or other chlorides for high temperature heat storage and transfer.

关键词： concentrated solar power (CSP) Mg corrosion inhibitor Mg–Ni intermetallic salt purification thermal energy storage (TES)

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铝电解用Fe-Ni-Co-Al2sub>O3sub>金属陶瓷惰性阳极

邱竹贤,石忠宁,徐君莉

《中国工程科学》 2004年第6卷第8期页码 35-39

摘要：

研制了一种新型铝电解金属陶瓷惰性阳极，阳极基体由Fe-Ni-CoAl2sub>O3sub>构成。在石墨坩埚中，960℃温度下，电解质中的氧化铝质量分数为6.0%，摩尔比为2.6；阳极电流密度为1.0 A/cm²，阳极尺寸大小为120 mm×80 mm×mm，石墨阴极尺寸大小为120 mm×40 mm×20 mm，通入的直流电为100～300 A，电解时间各为10 h；实验所得的电解铝产品纯度达到98%以上，杂质主要为Fe，Ni阳极的反电动势为2.45 V，比理论分解电压仅高出0.25 V证明该阳极为惰性阳极，在电解槽中进行的是Al2sub>O3sub>的分解反应。

关键词：铝电解惰性阳极反电动势

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Efficient degradation of orange II by ZnMn

Qingzhuo Ni, Hao Cheng, Jianfeng Ma, Yong Kong, Sridhar Komarneni

《化学科学与工程前沿（英文）》 2020年第14卷第6期页码 956-966 doi: 10.1007/s11705-019-1907-z

摘要： A ZnMn O catalyst has been synthesized via a sucrose-aided combustion method and characterized by various analytical techniques. It is composed of numerous nanoparticles (15–110 nm) assembled into a porous structure with a specific surface area (SSA) of 19.1 m ·g . Its catalytic activity has been investigated for the degradation of orange II dye using three different systems, i.e., the photocatalysis system with visible light, the chemocatalysis system with bisulfite, and the photo-chemical catalysis system with both visible light and bisulfite. The last system exhibits the maximum degradation efficiency of 90%, much higher than the photocatalysis system (15%) and the chemocatalysis system (67%). The recycling experiments indicate that the ZnMn O catalyst has high stability and reusability and is thus a green and eximious catalyst. Furthermore, the potential degradation mechanisms applicable to the three systems are discussed with relevant theoretical analysis and scavenging experiments for radicals. The active species such as Mn(III), O , h , e , SO and HO are proposed to be responsible for the excellent degradation results in the photo-chemical catalysis system with the ZnMn O catalyst.

关键词： ZnMn₂O₄ photo-chemical catalysis bisulfite dye degradation

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Ni-Co bimetallic catalyst for CH

Xiaohong LI, Jun AI, Wenying LI, Dongxiong LI

《化学科学与工程前沿（英文）》 2010年第4卷第4期页码 476-480 doi: 10.1007/s11705-010-0512-y

摘要： A co-precipitation method was employed to prepare Ni/Al O -ZrO , Co/Al O -ZrO and Ni-Co/Al O -ZrO catalysts. Their properties were characterized by N adsorption (BET), thermogravimetric analysis TGA , temperature-programmed reduction (TPR), temperature-programmed desorption (CO -TPD), and temperature-programmed surface reaction (CH -TPSR and CO -TPSR). Ni-Co/Al O -ZrO bimetallic catalyst has good performance in the reduction of active components Ni, Co and CO adsorption. Compared with mono-metallic catalyst, bimetallic catalyst could provide more active sites and CO adsorption sites (C+ CO = 2CO) for the methane-reforming reaction, and a more appropriate force formed between active components and composite support (SMSI) for the catalytic reaction. According to the CH -CO -TPSR, there were 80.9% and 81.5% higher CH and CO conversion over Ni-Co/Al O -ZrO catalyst, and its better resistance to carbon deposition, less than 0.5% of coke after 4 h reaction, was found by TGA. The high activity and excellent anti-coking of the Ni-Co/Al O -ZrO catalyst were closely related to the synergy between Ni and Co active metal, the strong metal-support interaction and the use of composite support.

关键词： Ni-Co bimetallic catalyst composite support CH₄ reforming with CO₂

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Laboratory study on high-temperature adsorption of HCl by dry-injection of Ca(OH)

Junjun TAN,Guohua YANG,Jingqiao MAO,Huichao DAI

《环境科学与工程前沿（英文）》 2014年第8卷第6期页码 863-870 doi: 10.1007/s11783-013-0618-9

摘要： Combustion-generated hydrogen chloride (HCl) is considered to be a very hazardous acid gaseous pollutant. This paper presents a laboratory study on the dry adsorption of HCl. The experiments were conducted in a dual-layer granular bed filter, at gas temperatures of 500°C–700°C and (Ca)/ (Cl)molar ratios of 1.0–5.0 using the silver nitrate titration method by dry adsorbent powders Ca(OH) . Mainly, the adsorption efficiency of HCl and utilization efficiency of Calcium were studied, by varying relevant factors including (Ca)/ (Cl), temperature, feeding method, water vapor and CO . With a relatively higher HCl concentration of 1000 ppm, the experimental results revealed that 600°C may be the optimum temperature for HCl adsorption when optimum (Ca)/ (Cl) was 2.5 in our tests. The results also demonstrated that the feeding at a constant pressure was more effective, and the HCl adsorption efficiency could rapidly reach over 90% with (Ca)/ (Cl) = 2.5 at 600°C. Furthermore, the HCl adsorption efficiency was found to be slightly promoted by water vapor, while could be impeded by CO , and the utilization efficiency of calcium could be up to 74.4% without CO , while was only 36.8% with CO when (Ca)/ (Cl) was 2.5 at 600°C.

关键词： acid gas HCl Ca(OH)₂ dry adsorption high temperature dual-layer granular bed filter

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Bamboo-like -doped carbon nanotubes encapsulating M(Co, Fe)-Ni alloy for electrochemical production of

《化学科学与工程前沿（英文）》 2022年第16卷第4期页码 498-510 doi: 10.1007/s11705-021-2082-6

摘要： The electrochemical conversion of CO₂-H₂O into CO-H₂ using renewable energy is a promising technique for clean syngas production. Low-cost electrocatalysts to produce tunable syngas with a potential-independent CO/H₂ ratio are highly desired. Herein, a series of N-doped carbon nanotubes encapsulating binary alloy nanoparticles (M_xNi-NCNT, M= Fe, Co) were successfully fabricated through the co-pyrolysis of melamine and metal precursors. The M_xNi-NCNT samples exhibited bamboo-like nanotubular structures with a large specific surface area and high degree of graphitization. Their electrocatalytic performance for syngas production can be tuned by changing the alloy compositions and modifying the electronic structure of the carbon nanotube through the encapsulated metal nanoparticles. Consequently, syngas with a wide range of CO/H₂ ratios, from 0.5:1 to 3.4:1, can be produced on M_xNi-NCNT. More importantly, stable CO/H₂ ratios of 2:1 and 1.5:1, corresponding to the ratio to produce biofuels by syngas fermentation, could be realized on Co₁Ni-NCNT and Co₂Ni-NCNT, respectively, over a potential window of –0.8 to –1.2 V versus the reversible hydrogen electrode. Our work provides an approach to develop low-cost and potential-independent electrocatalysts to effectively produce syngas with an adjustable CO/H₂ ratio from electrochemical CO₂ reduction.

关键词： electrochemical reduction of CO₂ syngas N-doped carbon nanotubes encapsulated alloy nanoparticles CO/H₂ ratio

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Generation of enhanced stability of SnO/In(OH)/InP for photocatalytic water splitting by SnO protection

《能源前沿（英文）》 2021年第15卷第3期页码 710-720 doi: 10.1007/s11708-021-0764-x

摘要： InP shows a very high efficiency for solar light to electricity conversion in solar cell and may present an expectation property in photocatalytic hydrogen evolution. However, it suffers serious corrosion in water dispersion. In this paper, it is demonstrated that the stability and activity of the InP-based catalyst are effectively enhanced by applying an anti-corrosion SnO layer and In(OH)₃ transition layer, which reduces the crystal mismatch between SnO and InP and increases charge transfer. The obtained Pt/SnO/In(OH)₃/InP exhibits a hydrogen production rate of 144.42 µmol/g in 3 h under visible light illumination in multi-cycle tests without remarkable decay, 123 times higher than that of naked In(OH)₃/InP without any electron donor under visible irradiation.

关键词： SnO/In(OH)₃/InP photocatalyst enhanced activity and stability for water splitting corrosion inhibition enhancing charge transfer and decreasing crystal mismatch

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Design and analysis of dual fuel methanol-power poly-generation

Minghua WANG , Zheng LI , Weidou NI ,

《能源前沿（英文）》 2009年第3卷第3期页码 341-347 doi: 10.1007/s11708-009-0023-z

摘要： A dual fuel head poly-generation flowsheet was designed based on coal gas and coke oven gas. To help clearly understand the system performance, a 1.2×10−3.2×10kg methanol and 274―496MW power poly-generation system was simulated by using the commercially available software ASPEN Plus and GT Pro. The technology scheme, the operating parameters, and the efficiency of the system were also analyzed and evaluated, which will be used for building industrial devices.

关键词： dual fuel methanol-power poly-generation CO₂ and CH₄ reforming splitting ratio

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以NH3sub>OH⁺/NH2sub>NH3sub>⁺作为B位阳离子的无金属六方钙钛矿含能材料 Article

尚宇, 余志鸿, 黄瑞康, 陈劭力, 刘德轩, 陈晓娴, 张伟雄, 陈小明

《工程（英文）》 2020年第6卷第9期页码 1013-1018 doi: 10.1016/j.eng.2020.05.018

摘要：文中通过合理地选择分子组分，经由易于规模放大的简单合成路线，以NH3sub>OH⁺和NH2sub>NH3sub>⁺分别作为B位点阳离子构筑了两例无金属六方钙钛矿含能材料(H2sub>dabco)B(ClO4sub>)3sub>（分别命名为DAP-6和DAP-7，其中H2sub>dabco²⁺是1,4-二氮杂双环[2.2.2]辛烷-1,4-二鎓离子）。与基于NH4sub>⁺阳离子构筑的立方钙钛矿类似物(H2sub>dabco)(NH4sub>)(ClO4sub>)特别地，DAP-7具有超高热稳定性（起始分解温度Tdsub> = 375.3 °C）、高爆速（D = 8.883 km·s^{关键词：

含能材料


单质炸药


固体推进剂


无金属六方钙钛矿


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Synergistic utilization of coal and other energy – Key to low carbon economy

Weidou NI, Zhen CHEN

《能源前沿（英文）》 2011年第5卷第1期页码 1-19 doi: 10.1007/s11708-010-0136-4

摘要： In China, coal is a dominant component of energy mix, and it is expected to remain as such over the next 30 to 40 years. Coal is expected to be used even more in power generation. The direct combustion of coal already has been causing severe pollution and ecological degradation, and it is quite difficult to address the need to reduce greenhouse gas (GHG) given the direct combustion of coal. Therefore, the polygeneration system based on coal gasification, which is one of the major examples of synergistic utilization of coal, is proposed. It is a comprehensive solution to meet the energy challenges China is facing. Furthermore, the synergy of fossil fuels (especially coal) with renewable energy, the synergy of different kinds of energy for energy storage, the synergy of centralized and distributed supply of different kinds of energy, and the synergy of different kinds of energy in smart energy grid (power, gas, heat, and water) are the keys to making China a low-carbon economy. Carbon dioxide (CO ) mitigation in China should begin from the coal-chemical industry given their accumulated relevant experiences. The mitigation process should gradually be transformed into the “IGCC+ polygeneration+ CCUS”. The objectives of this paper are to describe the synergistic utilization of coal, and to analyze the synergy of coal with other energy resources, and to propose the scientific and technological problems to achieve these synergies.

关键词： synergy clean and efficient utilization of coal coal-based polygenration CO₂ mitigation energy storage