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配位不饱和Au-O-Ti³⁺活性位点的构建及其在低温丙烯气相环氧化反应中强化氢气效率的研究 Article

宋钊宁, 闫昊, 袁俊聪, 马宏飞, 曹建琳, 王永祥, 王强, 彭冲, 邓风, 冯翔, 陈德, 杨朝合, 胡永康

《工程（英文）》 2023年第25卷第6期页码 144-156 doi: 10.1016/j.eng.2023.01.008

摘要：

自1998年以来，人们广泛认为Au/Ti基催化剂的Au-O-Ti⁴⁺位点是在相对高温条件下丙烯气相环氧化反应的活性位点，但该类催化剂的H2sub>有效利用率普遍较低值得注意的是，该活性位点主导反应时，最佳温度可从200 °C显著降低至138 °C，并使催化剂保持前所未有的43.6%的H2sub>有效利用率、90.7%的环氧丙烷（PO）选择性和超过100 h的稳定性。Ti³⁺位点促进了Au和Ti³⁺之间的电子转移，从而增强了催化剂对O2sub>的吸附能力，有效促进H2sub>O2sub本工作所报道的结果为强化丙烯直接气相环氧化反应的H2sub>有效利用率提供了新的思路，而且为低温下丙烯直接气相环氧化反应的工业化推进开辟了新的机会。

关键词：丙烯环氧化 H2sub>有效利用率 Au/Ti双功能催化剂配位不饱和Ti位点密度泛函理论

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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：

固体氧化物电解池（SOEC）作为一种新的能源利用方式，可以将电能转化为化学能，具有高效、洁净、环保等优点。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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Nickel(II) ion-intercalated MXene membranes for enhanced H2sub>/CO2sub> separation

Yiyi Fan, Jinyong Li, Saidi Wang, Xiuxia Meng, Yun Jin, Naitao Yang, Bo Meng, Jiaquan Li, Shaomin Liu

《化学科学与工程前沿（英文）》 2021年第15卷第4期页码 882-891 doi: 10.1007/s11705-020-1990-1

摘要： Hydrogen fuel has been embraced as a potential long-term solution to the growing demand for clean energy. A membrane-assisted separation is promising in producing high-purity H . Molecular sieving membranes (MSMs) are endowed with high gas selectivity and permeability because their well-defined micropores can facilitate molecular exclusion, diffusion, and adsorption. In this work, MXene nanosheets intercalated with Ni were assembled to form an MSM supported on Al O hollow fiber via a vacuum-assisted filtration and drying process. The prepared membranes showed excellent H /CO mixture separation performance at room temperature. Separation factor reached 615 with a hydrogen permeance of 8.35 × 10 mol·m ·s ·Pa . Compared with the original Ti C T /Al O hollow fiber membranes, the permeation of hydrogen through the Ni -Ti C T /Al O membrane was considerably increased, stemming from the strong interaction between the negatively charged MXene nanosheets and Ni . The interlayer spacing of MSMs was tuned by Ni . During 200-hour testing, the resultant membrane maintained an excellent gas separation without any substantial performance decline. Our results indicate that the Ni tailored Ti C T /Al O hollow fiber membranes can inspire promising industrial applications.

关键词： MXene H₂/CO₂ separation nickel ions hollow fiber

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NOxsub> and H2sub>S formation in the reductive zone of air-staged combustion of

Jinzhi CAI, Dan LI, Denggao CHEN, Zhenshan LI

《能源前沿（英文）》 2021年第15卷第1期页码 4-13 doi: 10.1007/s11708-020-0804-y

摘要： Low NO combustion of blended coals is widely used in coal-fired boilers in China to control NO emission; thus, it is necessary to understand the formation mechanism of NO and H S during the combustion of blended coals. This paper focused on the investigation of reductive gases in the formation of NO and H S in the reductive zone of blended coals during combustion. Experiments with Zhundong (ZD) and Commercial (GE) coal and their blends with different mixing ratios were conducted in a drop tube furnace at 1200°C–1400°C with an excessive air ratio of 0.6–1.2. The coal conversion and formation characteristics of CO, H S, and NO in the fuel-rich zone were carefully studied under different experimental conditions for different blend ratios. Blending ZD into GE was found to increase not only the coal conversion but also the concentrations of CO and H S as NO reduction accelerated. Both the CO and H S concentrations inblended coal combustion increase with an increase in the combustion temperature and a decrease in the excessive air ratio. Based on accumulated experimental data, one interesting finding was that NO and H S from blended coal combustion were almost directly dependent on the CO concentration, and the CO concentration of the blended coal combustion depended on the single char gasification conversion.Thus, CO, NO , and H S formation characteristics from blended coal combustion can be well predicted by single char gasification kinetics.

关键词： blended coal combustion NO_xformation H₂S formation air staged combustion

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growth of a-few-layered MoS on CdS nanorod for high efficient photocatalytic H production

《能源前沿（英文）》 2021年第15卷第3期页码 752-759 doi: 10.1007/s11708-021-0779-3

摘要： An ultrathin MoS₂ was grown on CdS nanorod by a solid state method using sulfur powder as sulfur source for photocatalytic H₂ production. The characterization result reveals that the ultrathin MoS₂ nanosheets loaded on CdS has a good contact state. The photoelectrochemical result shows that MoS₂ not only are beneficial for charge separation, but also works as active sites, thus enhancing photocatalytic activity. Compared with pure CdS, the photocatalytic activity of MoS₂ loaded CdS was significantly improved. The hydrogen evolution rate on m(MoS₂): m(CdS) = 1: 50 (m is mass) reaches 542 μmol/h, which is 6 times of that on pure CdS (92 μmol/h). This work provides a new design for photocatalysts with high photocatalytic activities and provides a deeper understanding of the effect of MoS₂ on enhancing photocatalytic activity.

关键词： photocatalytic H₂ production CdS MoS₂ cocatalyst charge separation

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H2sub> 对Pt-Ba-Ce /γ-Al2sub>O3sub> 催化剂NOxsub> 存储和还原机理的影响研究 Article

王攀, 裔静, 孙川, 罗鹏, 雷利利

《工程（英文）》 2019年第5卷第3期页码 568-575 doi: 10.1016/j.eng.2019.02.005

摘要：

本研究采用浸渍法制备了Pt-Ba-Ce/γ-Al2sub>O3sub>催化剂，利用实验评价了H2sub> 对NSR（NOxsub> storage and reduction）催化剂存储和还原机理的影响，并采用综合表征技术研究了Pt-Ba-Ce /γ-Al2sub>O3sub结果表明，透射电子显微镜（TEM）显示X 射线衍射（XRD）光谱中观察到的PtOxsub>、CeO2sub> 和BaCO3sub> 峰很好地分散在在NOxsub> 吸附和脱附循环实验中，随着H2sub>暴露时间（30 s、45 s 和60 s）延长，NOxsub> 的存储效率和转化率增加适当增加H2sub>量加速了硝酸盐或亚硝酸盐的分解，有利于NOxsub> 存储-还原，并促进了下一循环NSR吸附位点的再生。

关键词： Pt–Ba–Ce/γ-Al2sub>O3sub> 催化剂，物理化学性质，NOxsub>存储和还原，NOxsub> 排放，H2sub> 还原剂

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grown TiN/N-TiO composite for enhanced photocatalytic H evolution activity

《能源前沿（英文）》 2021年第15卷第3期页码 721-731 doi: 10.1007/s11708-021-0766-8

摘要： Titanium nitride (TiN) decorated N-doped titania (N-TiO₂) composite (TiN/N-TiO₂) is fabricated via an in situ nitridation using a hydrothermally synthesized TiO₂ and melamine (MA) as raw materials. After the optimization of the reaction condition, the resultant TiN/N-TiO₂ composite delivers a hydrogen evolution activity of up to 703 μmol/h under the full spectrum irradiation of Xe-lamp, which is approximately 2.6 and 32.0 times more than that of TiO₂ and TiN alone, respectively. To explore the underlying photocatalytic mechanism, the crystal phase, morphology, light absorption, energy band structure, element composition, and electrochemical behavior of the composite material are characterized and analyzed. The results indicate that the superior activity is mainly caused by the in situ formation of plasmonic TiN and N-TiO₂ with intimate interface contact, which not only extends the spectral response range, but also accelerates the transfer and separation of the photoexcited hot charge carrier of TiN. The present study provides a fascinating approach to in situ forming nonmetallic plasmonic material/N-doped TiO₂ composite photocatalysts for high-efficiency water splitting.

关键词： photocatalytic H₂ evolution TiN/N-TiO₂ composite plasmonic effect in-situ nitridation

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催化氧化净化黄磷尾气中的磷和硫

宁平,Hans-JörgBart,王学谦,马丽萍,陈梁

《中国工程科学》 2005年第7卷第6期页码 27-35

摘要：

利用黄磷尾气生产甲酸、乙酸以及甲醇等高附加值产品，净化预处理成为制药其应用的瓶颈问题。研究了用普通活性炭和自制催化剂KU2催化氧化净化黄磷尾气的方法；讨论了固定床系统中常压下、温度20～140℃，催化剂上磷和硫化氢的吸附特征。KU2和活性炭都能通过催化氧化过程有效脱除黄磷尾气中的P4sub>，PH3sub>和H2sub>S杂质，随着反应温度和氧含量增加可显著提高净化效果，在最优条件下

关键词：催化剂催化氧化 H2sub>S P4sub> PH3sub> 固定床

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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

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Photoelectrocatalytic generation of H and S from toxic HS by using a novel BiOI/WO nanoflake array photoanode

《能源前沿（英文）》 2021年第15卷第3期页码 744-751 doi: 10.1007/s11708-021-0775-7

摘要： In this paper, a photoelectrocatalytic (PEC) recovery of toxic H₂S into H₂ and S system was proposed using a novel bismuth oxyiodide (BiOI)/ tungsten trioxide (WO₃) nano-flake arrays (NFA) photoanode. The BiOI/WO₃ NFA with a vertically aligned nanostructure were uniformly prepared on the conductive substrate via transformation of tungstate following an impregnating hydroxylation of BiI₃. Compared to pure WO₃ NFA, the BiOI/WO₃ NFA promotes a significant increase of photocurrent by 200%. Owing to the excellent stability and photoactivity of the BiOI/WO₃ NFA photoanode and I^–/

I 3 −

catalytic system, the PEC system toward splitting of H₂S totally converted S^2– into S without any polysulfide (

S x n −

) under solar-light irradiation. Moreover, H₂ was simultaneously generated at a rate of about 0.867 mL/(h·cm). The proposed PEC H₂S splitting system provides an efficient and sustainable route to recover H₂ and S.

关键词： bismuth oxyiodide (BiOI)/ tungsten trioxide (WO₃) nano-flake arrays (NFA) photoelectrocatalytic (PEC) H₂S splitting H₂ S

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天然气提质过程中可有效回收丙烷和乙烷的高工业应用潜力金属有机框架材料 Article

咸士凯, 彭俊杰, Haardik Pandey, Timo Thonhauser, 王浩, 李静

《工程（英文）》 2023年第23卷第4期页码 56-63 doi: 10.1016/j.eng.2022.07.017

摘要：

开发具有高吸收和选择性的高效吸附剂用于从天然气中分离和回收C2sub>H6sub>和C3sub>H8sub>是一项重要但具有挑战性的任务。此外，MOF-303 也显示出很高的C2H6吸收能力（在10 kPa 时）和C2sub>H6sub>/CH4 sub>(10:85, V/sub>3sub>H8sub>和C2sub>H6sub>的亲和力，从而产生了对C3sub>H8sub>和C2sub>H6sub>的高负载能力和选择性。其优异的分离性能、高稳定性、低成本和良好的可扩展性，是天然气净化和回收C2sub>H6sub>和C3sub>H8sub>的理想吸附剂。

关键词：金属-有机框架，烃类吸附和分离，选择性，稳定性，放大合成

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Events and reaction mechanisms during the synthesis of an Al

ZAKERI, H. BAHMANPOUR

《化学科学与工程前沿（英文）》 2013年第7卷第2期页码 123-129 doi: 10.1007/s11705-013-1325-6

摘要： An Al O -TiB nanocomposite was successfully synthesized by the high energy ball milling of Al, B O and TiO . The structures of the powdered particles formed at different milling times were evaluated by X-ray diffraction (XRD), scanning electron microscopy (SEM) and transmission electron microscopy (TEM). Thermodynamic calculations showed that the composite formed in two steps via highly exothermic mechanically induced self-sustaining reactions (MSRs). The composite started to form at milling times of 9–10 h but the reaction was not complete. The remaining starting materials were consumed by increasing the milling time to 15 h. The XRD patterns of the annealed powders showed that aluminum borate is one of the intermediate products and that it is consumed at higher temperatures. Heat treatment of the 6-h milled sample at 1100 C led to a complete formation of the composite. Increasing the milling time to 15 h led to a refining of the crystallite sizes. A nanocomposite powder with a mean crystallite size of 35–40 nm was obtained after milling for 15 h.

关键词： ball milling nanocomposite Al₂O₃ TiB₂

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地热能储存与CO2sub>封存和利用的一体化框架 Article

刘月亮, 胡婷, 芮振华, 张政, 都凯, 杨涛, Birol Dindoruk, Erling Halfdan Stenby, Farshid Torabi, Andrey Afanasyevc

《工程（英文）》 2023年第30卷第11期页码 121-130 doi: 10.1016/j.eng.2022.12.010

摘要：此外，利用CO2sub>羽流进行地热储能可通过将CO2sub>储存于地质体中来缓解温室效应。本文提出了一个协同地热能储能和二氧化碳封存利用的一体化框架：CO2sub>首先被注入到地热层以进行能量积累。然后，将产生的高能CO2sub>引入到目标油藏中，用于CO2sub>利用和地热能储存。最后，将CO2sub>有效地封存在地质油藏体中。结果表明，随着高能CO2sub>的注入，整个目标油藏的平均温度大幅度提高。在地热能的协助下，CO2sub>的地质利用率更高，从而使驱油效率提高了10.1%。根据对模拟CO2sub>场地的封存潜力的评估，CO2sub>注入110年后，地质体的利用率将高达91.2%，场地内CO2sub>的最终注入量将高达9.529

关键词：地热能储存 CO2sub>封存碳中和大规模 CO2sub>利用

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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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encapsulating M(Co, Fe)-Ni alloy for electrochemical production of syngas with potential-independent CO/H

《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