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Bamboo-like -doped carbon nanotubes encapsulating M(Co, Fe)-Ni alloy for electrochemical production ofsyngas with potential-independent CO/H ratios

《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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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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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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山西沁水盆地柿庄北区块3#煤层注入埋藏CO2sub>提高煤层气采收率试验和评价

叶建平,张兵,Sam Wong

《中国工程科学》 2012年第14卷第2期页码 38-44

摘要：

对沁水盆地南部柿庄北区块进行了深煤层注入地质和工程评价，认为柿庄北区块适合进行深煤层注入CO2开采煤层气技术的应用；通过SX-001井的微型先导性试验通过现场试验，注入CO2后SX-001井的产气量是注入前的2.45倍；在小于煤岩破裂压力的条件下，每天注入20 t的CO2能够实现顺利注入，并且压力上升速度较慢；注入CO2后，煤岩发生膨胀，局部煤层的渗透率降低，排采一段时间后恢复；在目的煤层中注入的CO2的影响范围内，烃类气体总的置换效率达到14.18 cm3/g。该试验成果证明柿庄北区块通过注入CO2开采煤层气实现了CO2的埋藏，提高了煤层气井的采收率。

关键词：山西沁水盆地注入CO2sub> 煤层气采收率

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Impacts of CO2 and H2S on the risk of hydrate formation during pipeline transport of natural gas

Solomon A. Aromada, Bjørn Kvamme

《化学科学与工程前沿（英文）》 2019年第13卷第3期页码 616-627 doi: 10.1007/s11705-019-1795-2

摘要： Evaluation of maximum content of water in natural gas before water condenses out at a given temperature and pressure is the initial step in hydrate risk analysis during pipeline transport of natural gas. The impacts of CO and H S in natural gas on the maximum mole-fractions of water that can be tolerated during pipeline transport without the risk of hydrate nucleation has been studied using our novel thermodynamic scheme. Troll gas from the North Sea is used as a reference case, it contains very negligible amount of CO and no H S. Varying mole-fractions of CO and H S were introduced into the Troll gas, and the effects these inorganic impurities on the water tolerance of the system were evaluated. It is observed that CO does not cause any distinguishable impact on water tolerance of the system, but H S does. Water tolerance decreases with increase in concentration of H S. The impact of ethane on the system was also investigated. The maximum mole-fraction of water permitted in the gas to ensure prevention of hydrate formation also decreases with increase in the concentration of C H like H S. H S has the most impact, it tolerates the least amount of water among the components studied.

关键词： hydrate hydrogen Sulphide CO₂ dew point pipeline

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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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VALORIZATION OF BIOGAS THROUGH SIMULTANEOUS CO AND HS REMOVAL BY RENEWABLE AQUEOUS AMMONIA SOLUTION IN

《农业科学与工程前沿（英文）》 2023年第10卷第3期页码 468-478 doi: 10.15302/J-FASE-2022473

摘要：

● Simultaneous H₂S and CO₂ removal from biogas is studied.

关键词： biomethane biogas purification CO₂ removal H₂S removal membrane absorption

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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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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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Co anchored on porphyrinic triazine-based frameworks with excellent biocompatibility for conversion ofCO in H-mediated microbial electrosynthesis

《化学科学与工程前沿（英文）》 2022年第16卷第12期页码 1761-1771 doi: 10.1007/s11705-022-2195-6

摘要： Microbial electrosynthesis is a promising alternative to directly convert CO₂ into long-chain compounds by coupling inorganic electrocatalysis with biosynthetic systems. However, problems arose that the conventional electrocatalysts for hydrogen evolution may produce extensive by-products of reactive oxygen species and cause severe metal leaching, both of which induce strong toxicity toward microorganisms. Moreover, poor stability of electrocatalysts cannot be qualified for long-term operation. These problems may result in poor biocompatibility between electrocatalysts and microorganisms. To solve the bottleneck problem, Co anchored on porphyrinic triazine-based frameworks was synthesized as the electrocatalyst for hydrogen evolution and further coupled with Cupriavidus necator H16. It showed high selectivity for a four-electron pathway of oxygen reduction reaction and low production of reactive oxygen species, owing to the synergistic effect of Co–N_x modulating the charge distribution and adsorption energy of intermediates. Additionally, low metal leaching and excellent stability were observed, which may be attributed to low content of Co and the stabilizing effect of metalloporphyrins. Hence, the electrocatalyst exhibited excellent biocompatibility. Finally, the microbial electrosynthesis system equipped with the electrocatalyst successfully converted CO₂ to poly-β-hydroxybutyrate. This work drew up a novel strategy for enhancing the biocompatibility of electrocatalysts in microbial electrosynthesis system.

关键词： microbial electrosynthesis hydrogen evolution reaction metalloporphyrins biocompatibility CO₂ conversion

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Frontier science and challenges on offshore carbon storage

《环境科学与工程前沿（英文）》 2023年第17卷第7期 doi: 10.1007/s11783-023-1680-6

摘要：

● The main direct seal up carbon options and challenges are reviewed.

关键词： Offshore carbon storage Direct CO₂ injection CO₂-CH₄ replacement CO₂-EOR CCS hubs CO₂ transport

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Reduction potential of the energy penalty for CO capture in CCS

《能源前沿（英文）》 2023年第17卷第3期页码 390-399 doi: 10.1007/s11708-023-0864-x

摘要： CO₂ capture and storage (CCS) has been acknowledged as an essential part of a portfolio of technologies that are required to achieve cost-effective long-term CO₂ mitigation. However, the development progress of CCS technologies is far behind the targets set by roadmaps, and engineering practices do not lead to commercial deployment. One of the crucial reasons for this delay lies in the unaffordable penalty caused by CO₂ capture, even though the technology has been commonly recognized as achievable. From the aspects of separation and capture technology innovation, the potential and promising direction for solving this problem were analyzed, and correspondingly, the possible path for deployment of CCS in China was discussed. Under the carbon neutral target recently proposed by the Chinese government, the role of CCS and the key milestones for deployment were indicated.

关键词： CO₂ capture and storage (CCS) CO₂ separation energy penalty

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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