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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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Pilot scale autothermal gasification of coconut shell with CO

Bayu PRABOWO,Herri SUSANTO,Kentaro UMEKI,Mi YAN,Kunio YOSHIKAWA

《能源前沿（英文）》 2015年第9卷第3期页码 362-370 doi: 10.1007/s11708-015-0375-5

摘要： This paper explored the feasibility and benefit of CO utilization as gasifying agent in the autothermal gasification process. The effects of CO injection on reaction temperature and producer gas composition were examined in a pilot scale downdraft gasifier by varying the CO /C ratio from 0.6 to 1.6. O was injected at an equivalence ratio of approximately 0.33–0.38 for supplying heat through partial combustion. The results were also compared with those of air gasification. In general, the increase in CO injection resulted in the shift of combustion zone to the downstream of the gasifier. However, compared with that of air gasification, the long and distributed high temperature zones were obtained in CO -O gasification with a CO /C ratio of 0.6–1.2. The progress of the expected CO to CO conversion can be implied from the relatively insignificant decrease in CO fraction as the CO /C ratio increased. The producer gas heating value of CO -O gasification was consistently higher than that of air gasification. These results show the potential of CO -O gasification for producing high quality producer gas in an efficient manner, and the necessity for more work to deeply imply the observation.

关键词： biomass gasification CO₂ downdraft gasifier autothermal

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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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Reaction kinetics and internal diffusion of Zhundong char gasification with CO

Yun Liu, Jiangyuan Qu, Xuehui Wu, Kai Zhang, Yuan Zhang

《化学科学与工程前沿（英文）》 2021年第15卷第2期页码 373-383 doi: 10.1007/s11705-020-1949-2

摘要： Mass transfer usually affects the rate of chemical reactions in coal. The effect of internal diffusion on char gasification with CO in the temperature range from 1123 K to 1273 K was investigated via thermo-gravimetric analysis and assessment of char morphology features. The results revealed that the effect of internal diffusion on the initial reaction rate was more significant with an increase of particle size, due to the concentration gradient of the gasification agent within the solid particles. In the early stage of gasification, the generation of new micropores and the opening of closed pores led to an increase in specific surface area. As the reaction proceeded, the openings were gradually expanded and the specific surface area continued to increase. However, with further reaction, disappearance of edge pores, melting and collapse of the pore structure led to a decrease in specific surface area. The intrinsic activation energy and reaction order based on the th-order model were 157.67 kJ∙mol and 0.36, respectively. Thus, temperature zones corresponding to chemical reaction and diffusion control were identified. Moreover, the calculated effectiveness factor provided a quantitative estimation of internal diffusion in the initial stage.

关键词： coal char CO₂ gasification internal diffusion pore evolution

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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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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

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太阳能技术对我国未来减排CO2sub> 的贡献

赵玉文

《中国工程科学》 2003年第5卷第4期页码 38-40

摘要：

在“我国后续能源发展战略研究”基础上对太阳能技术在我国未来减排CO2sub>中的作用进行了估计，结果表明，在2010年后太阳能技术对CO2sub

关键词：太阳能，CO2减排

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Coupling the porous conditional moment closure with the random pore model: applications to gasificationand CO

D. N. SAULOV, C. R. CHODANKA, M. J. CLEARY, A. Y. KLIMENKO

《化学科学与工程前沿（英文）》 2012年第6卷第1期页码 84-93 doi: 10.1007/s11705-011-1164-2

摘要： Gasification of coal or biomass with in situ CO capture simultaneously allows production of clean hydrogen at relatively low cost and reduced emission of CO into the atmosphere. Clearly, this technology has a great potential for a future carbon constrained economy. Therefore, the development of a comprehensive, physically-based gasifier model is important. The sub-models that describe reactive transport processes in coal particles as well as in particles of CO sorbent material are among the key sub-models, which provide a necessary input for an overall gasifier model. Both coal and sorbent are materials that have complicated pore structures. The porous conditional moment closure (PCMC) model proves to be adequate for modeling reactive transport through porous media with fixed pore structure. Consumption of coal in the heterogeneous gasification reaction, however, widens the pores and reduces the surface area available for this reaction. At the same time, formation of a carbonate layer narrows the pores in the sorbent material and reduces the reaction rate of CO sorption. In both cases the pore structures are affected. Such changes are not taken into account in the existing PCMC model. In this study, we obtain the parameters of the diffusive tracer distribution based on the pore size distribution given by the widely applied random pore model (RPM), while coupling PCMC with RPM. Such coupling allows taking into account changes in pore structure caused by heterogeneous reactions and thus improves the accuracy of these key sub-models.

关键词： gasification CO₂ capture PCMC RPM

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A CO and CO

Guoxing Chen, Marc Widenmeyer, Binjie Tang, Louise Kaeswurm, Ling Wang, Armin Feldhoff, Anke Weidenkaff

《化学科学与工程前沿（英文）》 2020年第14卷第3期页码 405-414 doi: 10.1007/s11705-019-1886-0

摘要： A series of novel dense mixed conducting ceramic membranes based on K NiF -type (La Ca ) (Ni Cu )O was successfully prepared through a sol-gel route. Their chemical compatibility, oxygen permeability, CO and CO tolerance, and long-term CO resistance regarding phase composition and crystal structure at different atmospheres were studied. The results show that higher Ca contents in the material lead to the formation of CaCO . A constant oxygen permeation flux of about 0.63 mL·min ·cm at 1173 K through a 0.65 mm thick membrane was measured for (La Ca ) (Ni Cu )O , using either helium or pure CO as sweep gas. Steady oxygen fluxes with no sign of deterioration of this membrane were observed with increasing CO concentration. The membrane showed excellent chemical stability towards CO for more than 1360 h and phase stability in presence of CO for 4 h at high temperature. In addition, this membrane did not deteriorate in a high-energy CO plasma. The present work demonstrates that this (La Ca ) (Ni Cu )O membrane is a promising chemically robust candidate for oxygen separation applications.

关键词： K₂NiF₄ structure oxygen permeation membrane CO₂ and CO resistances CO₂ plasma resistance long-term robustness

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基于实时CT扫描技术的CO2sub>和N2sub>交替注入条件下煤吸附膨胀和解吸收缩规律研究 Article

张广磊, P.G. Ranjith, Herbert E. Huppert

《工程（英文）》 2022年第18卷第11期页码 88-95 doi: 10.1016/j.eng.2022.03.010

摘要：

深部煤层是分布最广泛的适宜二氧化碳（CO2sub>）地质封存的地层之一，且通常位于大型CO2sub>排放源附近。将CO2sub>注入到煤层中具有巨大的CO2sub>封存潜力，同时可以提高煤层气的采收率（CO2sub>-ECBM）。然而，目前CO2sub>-ECBM先导实验仍存在技术问题需要解决，即CO2sub>的注入会引起煤层渗透率降低进而影响长期注入能力。本文采用原位同步辐射X射线显微CT扫描技术，首次在原位条件下直接证明了注入氮气（N2sub>）可以置换解吸CO2sub>并减小因CO2sub>吸附引起的煤基质膨胀研究结果表明，煤层中注入经过简单处理的烟道气（主要成分为N2sub>和CO2sub>），是技术上可行的CO2sub>-ECBM 替代方案。

关键词： CCS CO2sub>-ECBM 碳中和 X 射线成像煤渗透率

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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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Chemical reactions of oily sludge catalyzed by iron oxide under supercritical water gasification condition

《化学科学与工程前沿（英文）》 2022年第16卷第6期页码 886-896 doi: 10.1007/s11705-021-2125-z

摘要： Supercritical water gasification is a promising technology in dealing with the degradation of hazardous waste, such as oily sludge, accompanied by the production of fuel gases. To evaluate the mechanism of Fe₂O₃ catalyst and the migration pathways of heteroatoms and to investigate the systems during the process, reactive force field molecular dynamics simulations are adopted. In terms of the catalytic mechanisms of Fe₂O₃, the surface lattice oxygen is consumed by small carbon fragments to produce CO and CO₂, improving the catalytic performance of the cluster due to more unsaturated coordination Fe sites exposed. Lattice oxygen combines with •H radicals to form water molecules, improving the catalytic performance. Furthermore, the pathway of asphaltene degradation was revealed at an atomic level, as well as products. Moreover, the adsorption of hydroxyl radical on the S atom caused breakage of the two C–S bonds in turn, forming •HSO intermediate, so that the organic S element was fixed into the inorganic liquid phase. The heteroatom O was removed under the effects of supercritical water. Heavy metal particles presented in the oily sludge, such as iron in association with Fe₂O₃ catalyst, helped accelerate the degradation of asphaltenes.

关键词： oily sludge SCWG ReaxFF Fe₂O₃ heteroatoms