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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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Characterization and catalytic activity of soft-templated NiO-CeO

Luciano Atzori, Maria Giorgia Cutrufello, Daniela Meloni, Barbara Onida, Delia Gazzoli, Andrea Ardu, Roberto Monaci, Maria Franca Sini, Elisabetta Rombi

《化学科学与工程前沿（英文）》 2021年第15卷第2期页码 251-268 doi: 10.1007/s11705-020-1951-8

摘要： Nanosized NiO, CeO and NiO-CeO mixed oxides with different Ni/Ce molar ratios were prepared by the soft template method. All the samples were characterized by different techniques as to their chemical composition, structure, morphology and texture. On the catalysts submitted to the same reduction pretreatment adopted for the activity tests the surface basic properties and specific metal surface area were also determined. NiO and CeO nanocrystals of about 4 nm in size were obtained, regardless of the Ni/Ce molar ratio. The Raman and X-ray photoelectron spectroscopy results proved the formation of defective sites at the NiO-CeO interface, where Ni species are in strong interaction with the support. The microcalorimetric and Fourier transform infrared analyses of the reduced samples highlighted that, unlike metallic nickel, CeO is able to effectively adsorb CO , forming carbonates and hydrogen carbonates. After reduction in H at 400 °C for 1 h, the catalytic performance was studied in the CO and CO co-methanation reaction. Catalytic tests were performed at atmospheric pressure and 300 °C, using CO/CO /H molar compositions of 1/1/7 or 1/1/5, and space velocities equal to 72000 or 450000 cm ∙h ∙g . Whereas CO was almost completely hydrogenated in any investigated experimental conditions, CO conversion was strongly affected by both the CO/CO /H ratio and the space velocity. The faster and definitely preferred CO hydrogenation was explained in the light of the different mechanisms of CO and CO methanation. On a selected sample, the influence of the reaction temperature and of a higher number of space velocity values, as well as the stability, were also studied. Provided that the Ni content is optimized, the NiCe system investigated was very promising, being highly active for the CO co-methanation reaction in a wide range of operating conditions and stable (up to 50 h) also when submitted to thermal stress.

关键词： soft template method NiO-CeO₂ catalysts CO and CO₂ co-methanation synthetic natural gas production

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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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Methanation of carbon dioxide: an overview

Wei WANG, Jinlong GONG

《化学科学与工程前沿（英文）》 2011年第5卷第1期页码 2-10 doi: 10.1007/s11705-010-0528-3

摘要： Although being very challenging, utilization of carbon dioxide (CO ) originating from production processes and flue gases of CO -intensive sectors has a great environmental and industrial potential due to improving the resource efficiency of industry as well as by contributing to the reduction of CO emissions. As a renewable and environmentally friendly source of carbon, catalytic approaches for CO fixation in the synthesis of chemicals offer the way to mitigate the increasing CO buildup. Among the catalytic reactions, methanation of CO is a particularly promising technique for producing energy carrier or chemical. This article focuses on recent developments in catalytic materials, novel reactors, and reaction mechanism for methanation of CO .

关键词： CO₂ methanation hydrogenation catalysis methane environmental science

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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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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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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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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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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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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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Review on cryogenic technologies for CO removal from natural gas

Yujing BI, Yonglin JU

《能源前沿（英文）》 2022年第16卷第5期页码 793-811 doi: 10.1007/s11708-022-0821-0

摘要： CO₂ in natural gas (NG) is prone to condense directly from gas to solid or solidify from liquid to solid at low temperatures due to its high triple point and boiling temperature, which can cause a block of equipment. Meanwhile, CO₂ will also affect the calorific value of NG. Based on the above reasons, CO₂ must be removed during the NG liquefaction process. Compared with conventional methods, cryogenic technologies for CO₂ removal from NG have attracted wide attention due to their non-polluting and low-cost advantages. Its integration with NG liquefaction can make rational use of the cold energy and realize the purification of NG and the production of by-product liquid CO₂. In this paper, the phase behavior of the CH₄-CO₂ binary mixture is summarized, which provides a basis for the process design of cryogenic CO₂ removal from NG. Then, the detailed techniques of design and optimization for cryogenic CO₂ removal in recent years are summarized, including the gas-liquid phase change technique and the gas-solid phase change technique. Finally, several improvements for further development of the cryogenic CO₂ removal process are proposed. The removal process in combination with the phase change and the traditional techniques with renewable energy will be the broad prospect for future development.

关键词： cryogenic CO₂ removal purification of natural gas (NG) biogas upgrading CH₄-CO₂ binary system

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Ultrasound-assisted co-precipitation synthesis of mesoporous Co3O4–CeO2 composite oxides for highly selective

《化学科学与工程前沿（英文）》 2022年第16卷第8期页码 1211-1223 doi: 10.1007/s11705-022-2145-3

摘要： The one-step highly selective oxidation of cyclohexane into cyclohexanone and cyclohexanol as the essential intermediates of nylon-6 and nylon-66 is considerably challenging. Therefore, an efficient and low-cost catalyst must be urgently developed to improve the efficiency of this process. In this study, a Co₃O₄–CeO₂ composite oxide catalyst was successfully prepared through ultrasound-assisted co-precipitation. This catalyst exhibited a higher selectivity to KA-oil, which was benefited from the synergistic effects between Co³⁺/Co²⁺ and Ce⁴⁺/Ce³⁺ redox pairs, than bulk CeO₂ and/or Co₃O₄. Under the optimum reaction conditions, 89.6% selectivity to KA-oil with a cyclohexane conversion of 5.8% was achieved over Co₃O₄–CeO₂. Its catalytic performance remained unchanged after five runs. Using the synergistic effects between the redox pairs of different transition metals, this study provides a feasible strategy to design high-performance catalysts for the selective oxidation of alkanes.

关键词： Co₃O₄–CeO₂ composite oxides cyclohexanone cyclohexanol ultrasonic-assisted co-precipitation selective oxidation solvent-free

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用于CO甲烷化的Ni/CeO2sub>催化剂还原过程重构行为调控研究 Article

曹昕宇, 浦天成, Bar Mosevitzky Lis, Israel E. Wachs, 彭冲, 朱明辉, 胡永康

《工程（英文）》 2022年第14卷第7期页码 94-99 doi: 10.1016/j.eng.2021.08.023

摘要：独特的活化方式使得催化剂上CO吸附得到增强，提高了CO甲烷化率。通过操纵活化条件来调整催化剂结构的策略也可以被用于指导其他负载型金属催化剂的理性设计。

关键词：镍-氧化铈催化剂催化剂活化结晶性甲烷化原位谱学

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基于一步法制备超高PEO负载的亲 CO2sub>气体分离膜用于高效碳捕集 Article

朱斌, 赫羴珊, 吴亚东, 李松伟, 邵路

《工程（英文）》 2023年第26卷第7期页码 220-228 doi: 10.1016/j.eng.2022.03.016

摘要：

针对日益增加的大气CO2sub>含量，膜技术被认为是一种有前景的碳捕集策略，其中亲CO2sub>分离膜已经展示出显著的应用潜力，特别是在CO2sub>/轻质气体分离方面。以聚环氧乙烷（PEO）为代表的CO2sub>亲和材料，因其与CO2sub>的特殊偶极-四极矩相互作用而吸引了广泛的研究关注。此外，高结构稳定性使得分离膜在高进料压力（高达20 bar）下表现出更好的CO2sub>渗透系数和气体选择性。

关键词：膜分离气体分离 CO2sub>捕集亲CO2sub>分离膜聚环氧乙烷

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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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标题作者时间类型操作

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

Kechao Zhao,Zhenhua Li,Li Bian

期刊论文

Characterization and catalytic activity of soft-templated NiO-CeO

Luciano Atzori, Maria Giorgia Cutrufello, Daniela Meloni, Barbara Onida, Delia Gazzoli, Andrea Ardu, Roberto Monaci, Maria Franca Sini, Elisabetta Rombi

期刊论文

以净零排放为目标的封存驱动型CO2sub>提高采收率方法

刘月亮, 芮振华

期刊论文

Methanation of carbon dioxide: an overview

Wei WANG, Jinlong GONG

期刊论文

Reduction potential of the energy penalty for CO capture in CCS

期刊论文

Frontier science and challenges on offshore carbon storage

期刊论文

固体氧化物电解池共电解H2sub>O/CO2sub>研究进展