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离岸碳捕集利用与封存技术体系研究

李姜辉,李鹏春,李彦尊,童峰

《中国工程科学》 2023年第25卷第2期页码 173-186 doi: 10.15302/J-SSCAE-2023.07.015

摘要：

离岸碳捕集、利用与封存（CCUS）技术是沿海国家或地区通过工程方式为实现CO₂减排而发展起来的解决方案与技术体系；相对于陆上离岸CCUS技术指从沿海大型或近海碳排放源捕集CO₂，加压并运输至离岸封存平台后注入海底地质储层中，实现CO₂与大气永久隔离或利用其生产价值产品的过程。本文概要回顾了全球及我国离岸CCUS技术的发展需求与产业现状，分析了发展离岸CCUS的技术性和社会性价值；梳理总结了代表性的离岸CCUS技术发展路线及其态势，如CO₂工厂捕集、CO₂管道运输、CO₂海底咸水层封存与驱油利用、CO₂化学利用以及其他技术架构。

关键词：离岸碳捕集、利用与封存；CO2捕集；CO2运输；CO2封存；CO2利用；沿海地区；近海沉积盆地

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Theoretical and experimental study on the fluidity performance of hard-to-fluidize carbon nanotubes-basedCO2 capture sorbents

《化学科学与工程前沿（英文）》 2022年第16卷第10期页码 1460-1475 doi: 10.1007/s11705-022-2159-x

摘要： Carbon nanotubes-based materials have been identified as promising sorbents for efficient CO₂ capture in fluidized beds, suffering from insufficient contact with CO₂ for the high-level CO₂ capture capacity. This study focuses on promoting the fluidizability of hard-to-fluidize pure and synthesized silica-coated amine-functionalized carbon nanotubes. The novel synthesized sorbent presents a superior sorption capacity of about 25 times higher than pure carbon nanotubes during 5 consecutive adsorption/regeneration cycles. The low-cost fluidizable-SiO₂ nanoparticles are used as assistant material to improve the fluidity of carbon nanotubes-based sorbents. Results reveal that a minimum amount of 7.5 and 5 wt% SiO₂ nanoparticles are required to achieve an agglomerate particulate fluidization behavior for pure and synthesized carbon nanotubes, respectively. Pure carbon nanotubes + 7.5 wt% SiO₂ and synthesized carbon nanotubes + 5 wt% SiO₂ indicates an agglomerate particulate fluidization characteristic, including the high-level bed expansion ratio, low minimum fluidization velocity (1.5 and 1.6 cm·s^–1), high Richardson−Zakin index (5.2 and 5.3 > 5), and low Π value (83.2 and 84.8 < 100, respectively). Chemical modification of carbon nanotubes causes not only enhanced CO ₂ uptake capacity but also decreases the required amount of silica additive to reach a homogeneous fluidization behavior for synthesized carbon nanotubes sorbent.

关键词： CO₂ capture CNT-based sorbents fluidization SiO₂ nanoparticles fluidized bed reactors

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Scale up of reactors for carbon dioxide reduction

《化学科学与工程前沿（英文）》 2023年第17卷第1期页码 116-122 doi: 10.1007/s11705-022-2178-7

摘要： In recent times there has been a great deal of interest in the conversion of carbon dioxide into more useful chemical compounds. On the other hand, the translation of these developments in electrochemical reduction of carbon dioxide from the laboratory bench to practical scale remains an underexplored topic. Here we examine some of the major challenges, demonstrating some promising strategies towards such scale-up, including increased electrode area and stacking of electrode pairs in different configurations. We observed that increasing the electrode area from 1 to 10 cm² led to only a 4% drop in current density, with similarly small penalties realised when stacking sub-cells together.

关键词： CO₂ reduction electrochemical cell electrosynthesis upscaling

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Encapsulation of 2-amino-2-methyl-1-propanol with tetraethyl orthosilicate for CO2 capture

Sidra Rama, Yan Zhang, Fideline Tchuenbou-Magaia, Yulong Ding, Yongliang Li

《化学科学与工程前沿（英文）》 2019年第13卷第4期页码 672-683 doi: 10.1007/s11705-019-1856-6

摘要： Carbon capture is widely recognised as an essential strategy to meet global goals for climate protection. Although various CO capture technologies including absorption, adsorption and membrane exist, they are not yet mature for post-combustion power plants mainly due to high energy penalty. Hence researchers are concentrating on developing non-aqueous solvents like ionic liquids, CO -binding organic liquids, nanoparticle hybrid materials and microencapsulated sorbents to minimize the energy consumption for carbon capture. This research aims to develop a novel and efficient approach by encapsulating sorbents to capture CO in a cold environment. The conventional emulsion technique was selected for the microcapsule formulation by using 2-amino-2-methyl-1-propanol (AMP) as the core sorbent and silicon dioxide as the shell. This paper reports the findings on the formulated microcapsules including key formulation parameters, microstructure, size distribution and thermal cycling stability. Furthermore, the effects of microcapsule quality and absorption temperature on the CO loading capacity of the microcapsules were investigated using a self-developed pressure decay method. The preliminary results have shown that the AMP microcapsules are promising to replace conventional sorbents.

关键词： carbon capture microencapsulated sorbents emulsion technique low temperature adsorption and absorption

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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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Newly-modeled graphene-based ternary nanocomposite for the magnetophotocatalytic reduction of CO2 with

《化学科学与工程前沿（英文）》 2022年第16卷第10期页码 1438-1459 doi: 10.1007/s11705-022-2166-y

摘要： The development of CO₂ into hydrocarbon fuels has emerged as a green method that could help mitigate global warning. The novel structured photocatalyst is a promising material for use in a photocatalytic and magneto-electrochemical method that fosters the reduction of CO₂ by suppressing the recombination of electron−hole pairs and effectively transferring the electrons to the surface for the chemical reaction of CO₂ reduction. In our study, we have developed a novel-structured AgCuZnS₂–graphene–TiO₂ to analyze its catalytic activity toward the selective evolution of CO₂. The selectivity of each nanocomposite substantially enhanced the activity of the AgCuZnS₂–graphene–TiO₂ ternary nanocomposite due to the successful interaction, and the selectivity of the final product was improved to a value 3 times higher than that of the pure AgCuZnS₂ and 2 times higher than those of AgCuZnS₂–graphene and AgCuZnS₂–TiO₂ under ultra-violet (UV)-light (λ = 254 nm) irradiation in the photocatalytic process. The electrochemical CO₂ reduction test was also conducted to analyze the efficacy of the AgCuZnS₂–graphene–TiO₂ when used as a working electrode in laboratory electrochemical cells. The electrochemical process was conducted under different experimental conditions, such as various scan rates (mV·s^–1), under UV-light and with a 0.07 T magnetic-core. The evolution of CO₂ substantially improved under UV-light (λ = 254 nm) and with 0.07 T magnetic-core treatment; these improvements were attributed to the facts that the UV-light activated the electron-transfer pathway and the magnetic core controlled the pathway of electron-transmission/prevention to protect it from chaotic electron movement. Among all tested nanocomposites, AgCuZnS₂–graphene–TiO₂ absorbed the CO₂ most strongly and showed the best ability to transfer the electron to reduce the CO₂ to methanol. We believe that our newly-modeled ternary nanocomposite opens up new opportunities for the evolution of CO₂ to methanol through an electrochemical and photocatalytic process.

关键词： ternary nanocomposite photocatalytic electrochemical CO₂ reduction UV-light magnetic core

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Tuning porosity of coal-derived activated carbons for CO2 adsorption

《化学科学与工程前沿（英文）》 2022年第16卷第9期页码 1345-1354 doi: 10.1007/s11705-022-2155-1

摘要： A simple method was developed to tune the porosity of coal-derived activated carbons, which provided a model adsorbent system to investigate the volumetric CO₂ adsorption performance. Specifically, the method involved the variation of the activation temperature in a K₂CO₃ induced chemical activation process which could yield activated carbons with defined microporous (< 2 nm, including ultra-microporous < 1 nm) and meso-micro-porous structures. CO₂ adsorption isotherms revealed that the microporous activated carbon has the highest measured CO₂ adsorption capacity (6.0 mmol∙g^–1 at 0 °C and 4.1 mmol∙g^–1 at 25 °C), whilst ultra-microporous activated carbon with a high packing density exhibited the highest normalized capacity with respect to packing volume (1.8 mmol∙cm⁻³ at 0 °C and 1.3 mmol∙cm^–3 at 25 °C), which is significant. Both experimental correlation analysis and molecular dynamics simulation demonstrated that (i) volumetric CO₂ adsorption capacity is directly proportional to the ultra-micropore volume, and (ii) an increase in micropore sizes is beneficial to improve the volumetric capacity, but may lead a low CO₂ adsorption density and thus low pore space utilization efficiency. The adsorption experiments on the activated carbons established the criterion for designing CO₂ adsorbents with high volumetric adsorption capacity.

关键词： coal-derived activated carbons porosity CO₂ adsorption molecular dynamics

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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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Enhancing the aromatic selectivity of cyclohexane aromatization by CO₂ coupling

《化学科学与工程前沿（英文）》 2023年第17卷第11期页码 1801-1808 doi: 10.1007/s11705-023-2325-9

摘要： Improving the aromatic selectivity in the alkane aromatization process is of great importance for its practical utilization but challenge to make because the high H/C ratio of alkanes would lead to a serious hydrogen transfer process and a large amount of light alkanes. Herein, CO₂ is introduced into the cyclohexane conversion process on the HZSM-5 zeolite, which can improve the aromatic selectivity. By optimizing the reaction conditions, an improved aromatic (benzene, toluene, xylene, and C₉₊) selectivity of 48.2% can be obtained at the conditions of 2.7 MPa (CO₂), 450 °C, and 1.7 h⁻¹, which is better than that without CO₂ (aromatic selectivity = 43.2%). In situ transmission Fourier transform infrared spectroscopy spectra illustrate that many oxygenated chemical intermediates (e.g., carboxylic acid, anhydride, unsaturated aldehydes/ketones or ketene) would be formed during the cyclohexane conversion process in the presence of CO₂. ¹³C isotope labeling experimental results demonstrate that CO₂ can enter into the aromatics through the formation of oxygenated chemical intermediates and thereby improve the aromatic selectivity. This study may open a green, economic, and promising way to improve the aromatic selectivity for alkane aromatization process.

关键词： aromatics carbon dioxide aromatization coupling reaction ZSM-5 zeolite

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地热能储存与CO₂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CO₂羽流进行地热储能可通过将CO₂储存于地质体中来缓解温室效应。然后，将产生的高能CO₂引入到目标油藏中，用于CO₂利用和地热能储存。最后，将CO₂有效地封存在地质油藏体中。结果表明，随着高能CO₂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，CO₂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CO₂场地的封存潜力的评估，CO₂注入110年后，地质体的利用率将高达91.2%，场地内CO₂的最终注入量将高达9.529 经过1000年封存，超临界相在CO₂封存中占主导地位，其次是液相，然后是矿化相。此外，由于残余油的存在，用于溶解捕获的CO₂封存量显著增加。

关键词：地热能储存 CO₂封存碳中和大规模 CO₂利用

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Decomposition analysis of energy-related carbon dioxide emissions in the iron and steel industry in China

Wenqiang SUN, Jiuju CAI, Hai YU, Lei DAI

《环境科学与工程前沿（英文）》 2012年第6卷第2期页码 265-270 doi: 10.1007/s11783-011-0284-8

摘要： This work aims to identify the main factors influencing the energy-related carbon dioxide (CO ) emissions from the iron and steel industry in China during the period of 1995–2007. The logarithmic mean divisia index (LMDI) technique was applied with period-wise analysis and time-series analysis. Changes in energy-related CO emissions were decomposed into four factors: emission factor effect, energy structure effect, energy consumption effect, and the steel production effect. The results show that steel production is the major factor responsible for the rise in CO emissions during the sampling period; on the other hand the energy consumption is the largest contributor to the decrease in CO emissions. To a lesser extent, the emission factor and energy structure effects have both negative and positive contributions to CO emissions, respectively. Policy implications are provided regarding the reduction of CO emissions from the iron and steel industry in China, such as controlling the overgrowth of steel production, improving energy-saving technologies, and introducing low-carbon energy sources into the iron and steel industry.

关键词： carbon dioxide (CO₂) emissions decomposition analysis logarithmic mean divisia index (LMDI) technique time-series analysis

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海底碳封存环境地质灾害风险及监测技术研究

张少鹏,刘晓磊,程光伟,朱超祁,李清平,何玉发

《中国工程科学》 2023年第25卷第3期页码 122-130 doi: 10.15302/J-SSCAE-2023.03.011

摘要：

海底CO2地质封存是我国实现“双碳”目标的重要组成部分，但CO2泄露具有诱发海底地质灾害的风险，威胁海洋工程的安全建设本文在简要介绍海底CO2地质封存示范案例的基础上，阐述了海底封存区CO2泄露的致灾机制，结合实例梳理了典型CO2控释试验中的海洋环境监测技术，重点分析了与CO2泄露相关的环境地质监测技术，包括地震调查与监测研究认为，今后应侧重封存区CO2泄露致灾机制与环境地质监测技术研究，建议在研发长时序、低成本并实时监测技术的基础上，结合封存区基线调查，建立和发展系统性、智能性的多维度灾害识别模型，构建多方面、多层次、

关键词：海底碳封存；环境地质；CO2泄露；灾害风险；监测技术

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海洋CO2管道输送技术现状与展望

王子明,李清平,李姜辉,范振宁,张建

《中国工程科学》 doi: 10.15302/J-SSCAE-2023.06.017

摘要：

管道输送是经济高效的CO2运输方式，海洋CO2运输是离岸碳捕集、利用与封存（CCUS）产业链的关键环节和规模化开展离岸CCUS工程建设所需的核心技术本文明晰了我国实施离岸CCUS的优势、典型海洋碳运输情境和海洋CO2运输方式，剖析了国内外海洋CO2管道输送的技术与工程概况；从CO2流体相态及流动安全，沿程腐蚀风险评估、监测及预警，CO2泄漏实时监测技术，高压CO2泄放及对环境的影响等方面梳理了海洋CO2管道输送工艺技术现状；从CO2管道材料断裂行为及止裂措施、高耐蚀及密封材料、碳钢管道长寿命运行的关键腐蚀控制技术、注采井筒的腐蚀风险评估等方面梳理了海洋CO2管道材料技术现状。研究认为，加快发展适应海洋CO2管道输送复杂工况的材料体系、全流程CO2管道的智慧管理与数字孪生技术、海底CO2管道全生命周期运行关键技术、在役海底管道改输评估与保障技术，采取加快推动我国近海碳封存CO2

关键词： CO2管道；离岸CCUS；海底管道；管道腐蚀；管道断裂；泄漏监测

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Activated carbons and amine-modified materials for carbon dioxide capture –– a review

Zhenhe CHEN, Shubo DENG, Haoran WEI, Bin WANG, Jun HUANG, Gang YU

《环境科学与工程前沿（英文）》 2013年第7卷第3期页码 326-340 doi: 10.1007/s11783-013-0510-7

摘要： Rapidly increasing concentration of CO in the atmosphere has drawn more and more attention in recent years, and adsorption has been considered as an effective technology for CO capture from the anthropogenic sources. In this paper, the attractive adsorbents including activated carbons and amine-modified materials were mainly reviewed and discussed with particular attention on progress in the adsorbent preparation and CO adsorption capacity. Carbon materials can be prepared from different precursors including fossil fuels, biomass and resins using the carbonization-activation or only activation process, and activated carbons prepared by KOH activation with high CO adsorbed amount were reviewed in the preparation, adsorption capacity as well as the relationship between the pore characteristics and CO adsorption. For the amine-modified materials, the physical impregnation and chemical graft of polyethylenimine (PEI) on the different porous materials were introduced in terms of preparation method and adsorption performance as well as their advantages and disadvantages for CO adsorption. In the last section, the issues and prospect of solid adsorbents for CO adsorption were summarized, and it is expected that this review will be helpful for the fundamental studies and industrial applications of activated carbons and amine-modified adsorbents for CO capture.

关键词： adsorption capacity CO₂ capture activated carbon amine-impregnated adsorbents