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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-based CO2capture 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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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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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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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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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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刘公平：面向CO₂捕集的混合基质膜设计制备（2022年4月16日）

2022年06月09日

关键词：绿色化工

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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Dynamic modelling and simulation of a post-combustion CO capture process for coal-fired power plants

《化学科学与工程前沿（英文）》 2022年第16卷第2期页码 198-209 doi: 10.1007/s11705-021-2057-7

摘要： Solvent-based post-combustion capture technologies have great potential for CO₂ mitigation in traditional coal-fired power plants. Modelling and simulation provide a low-cost opportunity to evaluate performances and guide flexible operation. Composed by a series of partial differential equations, first-principle post-combustion capture models are computationally expensive, which limits their use in real time process simulation and control. In this study, we propose a first-principle approach to develop the basic structure of a reduced-order model and then the dominant factor is used to fit properties and simplify the chemical and physical process, based on which a universal and hybrid post-combustion capture model is established. Model output at steady state and trend at dynamic state are validated using experimental data obtained from the literature. Then, impacts of liquid-to-gas ratio, reboiler power, desorber pressure, tower height and their combination on the absorption and desorption effects are analyzed. Results indicate that tower height should be designed in conjunction with the flue gas flow, and the gas-liquid ratio can be optimized to reduce the reboiler power under a certain capture target.

关键词： CO₂ capture post-combustion capture simulation dominant factor

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太阳能技术对我国未来减排CO₂ 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CO₂中的作用进行了估计，结果表明，在2010年后太阳能技术对CO₂

关键词：太阳能，CO2减排

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and measurements: Powerful tools for revealing the mechanism of alkali carbonate-based sorbents for COcapture in real conditions

《能源前沿（英文）》 2023年第17卷第3期页码 380-389 doi: 10.1007/s11708-023-0872-x

摘要： Alkali carbonate-based sorbents (ACSs), including Na₂CO₃- and K₂CO₃-based sorbents, are promising for CO₂ capture. However, the complex sorbent components and operation conditions lead to the versatile kinetics of CO₂ sorption on these sorbents. This paper proposed that operando modeling and measurements are powerful tools to understand the mechanism of sorbents in real operating conditions, facilitating the sorbent development, reactor design, and operation parameter optimization. It reviewed the theoretical simulation achievements during the development of ACSs. It elucidated the findings obtained by utilizing density functional theory (DFT) calculations, ab initio molecular dynamics (AIMD) simulations, and classical molecular dynamics (CMD) simulations as well. The hygroscopicity of sorbent and the humidity of gas flow are crucial to shifting the carbonation reaction from the gas−solid mode to the gas−liquid mode, boosting the kinetics. Moreover, it briefly introduced a machine learning (ML) approach as a promising method to aid sorbent design. Furthermore, it demonstrated a conceptual compact operando measurement system in order to understand the behavior of ACSs in the real operation process. The proposed measurement system includes a micro fluidized-bed (MFB) reactor for kinetic analysis, a multi-camera sub-system for 3D particle movement tracking, and a combined Raman and IR sub-system for solid/gas components and temperature monitoring. It is believed that this system is useful to evaluate the real-time sorbent performance, validating the theoretical prediction and promoting the industrial scale-up of ACSs for CO₂ capture.

关键词： CO₂ capture carbonation theoretical modeling operando techniques reaction visualization

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Al₂O₃ and CeO₂-promoted MgO sorbents for CO₂ 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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A coal-fired power plant integrated with biomass co-firing and CO capture for zero carbon emission

《能源前沿（英文）》 2022年第16卷第2期页码 307-320 doi: 10.1007/s11708-021-0790-8

摘要： A promising scheme for coal-fired power plants in which biomass co-firing and carbon dioxide capture technologies are adopted and the low-temperature waste heat from the CO₂ capture process is recycled to heat the condensed water to achieve zero carbon emission is proposed in this paper. Based on a 660 MW supercritical coal-fired power plant, the thermal performance, emission performance, and economic performance of the proposed scheme are evaluated. In addition, a sensitivity analysis is conducted to show the effects of several key parameters on the performance of the proposed system. The results show that when the biomass mass mixing ratio is 15.40% and the CO₂ capture rate is 90%, the CO₂ emission of the coal-fired power plant can reach zero, indicating that the technical route proposed in this paper can indeed achieve zero carbon emission in coal-fired power plants. The net thermal efficiency decreases by 10.31%, due to the huge energy consumption of the CO₂ capture unit. Besides, the cost of electricity (COE) and the cost of CO₂ avoided (COA) of the proposed system are 80.37 $/MWh and 41.63 $/tCO₂, respectively. The sensitivity analysis demonstrates that with the energy consumption of the reboiler decreasing from 3.22 GJ/tCO₂ to 2.40 GJ/ tCO₂, the efficiency penalty is reduced to 8.67%. This paper may provide reference for promoting the early realization of carbon neutrality in the power generation industry.

关键词： coal-fired power plant biomass co-firing CO₂ capture zero carbon emission performance evaluation