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

《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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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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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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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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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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Tuning the catalytic selectivity in electrochemical CO

Jiafang XIE,Yuxi HUANG,Hanqing YU

《环境科学与工程前沿（英文）》 2015年第9卷第5期页码 861-866 doi: 10.1007/s11783-014-0742-1

摘要： Electrochemical conversion of CO to hydrocarbons can relieve both environmental and energy stresses. However, electrocatalysts for this reaction usually suffer from a poor product selectivity and a large overpotential. Here we report that tunable catalytic selectivity for hydrocarbon formation could be achieved on Cu nanomaterials with different morphologies. By tuning the electrochemical parameters, either Cu oxide nanowires or nanoneedles were fabricated and then electrochemically reduced to the corresponding Cu nanomaterials. The Cu nanowires preferred the formation of C H , while the Cu nanoneedles favored the production of more CH , rather than C H . Our work provides a facile synthetic strategy for preparing Cu-based nanomaterials to achieve selective CO reduction.

关键词： electrochemical CO₂ reduction Cu oxide nanostructure selectivity hydrocarbon formation

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杨为民：石油化工CO2减排与转化中的催化技术（2021年5月21日）

2021年12月01日

关键词：碳中和

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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孙振宇：金属材料的表界面改性增强电催化CO2还原（2021年5月21日）

2021年11月22日

关键词：碳中和

侯阳：纳米碳基电极的结构设计与工业级电流密度下催化还原CO2机理（2021年5月21日）

2021年11月22日

关键词：碳中和

Electrochemical CO reduction to C products over CuZn intermetallic catalysts synthesized by electrodeposition

《能源前沿（英文）》 doi: 10.1007/s11708-023-0898-0

摘要： Electrocatalytic CO₂ reduction (ECR) offers an attractive approach to realizing carbon neutrality and producing valuable chemicals and fuels using CO₂ as the feedstock. However, the lack of cost-effective electrocatalysts with better performances has seriously hindered its application. Herein, a one-step co-electrodeposition method was used to introduce Zn, a metal with weak *CO binding energy, into Cu to form Cu/Zn intermetallic catalysts (Cu/Zn IMCs). It was shown that, using an H-cell, the high Faradaic efficiency of C₂₊ hydrocarbons/alcohols (

F E C 2 +

) could be achieved in ECR by adjusting the surface metal components and the applied potential. In suitable conditions, FE_C2+ and current density could be as high as 75% and 40 mA/cm², respectively. Compared with the Cu catalyst, the Cu/Zn IMCs have a lower interfacial charge transfer resistance and a larger electrochemically active surface area (ECSA), which accelerate the reaction. Moreover, the *CO formed on Zn sites can move to Cu sites due to its weak binding with *CO, and thus enhance the C–C coupling on the Cu surface to form C₂₊ products.

关键词： carbon dioxide electroreduction electrochemistry co-electrodeposition intermetallic catalysts value-added chemicals

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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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Theoretical and experimental study on the fluidity performance of hard-to-fluidize carbon nanotubes-based CO2

《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