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The catalytic effect of both oxygen-bearing functional group and ash in carbonaceous catalyst on CH 4-CO 2 reforming

Weidong ZHANG, Yongfa ZHANG,

《化学科学与工程前沿（英文）》 2010年第4卷第2期页码 147-152 doi: 10.1007/s11705-009-0242-1

摘要： A kind of new catalyst—carbonaceous catalyst—for CH-CO reformation has been developed in our laboratory. The effect of both oxygen-bearing functional group such as phenolic hydroxyl, carbonyl, carboxyl, and lactonic, and ash such as FeO, NaCO, and KCO in the carbonaceous catalyst on the CH-CO reforming has been investigated with a fixed-bed reactor. It has been found that the carbonaceous catalyst is an efficient catalyst on CO-CH reforming. With the decrease of oxygen-bearing functional group, the catalytic activity of carbonaceous catalyst decreases quickly. The oxygen-bearing functional groups play a significant role in the carbonaceous-catalyzed CO-CH reforming; the ash components in carbonaceous catalyst also have an important influence on the CO-CH reforming. FeO, NaCO, and KCO in the ash can catalyze the CO-CH reforming reaction; CaO has little effect on CO-CH reforming reaction. CaO can catalyze the gasification between carbonaceous catalyst and CO; AlO and MgO inhibit the CO-CH reforming.

关键词： oxygen-bearing functional carboxyl phenolic hydroxyl CH-CO reformation CO-CH reforming

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Effect of TiO

Navid Azizi, Mojgan Isanejad, Toraj Mohammadi, Reza M. Behbahani

《化学科学与工程前沿（英文）》 2019年第13卷第3期页码 517-530 doi: 10.1007/s11705-018-1781-0

摘要： Membranes have attracted much attention as economical methods for industrial chemical processes. The effects of the titanium dioxide nanoparticle load on the morphology and CO /CH separation performance of poly (ether-block-amide) (PEBAX-1657) mixed matrix membranes (MMMs) were investigated from pressures of 3–12 bar and temperatures of 30°C–60°C. The PEBAX membranes were characterized by scanning electron microscopy, Fourier transform infrared spectroscopy, X-ray diffraction, thermal gravimetric analysis, atomic force microscopy and tensile strength analysis. The incorporation of TiO nanoparticles into the polymeric MMMs improved the CO /CH gas separation performance (both the permeability and selectivity) of the membranes. The CO permeability and ideal CO /CH selectivity values of the nanocomposite membrane loaded with 8 wt-% TiO were 172.32 Barrer and 24.79, respectively whereas those of the neat membrane were 129.87 Barrer and 21.39, respectively.

关键词： mixed matrix membrane TiO₂ nanoparticles PEBAX-1657 CO₂/CH₄ separation

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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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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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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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Ni-Co bimetallic catalyst for CH

Xiaohong LI, Jun AI, Wenying LI, Dongxiong LI

《化学科学与工程前沿（英文）》 2010年第4卷第4期页码 476-480 doi: 10.1007/s11705-010-0512-y

摘要： A co-precipitation method was employed to prepare Ni/Al O -ZrO , Co/Al O -ZrO and Ni-Co/Al O -ZrO catalysts. Their properties were characterized by N adsorption (BET), thermogravimetric analysis TGA , temperature-programmed reduction (TPR), temperature-programmed desorption (CO -TPD), and temperature-programmed surface reaction (CH -TPSR and CO -TPSR). Ni-Co/Al O -ZrO bimetallic catalyst has good performance in the reduction of active components Ni, Co and CO adsorption. Compared with mono-metallic catalyst, bimetallic catalyst could provide more active sites and CO adsorption sites (C+ CO = 2CO) for the methane-reforming reaction, and a more appropriate force formed between active components and composite support (SMSI) for the catalytic reaction. According to the CH -CO -TPSR, there were 80.9% and 81.5% higher CH and CO conversion over Ni-Co/Al O -ZrO catalyst, and its better resistance to carbon deposition, less than 0.5% of coke after 4 h reaction, was found by TGA. The high activity and excellent anti-coking of the Ni-Co/Al O -ZrO catalyst were closely related to the synergy between Ni and Co active metal, the strong metal-support interaction and the use of composite support.

关键词： Ni-Co bimetallic catalyst composite support CH₄ reforming with CO₂

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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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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

Complete oxidation of methane on CoO-SnO catalysts

Xingfu TANG , Jiming HAO , Junhua LI ,

《环境科学与工程前沿（英文）》 2009年第3卷第3期页码 265-270 doi: 10.1007/s11783-009-0019-2

摘要： CoO-SnO hybrid oxides were prepared by the coprecipitation method and were used to oxidate methane (CH) in presence of oxygen. The CoO-SnO with a molar ratio of Co/(Co+Sn) at 0.75 exhibited the highest catalytic activity among all the CoO-SnO hybrid oxides. Experimental results showed that the catalysts were considerably stable in the CH combustion reaction, and were verified by X-ray photoelectron spectra (XPS). It was found that CoO was the active species, and SnO acted as a support or a promoting component in the CoO-SnO hybrid oxides. The surface area was not a major factor that affected catalytic activity. The hydrogen temperature-programmed reduction (H-TPR) results demonstrated that the interaction between cobalt and tin oxides accelerated the mobility of oxygen species of CoO-SnO, leading to higher catalytic activity.

关键词： Co₃O₄-SnO₂ complete oxidation methane (CH₄)

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Greenhouse gas emissions during co-composting of cattle feedlot manure with construction and demolition

Xiying Hao, Francis J. Larney

《环境科学与工程前沿（英文）》 2017年第11卷第3期 doi: 10.1007/s11783-017-0955-1

摘要： Manure management strategies should reflect current animal feeding practices and encourage recycling of organic waste to help protect our environment. This research investigated greenhouse gas (GHG) emissions during cattle manure stockpiling or composting with and without construction and demolition (C&D) waste. Manure was collected from cattle fed a typical finishing diet (CK manure) and from cattle on diets which included 30% dried distillers grains with solubles (DG manure). The CK and DG manures were co-composted with (4:1) C&D waste (treatments: CK_CD DG_CD), composted alone (treatments: CK and DG) in 13 m bins or stockpiled without C&D waste (treatments: CK_ST and DG_ST) for 99 days. Manure type (CK vs. DG manure) had no effect on GHG emissions over the 99 day manure composting or stockpiling. Composting with C&D waste produced similar CO emissions, about double that from manure stockpiling (7.0 kgC·m ). In contrast, CH emissions were reduced by the inclusion of C&D waste (64 gC·m with C&D vs. 244 gC·m without C&D) while the manure stockpile emitted the greatest amount of CH (464 gC·m ). Additionally, only 0.48% of C was emitted in CH form with C&D waste, compared to 1.68% when composting without C&D waste and 7.00% when cattle manure was stockpiled. The N O emissions (12.4 to 18.0 gN·m ) were similar across all treatments. The lower CH emissions with C&D waste are beneficial in reducing overall GHG emissions from manure composting, while reducing the amount of material entering landfills.

关键词： Livestock manure greenhouse gas flux straw bale compost bin N₂O CH₄ CO₂

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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