Journal of CO2 Utilization最新文献_第3页

Effect of electric furnace steel slag powder on the strength of green low-carbon concrete with high-titanium blast furnace slag 电炉钢渣粉对高钛高炉矿渣绿色低碳混凝土强度的影响

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-10-13 DOI: 10.1016/j.jcou.2024.102957

Yuehua Liang, Jie Wang

This study explores the application of electric furnace steel slag powder (EFSSP), fly ash (FA), and high-titanium heavy slag (HTHS) from Panzhihua City, China, in producing green low-carbon concrete. The properties of these waste materials were characterized, and the fluidity and hydration activity of the EFSSP-FA composite admixture in cement mortar were tested. Additionally, the strength of HTHSC mixed with EFSSP-FA composite admixture was evaluated at various curing times, and the microstructure of the concrete mortar layer was analyzed. The study shows that the 7-day activity indices of EFSSP and FA are 61 % and 51.96 %, respectively, with fluidity ratios of 92.53 % and 124.58 %. Mixing EFSSP and FA compensates for their individual limitations. At a 1:1 mass ratio, the composite admixture achieved a 69.89 % activity index and 114.46 % fluidity. The pozzolanic reaction within the composite admixture was evident, promoting the continuous formation of C-S-H in HTHSC, the compressive strength after curing periods of 520 days, 300 days, 180 days, and 90 days reached approximately 190 %, 170 %, 150 %, and 130 % of the 28-day strength, respectively. The XRD, SEM, TG, and DSC characterization results for the HTHSC mortar layer at different curing stages were consistent with the observed trends in compressive strength. Since the raw materials used for concrete preparation were industrial waste, this portion was excluded from carbon emissions calculations. The all-industrial waste HTHSC achieved approximately a 30 % reduction in carbon emissions, the carbon emissions per unit of strength at 520 days of curing were approximately 55 % of those at 28 days.

本研究探讨了中国攀枝花市电炉钢渣粉（EFSSP）、粉煤灰（FA）和高钛重渣（HTHS）在生产绿色低碳混凝土中的应用。对这些废弃材料的特性进行了表征，并测试了 EFSSP-FA 复合掺合料在水泥砂浆中的流动性和水化活性。此外，还评估了掺有 EFSSP-FA 复合外加剂的 HTHSC 在不同养护时间的强度，并分析了混凝土砂浆层的微观结构。研究表明，EFSSP 和 FA 的 7 天活性指数分别为 61 % 和 51.96 %，流动性比分别为 92.53 % 和 124.58 %。混合使用 EFSSP 和 FA 可以弥补它们各自的局限性。按照 1:1 的质量比，复合外加剂的活性指数为 69.89%，流动性为 114.46%。复合掺合料中的水青石反应明显，促进了 HTHSC 中 C-S-H 的持续形成，固化 520 天、300 天、180 天和 90 天后的抗压强度分别达到 28 天强度的约 190%、170%、150% 和 130%。不同养护阶段 HTHSC 砂浆层的 XRD、SEM、TG 和 DSC 表征结果与观察到的抗压强度趋势一致。由于用于制备混凝土的原材料是工业废料，因此在计算碳排放量时不包括这一部分。全工业废料 HTHSC 的碳排放量减少了约 30%，养护 520 天时单位强度的碳排放量约为养护 28 天时的 55%。

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引用次数: 0

A comprehensive review of post-combustion CO2 capture technologies for applications in the maritime sector: A focus on adsorbent materials 全面回顾应用于海事领域的燃烧后二氧化碳捕获技术：聚焦吸附材料

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-10-13 DOI: 10.1016/j.jcou.2024.102955

Esther Pancione , Alessandro Erto , Francesco Di Natale , Amedeo Lancia , Marco Balsamo

Onboard carbon capture systems are among the most promising strategies for decarbonization of the maritime sector in the short and medium term. These systems are based on post-combustion technologies, such as absorption, adsorption, calcium looping, membrane separation, and cryogenic technologies. They can be installed on existing ships without conflicting with other available carbon mitigation measures. Temperature Swing Adsorption (TSA) is one of the most proficient solutions; however, for effective use in the maritime sector, it is crucial to investigate adsorbent materials that are suitable for the specific conditions of flue gas deriving from ship engines. To this aim, attention should be focused on those materials that have i) high CO₂ adsorption capacities per unit of volume due to the expected space limitations on board ships, ii) good performances at relatively high temperatures in the presence of water and other chemical species (such as sulphur and nitrogen oxides and particulate matter), iii) easy regeneration patterns and iv) ideally highest possible efficiencies.

This paper provides an overview of the existing post-combustion technologies, focusing on their key technical aspects. Subsequently, starting from observing the great potentiality of TSA processes, a review of potential adsorbents for CO₂ capture in the maritime sector is reported. Functionalized materials, mainly with amines or potassium carbonate, show superior performance and are the most suitable option for on board ship applications. Ultimately, the paper aims to establish a baseline for possible TSA-based carbon capture applications in the maritime sector and stimulate further research in designing optimized CO₂ adsorption processes.

船载碳捕获系统是中短期内最有希望实现海运业脱碳的战略之一。这些系统基于燃烧后技术，如吸收、吸附、钙循环、膜分离和低温技术。这些系统可以安装在现有船舶上，不会与其他可用的碳减排措施发生冲突。变温吸附（TSA）是最有效的解决方案之一；然而，要在海事领域有效使用，关键是要研究适合船舶发动机烟气特定条件的吸附材料。为此，应重点关注以下材料：i) 由于船上空间有限，单位体积内的二氧化碳吸附能力强；ii) 在水和其他化学物质（如硫和氮氧化物以及颗粒物质）存在的相对高温条件下性能良好；iii) 易于再生；iv) 理想情况下具有尽可能高的效率。本文概述了现有的燃烧后技术，重点关注其关键技术方面。随后，从观察 TSA 工艺的巨大潜力入手，报告了海事领域二氧化碳捕获的潜在吸附剂。以胺或碳酸钾为主的功能化材料表现出卓越的性能，是最适合船上应用的选择。最终，本文旨在为海运领域可能的基于 TSA 的碳捕获应用建立一个基准，并激励在设计优化的二氧化碳吸附过程方面开展进一步的研究。

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引用次数: 0

Development of a novel bio char for CO2 capture and biogas upgrade: Static and dynamic testing 开发用于二氧化碳捕获和沼气升级的新型生物炭：静态和动态测试

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-10-13 DOI: 10.1016/j.jcou.2024.102958

Muhammad Imran-Masood , Enrique García-Díez , Muhammad Usman , Balaj Khan Lodhi , Muhammad Waqas , Susana García

The optimization of the pyrolysis of the spruce sawdust was conducted based on the yield, textural properties, and static capture capacity of the chars to generate a new micro porous char for biogas upgrade. The nature of the precursor (C: 45.68 %, H: 6.08 %, N: 0.15 %, and 0.34 % ash content) helped to tune the porosity of the char for capturing CO₂ from gas streams and biogas. The optimization of the pyrolysis at 700 °C, a heating rate of 10 °C / min and holding time of 1 hour, produced a microporous char with high yield, CO₂ capture capacity and CO₂/CH₄ selectivity. The presence of the oxygen and nitrogen-containing functional groups in the optimum char help in the selective capture of CO₂. The static CO₂ capture capacity of the optimum char was 1.98 mmol/g at atmospheric pressure and 25 °C (90 % CO₂ stream). The CSD (700−10−60) have capture capacity of 1.50 mmol/g (at a feed gas stream of 50 % CO₂ and adsorption temperature of 25 °C and 120 kPa) which is equivalent to Norit C and Calgon BPL. Hence, spruce sawdust can be used to produce efficient biochar for biogas upgrade (CO₂ capture) owing to high capture capacity and CO₂/CH₄ selectivity (around 3) and easy regeneration of the biochar for 10 consecutive cycles.

根据木炭的产量、质地特性和静态捕获能力，对云杉锯屑的热解进行了优化，以生成一种用于沼气升级的新型微孔木炭。前驱体的性质（C：45.68 %，H：6.08 %，N：0.15 %，灰分含量 0.34 %）有助于调节炭的孔隙率，以捕获气流和沼气中的二氧化碳。在 700 °C、10 °C/分钟的加热速率和 1 小时的保温时间条件下进行热解，可生产出具有高产率、二氧化碳捕获能力和二氧化碳/CH4 选择性的微孔炭。最佳炭中的含氧和含氮官能团有助于选择性捕获二氧化碳。在常压和 25 °C（90 % CO2 流）条件下，最佳炭的静态 CO2 捕获能力为 1.98 mmol/g。CSD（700-10-60）的捕集能力为 1.50 mmol/g（进料气流为 50 % CO2，吸附温度为 25 °C 和 120 kPa），相当于 Norit C 和 Calgon BPL。因此，云杉锯屑可用于生产高效的生物炭，用于沼气升级（二氧化碳捕集），因为它具有较高的捕集能力和二氧化碳/CH4 选择性（约为 3），而且生物炭易于连续再生 10 次。

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引用次数: 0

Strength and leaching behavior of CaO- and MgO-treated Cd-contaminated soils subjected to partial and full carbonation 经部分碳化和完全碳化的氧化钙和氧化镁处理的镉污染土壤的强度和浸出行为

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-10-01 DOI: 10.1016/j.jcou.2024.102953

Wentao Li , Junde Qin , Yaolin Yi

Cadmium (Cd)-contaminated soils may pose a significant threat on human health. They are often treated with quick lime (CaO) and reactive magnesia (MgO), but these treatments often result in low strength. Hence, in this study, partial and full carbonation are used to enhance the stabilization/solidification of CaO- and MgO-treated Cd-contaminated soils, aiming to achieve CO₂ sequestration, strength improvement, and Cd immobilization. Performance of treated contaminated soils is evaluated through unconfined compressive strength (UCS), leaching, X-ray diffraction (XRD), and thermogravimetric analysis (TGA) tests. The results indicate that carbonation significantly enhances the UCS of both CaO- and MgO-treated Cd-contaminated soils. After carbonation, MgO-treated soils exhibit higher UCS than CaO-treated soils. Partial and full carbonation yield similar UCS in CaO-treated soils, while full carbonation results in higher UCS in MgO-treated soils. For CaO-treated soils, partial carbonation keeps Cd leachability below the 1 mg/kg limit, but full carbonation increases it beyond this limit. In contrast, fully carbonated MgO-treated soils maintain Cd leachability below the limit, though partial carbonation leads to higher leachability. Formation of Ca and Mg carbonates contributes to the strength improvement of soils. Cd(OH)₂ and its complex, as well as CdCO₃ exist in partially and fully carbonated soils, lowering leached Cd concentration. Overall, partial carbonation is better for CaO-treated soils, while full carbonation is preferable for MgO-treated soils.

受镉 (Cd) 污染的土壤可能对人类健康构成严重威胁。人们通常使用生石灰（CaO）和活性氧化镁（MgO）来处理这些土壤，但这些处理方法通常会导致土壤强度较低。因此，本研究采用部分碳化和完全碳化的方法来提高经氧化钙和氧化镁处理过的镉污染土壤的稳定/固化程度，以实现二氧化碳封存、提高强度和固定镉的目的。通过无侧限抗压强度 (UCS)、浸出、X 射线衍射 (XRD) 和热重分析 (TGA) 测试评估了经处理的污染土壤的性能。结果表明，碳化能明显提高氧化钙和氧化镁处理过的镉污染土壤的无侧限抗压强度。碳化后，氧化镁处理过的土壤比氧化钙处理过的土壤显示出更高的 UCS。在氧化钙处理过的土壤中，部分碳化和完全碳化会产生相似的 UCS，而在氧化镁处理过的土壤中，完全碳化会产生更高的 UCS。对于氧化钙处理过的土壤，部分碳化可使镉浸出率保持在 1 毫克/千克的限度以下，但完全碳化则会使镉浸出率超过这一限度。相比之下，完全碳化的氧化镁处理过的土壤可使镉沥滤性保持在限值以下，但部分碳化会导致沥滤性升高。碳酸钙和碳酸镁的形成有助于提高土壤的强度。Cd(OH)2 及其复合物以及 CdCO3 存在于部分碳酸盐化和完全碳酸盐化的土壤中，从而降低了镉的浸出浓度。总体而言，部分碳酸盐化对 CaO 处理过的土壤更有利，而完全碳酸盐化对 MgO 处理过的土壤更有利。

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引用次数: 0

CO2 valorisation from lime production via Columbus process to produce E-methane for transport sector – A comprehensive life cycle assessment 通过哥伦布工艺将石灰生产过程中产生的二氧化碳变废为宝，为运输行业生产电子甲烷--综合生命周期评估

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-10-01 DOI: 10.1016/j.jcou.2024.102949

Jordy Motte , Erasmo Cadena , Yblin Roman Escobar , Jim Gripekoven , Koen Vlaeminck , Friso De Clercq , Pierre-Olivier Cambier , Nathalie Van Den Bogaert , Brecht De Roo , Jan Mertens , Jo Dewulf

In the next decades, CO₂ capture and utilisation (CCU) technologies can contribute to climate change mitigation. The Columbus project is an example of a CCU initiative in which CO₂ is captured from lime production and converted into E-methane via CO₂ methanation. E-methane can serve as fuel for ships and lorries to replace heavy fuel oil and diesel, respectively. This paper aims to assess the environmental impacts of E-methane production via the Columbus process, powered by renewable electricity, and its utilisation in the transport sector benchmarked to conventional fuel production (references) through life cycle assessment (LCA). A basket of products approach was used to also consider the co-products obtained from the Columbus process in the assessment. Both emission and resource based indicators were selected for the LCA. The results show that E-methane production and its utilisation in ships and lorries result in a decrease of the impact on climate change (35 %), particulate matter formation (94 %) and fossil resource use (85 %) compared to the references. For this comparison, the conventional production of the co-products was also taken into account. However, the production and utilisation of this fuel consumes more minerals and metals than the references. The higher mineral and metal extraction from the environment can be explained by the construction of the solar panels required to provide electricity for electrolysis. Future research should focus on the social acceptance and techno-economic assessment of the Columbus process.

在未来几十年中，二氧化碳捕集与利用（CCU）技术将有助于减缓气候变化。哥伦布项目（Columbus project）就是二氧化碳捕集与利用（CCU）技术的一个实例，该项目从石灰生产中捕集二氧化碳，并通过二氧化碳甲烷化将其转化为电子甲烷（E-methane）。电子甲烷可作为船舶和卡车的燃料，分别替代重油和柴油。本文旨在通过生命周期评估（LCA），以可再生电力为动力，评估哥伦布工艺生产的甲烷对环境的影响，以及甲烷在运输行业的使用情况，并以传统燃料生产（参考）为基准进行评估。在评估中还采用了一篮子产品的方法，以考虑哥伦布工艺获得的副产品。生命周期评估选择了基于排放和资源的指标。结果表明，与参照物相比，电子甲烷的生产及其在船舶和卡车中的使用可减少对气候变化的影响（35%）、颗粒物的形成（94%）和化石资源的使用（85%）。在进行比较时，还考虑了副产品的常规生产。然而，这种燃料的生产和利用比参考值消耗更多的矿物和金属。从环境中提取更多矿物和金属的原因可能是建造了为电解提供电力所需的太阳能电池板。今后的研究应侧重于哥伦布工艺的社会接受度和技术经济评估。

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引用次数: 0

Feedstock recycling of single-use garment simultaneously using CO2 and MSW incinerator bottom ash 同时利用二氧化碳和城市生活垃圾焚烧炉底灰回收一次性服装的原料

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-10-01 DOI: 10.1016/j.jcou.2024.102946

Doeun Choi , Jechan Lee

This study is aimed at proposing a feedstock recycling approach to make value-added monomer from single-use garment like stocking waste (SW) using incinerator bottom ash catalyst (IBAC). SW is made mainly of nylon 6 (>80 wt%) with minor components such as polyurethane. Thermochemical SW decomposition pathways are identified by evolved gas analysis and single-shot pyrolysis analysis, confirming that caprolactam (a value-added chemical re-used for manufacturing nylon 6) is the major product. IBAC is composed mainly of alkaline metal oxides (e.g., CaO). The use of IBAC in thermochemical SW conversion at 500 °C under CO₂ atmosphere increases the yield of caprolactam reaching 70.8 wt% (20 % higher than non-catalytic SW conversion (59.2 wt%)). Moreover, the caprolactam yield corrected to the nylon 6 content of SW is 86.8 wt%. The enhancement of caprolactam production by IBAC in CO₂ is most likely due to the synergistical effect of IBAC and CO₂ on promoting the molecular interaction of amide groups present on SW. It is hoped that this study brings the idea of new applications of concurrently reusing textile waste (e.g., SW) and municipal solid waste-treatment byproduct (e.g., IBAC).

本研究旨在提出一种原料循环利用方法，利用焚化炉底灰催化剂（IBAC）从一次性服装（如丝袜废料）中提取增值单体。SW 主要由尼龙 6（80%）和聚氨酯等次要成分制成。通过演化气体分析和单次热解分析确定了 SW 的热化学分解途径，证实己内酰胺（一种用于生产尼龙 6 的高附加值化学品）是主要产品。IBAC 主要由碱金属氧化物（如 CaO）组成。在二氧化碳气氛下于 500 °C 的热化学 SW 转化过程中使用 IBAC，可使己内酰胺的产率提高到 70.8%（比非催化 SW 转化（59.2%）高出 20%）。此外，根据 SW 中尼龙 6 含量校正的己内酰胺产量为 86.8 wt%。IBAC 在二氧化碳中提高己内酰胺产量的原因很可能是 IBAC 和二氧化碳在促进 SW 上酰胺基团分子相互作用方面的协同效应。希望这项研究能为同时再利用纺织废料（如 SW）和城市固体废物处理副产品（如 IBAC）带来新的应用思路。

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引用次数: 0

Effect of fly ash on hydration and carbonation of carbonation-cured Portland cements 粉煤灰对碳化固化硅酸盐水泥水化和碳化的影响

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-10-01 DOI: 10.1016/j.jcou.2024.102943

Geta Bekalu Belayneh , Naru Kim , Joonho Seo , Hansun Kim , Seunghee Park , H.M. Son , Solmoi Park

This study investigates the impact of fly ash on hydration and carbonation processes in carbonation-cured fly ash cements. Cement paste samples with fly ash replacement levels of 0 %, 5 %, 10 % and 30 % underwent carbonation curing for 28 days. Results reveal that the CaO content does not affect the final CO₂ absorption capacity. Instead, optimal fly ash replacement of 10 % enhances CO₂ uptake, yielding 52.9 g of CaCO₃ on the surface after 28 days of curing, compared to 43.4, 43.1 and 48.4 g for 0 %, 5 % and 30 % replaced samples, respectively. Additionally, fly ash incorporation significantly enhances belite reaction and improved CO₂ binding capacity. However, the reaction extent of alite was lower when exposed to CO₂-curing conditions. These findings advance understanding of blended cements in carbonation-curing, facilitating the development of environmentally friendly and durable concrete structures.

本研究探讨了粉煤灰对碳化固化粉煤灰水泥水化和碳化过程的影响。粉煤灰掺量分别为 0%、5%、10% 和 30% 的水泥浆样品经过 28 天的碳化固化。结果表明，氧化钙含量不会影响最终的二氧化碳吸收能力。相反，粉煤灰的最佳替代率为 10%，可提高二氧化碳吸收能力，固化 28 天后，表面产生 52.9 克 CaCO3，而替代率为 0%、5% 和 30%的样品分别为 43.4 克、43.1 克和 48.4 克。此外，粉煤灰的加入还能显著增强白云石反应，提高二氧化碳结合能力。然而，在二氧化碳固化条件下，白云石的反应程度较低。这些发现加深了人们对碳化固化过程中混合水泥的理解，有助于开发环保耐用的混凝土结构。

引用次数: 0

Effluent nozzles in reverse-vortex-stabilized microwave CO2 plasmas for improved energy efficiency 反向涡流稳定微波二氧化碳等离子体中的出流喷嘴，提高能源效率

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-10-01 DOI: 10.1016/j.jcou.2024.102952

C.F.A.M. van Deursen , H.M.S. van Poyer , W.A. Bongers , F.J.J. Peeters , F.M.A. Smits , M.C.M. van de Sanden

Energy efficiency and conversion in a reverse-vortex microwave CO₂ plasma are enhanced by optimizing the thermal trajectories using a converging diverging nozzle in subsonic flows. The nozzle mixes cold, unconverted gas at the edge of the flow with hot, active gas in the middle of the flow. Temperature measurements are taken of the quartz tube as well as just above the nozzle inlet and directly after the nozzle and presented to elucidate differences in performance. Measurements show significant improvements in conversion and energy efficiency, especially at pressures close to atmospheric pressure (500 – 900 mbar). In addition an improvement in plasma stability when adding a converging diverging nozzle. Thermal measurements also point towards a shift in energy loss mechanisms when changing flow configurations.

通过在亚音速流动中使用会聚发散喷嘴优化热轨迹，提高了反向涡流微波二氧化碳等离子体的能量效率和转换率。喷嘴将气流边缘未转化的冷气体与气流中间活跃的热气体混合在一起。对石英管、喷嘴入口正上方和喷嘴正后方进行温度测量，以阐明性能差异。测量结果表明，转换和能量效率有了显著提高，尤其是在压力接近大气压（500 - 900 毫巴）时。此外，当增加一个会聚发散喷嘴时，等离子体的稳定性也有所提高。热测量结果还表明，在改变流动配置时，能量损失机制也发生了变化。

引用次数: 0

Use of steel slag as carbonation material: A review of carbonation methods and evaluation, environmental factors and carbon conversion process 使用钢渣作为碳化材料：碳化方法与评估、环境因素和碳转化过程综述

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-10-01 DOI: 10.1016/j.jcou.2024.102947

Xiaozhe Zhang , Jihui Zhao , Yamei Liu , Jianxin Li

Steel slag, as a major solid waste in the steel industry, and its rational disposal is of significant meaning to the carbon emissions of the steel industry. Using steel slag as the carbon sequestration material to absorb the carbon dioxide from flue gases in the production process can realize the waste reuse and at the same time slow down the process of global warming. Although there have been many reports on the carbonation of steel slag, there is a lack of systematic reviews on the process and effect of steel slag carbonation. In this paper, the carbonation methods of steel slag and the evaluation methods of carbonation sequestration are reviewed in detail, and the effect of environmental factors on carbonation of steel slag are described. The mineral transformation and mechanism during carbonation are investigated, and the environmental and social benefits of steel slag carbonation are briefly explained. The study shows that aqueous carbonation is a widely used technical route, and temperature is the most significant factor affecting the carbonation effect of steel slag. Steel slag carbonation has a very broad application prospect and has significant technological advantages in the global warming background.

钢渣作为钢铁行业的主要固体废弃物，其合理处置对钢铁行业的碳排放具有重要意义。利用钢渣作为固碳材料，吸收生产过程中烟气中的二氧化碳，可以实现废物再利用，同时减缓全球变暖的进程。虽然关于钢渣碳化的报道很多，但缺乏对钢渣碳化过程和效果的系统综述。本文详细综述了钢渣的碳化方法和碳化固碳的评价方法，并阐述了环境因素对钢渣碳化的影响。研究了碳化过程中的矿物转化及机理，并简要阐述了钢渣碳化的环境效益和社会效益。研究表明，水碳化是一种广泛应用的技术路线，温度是影响钢渣碳化效果的最主要因素。在全球变暖的背景下，钢渣碳化具有非常广阔的应用前景和显著的技术优势。

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引用次数: 0

Evaluation of CO2 storage properties and mobility through NMR technique in post-grafting synthetized organically functionalized porous silica 通过核磁共振技术评估接枝后合成的有机功能化多孔二氧化硅的二氧化碳储存特性和流动性

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-10-01 DOI: 10.1016/j.jcou.2024.102945

Cataldo Simari , Giuseppe Conte , Ana-Maria Lacrămă , Roxana Nicola , Carlo Poselle Bonaventura , Giovanni Desiderio , Isabella Nicotera , Raffaele G. Agostino , Alfonso Policicchio

Functionalized porous silica materials were synthesized in alkaline conditions by post-grafting method using hexadecyltrimethylammonium bromide (CTAB) as templating agent, tetraethyl orthosilicate (TEOS) as silica precursors and trialkoxysilanes functionalised with different organic groups. Textural features, halfway between microporosity and mesoporosity, combined with the surface physico-chemical ones related to various organic groups, determined different CO₂ storage properties highlighting a strong interaction with the precursor 3-Aminopropyl)triethoxysilane. NMR spectroscopy also showed how physisorption is the mainstream mechanism for CO₂ adsorption in all the sorbents, except for the aforementioned organic group in which an important chemisorption contribution occurs. Diffusion and molecular mobility analysis revealed that at least two species coexist within the micro-/meso-pores of the sorbents, namely, CO₂ molecules powerfully interacting with the pore surface (pore-surface CO₂) and “bulk-like” CO₂ filling the central region of the pores. Furthermore, the post functionalization suppresses the diffusion of CO₂ molecules through the pore channels with all the functionalized materials exhibiting a single self-diffusion coefficient. On the other side, D// strictly depends on the average pore size of the sorbent.

以十六烷基三甲基溴化铵（CTAB）为模板剂，以正硅酸四乙酯（TEOS）为二氧化硅前驱体，以不同有机基团官能化的三烷氧基硅烷为载体，通过后接枝法在碱性条件下合成了官能化多孔二氧化硅材料。介于微孔和中孔之间的纹理特征，以及与各种有机基团相关的表面物理化学特征，决定了不同的二氧化碳储存特性，突出了与前驱体 3-氨基丙基三乙氧基硅烷的强烈相互作用。核磁共振光谱还显示，物理吸附是所有吸附剂吸附二氧化碳的主流机制，但上述有机基团除外，因为其中存在重要的化学吸附作用。扩散和分子迁移率分析表明，在吸附剂的微孔/介孔中至少有两种物质共存，即与孔表面有强烈相互作用的二氧化碳分子（孔表面二氧化碳）和填充在孔中心区域的 "大块 "二氧化碳。此外，后功能化抑制了二氧化碳分子在孔道中的扩散，所有功能化材料都表现出单一的自扩散系数。另一方面，D// 严格取决于吸附剂的平均孔径。

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引用次数: 0