Journal of CO2 Utilization最新文献

Liquid-phase CO2 hydrogenation to methanol synthesis: Solvent screening, process design and techno-economic evaluation 液相二氧化碳加氢合成甲醇：溶剂筛选、工艺设计和技术经济评估

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-11-16 DOI: 10.1016/j.jcou.2024.102976

Dongliang Wang , Yun Du , Zuwei Liao , Xiaodong Hong , Shilong Zhang

This paper focuses on a liquid-phase CO₂ hydrogenation process for methanol synthesis to enhance CO₂ conversion. The feasibility of a liquid-phase CO₂ hydrogenation process is comprehensively evaluated through a techno-economic analysis. The solvent tetraethylene glycol dimethyl ether is identified as one of the most favorable options following an analysis of the solubility data pertaining to various solvents and their influence on the reaction equilibrium of the substances within the system. The influence of process parameters, including temperature, pressure, solvent amount, and gas hourly space velocity (GHSV), on the conversion of CO₂ and the selectivity for methanol is examined and optimized in a liquid-phase CO₂ hydrogenation to methanol process without a gas recycle (Process 1), optimal reaction conditions are determined and a CO₂ conversion of 95.19 % and a CH₃OH yield of 94.77 % with a purity of 99.9 % are achieved. A liquid-phase process with a gas recycle (Process 2) is implemented to enhance the utilization of feed gas, achieving a CO₂ conversion rate of 95.23 % and a methanol yield of 99.69 %. The liquid-phase process is further optimized by incorporating reactive distillation technology (Process 3), to enhance reaction efficiency and reduce energy consumption. Following the techno-economic evaluation, the energy efficiency of Process 3 is 7.79 % and 4.99 % higher than that of Process 1 and Process 2, respectively. The product cost of Process 3 is reduced by 8.75 % compared to Process 1 and by 4.25 % compared to Process 2. This research offers insights into the challenges associated with the development of the liquid-phase method.

本文重点介绍一种用于甲醇合成的液相二氧化碳加氢工艺，以提高二氧化碳的转化率。通过技术经济分析，全面评估了液相二氧化碳加氢工艺的可行性。在分析了各种溶剂的溶解度数据及其对系统内物质反应平衡的影响后，确定溶剂四甘醇二甲醚是最有利的选择之一。在无气体循环的液相二氧化碳加氢制甲醇工艺（工艺 1）中，考察并优化了工艺参数（包括温度、压力、溶剂量和气体时空速度 (GHSV)）对二氧化碳转化率和甲醇选择性的影响，确定了最佳反应条件，二氧化碳转化率达到 95.19%，CH3OH 收率达到 94.77%，纯度达到 99.9%。为了提高原料气的利用率，采用了气体循环液相工艺（工艺 2），二氧化碳转化率达到 95.23%，甲醇产率达到 99.69%。通过采用反应蒸馏技术（工艺 3）进一步优化了液相工艺，以提高反应效率并降低能耗。经过技术经济评估，工艺 3 的能效分别比工艺 1 和工艺 2 高 7.79 % 和 4.99 %。工艺 3 的产品成本比工艺 1 降低了 8.75%，比工艺 2 降低了 4.25%。这项研究有助于深入了解与开发液相法相关的挑战。

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引用次数: 0

Recent advancements in integrating CO2 capture from flue gas and ambient air with thermal catalytic conversion for efficient CO2 utilization 将烟气和环境空气中的二氧化碳捕集与热催化转化相结合以高效利用二氧化碳的最新进展

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-11-01 DOI: 10.1016/j.jcou.2024.102973

Ruoyu Zhang , Zhenwei Xie , Qingfeng Ge , Xinli Zhu

Capturing CO₂ and converting it into valuable chemicals and fuels have been regarded as a pivotal strategy in addressing the environmental challenges of ever-growing CO₂ emissions. Combining CO₂ capture and conversion through material or process integration can eliminate the energy-intensive steps such as separation, compression, and transportation across a wide range of space and temperatures. The flue gas at high temperatures > 300 °C can be handled with dual-function materials consisting of sorbents and catalysts. The dual-function materials combine CO₂ capture and conversion through material integration, converting CO₂ with reactions such as methanation, reverse water-gas shift, dry reforming of CH₄, and oxidative dehydrogenation of propane. On the other hand, capturing CO₂ from air directly requires a long time to collect enough CO₂ for the subsequent conversion reaction. Consequently, direct air capture will likely combine with the conversion reactions in stepwise operations. The low latent heat in CO₂ from direct air capture makes it more suitable for reactions at a mild condition (< 250 °C), and stepwise operation allows the separate control of the capture and conversion conditions. Herein, we reviewed recent advancements in coupling CO₂ capture from flue gas and ambient air with thermal catalytic conversion. We discussed the requirements for materials, reactor configuration, and process operation for capturing and converting CO₂ from these sources and proposed that future research should focus on enhancing the efficiency, scalability, and sustainability of CO₂ capture and conversion technologies and optimizing the process design.

捕获二氧化碳并将其转化为有价值的化学品和燃料，一直被视为应对二氧化碳排放量不断增长所带来的环境挑战的关键战略。通过材料或工艺集成将二氧化碳捕集和转化结合起来，可以省去分离、压缩和跨空间、跨温度运输等高能耗步骤。由吸附剂和催化剂组成的双功能材料可处理 300 °C 高温烟气。双功能材料通过材料集成将二氧化碳捕获和转化结合在一起，通过甲烷化、反向水气变换、CH4 干重整和丙烷氧化脱氢等反应转化二氧化碳。另一方面，直接从空气中捕获二氧化碳需要很长时间才能收集到足够的二氧化碳进行后续转化反应。因此，直接从空气中捕获二氧化碳可能会与转化反应相结合，分步进行。直接从空气中捕获二氧化碳的潜热较低，因此更适合在温和的条件下（250 °C）进行反应，而且分步操作可以分别控制捕获和转化条件。在此，我们回顾了从烟道气和环境空气中捕集二氧化碳并进行热催化转化的最新进展。我们讨论了从这些来源捕集和转化二氧化碳对材料、反应器配置和工艺操作的要求，并建议未来的研究应侧重于提高二氧化碳捕集和转化技术的效率、可扩展性和可持续性，以及优化工艺设计。

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引用次数: 0

Progress in development of characterization capabilities to evaluate candidate materials for direct air capture applications 在开发表征能力以评估直接空气捕获应用的候选材料方面取得进展

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-11-01 DOI: 10.1016/j.jcou.2024.102975

Marcus Carter , Huong Giang T. Nguyen , Andrew J. Allen , Feng Yi , Wei-Chang D. Yang , Avery E. Baumann , W. Sean McGivern , Jeffrey A. Manion , Ivan Kuzmenko , Zois Tsinas , Charlotte M. Wentz , Malia Wenny , Daniel W. Siderius , Roger D. van Zee , Christopher M. Stafford , Craig M. Brown

As part of U.S. national efforts to combat the detrimental effect of global climate change, the National Institute of Standards and Technology (NIST) was recently tasked to support efforts in direct air capture (DAC) of carbon dioxide research and deployment. In order to develop test procedures, materials, and documentary standards, key characterization methods relevant to DAC materials have been investigated and used to identify desirable properties for a potential Standard Reference Material (SRM). Select amine-supported materials that previously showed potential for DAC applications have been characterized using commonly available laboratory methods. Further insights into the adsorption characteristics have been gained from developing and applying more specialized characterization tools ideal for probing low concentrations of carbon dioxide. A broad suite of capabilities that examine relevant properties under appropriate conditions gives the most profound insights into a material’s specific performance. We advocate for even more specialized capabilities to be developed and standardized to quantitatively monitor the interactions of CO₂ with molecular species in complex and often disordered systems to advance DAC and support carbon dioxide reduction (CDR) in general.

作为美国应对全球气候变化有害影响的国家努力的一部分，美国国家标准与技术研究院（NIST）最近受命支持二氧化碳直接空气捕集（DAC）的研究和部署工作。为了开发测试程序、材料和文件标准，对与 DAC 材料相关的关键表征方法进行了调查，并用于确定潜在标准参考材料 (SRM) 的理想属性。使用常见的实验室方法，对之前显示出 DAC 应用潜力的部分胺支持材料进行了表征。通过开发和应用非常适合探测低浓度二氧化碳的更专业的表征工具，我们对吸附特性有了更深入的了解。在适当的条件下对相关特性进行研究的广泛能力，可以最深入地了解材料的具体性能。我们主张开发更专业的能力并使之标准化，以定量监测二氧化碳与复杂且通常无序的系统中分子物种的相互作用，从而推动 DAC 的发展并支持二氧化碳减排 (CDR)。

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引用次数: 0

Evolution law of the pore structure of CO2-H2O-coal in liquid CO2-ECBM 液态 CO2-ECBM 中 CO2-H2O 煤孔隙结构的演变规律

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-11-01 DOI: 10.1016/j.jcou.2024.102971

Xiaojiao Cheng , Hu Wen , Shixing Fan , Bocong Liu , Rijun Li , Yanhui Xu , Wen Wang

Liquid CO₂ enhancing coalbed methane recovery (CO₂-ECBM) is an effective and intrinsically reliable gas drainage technology. Injection of liquid CO₂ into coal seam has the dual effect of increasing the permeability of the coal and rock and strengthening the recovery of gas, which is manifested primarily as “pressure cracking, low temperature frostbite, physical extraction and chemical corrosion, phase change pressurization, low viscosity permeability, competitive adsorption”. In this paper, the acidification and corrosion of CO₂-H₂O-coal was studied in physical and chemical extraction by experimental test and comparative analysis. The liquid CO₂ acidification reference group and the variable group experiment were designed. On the basis of the pH value of the aqueous solution, the content of major elements and minerals in coal, the minerals involved in chemical reaction, and their specific gravity were deduced. Variation in pore volume, specific surface area, and pore fractal characteristics were quantitatively and qualitatively analyzed. The experimental results show that the higher the pressure, the higher the content of carbonic acid dissolved in water and the amount of H⁺ ionized by carbonic acid. The longer the reaction time, the greater the mineral content involved in the chemical reaction, and the H⁺ in the water sample is consumed in large quantities. The elements of Na, K, Ca, Mg, Al, Si, S, P, and Ti decreased with increasing pressure, and the maximum decreases were 0.004 %, 0.024 %, 1.095 %, 0.028 %, 0.220 %, 0.304 %, 0.006 %, 0.003 % and 0.029 %, respectively. The decrease in Ca element was the largest, indicating that Ca-bearing minerals participate in the reaction. Calcite, kaolinite, and illite were the main minerals involved in the chemical reaction of CO₂-H₂O-coal. The pores (d > 100 nm) and transition pores (10 < d < 100 nm) in the sample were further developed, and the pore volume increased significantly, forming a good gas migration channel. In addition, the number of new micropores (2 < d < 10 nm) increases, the specific surface area increases significantly, and the complexity of the pores increases, forming a good reservoir.

液态二氧化碳提高煤层气采收率（CO2-ECBM）是一种有效且内在可靠的瓦斯抽采技术。向煤层注入液态 CO2 具有提高煤岩透气性和强化瓦斯采收的双重作用，主要表现为 "压力裂解、低温冻伤、物理抽采和化学腐蚀、相变增压、低粘度渗透、竞争吸附 "等。本文通过实验测试和对比分析，研究了 CO2-H2O 煤在物理萃取和化学萃取中的酸化和腐蚀问题。设计了液态 CO2 酸化参照组和变量组实验。根据水溶液的 pH 值，推断出煤中主要元素和矿物质的含量、参与化学反应的矿物质及其比重。对孔隙体积、比表面积和孔隙分形特征的变化进行了定量和定性分析。实验结果表明，压力越高，水中溶解的碳酸含量和碳酸电离出的 H+ 量越高。反应时间越长，参与化学反应的矿物质含量越高，水样中的 H+ 被大量消耗。随着压力的增加，Na、K、Ca、Mg、Al、Si、S、P、Ti 元素的含量分别减少了 0.004 %、0.024 %、1.095 %、0.028 %、0.220 %、0.304 %、0.006 %、0.003 % 和 0.029 %。钙元素的降幅最大，表明含钙矿物参与了反应。方解石、高岭石和伊利石是参与 CO2-H2O 煤化学反应的主要矿物。样品中的孔隙（d > 100 nm）和过渡孔隙（10 < d < 100 nm）进一步发育，孔隙体积明显增大，形成了良好的气体迁移通道。此外，新的微孔（2 < d < 10 nm）数量增加，比表面积显著增大，孔隙的复杂性增加，形成了良好的储层。

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引用次数: 0

A stable dual-function lanthanum MOF: Simultaneous CO2 capture and catalysis 稳定的双功能镧系 MOF：同时实现二氧化碳捕获和催化

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-11-01 DOI: 10.1016/j.jcou.2024.102974

Ying-chao Wang , Ming-ming Zhai , He-xiang Huang , Zheng-hui Shi , Yuan-zhe Li , Cheng-cheng Zhao , Kang-ning Xie , Xiu-yuan Li , Yan-fei Hu , Zhi-hua Qiao , Chi Tang , Chen-xu Zhang

Carbon dioxide (CO₂) capture has become a hot topic in recent years because of global warming issues. However, most research has focused primarily on gas capture, with limited methods available for achieving both CO₂ capture and conversion within a single material. Here, we synthesized FMU-101, a metal-organic framework (MOF) with metal-open sites, through the self-assembly of [1,1′-Biphenyl]-3,3′,5-tricarboxylic acid and lanthanide ions in a solvothermal environment. FMU-101 features hexagonal one-dimensional pores with a diameter of 1.4 nm. The presence of free dimethylamine cations and metal open sites in the channel contributes to its remarkable capability for selectively enriching CO₂ from CO₂/CH₄ mixtures in dynamic breakthrough experiments. Furthermore, the metal-open sites in FMU-101 play a crucial role in CO₂ fixation, serving as effective catalytic sites for converting the adsorbed CO₂ into high-value chloropropylene carbonate, a versatile chemical intermediate. The segregation and conversion mechanisms were further elucidated through density-functional theory (DFT) calculations and Grand Canonical Monte Carlo (GCMC) simulations, which highlighted the critical role of metal-open sites in CO₂ adsorption and transformation.

近年来，由于全球变暖问题，二氧化碳（CO2）捕集已成为一个热门话题。然而，大多数研究主要集中在气体捕集方面，在单一材料中同时实现二氧化碳捕集和转化的方法非常有限。在这里，我们通过[1,1′-联苯]-3,3′,5-三羧酸和镧离子在溶热环境中的自组装，合成了具有金属开放位点的金属有机框架（MOF）FMU-101。FMU-101 具有直径为 1.4 纳米的六角形一维孔隙。由于通道中存在游离的二甲基胺阳离子和金属开放位点，因此在动态突破实验中，FMU-101 能够从 CO2/CH4 混合物中选择性地富集二氧化碳。此外，FMU-101 中的金属开放位点在二氧化碳固定过程中发挥了关键作用，是将吸附的二氧化碳转化为高价值的碳酸氯丙烯酯（一种多功能化学中间体）的有效催化位点。通过密度函数理论（DFT）计算和大卡农蒙特卡罗（GCMC）模拟，进一步阐明了分离和转化机制，突出了金属开放位点在二氧化碳吸附和转化中的关键作用。

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引用次数: 0

In situ evolution of surface and bulk properties of Ni/La-doped CeO2 catalysts for CO2 reduction with hydrogen 用于氢气还原二氧化碳的掺镍/掺镭 CeO2 催化剂表面和块体性能的原位演化

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-11-01 DOI: 10.1016/j.jcou.2024.102969

Belén Bachiller-Baeza , João Elias F.S. Rodrigues , Maricarmen Capel-Sanchez , Javier Gainza , Victoria E. García-Sánchez , Ignacio J. Villar-García , Virginia Perez-Dieste , Carlo Marini , M. Teresa Fernández-Diaz , José A. Alonso , Consuelo Álvarez-Galván

In this work, key factors that affect catalytic activity of Ni/La-doped ceria catalysts for the reverse water gas shift reaction (RWGS) have been revealed by applying in situ advanced synchrotron techniques, such as X-ray Absorption Spectroscopy (XAS) and Near-ambient pressure X-ray Photoelectron spectroscopy (NAP-XPS). Complementary ex situ characterization techniques have been also used, adding valuable insights on different physicochemical properties of the catalysts. Lanthanum incorporates into the ceria lattice, increasing oxygen mobility, which has a role in the formation of H₂O during the reaction. The optimum substitution degree of Ce by La that maximizes CO yield is close to 10 %. It is found that both bulk and surface Ce³⁺ proportions depend on the proportion of La, increasing with La content. At a reaction temperature of 873 K, bulk Ce³⁺ proportions are higher than surface ones. These differences are due to oxidative phenomena, associated to the reactive mixture that take place on the surface, such as CO₂ adsorption and H₂O formation. Concerning Ni phase, NiO bulk reduction to metallic Ni is very fast (in the range 573–623 K), however, Ni⁰ and Ni²⁺ species coexist on the surface during the reaction. It is found that a higher proportion of surface metallic Ni promotes the selectivity towards the RWGS, inhibiting the competing methanation reaction. On the other hand, La doping is relevant for the formation of lanthanum oxycarbonate, which has a role gasifying carbon deposits.

在这项研究中，通过应用 X 射线吸收光谱（XAS）和近常压 X 射线光电子能谱（NAP-XPS）等原位先进同步辐射技术，揭示了影响用于反向水煤气变换反应（RWGS）的掺镍/掺镭铈催化剂催化活性的关键因素。此外，还使用了补充性的原位表征技术，为催化剂的不同物理化学特性增添了宝贵的见解。镧加入到铈晶格中，增加了氧的流动性，从而在反应过程中形成 H2O。铈对镧的最佳取代度接近 10%，可使 CO 产率最大化。研究发现，体积和表面 Ce3+ 的比例都取决于 La 的比例，随着 La 含量的增加而增加。在 873 K 的反应温度下，块状 Ce3+ 的比例高于表面 Ce3+ 的比例。这些差异是由于氧化现象造成的，与表面发生的反应混合物有关，如 CO2 吸附和 H2O 形成。关于镍相，NiO 体积还原成金属镍的速度非常快（在 573-623 K 范围内），但在反应过程中，Ni0 和 Ni2+ 物种在表面共存。研究发现，表面金属镍的比例越高，对 RWGS 的选择性越大，从而抑制了竞争性的甲烷化反应。另一方面，La 掺杂与氧碳酸镧的形成有关，而氧碳酸镧具有气化碳沉积物的作用。

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引用次数: 0

The development trends, technological competition situations and cooperation status of carbon-negative technology: A patent landscape analysis 负碳技术的发展趋势、技术竞争态势与合作现状：专利格局分析

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-11-01 DOI: 10.1016/j.jcou.2024.102966

Xin Li, Ning Gao, Fei Yuan, Lucheng Huang

In the context of carbon neutrality, carbon-negative technology is considered a crucial technology for reducing carbon emissions and achieving carbon neutrality. Carbon-negative technology has gained attention from governments, businesses and academia. To comprehend the overall development status of carbon-negative technology, including the core technologies, the patent landscape, competition, and cooperation among major countries and regions, this paper proposes an analytical framework for the patent landscape of carbon-negative technology. The research results demonstrate the rapid overall development of carbon-negative technology. The R&D strategies of major competing countries in the field of carbon-negative technology focus on specific technology areas, and their core technologies exhibit similarities as well as differences. In the field of technology-based solutions, the United States and China dominate with their leaders and active contributors in various technology domains. The collaboration largely revolves around the United States, while other nations engage in less partnership and interaction. Countries have not yet established technological leadership in carbon sinks technology, and the cooperation network is relatively limited. These findings contribute to our understanding of the current global development status of carbon-negative technology, as well as the competitive levels and positions of major countries in this field. These findings also provide a decision-making basis and support for the development of carbon-negative technology.

在碳中和的背景下，负碳技术被认为是减少碳排放和实现碳中和的关键技术。负碳技术已受到政府、企业和学术界的关注。为了解负碳技术的整体发展状况，包括核心技术、专利格局、竞争以及主要国家和地区之间的合作情况，本文提出了负碳技术专利格局的分析框架。研究结果表明，负碳技术总体发展迅速。主要竞争国家在负碳技术领域的研发战略都集中在特定的技术领域，其核心技术既有相似之处，也有不同之处。在以技术为基础的解决方案领域，美国和中国以其在各个技术领域的领导者和积极贡献者而占据主导地位。合作主要围绕美国展开，其他国家的合作和互动较少。各国尚未在碳汇技术领域确立技术领导地位，合作网络也相对有限。这些发现有助于我们了解目前全球碳负技术的发展状况，以及主要国家在该领域的竞争水平和地位。这些发现也为发展碳负技术提供了决策依据和支持。

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引用次数: 0

Reactivity of aqueous carbonated cement pastes: Effect of chemical composition and carbonation conditions 水性碳化水泥浆的反应性：化学成分和碳化条件的影响

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-11-01 DOI: 10.1016/j.jcou.2024.102970

Fábio Maia Neto , Ruben Snellings , Jørgen Skibsted

Aqueous carbonation of end-of-life concrete fines is a promising method to alleviate greenhouse gas emissions by CO₂ sequestration from point-source emitters. This produces a valuable material that can be utilized in new cement formulations. This study investigates effects of the composition of cement pastes and of the carbonation conditions on the reactivity and phase assemblage for aqueous carbonated Portland cement pastes incorporating silica fume, fly ash, and blast furnace slag. Results from ²⁷Al and ²⁹Si NMR show that hydration of the carbonated pastes under reactivity test conditions lead to phase assemblages dominated by a C-(A)-S-H phase, with reduced Al/Si ratio, as well as by ettringite and hemi/monocarbonate AFm phases. The results from the reactivity tests demonstrate that the carbonated blended cement pastes exhibit superior reactivity compared to carbonated neat Portland cement paste because of their increased fraction of reactive alumina and silica species. The variations in carbonation conditions (i.e., temperature, CO₂ gas concentration, and solution composition) do not alter significantly the reactivity of the carbonated pastes. These findings demonstrate the robustness of aqueous carbonation of concrete fines and support its wider application as a mean to reduce CO₂ emissions and enhance circularity of cement-based materials.

对报废混凝土细料进行水碳化是一种很有前景的方法，可通过对点源排放者的二氧化碳进行封存来减少温室气体排放。这种方法产生的宝贵材料可用于新的水泥配方。本研究调查了水泥浆的成分和碳化条件对掺入硅灰、粉煤灰和高炉矿渣的水性碳化波特兰水泥浆的反应性和相组合的影响。27Al 和 29Si NMR 的结果表明，碳化浆料在反应性试验条件下进行水化，会产生以 C-(A)-S-H 相（铝/硅比率降低）为主的相组合，以及埃特林岩相和半碳酸盐/单碳酸盐 AFm 相。反应性测试结果表明，碳化混合水泥浆的反应性优于碳化纯波特兰水泥浆，这是因为它们的反应性氧化铝和二氧化硅种类的比例增加了。碳化条件（即温度、二氧化碳气体浓度和溶液成分）的变化不会显著改变碳化浆料的反应性。这些发现证明了混凝土细料水溶液碳化的稳健性，并支持将其作为减少二氧化碳排放和提高水泥基材料循环性的一种手段加以广泛应用。

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引用次数: 0

Study on the deterioration and damage evolution characteristics of mechanical properties of siltstone after supercritical CO2 treatment 超临界二氧化碳处理后粉砂岩力学性能劣化和损伤演变特征研究

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-11-01 DOI: 10.1016/j.jcou.2024.102972

Jianfeng Hao , Chunyu Guo , Weiji Sun , Bing Liang , Bing Qin , Leilei Li

To quantitatively represent the deterioration law of the mechanical properties of siltstone after exposure to supercritical CO₂(SC-CO₂), experiments were conducted to test the mechanical parameters of rocks under the coupling effect of CO₂–water–rock interactions. The purpose of this study is to determine the evolution law and damage characteristics of each siltstone mechanical parameter under the action of SC-CO₂. In combination with numerical simulation results, this study revealed the damage evolution characteristics of rocks in a CO₂ geological storage reservoir. The research findings indicate that SC-CO₂ exhibits a certain time effect and causes non-uniform damage to siltstone. Both the deterioration law of the mechanical parameters and soaking time exhibited an exponential relationship. With increasing soaking time, both the uniaxial compressive strength and elastic modulus showed a decreasing tendency, whereas the Poisson's ratio showed a varying degree of increase. The total degree of deterioration gradually increased as the soaking time increased and approached a stable value. After exposure to SC-CO₂, the damage deformation and failure mode transitioned from brittle to plastic in the siltstone samples. In addition, there was a shift from a single axial crack failure pattern to a complex failure mode with multiple cracks. This study also derived a uniaxial compressive strength prediction model for siltstone based on soaking time, constructed an elastic modulus damage model, and established a fluid–solid coupling model considering damage in the CO₂ geological storage process. The experimental and numerical simulation results revealed that microstructural alterations occurred in the siltstone after exposure to SC-CO₂. Furthermore, it was discovered that damage accumulation from the micro- to macroscale ultimately led to a gradual deterioration in mechanical properties. The research results provide a theoretical basis for mechanical stability evaluation in CO₂ geological storage.

为了定量地反映粉砂岩在暴露于超临界二氧化碳（SC-CO2）后力学性能的劣化规律，进行了二氧化碳-水-岩石相互作用耦合效应下的岩石力学参数试验。本研究的目的是确定粉砂岩各力学参数在 SC-CO2 作用下的演变规律和破坏特征。结合数值模拟结果，本研究揭示了二氧化碳地质封存储层中岩石的损伤演化特征。研究结果表明，SC-CO2 具有一定的时间效应，会对粉砂岩造成不均匀的破坏。力学参数的劣化规律与浸泡时间呈指数关系。随着浸泡时间的延长，单轴抗压强度和弹性模量均呈下降趋势，而泊松比则呈不同程度的上升。随着浸泡时间的延长，总劣化程度逐渐增加，并接近稳定值。暴露于 SC-CO2 后，粉砂岩样品的破坏变形和破坏模式从脆性转变为塑性。此外，破坏模式也从单一轴向裂纹转变为多裂纹的复杂破坏模式。该研究还得出了基于浸泡时间的粉砂岩单轴抗压强度预测模型，构建了弹性模量损伤模型，并建立了考虑 CO2 地质封存过程中损伤的流固耦合模型。实验和数值模拟结果表明，粉砂岩暴露于 SC-CO2 后发生了微结构改变。此外，研究还发现，从微观到宏观尺度的损伤累积最终导致了力学性能的逐渐恶化。研究成果为二氧化碳地质封存中的力学稳定性评估提供了理论依据。

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引用次数: 0

Effects of the use of acetone as co-solvent on the financial viability of bio-crude production by hydrothermal liquefaction of CO2 captured by microalgae 使用丙酮作为助溶剂对通过热液液化微藻类捕获的二氧化碳生产生物原油的经济可行性的影响

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2024-11-01 DOI: 10.1016/j.jcou.2024.102960

David Ocampo , Elkin A. Gómez , Luis A. Ríos , Gabriel J. Vargas

Hydrothermal Liquefaction (HTL) is a promising technology to produce biocrude from microalgal biomass that has captured gaseous CO₂. However, several problems of this technology must still be solved to make it economically and technically feasible. One of the main problems in the financial viability of the HTL process is the low yield obtained when only water is used as a solvent, with results close to or lower than 30 wt%. This, in turn, increases the production cost to over 120 USD/BBL. In recent years, some authors have focused their efforts on increasing biocrude production through the extensive use of organic solvents, without considering the effects on economic viability. The present work evaluated the financial effect of using acetone as an organic co-solvent, finding that high acetone contents increased operating costs of the process, mainly due to losses in its handling and recovery. On the contrary, very low acetone contents had very little effect on the biocrude yield. It was possible to establish that concentrations close to 5 wt% of acetone, mixed with water, resulted in a yield of about 60 wt% and a production cost of 50 USD/BBL of biocrude, with an energetic densification of 30.25 MJ/kg and 8.60^∘ API, classifying it as heavy crude, which makes it necessary to include refining processes for heteroatom removal. Chemical characterization of biocrude revealed a high content of nitrogenous compounds (23.6 wt%) and oxygenated compounds (10.7 wt%), which have to be removed for the subsequent production of commercial liquid fuels. It is concluded that the use of a water-acetone mixture allows for obtaining positive operating profits, which helps to the high capital costs involved in this type of technology, making it more financially comparable with the conventional petroleum industry.

水热液化（HTL）是一种利用捕获气态二氧化碳的微藻生物质生产生物原油的前景广阔的技术。然而，要使这项技术在经济和技术上可行，还必须解决它的几个问题。HTL 工艺在经济可行性方面的一个主要问题是，仅用水作为溶剂时，产量较低，接近或低于 30 wt%。这反过来又将生产成本提高到 120 美元/BBL 以上。近年来，一些学者致力于通过大量使用有机溶剂来提高生物原油的产量，但并未考虑其对经济可行性的影响。本研究评估了使用丙酮作为有机辅助溶剂的经济效果，发现丙酮含量高会增加工艺的运营成本，主要原因是丙酮处理和回收过程中的损失。相反，极低的丙酮含量对生物原油产量的影响很小。可以确定的是，丙酮浓度接近 5 wt%（与水混合）时，生物原油的产量约为 60 wt%，生产成本为 50 美元/BBL，能量密度为 30.25 MJ/kg，API 为 8.60∘，属于重质原油，因此必须采用精炼工艺去除杂原子。生物原油的化学特征显示，含氮化合物（23.6 重量%）和含氧化合物（10.7 重量%）的含量较高，必须去除这些物质才能生产商业液体燃料。结论是，使用水-丙酮混合物可以获得积极的经营利润，这有助于降低这类技术所涉及的高昂资本成本，使其在财务上与传统石油工业更具可比性。

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引用次数: 0