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Enhanced solar-light driven CO2 conversion using Pt-doped graphitic carbon nitride photocatalyst 利用掺铂氮化石墨碳光催化剂提高太阳光驱动的二氧化碳转化率
IF 2.2 4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2023-12-06 DOI: 10.1002/ghg.2247
Thi Huong Pham, Minh Viet Nguyen, Thi Thu Hien Chu, Sung Hoon Jung, Taeyoung Kim

The increasing levels of carbon dioxide (CO2) in our atmosphere demand innovative and efficient methods for its reduction. In this context, we present an advanced solar-driven photocatalyst, Pt-doped graphitic carbon nitride (Pt/g-C3N4), specifically engineered for enhanced photoreduction of CO2. Our findings highlight the dual advantage of Pt/g-C3N4: enhanced visible light absorption and electron-hole pair dynamics, ensuring efficient carrier separation. Notably, the CO and CH4 yields, when employing Pt/g-C3N4, surpassed those with the pristine g-C3N4 catalyst by factors of 3.1 and 4.3, respectively. Moreover, the Pt/g-C3N4 catalyst exhibited consistent high-efficiency of CO2 conversion over successive cycles, emphasizing the catalyst's robustness. This work underscores the potential of Pt/g-C3N4 as a viable tool against escalating CO2 levels, paving the way for a green and sustainable conversion of this predominant greenhouse gas into beneficial chemicals. © 2023 Society of Chemical Industry and John Wiley & Sons, Ltd.

随着大气中二氧化碳(CO2)含量的不断增加,我们需要创新、高效的方法来减少二氧化碳。在此背景下,我们提出了一种先进的太阳能光催化剂--掺铂氮化石墨(Pt/g-C3N4),专门用于增强二氧化碳的光还原。我们的研究结果凸显了 Pt/g-C3N4 的双重优势:增强的可见光吸收和电子-空穴对动力学,确保了高效的载流子分离。值得注意的是,使用 Pt/g-C3N4 催化剂的 CO 和 CH4 产率分别比使用原始 g-C3N4 催化剂的产率高出 3.1 倍和 4.3 倍。此外,Pt/g-C3N4 催化剂在连续循环中表现出持续的高效二氧化碳转化率,突出了催化剂的稳健性。这项研究强调了 Pt/g-C3N4 作为一种可行工具来应对二氧化碳含量不断攀升的潜力,为将这种主要温室气体转化为有益化学品的绿色和可持续发展铺平了道路。© 2023 化学工业协会和 John Wiley & Sons, Ltd. 保留所有权利。
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引用次数: 0
Signal propagation from portable active seismic source (PASS) to km-scale borehole DAS for continuous monitoring of CO2 storage site 从便携式有源地震源(PASS)到千米级井眼DAS的信号传播,用于连续监测CO2储存地点
IF 2.2 4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2023-12-04 DOI: 10.1002/ghg.2249
Takeshi Tsuji, Eiichi Arakawa, Hitoshi Tsukahara, Fumitoshi Murakami, Naoshi Aoki, Susumu Abe, Takuya Miura

We have developed a portable active seismic source (PASS) to monitor CO2 storage reservoirs at a depth of approximately 1 km. Despite its small size, stacking the signals generated by the PASS improves the signal-to-noise ratio of the seismometer data far from the source. The smaller size and lower cost of the PASS enables its permanent deployment in many locations to continuously monitor CO2 storage reservoirs. To achieve continuous monitoring, distributed acoustic sensing (DAS) is also a vital technology. Based on DAS, we can continuously record the signal from the PASS in an extensive area, including within boreholes and offshore fields. Here we report application of the PASS for the borehole DAS system. We confirmed the PASS signal propagation to a depth of ∼1 km when we used a PASS with 630N at 50 Hz close to the wellhead and recorded the signal by the borehole fiber optic cable. The ability of the system to propagate the PASS signal to a depth of ∼1 km enables continuous monitoring of most CO2 storage reservoirs with high temporal resolution. Furthermore, deploying multiple PASS systems could improve the spatial resolution of monitoring results. © 2023 Society of Chemical Industry and John Wiley & Sons, Ltd.

我们开发了一种便携式活动地震源(PASS),用于监测深度约1公里的二氧化碳储层。尽管它的体积很小,但叠加由PASS产生的信号可以提高远离震源的地震仪数据的信噪比。由于PASS的体积更小,成本更低,因此可以在许多地方永久部署,持续监测二氧化碳储存库。为了实现连续监测,分布式声传感(DAS)也是一项至关重要的技术。基于DAS,我们可以在大范围内连续记录来自PASS的信号,包括井眼内和海上油田。本文报道了PASS在井下DAS系统中的应用。当我们在井口附近使用630N, 50 Hz的PASS时,我们确认了PASS信号的传播深度为1公里,并通过钻孔光纤电缆记录了信号。该系统能够将PASS信号传播到~ 1公里的深度,从而能够以高时间分辨率连续监测大多数二氧化碳储存库。此外,部署多个PASS系统可以提高监测结果的空间分辨率。©2023化学工业协会和John Wiley &儿子,有限公司
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引用次数: 0
Two-phase flow behavior in CO2 geological storage considering spatial parameter heterogeneity 考虑空间参数非均质性的CO2地质储层两相流动特性
IF 2.2 4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2023-12-01 DOI: 10.1002/ghg.2248
Yiyan Zhong, Qi Li, Liang Xu, Yiping Wen, Yunlu Hou, Wenbin Gao

Saline aquifer rocks exhibit significant spatial randomness due to geological sedimentation processes. To address the issue of the heterogeneity of rock formations in numerical simulations, it is common practice to homogenize rock layers with similar lithologies. However, the acceptability of the errors generated during homogenized computations is a major concern and should be investigated. Therefore, to study the influence of heterogeneity at the storage site on the CO2 migration behavior, the Monte Carlo simulation–random finite element method (MCS-RFEM) was combined with a CO2 two-phase flow model to compare the effects of the coefficient of variation (Cv) and correlation length (λx) of random reservoir permeability fields on the migration distance and extent of CO2 storage under the same mean conditions. The results showed that higher Cv and λx values significantly reduced the CO2 migration distance while increasing the spread extent. Compared to the homogeneous model, at a λx value of 100 m, the CO2 migration distance decreased by 5.05%, while the profile sweep area increased by 6.20%. Concurrently, with increasing Cv, the area with a CO2 volume fraction higher than 0.75 decreased by 20.22%, while an increase in λx resulted in a 42.35% increase in the area with a CO2 volume fraction higher than 0.75. Therefore, reservoirs with high Cv and low λx values are more suitable for safely storing CO2. © 2023 Society of Chemical Industry and John Wiley & Sons, Ltd.

由于地质沉积过程,含盐含水层表现出明显的空间随机性。为了解决数值模拟中岩层的非均质性问题,通常的做法是对具有相似岩性的岩层进行均质化。然而,在均匀化计算过程中产生的误差的可接受性是一个主要问题,应该进行研究。因此,为了研究储层非均质性对CO2迁移行为的影响,将蒙特卡罗模拟-随机有限元法(MCS-RFEM)与CO2两相流模型相结合,比较在相同平均条件下随机储层渗透率场的变异系数(Cv)和相关长度(λx)对CO2迁移距离和封存程度的影响。结果表明,较高的Cv和λx值显著减小了CO2的迁移距离,增加了CO2的扩散范围。与均匀模型相比,λx值为100 m时,CO2迁移距离减小了5.05%,剖面扫描面积增大了6.20%。同时,随着Cv的增大,CO2体积分数大于0.75的面积减少了20.22%,而λx的增大导致CO2体积分数大于0.75的面积增加了42.35%。因此,高Cv值和低λx值的储层更适合安全储存CO2。©2023化学工业协会和John Wiley &儿子,有限公司
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引用次数: 0
Experimental study on the flow characteristics of supercritical CO2 in reservoir sandstones from the Ordos Basin, China 鄂尔多斯盆地储层砂岩超临界CO2流动特征实验研究
IF 2.2 4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2023-11-29 DOI: 10.1002/ghg.2246
Qianlin Zhu, Dongbao Chen, Shijian Lu, Shaojin Jiang

Understanding the flow characteristics of supercritical CO2 in dry sandstones or those with low water content provides crucial information on the flow behavior in near-wellbore zone. We conducted supercritical CO2 core flooding experiments using sandstone cores extracted from potential CO2 reservoirs in the Ordos Basin, China. During the experiments, we reduced the water content of saturated cores by flushing with dry CO2 and subsequently vacuumizing them at a temperature of 35°C to simulate sandstones with low water content. The experimental results demonstrate that the CO2 permeability was initially high during the low differential pressure stage and remained constant as the differential pressure increased. In the carbonic acid solution injection experiment, we observed an increase in the flow rate of the solution with the continuous interaction in the cores from the Shanxi and Shihezi groups, while the Yanchang group exhibited the opposite effect. This increase in permeability can be attributed to mineral dissolution and the loss of fine particles. Conversely, the blockage of fine particles or the precipitation of dissolved minerals may lead to a decrease in permeability. After the CO2–water–rock interaction, the CO2 permeability decreased compared to before the interaction, indicating that adsorbed water, the precipitation of dissolved mineral, or pore throat blockage by fine particles could induce this permeability decrease. The impact of adsorbed water on the decrease in CO2 permeability is significant. Additionally, the CO2–water–rock interaction caused corrosion on the anorthite surface. Furthermore, calcite dispersed in connected pores displayed a more pronounced dissolution compared to cemented calcite. © 2023 Society of Chemical Industry and John Wiley & Sons, Ltd.

了解超临界CO2在干砂岩或低含水率砂岩中的流动特征,为研究近井带的流动特性提供了重要信息。利用鄂尔多斯盆地潜在CO2储层砂岩岩心进行了超临界CO2岩心驱替实验。在实验中,我们通过用干燥的CO2冲洗饱和岩心,然后在35℃的温度下抽真空,来降低岩心的含水量,模拟低含水量的砂岩。实验结果表明,低压差阶段CO2渗透率较高,随着压差的增大,渗透率保持不变。在碳酸溶液注入实验中,我们观察到随着碳酸溶液在山西组和石河子组岩心中的持续相互作用,碳酸溶液的流速增加,而延长组岩心则相反。渗透性的增加可归因于矿物溶解和细颗粒的损失。相反,细颗粒的堵塞或溶解矿物的沉淀可能导致渗透率降低。CO2 -水-岩相互作用后,CO2渗透率较相互作用前降低,说明吸附水、溶解矿物沉淀或细颗粒堵塞孔喉可能导致渗透率降低。吸附水对CO2渗透率降低的影响是显著的。此外,co2 -水-岩相互作用导致钙长石表面腐蚀。此外,与胶结方解石相比,分散在连通孔隙中的方解石表现出更明显的溶解。©2023化学工业协会和John Wiley &儿子,有限公司
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引用次数: 0
Developing a roadmap for carbon capture, and storage in Oklahoma by assessing the viability of stacked storage 通过评估堆叠储存的可行性,为俄克拉荷马州的碳捕获和储存制定路线图
IF 2.2 4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2023-11-09 DOI: 10.1002/ghg.2244
Marcos W. Miranda, Jonathan D. Ogland-Hand, Jeffrey M. Bielicki, Rouzbeh G. Moghanloo, Jamal DaneshFar, Richard S. Middleton

The Intergovernmental Panel on Climate Change concludes that CO2 capture and storage (CCS) is critical for climate-stabilizing energy transitions. In CCS, captured CO2 is sequestered in saline aquifers within sedimentary basins. The CO2 storage capacity and the rate of injection are functions of the geology of the saline aquifer, which is uncertain. To minimize impacts of this uncertainty, CCS projects could include backup plans, such as co-locating geologic CO2 storage (GCS) sites with or near existing CO2-enhanced oil recovery (CO2-EOR) operations. These “stacked storage” projects could hedge against uncertainty in the saline formation performance because captured CO2 could be injected into either location in the event of unexpected events (e.g., the injectivity decreases). Here, we investigate the possibility and ramifications of developing CCS networks in Oklahoma that are amendable to stacked storage. We find that stacked storage is possible in Oklahoma but the counties with the lowest-cost saline storage resources do not have existing CO2-EOR operations. At the systems level, we find it is slightly more expensive (e.g., $1/tCO2 to $5/tCO2) to site GCS in counties with CO2-EOR projects. This increased expense is largely due to increased CO2 transportation costs because hundreds of km of additional pipeline is required to capture CO2 from the lowest-cost sources. Overall, our results suggest that it is optimal to build more pipelines and avoid injecting CO2 in some of the lowest-cost saline storage resources, to enable capturing CO2 from the least-cost sources. © 2023 Society of Chemical Industry and John Wiley & Sons, Ltd.

政府间气候变化专门委员会得出结论,二氧化碳捕集与封存(CCS)对于稳定气候的能源转型至关重要。在CCS中,捕获的二氧化碳被隔离在沉积盆地的含盐含水层中。CO2储存量和注入速率是咸水层地质的函数,具有不确定性。为了最大限度地减少这种不确定性的影响,CCS项目可以包括备用计划,例如将地质二氧化碳储存(GCS)地点与现有的二氧化碳提高采收率(CO2- eor)作业共同安置或靠近。这些“堆叠储存”项目可以对冲含盐地层性能的不确定性,因为在发生意外事件(例如,注入能力下降)时,捕获的二氧化碳可以注入到任何一个位置。在这里,我们研究了在俄克拉荷马州开发CCS网络的可能性和后果,这些网络可以修改为堆叠存储。我们发现叠储在俄克拉何马州是可行的,但拥有成本最低的盐储资源的县没有现有的二氧化碳提高采收率作业。在系统层面,我们发现在有CO2-EOR项目的县部署GCS的成本略高(例如,1美元/吨二氧化碳到5美元/吨二氧化碳)。增加的费用主要是由于二氧化碳运输成本的增加,因为从成本最低的来源捕获二氧化碳需要数百公里的额外管道。总的来说,我们的研究结果表明,建设更多的管道,避免在一些成本最低的盐水储存资源中注入二氧化碳,从而从成本最低的来源捕获二氧化碳是最理想的。©2023化学工业协会和John Wiley &儿子,有限公司
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引用次数: 0
Optimization of calcium carbide residue utilization for producing high-quality calcium carbonate 电石渣生产优质碳酸钙的优化利用
IF 2.2 4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2023-10-28 DOI: 10.1002/ghg.2245
Yuhang Yang, Wenxiu Li, Zhiwei Xun, Zhenwei Yi, Tao Wang, Zitao Yu, Yan Huang, Yongzheng Gu

In light of the current situation where the utilization of calcium carbide slag yields low profits but holds significant potential for reducing carbon emissions, ammonium acetate was employed to leach calcium carbide slag. It also played a crucial role in regulating the products of indirect carbon dioxide carbonation when mixed with glycine and lye. Ammonium acetate's significance underscores its dual role in both the leaching and carbonation processes. This process yielded calcium carbonate with particle sizes smaller than 100 nm, with a purity of 98% and a single vaterite phase. The calcium carbide residue demonstrated an impressive CO2 uptake rate of 23.5%. Ammonium acetate exhibited an efficiency of 79.2% as a leaching agent. The ammonium acetate method demonstrated enhanced environmental friendliness and facilitated a more efficient carbon uptake rate of 23.5% compared to conventional indirect methods. Furthermore, the addition of lye, glycine, and ammonium acetate effectively extended the nucleation time of the calcium carbonate crystals and induced the formation of more vaterite intermediates with smaller particle sizes. The influence mechanism of compound additives on the carbonation reaction was revealed through kinetic analysis and molecular dynamics. This innovative approach offers a promising avenue for simultaneously treating solid waste and reducing CO2 emission. © 2023 Society of Chemical Industry and John Wiley & Sons, Ltd.

针对电石渣利用效益低但碳减排潜力大的现状,采用醋酸铵对电石渣进行浸出。它在调节二氧化碳与甘氨酸和碱液混合时的间接碳酸化产物中也起着至关重要的作用。乙酸铵的意义在于它在浸出和碳酸化过程中的双重作用。该工艺制得的碳酸钙粒径小于100 nm,纯度为98%,且为单一水晶石相。电石渣的CO2吸收率高达23.5%。乙酸铵的浸出率为79.2%。与传统的间接方法相比,乙酸铵法具有更高的环境友好性,碳吸收率为23.5%。此外,碱液、甘氨酸和乙酸铵的加入有效延长了碳酸钙晶体的成核时间,诱导形成了更多粒径更小的水晶石中间体。通过动力学分析和分子动力学,揭示了复合添加剂对碳酸化反应的影响机理。这种创新的方法为同时处理固体废物和减少二氧化碳排放提供了一条有前途的途径。©2023化学工业协会和John Wiley &儿子,有限公司
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引用次数: 0
Influence of Hydrogen on the Performance and Emissions Characteristics of a Spark Ignition Ammonia Direct Injection Engine 氢气对火花点火式氨直喷发动机性能及排放特性的影响
4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2023-10-16 DOI: 10.3390/gases3040010
Cheolwoong Park, Yonghun Jang, Seonyeob Kim, Yongrae Kim, Young Choi
Because ammonia is easier to store and transport over long distances than hydrogen, it is a promising research direction as a potential carrier for hydrogen. However, its low ignition and combustion rates pose challenges for running conventional ignition engines solely on ammonia fuel over the entire operational range. In this study, we attempted to identify a stable engine combustion zone using a high-pressure direct injection of ammonia fuel into a 2.5 L spark ignition engine and examined the potential for extending the operational range by adding hydrogen. As it is difficult to secure combustion stability in a low-temperature atmosphere, the experiment was conducted in a sufficiently-warmed atmosphere (90 ± 2.5 °C), and the combustion, emission, and efficiency results under each operating condition were experimentally compared. At 1500 rpm, the addition of 10% hydrogen resulted in a notable 20.26% surge in the maximum torque, reaching 263.5 Nm, in contrast with the case where only ammonia fuel was used. Furthermore, combustion stability was ensured at a torque of 140 Nm by reducing the fuel and air flow rates.
由于氨比氢更容易储存和长距离运输,它作为氢的潜在载体是一个很有前途的研究方向。然而,它的低点火和燃烧速率给在整个工作范围内仅使用氨燃料的传统点火发动机带来了挑战。在这项研究中,我们试图通过向2.5 L火花点火发动机高压直喷氨燃料来确定稳定的发动机燃烧区域,并研究了通过添加氢气来延长工作范围的潜力。由于在低温气氛下难以保证燃烧稳定性,实验在足够温暖的气氛下(90±2.5℃)进行,并对各工况下的燃烧、排放和效率结果进行了实验比较。在1500转/分时,加入10%的氢气,与只使用氨燃料的情况相比,最大扭矩增加了20.26%,达到263.5 Nm。此外,通过降低燃料和空气流量,在140 Nm的扭矩下确保了燃烧稳定性。
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引用次数: 0
Effect of Mixing Technique on Physico-Chemical Characteristics of Blended Membranes for Gas Separation 混合技术对气体分离混合膜理化特性的影响
4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2023-09-26 DOI: 10.3390/gases3040009
Danial Qadir, Humbul Suleman, Faizan Ahmad
Polymer blending has attracted considerable attention because of its ability to overcome the permeability–selectivity trade-off in gas separation applications. In this study, polysulfone (PSU)-modified cellulose acetate (CA) membranes were prepared using N-methyl-2-pyrrolidone (NMP) and tetrahydrofuran (THF) using a dry–wet phase inversion technique. The membranes were characterized using scanning electron microscopy (SEM) for morphological analysis, thermogravimetric analysis (TGA) for thermal stability, and Fourier transform infrared spectroscopy (FTIR) to identify the chemical changes on the surface of the membranes. Our analyses confirmed that the mixing method (the route chosen for preparing the casting solution for the blended membranes) significantly influences the morphological and thermal properties of the resultant membranes. The blended membranes exhibited a transition from a finger-like pore structure to a dense substructure in the presence of macrovoids. Similarly, thermal analysis confirmed the improved residual weight (up to 7%) and higher onset degradation temperature (up to 10 °C) of the synthesized membranes. Finally, spectral analysis confirmed that the blending of both polymers was physical only.
聚合物共混由于能够克服气体分离中渗透性与选择性之间的权衡而引起了广泛的关注。本研究以n -甲基-2-吡罗烷酮(NMP)和四氢呋喃(THF)为原料,采用干湿相转化技术制备了聚砜(PSU)改性醋酸纤维素(CA)膜。采用扫描电镜(SEM)对膜进行形貌分析,热重分析(TGA)对膜进行热稳定性分析,傅里叶变换红外光谱(FTIR)对膜表面的化学变化进行表征。我们的分析证实,混合方法(为混合膜制备浇铸溶液所选择的路线)显著影响所得膜的形态和热性能。混合膜表现出从指状孔结构向存在大孔洞的致密亚结构的转变。同样,热分析证实了合成膜的残余重量(高达7%)和更高的起始降解温度(高达10°C)。最后,光谱分析证实了这两种聚合物的共混只是物理性质的。
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引用次数: 0
Handling heat-stable salts in post-combustion CO2 capture: A detailed survey 燃烧后CO2捕集处理热稳定盐:详细调查
IF 2.2 4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2023-09-11 DOI: 10.1002/ghg.2242
Wilfred Emori, Inime I. Udoh, Okpo O. Ekerenam, Alexander I. Ikeuba, IniIbehe N. Etim, Chigoziri N. Njoku, Enobong F. Daniel, Demian I. Njoku, Paul C. Uzoma, Sharafadeen K. Kolawole, Olajire S. Olanrele

The generation of heat-stable salts (HSSs) in alkanolamine solutions for CO2 capture processes, which is adapted for power plant technologies, exists irrespective of the class of amine solution used for the capture process. Their presence do not only trigger decrements in the CO2 absorption capacities of the solvents and contribute to further alkanolamine degradation, but also result in foaming and loss of solvents, which impacts system economics and threatens the environment. HSSs also promote the corrosiveness of the metallic structures of capture systems by lowering the pH and increasing the conductivity of the absorbent solutions. Overall, these effects substantially subvert the reliability and integrity of CO2 capture units. This survey affords sufficient background on the existence of HSSs by unraveling the flow process in a typical alkanolamine-based CO2 capture unit with respect to their formation points and potential threats. Furthermore, the major HSSs removal and alkanolamine reclamation methodologies (electrodialysis, distillation, ion exchange, electromagnetic separation, and solvent extraction) were comprehensively explored. We believe that this review paper will benefit researchers across disciplines as we continue to explore new and complex solvent formulations to minimize the cost of CO2 capture while maximizing efficiency. © 2023 Society of Chemical Industry and John Wiley & Sons, Ltd.

在用于二氧化碳捕获过程的烷醇胺溶液中产生热稳定盐(hss)适用于发电厂技术,无论用于捕获过程的胺溶液的类别如何都存在。它们的存在不仅会导致溶剂对CO2的吸收能力下降,导致烷醇胺的进一步降解,而且还会导致溶剂的起泡和损失,从而影响系统的经济性并威胁环境。hss还通过降低pH值和增加吸收溶液的导电性来促进捕获系统金属结构的腐蚀性。总的来说,这些影响大大破坏了二氧化碳捕集装置的可靠性和完整性。这项调查通过揭示典型的烷醇胺基二氧化碳捕集装置中关于其形成点和潜在威胁的流动过程,为hss的存在提供了充分的背景。并对电渗析、精馏、离子交换、电磁分离和溶剂萃取等主要的高磺酸盐脱除和烷醇胺回收方法进行了全面探讨。我们相信,这篇综述论文将使跨学科的研究人员受益,因为我们将继续探索新的和复杂的溶剂配方,以最大限度地降低二氧化碳捕获的成本,同时最大化效率。©2023化学工业协会和John Wiley &儿子,有限公司
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引用次数: 0
CO2-Induced alterations due to thermal maturation in shale: Implications for CO2 utilization and storage 页岩热成熟引起的CO2引起的变化:对CO2利用和储存的影响
IF 2.2 4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2023-09-06 DOI: 10.1002/ghg.2243
Chioma Onwumelu, Oladoyin Kolawole, Imene Bouchakour, Ogochukwu Ozotta, Stephan Nordeng, Moones Alamooti
<p>Shales have low to ultra-low porosity and permeability, which makes them an attractive candidate for CO<sub>2</sub> utilization during CO<sub>2</sub>-enhanced oil recovery (CO<sub>2</sub>-EOR) or for geologic CO<sub>2</sub> storage (GCS). Shale are source rocks, and thus, there is a continuous induced diagenetic process that can alter their properties as they reaches maturity at greater in situ temperature. However, there are significant knowledge gaps in the possibility of CO<sub>2</sub> utilization during this diagenetic process (thermal maturation) to achieve long-term CO<sub>2</sub> storage. This experimental study investigates the potential for CO<sub>2</sub> utilization in shale due to induced thermal maturation at in situ conditions, and the implications of pre-maturation CO<sub>2</sub> injection in shale for GCS and CO<sub>2</sub>-EOR. Here, we used subsurface hydrocarbon-rich Bakken and Green River shales exposed to CO<sub>2</sub> for a specific period. This is followed by inducing the unexposed and CO<sub>2</sub>-exposed shales to thermal maturity. Subsequently, we evaluated the total organic carbon (TOC), liberated hydrocarbons (<i>S</i><sub>2</sub>), and the mineralogical and mechanical properties of the mature and CO<sub>2</sub>-exposed mature shales. We further assessed the implications of CO<sub>2</sub> utilization and storage in thermally matured Bakken and Green River shales for long-term storage or CO<sub>2</sub>-EOR. The results indicate that if CO<sub>2</sub> is injected into shales before attaining maturity, higher hydrocarbon production and more significant mechanical weakness can be expected when they attain maturity in Bakken shales (+30% liberated hydrocarbons; −31% Young's modulus; −34% hardness) and Green Rivers shales (+8% liberated hydrocarbons; −40% Young's modulus; −30% hardness), and this is relative to Bakken and Green River shales without CO<sub>2</sub> injection before attaining thermal maturity. Further, CO<sub>2</sub>-exposed mature Bakken and Green River shales can alter the minerals in shales with the dissolution of dolomite and precipitation of calcite, which promotes mineral trapping and achieve a lower TOC (Bakken shale = −24%; Green River shale = −26%), and this is relative to Bakken and Green River shales without CO<sub>2</sub> injection before attaining maturity. Analyses of the results suggest that the application of this proposed CO<sub>2</sub> injection and utilization in immature shales could access more excellent CO<sub>2</sub>-storage reservoirs in Bakken and Green River shales without waiting for a more extended period for the shales to become viable and mature, which is the case with the present GCS and CO<sub>2</sub>-EOR operations in shale reservoirs globally. Also, our proposed pre-maturation CO<sub>2</sub> injection could rejuvenate mature shales for increased hydrocarbon production through CO<sub>2</sub>-EOR, yield a greater sealing efficiency, and mitigate leakage risks for long-term C
页岩具有低至超低的孔隙度和渗透率,这使其成为CO2强化采油(CO2 EOR)或地质CO2储存(GCS)过程中CO2利用的有吸引力的候选者。页岩是烃源岩,因此,存在一个连续的诱导成岩过程,当它们在更高的原位温度下达到成熟度时,会改变它们的性质。然而,在该成岩过程(热成熟)中利用CO2以实现长期CO2储存的可能性方面存在重大知识差距。本实验研究调查了由于在原位条件下诱导热成熟而在页岩中利用CO2的潜力,以及在页岩中注入成熟前CO2对GCS和CO2提高采收率的影响。在这里,我们使用了暴露在CO2中一段特定时期的地下富烃Bakken和Green River页岩。然后将未暴露和暴露于CO2的页岩诱导至热成熟期。随后,我们评估了总有机碳(TOC)、释放的碳氢化合物(S2)以及成熟页岩和暴露于CO2的成熟页岩的矿物学和力学性质。我们进一步评估了热成熟Bakken和Green River页岩中CO2利用和储存对长期储存或CO2 EOR的影响。结果表明,如果在达到成熟度之前将CO2注入页岩,那么当巴肯页岩(+30%释放的碳氢化合物;−31%杨氏模量;−34%硬度)和格林河页岩(+8%释放的烃;−40%杨氏模量;–30%硬度)达到成熟度时,预计会有更高的碳氢化合物产量和更显著的机械弱点,这是相对于在达到热成熟度之前没有注入CO2的Bakken和Green River页岩而言的。此外,暴露于CO2的成熟Bakken和Green River页岩可以通过白云石的溶解和方解石的沉淀改变页岩中的矿物,从而促进矿物捕获并实现较低的TOC(Bakken页岩=−24%;Green River页岩=−26%),这与成熟前未注入CO2的Bakken或Green River页岩有关。对结果的分析表明,在未成熟页岩中应用这种拟议的CO2注入和利用可以在Bakken和Green River页岩中获得更优秀的CO2储存储层,而无需等待更长的时间使页岩变得可行和成熟,这就是目前全球页岩储层的GCS和CO2 EOR操作的情况。此外,我们提出的预成熟CO2注入可以通过CO2 EOR使成熟页岩恢复活力,增加碳氢化合物产量,提高密封效率,并降低长期CO2储存的泄漏风险。这项研究的结果提供了新的见解,可以促进未成熟Bakken和Green River页岩未来GCS和/或CO2 EOR的CO2利用,同时通过消耗大气中的CO2来提供一个即时可行的储存选择,以在2050年前实现全球净零排放。©2023化学工业协会和John Wiley&Sons,有限公司。
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Greenhouse Gases: Science and Technology
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