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Response Surface Optimisation of Carbon Dioxide Adsorption Onto Palm Shell Activated Carbon Functionalised With Natural Amino Acids 天然氨基酸功能化棕榈壳活性炭吸附二氧化碳的响应面优化
IF 2.8 4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2025-01-25 DOI: 10.1002/ghg.2321
Nur Syahirah Mohamed Hatta, Farihahusnah Hussin, Lai Ti Gew, Mohamed Kheireddine Aroua

Amino acids have shown promising results for carbon dioxide (CO2) capture when functionalised on solid materials; however, the functionalisation often relies on commercial synthetic amino acids. This study investigated the optimal CO2 adsorption performance of amino acid–functionalised material synthesised from palm shell–based activated carbon and natural amino acids, specifically egg white (EW) solution, in a continuous adsorption column. The process conditions of the column were optimised using response surface methodology. Four parameters, namely, the gas flow rate, adsorption temperature, CO2 concentration and EW concentration in the impregnation solution, were identified as significantly affecting CO2 adsorption performance. Good agreements were obtained between the predicted and experimental data, with the coefficients of determination ranging from 0.9639 to 0.9784. A maximum CO2 adsorption capacity of 1.1793 mmol/g was achieved under optimal process conditions: a gas flow rate of 200 mL/min, an adsorption temperature of 25°C, a CO2 concentration of 25 vol.%, and an EW concentration of 15 wt.%. The validation results further confirmed the reliability of the developed model equation in predicting the maximum CO2 adsorption capacity at a fixed 15 vol.% CO2 concentration, with low estimation error. The comparable results obtained using EW waste in this study represent a significant finding in the potential for waste valorisation, aligning with Sustainable Development Goal (SDG) 12 of the United Nations Sustainable Development Goals, as well as contributing to climate action as outlined in SDG 13.

氨基酸在固体材料上功能化后,在捕获二氧化碳(CO2)方面显示出有希望的结果;然而,功能化往往依赖于商业合成氨基酸。研究了棕榈壳活性炭与天然氨基酸,特别是蛋清(EW)溶液合成的氨基酸功能化材料在连续吸附柱上的最佳CO2吸附性能。采用响应面法对色谱柱的工艺条件进行了优化。确定了浸渍液中气体流速、吸附温度、CO2浓度和EW浓度等4个参数对CO2吸附性能有显著影响。预测值与实验值吻合较好,决定系数在0.9639 ~ 0.9784之间。最佳工艺条件为:气体流速200 mL/min,吸附温度25℃,CO2浓度25 vol.%, EW浓度15 wt.%,最大CO2吸附量为1.1793 mmol/g。验证结果进一步证实了所建立的模型方程在固定CO2浓度为15 vol.%时预测最大CO2吸附量的可靠性,且估计误差小。本研究中利用电子废弃物获得的可比结果代表了废物价值化潜力的重大发现,与联合国可持续发展目标中的可持续发展目标(SDG) 12一致,并有助于SDG 13中概述的气候行动。
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引用次数: 0
Impact of Relative Permeability Hysteresis on CO2 Storage in Saline Aquifers 相对渗透率滞后效应对含盐含水层CO2储存量的影响
IF 2.8 4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2024-12-27 DOI: 10.1002/ghg.2319
Reza Khoramian, Ibraheem Salaudeen, Peyman Pourafshary, Masoud Riazi, Riyaz Kharrat

The urgent challenge of climate change, driven by rising carbon emissions, necessitates innovative strategies for carbon capture and storage (CCS). This study examines the impact of hysteresis in relative permeability on CO2 entrapment efficiency within saline aquifers, known for their significant storage capabilities. An aquifer model was analyzed through numerical simulation by varying hysteresis values from 0.2 to 0.5 to evaluate their impact on CO2 plume behavior, retention during water-alternating-gas (WAG) injection, and plume morphology. The CO2 plume exhibits a funnel-shaped configuration at low hysteresis with a narrow, pointed base, indicating a concentrated upward migration trajectory. In contrast, a hysteresis value of 0.5 results in diminished gas movement toward the upper aquifer, transforming the plume into a more oval shape. Results from the land trapping model further support our findings, revealing an inverse relationship where increased hysteresis enhances residual CO2 entrapment, reflected in trapping coefficient values ranging from 0.5 to 4. This underscores the model's efficacy in verifying gas trapping efficiency and safety during sequestration. Moreover, increased water flow generates stronger forces, pushing CO2 into narrower pore spaces, where it becomes trapped. Our findings indicate that increased hysteresis enhances CO2 retention by limiting vertical migration and significantly influences plume geometry, promoting stable and predictable distribution patterns. At higher hysteresis values, CO2 migration is significantly restricted, resulting in near-complete immobilization of the injected gas. This research highlights hysteresis's critical role in refining injection methodologies and enhancing plume stability for long-term CO2 storage. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.

由碳排放上升所驱动的气候变化的紧迫挑战,需要创新的碳捕获与封存(CCS)战略。本研究考察了相对渗透率的滞后对含盐含水层中二氧化碳捕获效率的影响,含盐含水层以其显著的储存能力而闻名。通过对含水层模型进行数值模拟,分析了迟滞值在0.2 ~ 0.5范围内的变化,以评估其对CO2羽流行为、水-气交替(WAG)注入过程中的滞留以及羽流形态的影响。CO2羽流在低迟滞时呈漏斗状结构,底部窄而尖,呈集中向上运移轨迹。相反,滞后值为0.5时,气体向上层含水层的运动减少,使羽流变成更椭圆形的形状。陆地捕获模型的结果进一步支持了我们的发现,揭示了一个反比关系,即滞后增加会增加剩余二氧化碳的捕获,这反映在捕获系数的0.5到4之间。这强调了该模型在验证封存期间的气体捕获效率和安全性方面的有效性。此外,增加的水流产生更强的力,将二氧化碳推入更窄的孔隙空间,在那里被困住。研究结果表明,迟滞的增加通过限制垂直迁移来增强CO2的滞留,并显著影响羽流的几何形状,促进稳定和可预测的分布模式。在较高的迟滞值下,二氧化碳的运移受到明显限制,导致注入气体几乎完全不动。这项研究强调了迟滞在改进注入方法和提高长期二氧化碳储存羽流稳定性方面的关键作用。©2024化学工业协会和John Wiley &;儿子,有限公司
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引用次数: 0
Techno-Economic Analysis of Glycerol Steam Reforming with Amine-Based Carbon Capture for Blue Hydrogen Production: A Rate-Based Kinetic Model Approach 氨基碳捕集甘油蒸汽重整蓝色制氢的技术经济分析:基于速率的动力学模型方法
IF 2.8 4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2024-12-06 DOI: 10.1002/ghg.2320
Pali Rosha, Mohammad Sajjadi, Hussameldin Ibrahim

This study outlines a comprehensive process design utilising glycerol-steam reforming for an H2-enriched gas stream, coupled with carbon dioxide removal via a chemical absorption system, followed by a techno-economic analysis. The Aspen Plus economic analyser assesses the developed model, incorporating simulation results and literature data. Initially, the CO2 capture unit was planned with a standalone absorber and stripper, later integrated for solvent makeup calculation. Findings reveal that as catalyst loading increased from 5 to 50 kg, glycerol conversion and product molar fraction improved. For a targeted H2 production of 10 t/day, optimal reactor dimensions are 3.2 m diameter and 30 m length, corresponding to a reactant flow of 105 t/day and a 2.52 MW heat duty at stoichiometry conditions. To capture 95% CO2 from the reformed product stream, absorber and stripper packing heights of 12 and 7 m, respectively, with column diameters of 1.25 and 2.71 m are necessary. The production cost of H2 is determined to be $3.8 per kg, as revealed by the techno-economic analysis. Calculated values for net present value, discounted payback period, and internal rate of return stand at $30 million, 5 years, and 25.0%, respectively. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.

本研究概述了一个综合的工艺设计,利用甘油-蒸汽重整的h2富集气流,通过化学吸收系统去除二氧化碳,然后进行技术经济分析。Aspen Plus经济分析师评估开发的模型,结合模拟结果和文献数据。最初,CO2捕集装置计划有一个独立的吸收器和汽提器,后来集成用于溶剂组成计算。结果表明,当催化剂负载从5 kg增加到50 kg时,甘油转化率和产物摩尔分数都有所提高。为了达到10吨/天的目标氢气产量,反应器的最佳尺寸为直径3.2米,长度30米,对应于化学计量条件下的反应物流量为105吨/天,热负荷为2.52兆瓦。要从重整产物流中捕集95%的CO2,吸收塔和汽提塔的填料高度分别为12米和7米,塔直径分别为1.25米和2.71米。根据技术经济分析,H2的生产成本确定为每公斤3.8美元。净现值、贴现回收期和内部收益率的计算值分别为3000万美元、5年和25.0%。©2024化学工业协会和John Wiley &;儿子,有限公司
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引用次数: 0
Study on the effect of alcohol additives on ammonia decarburization performance and ammonia escape 醇类添加剂对氨脱碳性能及氨逸出的影响研究
IF 2.8 4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2024-11-28 DOI: 10.1002/ghg.2317
Yu Bin Wang, Jie Rui Yu, Xiao Xian Zhang, Hao Chen, Han Bang Ruan, Guo Hua Yang

Ammonia carbon capture is characterized by low corrosion, resistance to oxidation and degradation, and low energy consumption for regeneration. However, it also presents challenges such as a slow absorption rate and notable ammonia escape. Current ammonia decarbonization research primarily focuses on the flue gas from power plants, which differs in composition from ship exhaust gas. To address this, we constructed a small carbon absorption test bench and used a mixture of CO2 and N2 as the ship exhaust gas. Ammonia solution and alcohol served as absorbents and additives, respectively, to explore the effects of the additive hydroxyl number, the concentrations of the additive and ammonia solution, and the reaction temperature on carbon loading, absorption rate, and ammonia escape. Results indicated that n-propanol was most effective in inhibiting ammonia escape, and a low concentration of ammonia solution was more suitable for absorbing CO2. Specifically, when the concentration of ammonia was 4% and the concentration of n-propanol was 0.2 mol/L, the cumulative ammonia escape was reduced by 34% compared to the scenario without additives. Additionally, the carbon loading and average absorption rate reached 0.49 mol CO2/mol NH3 and 2.33 × 10−3 mol·kg−1·min−1, respectively, representing increases of 34.2 and 60.7%. However, as the reaction temperature increased, the effectiveness of n-propanol in enhancing ammonia absorption diminished. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.

氨碳捕集具有低腐蚀、抗氧化、抗降解、再生能耗低等特点。然而,它也面临着诸如吸收率慢和明显的氨逸出等挑战。目前的氨脱碳研究主要集中在电厂烟气中,其成分与船舶废气不同。为了解决这个问题,我们建造了一个小型碳吸收试验台,并使用二氧化碳和N2的混合物作为船舶废气。以氨溶液和醇分别作为吸附剂和助剂,考察助剂羟基数、助剂和氨溶液浓度、反应温度对碳负荷、吸收率和氨逸出的影响。结果表明,正丙醇抑制氨逸的效果最好,低浓度的氨溶液更适合吸收CO2。其中,当氨浓度为4%,正丙醇浓度为0.2 mol/L时,与不添加添加剂的情况相比,氨的累积逸出量减少了34%。碳负荷和平均吸收率分别达到0.49 mol CO2/mol NH3和2.33 × 10−3 mol·kg−1·min−1,分别增加了34.2和60.7%。但随着反应温度的升高,正丙醇促进氨吸收的效果减弱。©2024化学工业协会和John Wiley &;儿子,有限公司
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引用次数: 0
Enhanced sintering resistance of NiFe-based RWGS catalysts through Cu doping 通过掺杂铜提高 NiFe 基 RWGS 催化剂的抗烧结性
IF 2.8 4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2024-11-19 DOI: 10.1002/ghg.2314
Jiayi Wu, Wenhao Zhang, Hecao Chen, Weifeng Yu, Bo Sun, Minghui Zhu, Yi-Fan Han

The reverse water-gas shift (RWGS) reaction offers an effective method for mitigating CO2 emissions. Due to its affordability and physicochemical stability, iron has garnered significant attention as a potential catalyst for RWGS. The incorporation of nickel and copper promoters can enhance CO2 conversion and CO selectivity in Fe-based catalysts. This study focuses on modifying the strength of the Strong Metal-Support Interaction (SMSI) through particle size optimization. Doping Cu into NiFe-based catalysts restricts particle size, which influences the curvature of the Ni0@FeOx interface. This curvature enhances the electron coupling between Ni0 and FeOx, promoting the formation of a denser and thicker Ni0 and FeOx layer. This results in a nearly 90% increase in the CO2 reaction rate during the sintering resistance test by anchoring Ni0 and facilitating electron transfer to active sites. Such morphological evolution improves high-temperature resistance to sintering during RWGS. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.

逆向水气转换(RWGS)反应为减少二氧化碳排放提供了一种有效的方法。由于其可负担性和物理化学稳定性,铁作为RWGS的潜在催化剂受到了广泛关注。在铁基催化剂中加入镍和铜促进剂可以提高CO的选择性和CO的转化率。本研究的重点是通过粒度优化来改变强金属-载体相互作用(SMSI)的强度。在nife基催化剂中掺杂Cu会限制催化剂的粒径,从而影响Ni0@FeOx界面的曲率。这种曲率增强了Ni0和FeOx之间的电子耦合,促进了Ni0和FeOx层的致密和厚度的形成。通过锚定Ni0和促进电子转移到活性位点,在抗烧结测试中,二氧化碳反应速率提高了近90%。这种形态的演变提高了RWGS过程中的高温烧结性能。©2024化学工业协会和John Wiley &;儿子,有限公司
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引用次数: 0
Data-driven framework for predicting the sorption capacity of carbon dioxide and methane in tight reservoirs 致密储层二氧化碳和甲烷吸附能力预测的数据驱动框架
IF 2.8 4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2024-11-17 DOI: 10.1002/ghg.2318
Fahd Mohamad Alqahtani, Mohamed Riad Youcefi, Hakim Djema, Menad Nait Amar, Mohammad Ghasemi

As energy demand continues to rise and conventional fuel sources dwindle, there is growing emphasis on previously overlooked reservoirs, such as tight reservoirs. Shale and coal formations have emerged as highly attractive options due to their substantial contributions to global gas reserves. Enhanced shale gas recovery (ESGR) and enhanced coalbed methane recovery (ECBM) based on gas injection are advanced techniques used to increase the extraction of gas from shale and coal formations. One of the key challenges associated with these formations and their enhanced recovery methods is accurately predicting the sorption process and its profile. This is crucial because it affects how methane (CH4) and carbon dioxide (CO2) are stored and released from the rock, and it significantly impacts the evaluation of gas content and the potential productivity of these formations. Due to the high cost of experimental procedures and the moderate accuracy of existing predictive approaches, this study proposes various cheap and consistent data-driven schemes for predicting the sorption of CH4 and CO2 in shale and coal formations. In this regard, three intelligent models, including generalized regression neural network (GRNN), radial basis function neural network (RBFNN), and categorical boosting (CatBoost), were taught and tested using more than 3800 real measurements of CH4 and CO2 sorption in shale and coal formations. To find automatically their appropriate control parameters and improve their prediction ability, RBFNN and CatBoost were evolved using grey wolf optimization (GWO). The obtained results exhibited the encouraging prediction capabilities of the suggested models. In addition, it was found that CatBoost-GWO is the most accurate scheme with total root mean square (RMSE) and determination coefficient (R2) of 0.1229 and 0.9993 for CO2 sorption, and 0.0681 and 0.9970 for CH4 sorption, respectively. Additionally, this approach demonstrated its physical validity by respecting the real sorption tendencies with respect to operational parameters. Furthermore, the CatBoost-GWO model outperforms recently published machine learning approaches. Lastly, the findings of this study offer a significant contribution by demonstrating that the suggested model can greatly improve the ease of estimating CO2 and CH4 sorption in tight formations, thereby facilitating the simulation of other parameters related to this process. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.

随着能源需求的持续增长和传统燃料来源的减少,人们越来越重视以前被忽视的储层,如致密储层。由于页岩和煤田对全球天然气储量的巨大贡献,它们已成为极具吸引力的选择。基于注气的提高页岩气采收率(ESGR)和提高煤层气采收率(ECBM)是用于提高页岩和煤层天然气采收率的先进技术。与这些地层及其提高采收率方法相关的关键挑战之一是准确预测吸附过程及其剖面。这一点至关重要,因为它会影响甲烷(CH4)和二氧化碳(CO2)从岩石中储存和释放的方式,并对这些地层的气体含量和潜在产能的评估产生重大影响。由于实验程序的高成本和现有预测方法的中等准确性,本研究提出了各种廉价和一致的数据驱动方案来预测页岩和煤层中CH4和CO2的吸附。在这方面,三种智能模型,包括广义回归神经网络(GRNN)、径向基函数神经网络(RBFNN)和分类增压(CatBoost),被教授并使用超过3800个页岩和煤层中CH4和CO2吸附的实际测量结果进行测试。为了自动找到合适的控制参数,提高其预测能力,RBFNN和CatBoost采用灰狼优化(GWO)进行进化。所得结果显示了所建议模型令人鼓舞的预测能力。此外,CatBoost-GWO是最准确的方案,CO2吸附的总均方根(RMSE)和决定系数(R2)分别为0.1229和0.9993,CH4吸附的总均方根和决定系数(R2)分别为0.0681和0.9970。此外,该方法通过尊重实际吸附趋势与操作参数的关系,证明了其物理有效性。此外,CatBoost-GWO模型优于最近发表的机器学习方法。最后,本研究的发现提供了重要的贡献,表明所建议的模型可以大大提高估计致密地层中CO2和CH4吸附的便利性,从而促进了与该过程相关的其他参数的模拟。©2024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 sequestration and soil improvement in enhanced rock weathering: A review from an experimental perspective 增强岩石风化过程中的二氧化碳封存和土壤改良:从实验角度综述
IF 2.8 4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2024-11-12 DOI: 10.1002/ghg.2313
Lianghan Cong, Shuaiyi Lu, Pan Jiang, Tianqi Zheng, Ziwang Yu, Xiaoshu Lü

Enhanced rock weathering (ERW) is an emerging negative emission technology (NET) with significant potential for mitigating climate change and improving soil health through the accelerated chemical weathering of silicate minerals. This study adopts a critical research approach to review existing ERW experiments, focusing on the mechanisms of soil improvement and CO₂ sequestration, as well as the economic costs and environmental risks associated with its large-scale implementation. The results demonstrate that while ERW effectively enhances soil pH and provides essential nutrients for crops, its CO₂ sequestration capacity is highly dependent on variables such as soil type, rock type, application rate, and particle size. Furthermore, the economic feasibility of ERW is challenged by high costs related to mining, grinding, and transportation, and environmental risks posed by the release of heavy metals like Ni and Cr during the weathering process. Notably, significant discrepancies exist between laboratory experiments and field applications, highlighting the need for extensive in-situ monitoring and adjustment of ERW practices. This study underscores the importance of optimizing ERW strategies to maximize CO₂ sequestration while minimizing environmental impacts. Future research should focus on long-term field experiments, understanding secondary mineral formation, and refining the application techniques to enhance the overall efficiency and sustainability of ERW. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.

增强岩石风化(ERW)是一种新兴的负排放技术(NET),通过加速硅酸盐矿物的化学风化,具有减缓气候变化和改善土壤健康的巨大潜力。本研究采用批判性的研究方法,回顾了现有的ERW实验,重点研究了土壤改良和CO 2固存的机制,以及大规模实施的经济成本和环境风险。结果表明,虽然ERW有效地提高了土壤pH值,并为作物提供了必需的养分,但其CO 2固存能力与土壤类型、岩石类型、施用量和粒径等变量高度相关。此外,战争遗留爆炸物的经济可行性受到采矿、研磨和运输的高成本以及风化过程中Ni和Cr等重金属释放带来的环境风险的挑战。值得注意的是,实验室实验和实地应用之间存在重大差异,突出表明需要广泛的现场监测和调整战争遗留爆炸物的做法。这项研究强调了优化剩余物处理策略的重要性,以最大限度地减少二氧化碳的吸收,同时最大限度地减少对环境的影响。未来的研究应着眼于长期的野外试验,了解次生矿物的形成,完善应用技术,以提高剩余物的整体效率和可持续性。©2024化学工业协会和John Wiley &;儿子,有限公司
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引用次数: 0
Quantitative assessment of CO2 leakage risk in geologic carbon storage management 地质储碳管理中CO2泄漏风险定量评价
IF 2.8 4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2024-11-12 DOI: 10.1002/ghg.2315
Meng Jing, Qi Li, Guizhen Liu, Quan Xue

Large-scale geological storage of carbon dioxide (CO2) is indispensable for mitigating climate change but faces significant challenges, especially in the accurate quantitative assessment of leakage risks to ensure long-term security. Given these circumstances, this paper proposes an innovative approach for quantitatively assessing CO2 leakage risk to address the previous limitations of limited accuracy and insufficient data. We construct a fault tree and transform it into a Bayesian network–directed acyclic graph, and then use judgment sets along with fuzzy set theory to obtain prior probabilities of root nodes. The feature, event, and process method was utilized to identify key components and subsequently determine the conditional probability table (CPT) of the leaf node. The subjective experience assessments from experts are defuzzified to obtain the CPTs of intermediate nodes. The obtained basic probability parameters are input into the directed acyclic graph to complete the model construction. After calculating the leakage probability using this model, it is combined with the severity of impacts to conduct a comprehensive risk assessment. Furthermore, critical CO2 risk sources can be determined through posterior probability calculations when intermediate nodes are designated as deterministic risk events. The gradual implementation process of the proposed model is demonstrated via a typical case study. The results indicate an overall CO2 leakage probability of 29%, with probabilities of leakage along faults/fractures, caprock, and well identified as 32%, 28%, and 19%, respectively. The project is categorized as a medium-low risk level. When leakage is confirmed, tectonic movement, thickness, and delamination at interface connections/the presence of cracks are the critical risk sources, and measures to mitigate key risks are outlined. The identified key risk factors conform to empirical evidence and previous research, validating the accuracy of the model. This study is instrumental in CO2 geological storage risk assessment and scalable development program design. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.

大规模的二氧化碳地质封存对于减缓气候变化是必不可少的,但也面临着重大挑战,特别是在准确定量评估泄漏风险以确保长期安全方面。鉴于这些情况,本文提出了一种创新的CO2泄漏风险定量评估方法,以解决以往准确性有限和数据不足的局限性。构造故障树并将其转化为贝叶斯网络有向无环图,然后利用判断集和模糊集理论求出根节点的先验概率。利用特征、事件和过程方法识别关键组件,然后确定叶节点的条件概率表(CPT)。对专家的主观经验评价进行去模糊化,得到中间节点的cpt。将得到的基本概率参数输入到有向无环图中,完成模型的构造。利用该模型计算泄漏概率后,结合影响的严重程度进行综合风险评估。此外,将中间节点指定为确定性风险事件时,可以通过后验概率计算确定临界CO2风险源。通过一个典型的案例研究,说明了该模型的逐步实施过程。结果表明,总体CO2泄漏概率为29%,其中沿断层/裂缝、盖层和井识别的泄漏概率分别为32%、28%和19%。该项目被划分为中低风险级别。当确认泄漏时,构造运动、厚度和界面连接处的分层/裂缝的存在是关键的风险来源,并概述了减轻关键风险的措施。确定的关键风险因素符合经验证据和先前的研究,验证了模型的准确性。该研究对二氧化碳地质封存风险评估和可扩展开发方案设计具有重要意义。©2024化学工业协会和John Wiley &;儿子,有限公司
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引用次数: 0
Accelerated weathering of construction-grade limestone for CO2 absorption 加速建筑级石灰石的风化以吸收二氧化碳
IF 2.8 4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2024-11-12 DOI: 10.1002/ghg.2311
Daniel Nyuin Alfred Damu, Alvin Guo Jian Lee, Slyvester Yew Wang Chai, Lock Hei Ngu

Accelerated weathering of limestone (AWL) process efficiently captures CO2 from point source emissions. However, despite achieving an outstanding capture efficiency of 73.51 %, lab-grade (LG) limestone with 99.90 % CaCO3 as an absorbent is costly ($2757.70/t), making commercialization of AWL impractical. This work delves into the viability of utilizing construction-grade (CG) limestone (93.26% purity) for the AWL process facilitated by potable water in an absorption tower for post-combustion capture. The result shows that CG limestone achieves comparable CO2 capture efficiency of 8.0–74.68% and bicarbonate (Ca(HCO3)2) concentration of 0.63–3.10 mM compared with LG limestone. However, LG limestone has 0.29 mol CO2/mol CaCO3 higher CO2 absorption capacity and a faster absorption rate than CG limestone, indicating a somewhat better CO2 capture performance. Nevertheless, CG limestone offered a more cost-effective alternative, with a $2735.24 lower cost per ton of CaCO3 and a $2651.63 per ton CO2 lower CO2 capturing cost at the highest carbon capture efficiency (HCCE) condition compared to LG limestone. The kinetic analysis shows that the forward reactions in the AWL process are significantly faster at elevated CO2 concentration, with the mass transfer coefficient affirming that CO2 dissolves faster than CaCO3, in line with prior research. Thus, this work validates that CG limestone-based AWL achieves comparable CO2 capture performance to that of LG limestone, offering a cost-efficient alternative. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.

石灰石加速风化(AWL)工艺可从点源排放中有效捕集二氧化碳。然而,尽管实现了 73.51 % 的出色捕集效率,但使用含 99.90 % CaCO3 的实验室级(LG)石灰石作为吸收剂成本高昂(2757.70 美元/吨),使得 AWL 的商业化不切实际。这项研究探讨了利用建筑级(CG)石灰石(纯度为 93.26%)进行燃烧后捕集(AWL)工艺的可行性,在吸收塔中利用饮用水进行燃烧后捕集。结果表明,与 LG 石灰石相比,CG 石灰石的二氧化碳捕集效率为 8.0-74.68%,碳酸氢盐(Ca(HCO3)2)浓度为 0.63-3.10 mM。然而,与 CG 石灰岩相比,LG 石灰岩的二氧化碳吸收能力高 0.29 摩尔 CO2/摩尔 CaCO3,吸收速度快,表明其二氧化碳捕集性能更好。尽管如此,与 LG 石灰岩相比,CG 石灰岩提供了更具成本效益的选择,在最高碳捕集效率(HCCE)条件下,每吨 CaCO3 的成本比 LG 石灰岩低 2735.24 美元,每吨 CO2 的捕集成本比 LG 石灰岩低 2651.63 美元。动力学分析表明,在二氧化碳浓度升高的情况下,AWL 工艺中的正向反应速度明显加快,传质系数证实二氧化碳的溶解速度快于 CaCO3,这与之前的研究结果一致。因此,这项工作验证了基于 CG 石灰石的 AWL 可实现与 LG 石灰石相当的二氧化碳捕集性能,提供了一种具有成本效益的替代方法。© 2024 化学工业协会和约翰威利父子有限公司版权所有。
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引用次数: 0
Oxidative degradation of glycine in aqueous KOH/K2CO3 solutions for CO2 capture 甘氨酸在KOH/K2CO3水溶液中氧化降解以捕获CO2
IF 2.8 4区 环境科学与生态学 Q3 ENERGY & FUELS Pub Date : 2024-11-11 DOI: 10.1002/ghg.2310
Friday O. Ochedi, John Andresen, Mijndert van der Spek

Potassium hydroxide and potassium carbonate, being cost-effective and environmentally friendly CO2 capture solvents, are promising candidates for carbon capture applications. Their slow absorption kinetics, however, necessitate strategies to enhance their rates, thereby reducing the capital costs of absorption equipment and saving energy for regenerating large volumes of solvent. Glycine, a potential additive, is explored for this purpose. While glycine-based solvents are more stable than MEA, their amino functional group renders them susceptible to oxidative degradation. This study investigates the degradation of these solvents and the influence of potassium hydroxide and potassium carbonate on their stability. The experiment was performed under 100% O2 at 90 °C and 3 bar for about 3 weeks. It was observed that glycinate degraded by 53% for the glycinate-only solution. The results also show that the addition of potassium hydroxide and potassium carbonate to a glycinate-only solution had a mixed effect on the degradation of glycinate. Potassium hydroxide increased degradation by 5% compared to the glycinate-only solution, while potassium carbonate decreased degradation by 4%. This order is supported by the degradation rate constants. Meanwhile, under N2, no significant change was observed in glycine concentration. Glycine's susceptibility to oxidative degradation is likely attributed to its less compact and rigid structure, resulting in weaker bonding and increased vulnerability to external factors. This instability leads to the formation of formate, carbonate, acetate, and oxalate as the primary degradation products across all studied solutions. A proposed mechanism for glycinate oxidative degradation sheds light on this process. These findings are crucial for informed decision making regarding performance trade-offs in point source carbon capture and direct air capture, where oxygen is a prevalent gas component and potassium-based solutions are commonly employed as absorbents. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.

氢氧化钾和碳酸钾作为具有成本效益和环境友好型的二氧化碳捕获溶剂,是碳捕获应用的有希望的候选者。然而,它们缓慢的吸收动力学需要提高其吸收速率的策略,从而降低吸收设备的资本成本并节省再生大量溶剂的能源。甘氨酸,一种潜在的添加剂,探讨了这一目的。虽然甘氨酸基溶剂比MEA更稳定,但它们的氨基官能团使它们容易氧化降解。本研究考察了这些溶剂的降解以及氢氧化钾和碳酸钾对其稳定性的影响。实验在100% O2条件下,90℃,3 bar,持续约3周。结果表明,甘氨酸在纯甘氨酸溶液中降解率为53%。结果还表明,在甘氨酸溶液中加入氢氧化钾和碳酸钾对甘氨酸的降解有混合效果。与仅甘氨酸盐溶液相比,氢氧化钾的降解率提高了5%,而碳酸钾的降解率降低了4%。退化速率常数支持这个顺序。同时,在N2条件下,甘氨酸浓度无明显变化。甘氨酸对氧化降解的易感性可能是由于其结构不致密和刚性,导致结合较弱,对外部因素的脆弱性增加。这种不稳定性导致甲酸盐、碳酸盐、醋酸盐和草酸盐的形成,成为所有研究溶液的主要降解产物。提出的甘氨酸氧化降解机制揭示了这一过程。这些发现对于点源碳捕获和直接空气捕获的性能权衡的明智决策至关重要,其中氧气是普遍的气体成分,钾基溶液通常被用作吸收剂。©2024化学工业协会和John Wiley &;儿子,有限公司
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引用次数: 0
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Greenhouse Gases: Science and Technology
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