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CO2 and steam-CO2 reforming of ethanol over CuО/Al2O3 catalysts: Influence of additives on catalyst coking 乙醇在CuО/Al2O3催化剂上的CO2和蒸汽-CO2重整:添加剂对催化剂焦化的影响
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-01-20 DOI: 10.1016/j.jcou.2026.103333
Gaukhar Yergaziyeva , Moldir Anissova , Nursaya Makayeva , Laura Myltykbayeva , Manshuk Mambetova , Zhengisbek Kuspanov , Chingis Daulbayev , Madina Bissenova
The effect of γ-Al₂O₃ modification with CeO₂ and La₂O₃ oxides on the catalytic and performance characteristics of copper catalysts in CO₂ reforming and steam–CO₂ reforming of ethanol is investigated. Catalysts with compositions of 10 wt% CuO/Al₂O₃, 10 wt% CuO/2 wt% CeO₂–Al₂O₃ and 10 wt% CuO/2 wt% La₂O₃–Al₂O₃ were synthesized, characterized by TPD-CO₂, TPR-H₂, TPO, TGA/DTA and XRD techniques, and tested in the temperature range of 500–800 °C. The addition of La₂O₃ was shown to generate the strongest basic sites and suppress the formation of the CuAl₂O₄ spinel phase, resulting in an optimal combination of high CO₂ conversion (95 %), maximum hydrogen concentration (55.3 vol%), and minimal coking under steam–CO₂ reforming conditions. In contrast, CeO₂ addition enhances oxygen mobility and promotes ethanol dehydration activity but leads to the highest ethylene yield (67.5 vol%) and the greatest coke deposition (167 mgC/gcat), particularly in the presence of steam. A linear correlation (R² ≈ 0.98) between ethylene yield and the amount of deposited carbon was identified, indicating the key role of ethylene as a coke precursor in the investigated systems. Thermogravimetric analysis of spent catalysts revealed that the La-modified catalyst accumulated the lowest amount of predominantly reactive carbon species and exhibited the lowest deactivation rate. The obtained results establish the relationship between basicity, redox properties, and coking tendency in CuO/Al₂O₃–CeO₂/La₂O₃ systems, providing a rational basis for the design of stable copper catalysts for ethanol reforming with simultaneous CO₂ utilization.
研究了用ceo2和La₂O₃氧化物改性γ-Al₂O₃对铜催化剂在乙醇CO₂重整和蒸汽- CO₂重整过程中的催化性能和性能的影响。合成了10 wt% CuO/Al₂O₃、10 wt% CuO/2 wt% CeO₂-Al₂O₃和10 wt% CuO/2 wt% La₂O₃-Al₂O₃的催化剂,采用TPD-CO₂、TPR-H₂、TPO、TGA/DTA和XRD技术对催化剂进行了表征,并在500 ~ 800℃的温度范围内进行了测试。结果表明,在蒸汽- CO₂重整条件下,La₂O₃的加入产生了最强的碱性位点,抑制了CuAl₂O₄尖晶石相的形成,从而实现了高CO₂转化率(95% %)、最大氢浓度(55.3 vol%)和最小结焦的最佳组合。相比之下,添加CeO 2可以提高氧的流动性,促进乙醇脱水活性,但导致最高的乙烯收率(67.5 vol%)和最大的焦炭沉积(167 mgC/gcat),特别是在有蒸汽存在的情况下。乙烯产率与沉积碳量呈线性相关(R²≈0.98),表明乙烯作为焦炭前驱体在研究体系中起着关键作用。对废催化剂的热重分析表明,la改性催化剂的主要活性碳含量最低,失活率最低。所得结果建立了CuO/Al₂O₃-CeO₂/La₂O₃体系的碱度、氧化还原性能和结焦倾向之间的关系,为设计稳定的铜催化剂用于乙醇重整同时利用CO₂提供了合理的依据。
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引用次数: 0
Engineering long-term antibacterial PLA packaging: Controlled release of thymol co-amorphous pairs via supercritical solvent impregnation 工程长效抗菌PLA包装:超临界溶剂浸渍法控释百里香酚共无定形对
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-01-23 DOI: 10.1016/j.jcou.2026.103341
Adrián Rojas , Irena Zizovic , Paulina Cheuquepan , Hans Lagos , Mariusz Nowak , Gonzalo Aguila , María Galotto , Ximena Valenzuela
The rapid release of active compounds often limits the development of active food packaging with long-term antimicrobial effects. This study proposes an innovative and sustainable solution by integrating cocrystallization and supercritical fluid technologies to create a controlled-release system. Herein is investigated the impregnation of poly(lactic acid) (PLA) foams with thymol (THY) - phenazine (PHE) cocrystal pairs via supercritical solvent impregnation at 40 °C and 12–18 MPa, analyzing the impact of different isobaric cooling rates (0.3 and 1.5 °C/min) on particle deposition and release kinetics. Submicron THY-PHE co-amorphous pairs were successfully deposited within the PLA matrix, with particle size dependent on the cooling rate. These pairs exhibited significantly slower release kinetics than pure THY, with a release rate constant up to 12 times lower. Consequently, PLA foams loaded with THY-PHE pairs demonstrated prolonged antibacterial activity, completely inhibiting Staphylococcus aureus and Escherichia coli for up to 192 h with concentrations three times lower than those required for pure THY. This work presents a robust, environmentally friendly, method for engineering advanced packaging materials with tailored, long-term release of active agents.
活性化合物的快速释放往往限制了具有长期抗菌作用的活性食品包装的发展。本研究提出了一种创新和可持续的解决方案,将共结晶和超临界流体技术相结合,创建一个控释系统。研究了百里香酚(THY) -苯那嗪(PHE)共晶对在40℃、12-18 MPa条件下的超临界溶剂浸渍法制备聚乳酸(PLA)泡沫,分析了不同等压冷却速率(0.3和1.5 ℃/min)对颗粒沉积和释放动力学的影响。亚微米THY-PHE共非晶对成功沉积在PLA基体中,其颗粒大小取决于冷却速度。这些药物对的释放动力学比纯THY慢得多,释放速率常数低12倍。因此,负载THY- phe对的PLA泡沫显示出持久的抗菌活性,完全抑制金黄色葡萄球菌和大肠杆菌高达192 h,浓度比纯THY所需的浓度低3倍。这项工作提出了一个强大的,环保的,工程先进的包装材料与定制的方法,长期释放活性剂。
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引用次数: 0
Boron-driven oxygen-vacancy enrichment and VOX dispersion in SAPO-34 for robust CO2-ODHP 硼驱动的SAPO-34中氧空位富集和VOX分散对CO2-ODHP的影响
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-02-04 DOI: 10.1016/j.jcou.2026.103352
Reza Asadi, Jafar Towfighi Darian, Masoud Safari Yazd
We report a boron-modified vanadia@SAPO-34 catalyst (V@SP-B) that integrates Lewis-acidic B3 + sites with redox-active VOX species to enhance CO2-assisted oxidative dehydrogenation of propane (CO2-ODHP). The catalyst, synthesized via H3BO3 etching and VO(acac)2 impregnation, forms a hierarchical micro–mesoporous nanoreactor. XRD confirms CHA framework retention with smaller crystallites (31 vs 37 nm), while FT-IR and Raman reveal new B–O/B–O–B bonds, intensified VO vibrations, and vacancy markers indicating increased defect density. HR-XPS shows framework reorganization with higher B3+ incorporation (66 %), elevated V4+/V5+ ratio (1.3), and a significantly higher oxygen-vacancy ratio (OV/OL = 2.4). Textural analysis demonstrates enhanced surface area (515 m2 g−1) and pore volume (0.46 cm3 g−1). Redox and acid–base studies confirm easier reducibility, stronger hydrogen spillover, enhanced dispersion of active sites (11.4 %), increased acidity (828 µmol g−1), and improved CO2 binding (155 µmol g−1). MD simulations support these findings, revealing stronger CO2 adsorption and lower vacancy formation and reaction barriers. Catalytically, at 550 °C and C3H8/CO2 = 2, V@SP-B achieves 18.1 % conversion, 13.7 % yield, and ∼77 % selectivity, maintaining stability over 36 h. The study establishes a direct structure–property–performance relationship driven by boron-induced acid–redox synergy, oxygen-vacancy enrichment, and hierarchical porosity for selective, durable CO2-ODHP.
我们报道了一种硼修饰的vanadia@SAPO-34催化剂(V@SP-B),它将lewis -酸性B3 +位点与氧化还原活性VOX物质结合在一起,以增强二氧化碳辅助丙烷的氧化脱氢(CO2-ODHP)。催化剂通过H3BO3蚀刻和VO(acac)2浸渍合成,形成了层次微介孔纳米反应器。XRD证实CHA骨架保留了更小的晶体(31 vs 37 nm),而FT-IR和Raman显示新的B-O / B-O - b键,增强的VO振动和空位标记表明缺陷密度增加。HR-XPS显示出更高的B3+掺入率(66. %),V4+/V5+比值升高(1.3),氧空位比显著升高(OV/OL = 2.4)。纹理分析显示增强的表面积(515 m2 g−1)和孔隙体积(0.46 cm3 g−1)。氧化还原和酸碱研究证实更容易还原性,更强的氢溢出,增强活性位点的分散(11.4 %),增加酸度(828µmol g−1),改善CO2结合(155µmol g−1)。MD模拟支持这些发现,揭示了更强的CO2吸附和更低的空位形成和反应障碍。催化,在550°C和C3H8/CO2 = 2下,V@SP-B的转化率为18.1 %,产率为13.7 %,选择性为~ 77 %,在36 h内保持稳定。该研究建立了一种直接的结构-性能-性能关系,由硼诱导的酸-氧化还原协同作用、氧空位富集和选择性、耐用的CO2-ODHP的分层孔隙度驱动。
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引用次数: 0
Ferrocene-linked triazine-based porous organic polymers as multifunctional platforms for CO2 recognition, separation and utilization 二茂铁连接三嗪基多孔有机聚合物作为CO2识别、分离和利用的多功能平台
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-02-10 DOI: 10.1016/j.jcou.2026.103356
Mohamed Gamal Mohamed , Wei-Chun Huang , Mohsin Ejaz , Yang-Chin Kao , Yen-Min Lo , Ahmed A.K. Mohammed , Yen-Ling Kuan , Shiao-Wei Kuo
The development of efficient materials that can capture CO2 and catalyze its conversion into value-added organic compounds is critically important. The concept of CO2 Capture and Utilization (CCU) is gradually gaining the attention of researchers. In this study, we designed and synthesized ferrocene and triazine-based porous organic polymers (POP), named FC-TPT-POP and FC-TPT-Ph-POP, through a Schiff base reaction for CO2 capture, and utilized them as catalysts to transform CO2 and various epoxides into cyclic carbonates via a cycloaddition process. The FC-TPT-POP showed high surface area (797 m2 g−1) and microporosity. The presence of high surface area, porosity, and triazine units having nitrogen basic sites showed excellent selective CO2 capture (3.34 mmol g−1 at 1 bar pressure/273 K, Qst of 34 kJ mol−1). Both POPs show strong CO2 selectivity at low pressures due to interactions between nitrogen sites and the highly polar, high-quadrupole CO2 molecules. FC-TPT-POP outperforms FC-TPT-Ph-POP, achieving a CO2/N2 selectivity of about 40 at 273 K. Moreover, it demonstrates outstanding catalytic performance in transforming simple terminal epoxides into cyclic carbonates using CO2 as a reactant. For example, under mild conditions (120 °C, 400 psi, 8 h), FC-TPT-POP achieved a high conversion of 99.5 % toward propylene oxide (PO). The catalytic effect arises from the synergistic interaction of Lewis basic nitrogen atoms in the triazine units and the metal active sites of ferrocene. Therefore, the development of ferrocene-triazine-based POP catalysts in this study offers a promising strategy for lowering atmospheric CO2 levels through efficient capture and catalytic conversion.
开发能够捕获二氧化碳并催化其转化为增值有机化合物的高效材料至关重要。二氧化碳捕集与利用(CCU)的概念正逐渐受到研究人员的重视。在本研究中,我们设计并合成了二茂铁和三嗪基多孔有机聚合物(POP),命名为FC-TPT-POP和FC-TPT-Ph-POP,通过席夫碱反应捕获CO2,并利用它们作为催化剂,通过环加成工艺将CO2和各种环氧化物转化为环状碳酸盐。FC-TPT-POP具有较高的比表面积(797 m2 g−1)和微孔隙度。高表面积、孔隙度和具有氮基位的三嗪单元的存在表现出良好的选择性CO2捕获(在1 bar压力/273 K下3.34 mmol g−1,Qst为34 kJ mol−1)。由于氮位点与高极性、高四极CO2分子之间的相互作用,这两种持久性有机污染物在低压下都表现出很强的CO2选择性。FC-TPT-POP优于FC-TPT-Ph-POP,在273 K下达到约40的CO2/N2选择性。此外,它在以CO2为反应物将简单末端环氧化物转化为环状碳酸盐方面表现出优异的催化性能。例如,在温和条件下(120°C, 400 psi, 8 h), FC-TPT-POP对环氧丙烷(PO)的转化率高达99.5% %。催化作用是由三嗪单元中的路易斯碱态氮原子与二茂铁的金属活性位点的协同作用引起的。因此,本研究中二茂铁-三嗪基POP催化剂的开发为通过高效捕获和催化转化降低大气CO2水平提供了一种有前途的策略。
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引用次数: 0
Evaluating operating trade-offs in CO2 hydrogenation to methanol: Conversion, energy efficiency, and techno-economic implications 评估二氧化碳加氢制甲醇的操作权衡:转换、能源效率和技术经济影响
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-02-12 DOI: 10.1016/j.jcou.2026.103359
Giovana Chinaglia Tonon Petrielli, Rubens Maciel Filho
The direct hydrogenation of carbon dioxide (CO2) to methanol presents a promising approach to mitigate atmospheric CO2 levels while producing a valuable chemical feedstock. However, the technical and economic feasibility of renewable methanol is still under evaluation, making it essential to identify optimal operational conditions and develop predictive models to enhance its competitiveness. This study investigates the optimization of the methanol production process via CO2 hydrogenation in a conventional catalytic reactor, combining simulation and statistical analysis to enhance both CO2 conversion and energy conversion efficiency (ηPtF). Aspen Plus simulations were conducted under varying pressures, temperatures, and hydrogen-to-CO2 feed ratios, and response surface methodology (RSM) was applied to identify optimal conditions. The results revealed that the maximum CO2 conversion (91.1 %) occurs at 83 bar, 247°C, and a hydrogen-to-CO2 ratio of 5:1, while the optimal ηPtF (58.4 %) is achieved at 50 bar, 210°C and a ratio of 3:1. A techno-economic assessment shows that the high-conversion scenario demands substantially higher hydrogen recycle and compression, increasing capital and operating costs. In contrast, the ηPtF-optimized condition offers lower energy demand and improved economic performance. CO2 conversion and ηPtF reached values comparable to or exceeding those in state-of-the-art studies, while highlighting the trade-off between maximizing conversion and optimizing energy efficiency. This underscores the need for tailored operating conditions. The generated surrogate models accurately predict the process outcomes, offering valuable insights for future studies, and demonstrating the potential for different economic and energy outcomes depending on the optimization strategy.
二氧化碳(CO2)直接加氢制甲醇是一种很有前途的方法,可以在生产有价值的化学原料的同时降低大气中的二氧化碳水平。然而,可再生甲醇的技术和经济可行性仍在评估中,因此确定最佳操作条件和开发预测模型以提高其竞争力至关重要。本研究对传统催化反应器中CO2加氢制甲醇工艺进行了优化研究,将模拟与统计分析相结合,以提高CO2转化率和能量转换效率(ηPtF)。Aspen Plus在不同的压力、温度和氢气/二氧化碳进料比下进行了模拟,并应用响应面法(RSM)确定了最佳条件。结果表明,在83 bar, 247℃,氢/二氧化碳比为5:1时,CO2转化率最高(91.1 %),而在50 bar, 210℃,氢/二氧化碳比为3:1时,ηPtF达到最佳(58.4 %)。技术经济评估表明,高转化率方案需要更高的氢气回收和压缩,从而增加资本和运营成本。相比之下,η ptf优化条件具有更低的能源需求和更高的经济效益。二氧化碳转化率和ηPtF达到了与最新研究相当或超过的值,同时强调了最大化转化率和优化能源效率之间的权衡。这强调了定制操作条件的必要性。生成的代理模型准确地预测了过程结果,为未来的研究提供了有价值的见解,并展示了取决于优化策略的不同经济和能源结果的潜力。
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引用次数: 0
Mineral carbonation: Thermal activation of serpentine as flexible component in energy systems 矿物碳酸化:作为能源系统中柔性组分的蛇纹石的热活化
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-02-12 DOI: 10.1016/j.jcou.2026.103353
Sampo Mäkikouri , Marjut Mälkki , Timo Leino , Juho Kauppinen , Fanni Hakanen , Henrik Tolvanen
In this article, the thermal activation of serpentine for mineral carbonation using an electrically heated fluidised bed was studied. This process step is combined into a novel process configuration with rapid thermal activation and a thermal energy storage. For the studied serpentinite mine tailings, the thermal activation durations corresponding with desired mineralogical changes were < 2 min at 700 °C, 4–8 min at 650 °C, 16–75 min at 600 °C and > 75 min at 550°C, improving reaction kinetics compared to chamber furnace processing at 650°C for 30 min or 750 °C for 15 min. In all fluidised bed experiments, the preferred mineralogical changes corresponded to a dehydroxylation degree of 52–72 % determined with simultaneous thermal analysis. Fourier-transform infrared analyser was used for online determination of the dehydroxylation degree and could be used for process control if the measurement delay was considered better. The mass and energy balances for an industrial-scale thermal activation plant matching 100,000 tCO2/a storage were calculated. The average electrical power demand was 17.4 MW, of which 22.9 % was recovered from steam and 61.7 % was stored in the thermal energy storage silos. Twelve-hour and 7-day buffering times resulted in silo volumes of 452.5 m3 and 3167 m3 and thermal energy storage capacities of 129.0 MWh and 903.2 MWh, respectively. Further studies should include process parameter optimisation as well as techno-economic and life cycle assessments to holistically improve the concept.
本文研究了电加热流化床对蛇纹石矿物碳化的热活化。该工艺步骤被结合到一个具有快速热激活和热能储存的新工艺配置中。对于所研究的蛇纹岩尾矿,与期望矿物学变化相对应的热活化时间为700°C时 2 min, 650°C时4-8 min, 600°C时16-75 min和550°C时 75 min,与在650°C下30 min或750°C下15 min的炉内处理相比,提高了反应动力学。在所有流化床实验中,优选的矿物学变化对应于同时热分析确定的52-72 %的脱羟基程度。采用傅里叶变换红外分析仪在线测定脱羟基化程度,如果考虑到测量延迟,可用于过程控制。计算了与100,000 tCO2/a储存量相匹配的工业规模热活化工厂的质量和能量平衡。平均电力需求为17.4 MW,其中22.9 %从蒸汽中回收,61.7 %储存在蓄热筒仓中。12小时和7天的缓冲时间使筒仓容积分别达到452.5 m3和3167 m3,蓄热容量分别达到129.0 MWh和903.2 MWh。进一步的研究应包括工艺参数优化以及技术经济和生命周期评估,以全面改进这一概念。
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引用次数: 0
Sustainable CO2 fixation under low CO2 pressure, solvent free conditions using a recyclable Zn-dehydroacetic acid catalyst supported on SBA-15 使用SBA-15负载的可回收锌-脱氢乙酸催化剂,在低CO2压力、无溶剂条件下进行可持续CO2固定
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-01-26 DOI: 10.1016/j.jcou.2026.103320
Salimeh Nazari Mazidi, Elham Safaei
A heterogeneous catalyst has been synthesized by immobilizing a zinc complex of the bio- derived dehydroacetic acid (DHA) ligand onto SBA-15. This catalyst was characterized by BET, XPS, FTIR, TGA, TEM, SEM, XRD, and ICP-OES, which confirmed the successful incorporation of Zn-DHA complex into the SBA-15. In combination with KI (3 mol%) as simple and inexpensive co-catalyst, the minimal amount (20 mg) of the catalyst, promoted the solvent free cycloaddition of CO₂ to epoxides at 50 °C under ambient to low CO₂ pressure (2 bar to balloon). This mesoporous catalyst exhibited excellent activity and selectivity across a broad substrate scope and could be reused for six cycles, with minimal loss in performance. Hot filtration test and ICP analysis confirmed the structural stability and heterogeneous nature of the catalytic process with negligible leaching. A key distinguishing feature of this catalyst is the modulation of Lewis acidity at Zn(II) center by the oxygen-rich DHA ligand, promotes catalyst dispersibility and improves epoxide activation. Notably, this cost-effective and reusable catalyst system avoids high CO₂ pressure and costly quaternary ammonium salts, significantly improving sustainable CO2 valorization and practical applicability.
将生物源脱氢乙酸(DHA)配体的锌配合物固定在SBA-15上,合成了一种多相催化剂。通过BET、XPS、FTIR、TGA、TEM、SEM、XRD、ICP-OES等手段对催化剂进行了表征,证实了锌- dha配合物成功掺入SBA-15中。以KI(3 mol%)作为简单廉价的助催化剂,少量(20 mg)催化剂,在50°C的环境至低CO₂压力(2 bar至气球)下,促进了CO₂对环氧化物的无溶剂环加成。该介孔催化剂在广泛的底物范围内表现出优异的活性和选择性,并且可以重复使用6次,性能损失最小。热过滤试验和ICP分析证实了催化过程的结构稳定性和非均相性,浸出可以忽略不计。该催化剂的一个重要特征是富氧DHA配体对Zn(II)中心Lewis酸度的调节,促进了催化剂的分散性,提高了环氧化物的活化。值得注意的是,这种具有成本效益和可重复使用的催化剂系统避免了高CO₂压力和昂贵的季铵盐,显著提高了CO2的可持续增值和实用性。
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引用次数: 0
Study of CO2 absorption into monoethanolamine solution in a rotating packed bed 旋转填料床中单乙醇胺溶液吸收CO2的研究
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-01-27 DOI: 10.1016/j.jcou.2026.103345
Jaesu Jang , Gwan Hong Min , Sung Chan Nam , Kibong Lee , Sunghoon Lee
Conventional packed bed (PB) absorbers for post-combustion CO2 capture are hindered by large equipment size and high regeneration energy. Rotating packed bed (RPB) has emerged as a promising alternative by intensifying mass transfer and reducing process footprint. In this study, a lab-scale RPB system employing high-concentration monoethanolamine (MEA) solutions at concentrations of 30–70 wt% was investigated for CO2 absorption. Sensitivity analysis was conducted by varying motor speed (300–800 RPM), liquid flow rate, gas flow rate (3–6 Nm3/h), and reboiler temperature, while maintaining a CO2 capture efficiency of 90 %. The results revealed that higher motor speeds and concentrated MEA solutions enhanced mass transfer and cyclic capacity, while reducing overall power consumption. In addition, an optimal L/G ratio of 6.90 L/m3 minimized the total energy demand, while a regeneration temperature of 102 °C was found to be the minimum required. Lastly, the electricity consumption of the RPB was measured and compared with the regeneration energy in the stripper to evaluate the relative magnitude of the RPB power usage. As a result, the electrical energy consumption of the RPB accounted for about 2 % less than the heat duty required by the reboiler. This study demonstrates that an RPB-based CO2 capture system outperforms a PB despite its reduced packing height and reactor volume. The use of highly concentrated MEA solutions further enhances RPB process intensification, offering valuable guidance for industrial-scale CO2 capture system design and optimization.
传统的填料床(PB)吸收体存在设备体积大、再生能量高的问题。旋转填料床(RPB)已成为一种有前途的替代方案,通过加强传质和减少过程足迹。在本研究中,采用浓度为30-70 wt%的高浓度单乙醇胺(MEA)溶液,研究了实验室规模的RPB系统对CO2的吸收。在保持90% %的CO2捕集效率的情况下,通过改变电机转速(300-800 RPM)、液体流速、气体流速(3-6 Nm3/h)和再沸器温度进行敏感性分析。结果表明,较高的电机转速和集中的MEA解决方案增强了传质和循环容量,同时降低了总体功耗。此外,最佳L/G比为6.90 L/m3时,总能量需求最小,而再生温度为102℃时,所需能量最小。最后,测量了RPB的用电量,并与汽提塔的再生能量进行了比较,以评估RPB用电量的相对幅度。结果,RPB的电能消耗比再沸器所需的热负荷低约2% %。该研究表明,基于rpb的CO2捕集系统尽管降低了填料高度和反应器体积,但其性能优于PB。高浓度MEA解决方案的使用进一步增强了RPB过程的集约化,为工业规模的CO2捕集系统设计和优化提供了有价值的指导。
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引用次数: 0
Revealing the structure-activity relationship of Mn3O4/TiO2 via phase engineering for enhanced photocatalytic CO₂ reduction 通过相工程揭示Mn3O4/TiO2增强光催化CO 2还原的构效关系
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-02-16 DOI: 10.1016/j.jcou.2026.103357
Eunhee Gong , Hye Rim Kim , Yunju Hwang , Jeonghyeon Lee , Jin-Woo Jung , Chang-Hee Cho , In Young Kim , Su-Il In
The structure-activity relationship plays a crucial role for enhanced photocatalytic performance, nevertheless, precisely controlling the phase of transition metal oxides remains a significant challenge. Herein, we developed 2D-layered Mn3O4 decorated with TiO2 catalyst to investigate the effects of manganese oxide phase on photocatalytic CO2 reduction activity. We optimized the manganese oxide phase by varying the amount of the TiCl4 precursor. During the synthesis reaction, TiCl4 is a key role for determining the oxidation state of manganese oxide. We identified that Mn3O4 is the best phase for photocatalytic CO2 reduction, and Mn3O4/TiO2 exhibits 20.1-, 7.8-fold enhanced photocatalytic CO2 reduction performance than pristine TiO2 and Mn3O4, respectively. The improved photocatalytic activity is relevant to the phase of manganese oxide, the enhanced separation of charge carriers and prolonged lifetimes of charge carriers. In situ X-ray Absorption Near-Edge Structure (XANES) confirms the changes of oxidation state under photocatalytic CO2 reduction conditions. Furthermore, the photocatalytic mechanism is proposed by in situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) analysis. This study provides an effective design strategy for modulating oxidation state of transition metal oxide-based photocatalyst for enhanced solar fuels generation.
结构-活性关系对增强光催化性能起着至关重要的作用,然而,精确控制过渡金属氧化物的相仍然是一个重大的挑战。在此,我们开发了二氧化钛催化剂修饰的二维层状Mn3O4,以研究锰氧化物相对光催化CO2还原活性的影响。我们通过改变二氧化钛前驱体的量来优化氧化锰相。在合成反应中,TiCl4是决定氧化锰氧化态的关键因素。我们发现Mn3O4是光催化CO2还原的最佳相,Mn3O4/TiO2的光催化CO2还原性能分别比原始TiO2和Mn3O4提高20.1倍和7.8倍。光催化活性的提高与氧化锰的相态、载流子分离的增强和载流子寿命的延长有关。原位x射线吸收近边结构(XANES)证实了光催化CO2还原条件下氧化态的变化。此外,通过漫反射红外傅立叶变换光谱(DRIFTS)原位分析,提出了光催化机理。本研究为过渡金属氧化物基光催化剂的氧化态调控提供了一种有效的设计策略。
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引用次数: 0
Mechanisms of CO2 flooding front migration and injection-production regulation in heterogeneous reservoirs: A large-scale visual physical simulation study 非均质油藏CO2驱前运移及注采调控机理:大规模可视化物理模拟研究
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-01-21 DOI: 10.1016/j.jcou.2026.103339
Yutong Yan , Weifeng Lyu , Hongwei Yu , Wenfeng Lv , Shumin Ni
The unclear migration mechanisms of CO2 flooding fronts in heterogeneous reservoirs significantly constrain the efficiency enhancement of CCUS-EOR technology. This study, employing a self-designed large-scale two-dimensional visual physical model, systematically reveals for the first time the dominant control mechanism of interlayer spatial configuration on channeling pathways and the laws of injection-production regulation. Experiments demonstrate that when gas is injected on the side with a developed interlayer, CO2 preferentially migrates horizontally along the high-permeability layer and, after breakthrough, channels laterally into the low-permeability layer through the non-interlayer interface. Conversely, gas injection on the non-interlayer side induces vertical channeling. The mode of “gas injection at the non-interlayer end + oil production at the interlayer end” coupled with early soaking expanded the miscible zone by 29.81 % and achieved a total recovery factor of 91.04 %. Although increasing the pressure difference in the low-permeability layer by 1.5 times can forcibly initiate oil mobilization, channeling must be suppressed to avoid inter-layer imbalance. The evolution of the miscible zone exhibits a two-stage characteristic of “synergistic growth - competitive substitution”: dominated by mass transfer-displacement synergy before breakthrough, and by gas channeling and phase competition afterwards. The high-permeability layer readily forms an arc-shaped miscible enrichment zone, while the low-permeability layer exhibits narrow, strip-like expansion limited by mass transfer. Future work needs to focus on enhancing dynamic identification of the miscible zone, optimizing soaking timing, and combining numerical simulation to study the influence of interlayer spatial configuration on inter-layer channeling. These results provide key experimental evidence for CCUS-EOR development in heterogeneous reservoirs, promoting the advancement of inter-layer conflict regulation from mechanistic understanding to engineering optimization.
非均质油藏中CO2驱前沿运移机制不明确,严重制约了CCUS-EOR技术的效率提升。本研究采用自行设计的大尺度二维可视化物理模型,首次系统揭示了层间空间构型对窜流路径的主导控制机制和注采调节规律。实验表明,在夹层发育的一侧注气时,CO2优先沿高渗透层水平运移,突破后通过非夹层界面向低渗透层横向运移。相反,非层间侧的注气会引起垂直通道。采用“非层间端注气+层间端 采油”的模式,再加上早期浸泡,可将混相层扩大29.81 %,总采收率达到91.04 %。虽然将低渗透层压差提高1.5倍可以强制启动石油动员,但必须抑制窜流,以避免层间不平衡。混相带的演化呈现出“协同生长-竞争替代”的两个阶段特征:突破前以传质-驱替协同为主,突破后以气窜和相竞争为主。高渗层易形成弧形混相富集带,低渗层受传质限制呈窄条状扩张。今后的工作需要加强对混相带的动态识别,优化浸泡时间,并结合数值模拟研究层间空间构型对层间通道的影响。这些结果为非均质储层CCUS-EOR开发提供了关键的实验依据,促进了层间冲突调控从机理认识向工程优化的推进。
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引用次数: 0
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Journal of CO2 Utilization
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