Chemical Engineering Science最新文献_第3页

Droplet deformation and breakup in 3D-printed millichannels featuring arrays of rectangular obstacles with different configurations 具有不同结构的矩形障碍物阵列的3d打印微通道中的液滴变形和破裂

IF 4.3 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2026-05-15 Epub Date: 2026-01-31 DOI: 10.1016/j.ces.2026.123493

A.T.S. Cerdeira, J.B.L.M. Campos, J.M. Miranda, J.D.P. Araújo

The present study investigates the deformation and breakup of droplets in 3D-printed millichannels containing an array of rectangular obstacles with different configurations: transverse, longitudinal, and herringbone. Experiments were performed with two different viscosity ratios between phases (X = 0.026 and X = 30) under a range of flow conditions, with systematic variations of the flow rate ratio (Ø) and the Capillary number of the dispersed phase (Ca_d). Flow visualization combined with image processing techniques enables a quantitative characterization of droplet area and velocity distributions at the inlet, across the array of obstacles, and at the outlet region. The results show that, while the droplet area at the inlet region is determined by the flow rate, the outlet area distributions are predominantly governed by the configuration of the array of rectangular obstacles and porosity, with negligible influence from Ø. For a constant Ø, as Ca_d increases, viscous stresses become stronger relative to interfacial tension, promoting droplet deformation and breakup. Among the tested designs, the herringbone configuration produced the smallest droplets, followed by the transverse and longitudinal arrays. Additionally, porosity was found to play a critical role: lower porosity enhanced droplet confinement and promoted faster breakup, while higher porosity weakened droplet-obstacle interactions and reduced breakup efficiency. These findings highlight the effectiveness of array of obstacles as a passive strategy to promote droplet breakup and size uniformity, offering new design guidelines for droplet manipulation in millifluidic devices.

本研究研究了3d打印微通道中液滴的变形和破裂，这些微通道包含一系列具有不同构型的矩形障碍物：横向、纵向和人字形。实验采用两种不同的相黏度比（X = 0.026和X = 30），在一定的流动条件下，系统地改变了流速比（Ø）和分散相毛细管数（Cad）。流动可视化与图像处理技术相结合，可以定量表征液滴在入口、穿过障碍物阵列和出口区域的面积和速度分布。结果表明，进口区域的液滴面积由流量决定，而出口区域的分布主要受矩形障碍物阵列的配置和孔隙率的影响，Ø的影响可以忽略不计。对于Ø常数，随着Cad的增加，黏性应力相对于界面张力变得更强，促进液滴变形和破裂。在测试设计中，人字排列产生的液滴最小，其次是横向排列和纵向排列。此外，孔隙度也起到了关键作用：较低的孔隙度增强了液滴的束缚，促进了更快的破碎，而较高的孔隙度减弱了液滴与障碍的相互作用，降低了破碎效率。这些发现突出了障碍物阵列作为一种被动策略来促进液滴破碎和尺寸均匀性的有效性，为微流控装置中的液滴操作提供了新的设计指导。

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引用次数: 0

Process parameters optimization of ohmic heat-assisted vacuum evaporation of sapodilla juice and quality modelling of its concentrate 欧姆热辅助真空蒸发皂角汁工艺参数优化及浓缩液质量建模

IF 4.3 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2026-05-15 Epub Date: 2026-02-09 DOI: 10.1016/j.ces.2026.123561

Vasudeva Rao Vangapandu, Venkata S.P. Bitra

Using an ohmic heat-assisted vacuum evaporation (OHVE) system, concentration of clarified sapodilla fruit juice was carried out and it was compared to rotary vacuum evaporation (VE) method in order to maximize total soluble solids (TSS) content of concentrated sapodilla juice and compare the quality of concentrated sapodilla juice using both methods. A laboratory-scale OHVE system was designed and fabricated to achieve the targeted objective. Using Box-Behnken design of response surface methodology, optimized the OHVE process parameters, including temperature (50, 60, and 70 °C), holding time (40, 80, and 120 min), voltage gradient (9, 12, and 15 V/cm), and vacuum pressure (400, 500, and 600 mmHg), to achieve the desired TSS for concentrated sapodilla fruit juice. Sapodilla juice concentrate was produced using both OHVE and VE methods. OHVE was performed under optimized conditions voltage gradient of 14.50 V/cm and vacuum pressure of 574 mm Hg (gauge) while varying the temperature (50–70 °C) and processing time (0–120 min) to assess their effects on the concentration process. Quality characteristics of OHVE sapodilla fruit juice concentrate were in the range of pH: 4.0 to 4.634, density: 1064 to 1098 kg/m³, ascorbic acid: 0.033 to 0.039 mg/100 mL, non-enzymatic browning index: 0.101 to 0.544 at OD_420nm, titratable acidity: 5.37% to 6.03%, viscosity: 5.37 to 35.1 cP, L*: 20.92 to 10.59, a*: 0.07 to 8.7, b*: 11.02 to 16.39, hue angle: 55.67° to 89.99°, and chroma: 11.06 to 15.42. Results showed that integrating ohmic heating with vacuum evaporation significantly improved juice quality retention compared to conventional rotary vacuum evaporation.

利用欧姆热辅助真空蒸发（OHVE）系统对皂角果汁进行浓缩，并与旋转真空蒸发（VE）法进行比较，以最大限度地提高皂角果汁浓缩液的总可溶性固形物（TSS）含量，比较两种方法对皂角果汁浓缩液的质量。为实现上述目标，设计并制作了实验室规模的OHVE系统。采用响应面法的Box-Behnken设计，优化OHVE工艺参数，包括温度（50、60和70℃）、保温时间（40、80和120 min）、电压梯度（9、12和15 V/cm）和真空压力（400、500和600 mmHg），以获得浓缩皂苷果汁所需的TSS。采用OHVE法和VE法生产皂角浓缩汁。在电压梯度为14.50 V/cm、真空压力为574 mm Hg（压力表）、温度（50 ~ 70℃）和处理时间（0 ~ 120 min）变化的优化条件下进行OHVE，评估其对浓缩过程的影响。OHVE枇杷汁浓缩液的质量特征为pH: 4.0 ~ 4.634，密度：1064 ~ 1098 kg/m3，抗坏血酸：0.033 ~ 0.039 mg/100 mL，非酶褐变指数：0.101 ~ 0.544 (OD420nm)，可滴定酸度：5.37% ~ 6.03%，粘度：5.37 ~ 35.1 cP, L*: 20.92 ~ 10.59, a*: 0.07 ~ 8.7, b*: 11.02 ~ 16.39，色相角：55.67°~ 89.99°，色度：11.06 ~ 15.42。结果表明，与传统的旋转真空蒸发相比，欧姆加热与真空蒸发相结合显著提高了果汁品质的保持性。

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引用次数: 0

Water state engineering of Nanodiamond-Modified hydrogels for antifreeze and high toughness 纳米金刚石改性抗冻高韧性水凝胶的水态工程

IF 4.3 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2026-05-15 Epub Date: 2026-02-06 DOI: 10.1016/j.ces.2026.123551

Jianan Xie , Wenhao Ding , Mingyu Yang , Jingbo Xu , Zhenjie Lu , Xiao Cheng , Shugang Pan , Xin Wang , Junwu Zhu , Yongsheng Fu

The water contained within hydrogels can be categorized into bound water, intermediate water, and free water. Among these, free water readily freezes at subzero temperatures, leading to ice formation and ultimately compromising hydrogel performance. Conventional antifreeze hydrogel designs mainly rely on the introduction of exogenous antifreeze agents, while it often directly sacrifices the water content of the system, thereby neglecting the fundamental role of water state distribution within the polymer network and undermining the core properties that water imparts to hydrogels. In this study, we propose a “water state engineering” strategy that addresses the root cause of freezing by tailoring the interfacial water interactions. By incorporating amine-functionalized nanodiamonds (aND) as interfacial bound water regulators into polyvinyl alcohol (PVA) and xanthan gum (XG), we constructed a PVA/XG-aND double-network hydrogel. This structure facilitates the formation of a molecular-scale interfacial bound water network, effectively modulating the free-to-bound water ratio. The hydrogel prepared by this method exhibits biological non-toxicity, demonstrating superior tensile strength (2088 kPa) and fracture elongation (380%) while maintaining its original water content, along with a reduced freezing point of −26 °C. This work highlights the crucial role of water state regulation in enhancing the cryo-resistance of hydrogels.

水凝胶中所含的水可分为结合水、中间水和自由水。其中，自由水很容易在零度以下结冰，导致结冰，最终影响水凝胶的性能。传统的防冻水凝胶设计主要依赖于外源防冻剂的引入，而这往往直接牺牲了体系的含水量，从而忽略了聚合物网络中水态分布的基本作用，破坏了水赋予水凝胶的核心性质。在这项研究中，我们提出了一种“水状态工程”策略，通过调整界面水的相互作用来解决冻结的根本原因。通过将胺功能化纳米金刚石（aND）作为界面结合水调节剂掺入聚乙烯醇（PVA）和黄原胶（XG）中，构建了PVA/XG-aND双网络水凝胶。这种结构促进了分子尺度界面结合水网络的形成，有效地调节了自由结合水比。通过该方法制备的水凝胶具有生物无毒性，在保持其原始含水量的同时，具有优异的抗拉强度（2088 kPa）和断裂伸长率（380%），并且冰点降低到- 26°C。这项工作强调了水状态调节在增强水凝胶抗冻性方面的关键作用。

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引用次数: 0

Fabrication of long aliphatic chains (C18)-based adhesive with strong underwater adhesion strength 具有较强水下粘附力的长脂肪链（C18）基粘合剂的制备

IF 4.3 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2026-05-15 Epub Date: 2026-02-09 DOI: 10.1016/j.ces.2026.123558

Huizhen Jiang , Bin Yang , Yuhang Wu , Funing Zhang , Huaiyuan Wang , Weina Kong , Fatang Liu

Conventional adhesives typically form strong and durable bonds only on dry surfaces, and their adhesion effectiveness often weakens or disappears entirely in the presence of water at the bonding interface. Thus, developing high-performance adhesives suitable for underwater applications is crucial. In this study, we successfully developed a high-strength (4.13 MPa) epoxy-based underwater adhesive (called MGEO) using a simple one-step, solvent-free strategy. After underwater adhesion, the adhesive rapidly transforms from liquid to solid at room temperature, forming a strong adhesion that requires no additional processing. The hydrophobic effect of the long aliphatic chain (C18) effectively facilitated water displacement at the interface, while multiple intermolecular interactions enhanced interfacial adhesion, ensuring strong and reliable underwater performance. Additionally, the adhesive exhibited excellent adhesive stability after it was immersed in different aqueous solutions for 20 d [alkali (3.39 MPa), salt (4.37 MPa), and artificial seawater (4.28 MPa)]. Moreover, the adhesive exhibited outstanding long-term stability in water and a strength of 3.87 MPa after 50 d of immersion. After the adhesive underwent 50 cold-hot shock cycles, it exhibited a strength of 3.59 MPa. After it underwent five underwater adhesion cycles, its strength was 2.29 MPa. The long-term durability of MGEO adhesive underwater demonstrates its excellent application potential in underwater repair.

传统的粘合剂通常只能在干燥的表面上形成牢固而持久的粘合，并且在粘合界面存在水时，其粘合效果往往会减弱或完全消失。因此，开发适用于水下应用的高性能粘合剂至关重要。在这项研究中，我们通过简单的一步无溶剂策略，成功开发了一种高强度（4.13 MPa）的环氧基水下粘合剂（MGEO）。胶粘剂在水下粘合后，在室温下迅速由液体转变为固体，形成不需要额外处理的强附着力。长脂肪链（C18）的疏水作用有效地促进了界面处的水位移，而多重分子间相互作用增强了界面粘附，确保了强大可靠的水下性能。在不同的水溶液[碱（3.39 MPa）、盐（4.37 MPa）、人工海水（4.28 MPa）]中浸泡20 d后，胶粘剂表现出优异的粘接稳定性。此外，该胶粘剂在水中表现出良好的长期稳定性，浸泡50 d后强度达到3.87 MPa。经50次冷热冲击循环后，胶粘剂的强度为3.59 MPa。经过5次水下黏附循环后，其强度为2.29 MPa。MGEO胶粘剂在水下的长期耐久性表明其在水下修复中具有良好的应用潜力。

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引用次数: 0

Development of a compartment modeling framework from axisymmetric CFD models: Extracting flow topology for industrial fermenters 基于轴对称CFD模型的隔室建模框架的开发：提取工业发酵罐的流动拓扑

IF 4.3 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2026-05-15 Epub Date: 2026-02-05 DOI: 10.1016/j.ces.2026.123502

Parth Shah , Satchit Nagpal , Dong Hun Kwak , Jung Ho Kim , Jae Hoon Cho , Sang Min Park , Kosan Roh , Jun-Woo Kim , Joseph Sang-Il Kwon

Industrial-scale fermentation processes often suffer from insufficient mixing, which leads to significant spatial heterogeneity in key variables such as dissolved oxygen and substrate concentrations. These gradients adversely impact oxygen transfer, microbial physiology, and overall process productivity. While computational fluid dynamics (CFD) simulations offer detailed insights into flow behavior, their computational requirements limit their applicability to large-scale systems. This study presents the development of a computationally efficient compartment modeling (CM) framework as an alternative to CFD for industrial fermenters. To this end, first, an axisymmetric CFD model was constructed to represent the industrial fermenter geometry. This approach was chosen over a full three-dimensional model to leverage the symmetry inherent in many reactor designs, thereby reducing computational costs while still capturing essential hydrodynamic features, such as axial and radial velocity components and turbulent kinetic energy, across different time instances. These variables were extracted to define flow topology and intercompartment flow rates within the CM. By averaging velocity fields and smoothing gradients, a stable and scalable compartmental representation of reactor hydrodynamics was achieved. The model was validated against CFD data through visualizations of flow patterns and velocity profiles, demonstrating its ability to capture spatial heterogeneity while significantly reducing computational costs. This CM framework offers a versatile tool for integrating kinetic models, facilitating process optimization, and improving design in complex fermenter systems.

工业规模的发酵过程经常受到混合不足的影响，这导致了溶解氧和底物浓度等关键变量的显著空间异质性。这些梯度对氧传递、微生物生理和整个过程的生产率产生不利影响。虽然计算流体动力学（CFD）模拟提供了对流动行为的详细见解，但其计算要求限制了其在大规模系统中的适用性。本研究提出了一种计算效率高的隔间建模（CM）框架的发展，作为工业发酵罐CFD的替代方案。为此，首先建立了代表工业发酵罐几何结构的轴对称CFD模型。这种方法被选择在一个完整的三维模型中，以利用许多反应堆设计中固有的对称性，从而降低计算成本，同时仍然捕获基本的流体动力学特征，如轴向和径向速度分量和湍流动能，跨越不同的时间实例。提取这些变量来定义CM内的流动拓扑和隔室间流速。通过平均速度场和平滑梯度，获得了一个稳定的、可扩展的反应堆流体力学分区表示。通过流动模式和速度剖面的可视化，该模型通过CFD数据进行了验证，证明了其能够在显著降低计算成本的同时捕获空间异质性。这个CM框架提供了一个多功能的工具，用于整合动力学模型，促进过程优化，并改善复杂发酵系统的设计。

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引用次数: 0

Ambient-temperature recovery of high-boiling solvent by solar-driven interfacial evaporation 太阳能驱动界面蒸发法在室温下回收高沸点溶剂

IF 4.3 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2026-05-15 Epub Date: 2026-02-12 DOI: 10.1016/j.ces.2026.123597

Qiuyu Mei, Cailin Yang, Youzhou Jiang, Kai Han

The recovery of high-boiling solvents is significant due to their wide application in fields such as drug synthesis. Solar-driven interfacial evaporation (SIE) technology is a green and energy-efficient technology with thermal localization, offering a promising strategy for separating and recovering high-boiling solvents. In this study, a black silicon-based evaporator was fabricated, achieving high evaporation rates of 4.25, 1.69, and 1.50 kg m⁻² h⁻¹ for the high-boiling solvents N,N-dimethylformamide (DMF), dimethyl sulfoxide (DMSO), and N-methyl-2-pyrrolidone (NMP), respectively, under ambient temperature and pressure. During evaporation and recovery from a 1 wt% Clindamycin hydrochloride (Clin)/DMF solution under 1sun, the membrane interfacial temperature was only 72°C, while the bulk solution remained at ambient temperature. Consequently, the chemical structure of Clin remained stable during the DMF evaporation process. The high purity (97.44%) of the recovered DMF, with water detected as the sole residual impurity, underscores the efficiency and selectivity of this solar-driven evaporation process. Using a 40 mm-diameter photothermal membrane, 8 h of interfacial evaporation achieved a solvent recovery of 40%. This work provides a novel and effective SIE approach for ambient temperature and pressure recovery of high-boiling solvents.

高沸点溶剂在药物合成等领域有着广泛的应用，其回收具有重要意义。太阳能驱动界面蒸发（SIE）技术是一种绿色节能的热局部化技术，为高沸点溶剂的分离和回收提供了一种很有前景的策略。本研究制备了黑硅基蒸发器，在常温常压下，对高沸点溶剂N，N-二甲基甲酰胺（DMF），二甲基亚砜（DMSO）和N-甲基-2-吡咯烷酮（NMP）分别实现了4.25,1.69和1.50 kg m−2 h−1的高蒸发速率。在1wt %盐酸克林霉素(Clin)/DMF溶液的蒸发和回收过程中，在1个太阳下，膜界面温度仅为72℃，而主体溶液保持在环境温度。因此，在DMF蒸发过程中，Clin的化学结构保持稳定。回收的DMF纯度高（97.44%），其中水是唯一残留杂质，强调了这种太阳能驱动蒸发过程的效率和选择性。采用直径40 mm的光热膜，界面蒸发8 h，溶剂回收率为40%。本研究为高沸点溶剂的环境温度和压力回收提供了一种新颖有效的SIE方法。

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引用次数: 0

Kinetic study and reaction model of chlorotrimethylsilane hydrolysis to hexamethyldisiloxane 氯三甲基硅烷水解成六甲基二硅氧烷的动力学研究及反应模型

IF 4.3 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2026-05-15 Epub Date: 2026-02-08 DOI: 10.1016/j.ces.2026.123542

Yue Zhang , Rui-Qi Jia , Guang-Wen Chu , Bao-Chang Sun , Liang-Liang Zhang , Jian-Feng Chen

As an important organosilicon intermediate, hexamethyldisiloxane (HMDSO) is widely used in the fabrication of silicone resins, functional coatings, and fine chemicals. However, the reaction kinetics remain insufficiently quantified, limiting process optimization. In this study, the reaction mechanism and pathway of HMDSO formation from chlorotrimethylsilane (CTMS) via hydrolysis were first elucidated using density functional theory simulations. The reaction network was simplified into two consecutive reactions: substitution and condensation. The reversibility and kinetic parameters of both reactions were experimentally determined using conductance and other methods, exhibiting that the substitution reaction is a rapid and irreversible process, while the condensation reaction is reversible and the rate-limiting step. Moreover, an apparent reaction model coupling reaction and mass transfer was developed for the practical liquid–liquid heterogeneous CTMS hydrolysis process. The predicted performance of the reaction by the model, including conversion ratio and reaction time, was in good agreement with experimental results.

六甲基二硅氧烷（HMDSO）是一种重要的有机硅中间体，广泛应用于有机硅树脂、功能涂料和精细化学品的制备。然而，反应动力学仍然不够量化，限制了工艺优化。本研究首次利用密度泛函理论模拟阐明了氯三甲基硅烷（CTMS）水解生成HMDSO的反应机理和途径。将反应网络简化为两个连续的反应：取代反应和缩合反应。用电导等方法测定了两种反应的可逆性和动力学参数，表明取代反应是一个快速的不可逆过程，而缩合反应是可逆的，是限速步骤。此外，建立了实际液-液非均相CTMS水解反应耦合传质的表观反应模型。模型预测的反应性能，包括转化率和反应时间，与实验结果吻合较好。

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引用次数: 0

Unveiling the synergistic effect between dielectric barrier discharge plasma and ZSM-5 in cracking of n-hexane: experimental and mechanistic study 揭示介质阻挡放电等离子体与ZSM-5在正己烷裂解中的协同作用：实验与机理研究

IF 4.3 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2026-05-15 Epub Date: 2026-02-08 DOI: 10.1016/j.ces.2026.123548

Ketao Shi , Nianming Jiao , Youbing Zhu , Zhen Xu , Ningjing Tang , Hui Wang

Plasma, with its highly energetic and reactive nature, was proposed as an effective external field to intensify the catalytic cracking of n-hexane over ZSM-5 zeolite. The effects of zeolite acidity, reaction temperature, plasma power, catalyst bed location vs the discharge region, and discharge atmosphere were systematically investigated. It was found that plasma significantly enhanced the cracking of n-hexane, and when the catalyst was placed in the plasma discharge region the reaction performance was the best, indicating a synergistic effect between plasma and ZSM-5. Compared with conventional catalytic cracking, the introduction of plasma increased the n-hexane conversion from 20.8% to 59.3% and the light olefins yield from 6.3% to 27.1% at 400 °C in the argon atmosphere. In-situ optical emission spectroscopy (OES), n-hexane-TPD, and electron collision reaction calculations based on the Boltzmann equation demonstrated that plasma effectively promoted the cleavage of C–C/C–H bonds, facilitating the formation of reactive radicals (e.g., CH, C₂, and H) and leading to the formation of smaller species. These reactive intermediates were more likely to undergo subsequent transformations over zeolite acid sites, thereby enhancing the radical-driven reaction pathway and significantly increasing the yield of light olefins. These findings demonstrate the synergistic effect between plasma and catalysts in promoting alkane cracking under moderate conditions, offering a promising strategy for the production of light olefins in an energy-efficient way.

等离子体具有高能量和反应性，可作为强化正己烷在ZSM-5沸石上催化裂化的有效外场。系统考察了沸石酸度、反应温度、等离子体功率、催化剂床位对放电区域和放电气氛的影响。实验发现，等离子体对正己烷的裂解有明显的促进作用，且当催化剂放置在等离子体放电区域时，反应性能最好，说明等离子体与ZSM-5之间存在协同作用。与传统催化裂化反应相比，等离子体的引入使正己烷转化率从20.8%提高到59.3%，轻烯烃收率从6.3%提高到27.1%。原位发射光谱（OES）、正己烷- tpd和基于玻尔兹曼方程的电子碰撞反应计算表明，等离子体有效地促进了C-C / C-H键的裂解，促进了活性自由基（如CH、C2和H）的形成，并导致了更小物质的形成。这些活性中间体更有可能在沸石酸位点上进行后续转化，从而增强了自由基驱动的反应途径，显著提高了轻质烯烃的收率。这些发现证明了等离子体和催化剂在促进烷烃在中等条件下裂解的协同作用，为节能生产轻质烯烃提供了一种有希望的策略。

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引用次数: 0

Coupled evolution of pore and carbon skeleton structure during coal and biomass pyrolysis up to 1400 °C: Mechanistic Insights and predictive Modeling 煤和生物质热解至1400 °C时孔隙和碳骨架结构的耦合演化：机理见解和预测建模

IF 4.3 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2026-05-15 Epub Date: 2026-02-09 DOI: 10.1016/j.ces.2026.123552

Dezhi Chen , Junmeng Li , Ji Long , Shihao Zhou , Jun Xu , Kai Xu , Long Jiang , Yi Wang , Sheng Su , Song Hu , Jun Xiang

This study systematically investigates the nonlinear evolution of pore structure and its coupled mechanism with chemical structural changes of the char from the pyrolysis of six biomass and three coal samples across 350–1400 °C. The results revealed that the BET surface area (S_BET) and pore volume (V_total) exhibit a distinct three-stage trend of “increase–decrease-increase” with increasing temperature, whereas the average pore diameter (D_average) follows the opposite trend. The first inflection point (FIP) and second inflection point (SIP) are primarily observed at 600 °C and 1000 °C for biochar, whereas around 700 °C and 1100 °C for coal chars. FIP and SIP correlate closely with the sum of the raw sample’s moisture and volatile contents, and the ratio of small to large aromatic rings of the char, respectively. In addition, in Stage I (350 °C-FIP), the increase in S_BET is strongly governed by the decline in H/C atomic ratio, Raman parameter α and A_(GR+VL+VR)/A_D, indicating that volatile release and the breakdown of aliphatic structures dominate pore generation. In Stage Ⅱ (FIP-SIP), the magnitude of S_BET reduction correlates positively with A_(GR+VL+VR)/A_D, reflecting partial collapse of pores induced by carbon skeleton compression. In Stage Ⅲ (SIP-1400 °C), S_BET exhibits strong positive correlation with structural index A_(GR+VL+VR)/A_G·C_RM, Mg and Ca volatilization disturbs carbon layers, creating inter-cluster dislocations, promoting new pores. Based on these findings, a three-stage mechanistic model was established. Furthermore, a unified pore structure prediction model across wide temperature range was constructed and validated, with S_BET average absolute error of only 5.41 m²/g.

本研究系统地研究了6种生物质和3种煤样在350-1400 °C范围内热解成焦的孔隙结构的非线性演化及其与化学结构变化的耦合机制。结果表明：随着温度的升高，孔隙比表面积（SBET）和孔隙体积（Vtotal）呈现出明显的“增大-减小-增大”的三阶段趋势，而平均孔径（daaverage）则呈现相反的趋势；生物炭的第一拐点（FIP）和第二拐点（SIP）主要在600 °C和1000 °C时观察到，而煤焦在700 °C和1100 °C左右观察到。FIP和SIP分别与原料样品的水分和挥发物含量的总和和焦炭的小环与大环的比例密切相关。此外，在第I阶段（350 °C- fip）， SBET的增加受到H/C原子比、拉曼参数α和A(GR+VL+VR)/AD的下降的强烈控制，表明挥发性释放和脂肪族结构的分解主导了孔隙的生成。在Ⅱ阶段（FIP-SIP）， SBET的减少幅度与A(GR+VL+VR)/AD呈正相关，反映了碳骨架压缩导致孔隙部分塌陷。在Ⅲ阶段（SIP-1400 °C）， SBET与结构指数A(GR+VL+VR)/AG·CRM呈强正相关，Mg和Ca的挥发扰乱了碳层，造成簇间位错，促进了新孔隙的形成。在此基础上，建立了一个三阶段的机制模型。建立并验证了宽温度范围内统一的孔隙结构预测模型，SBET平均绝对误差仅为5.41 m2/g。

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引用次数: 0

Low-concentration CO2 adsorption performance of MCM-41 molecular sieve doped with heterometals inherent in fly ash 掺粉煤灰异质金属的MCM-41分子筛低浓度CO2吸附性能研究

IF 4.3 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2026-05-15 Epub Date: 2026-02-05 DOI: 10.1016/j.ces.2026.123503

Kong Haowen , Wu Hong , Zhang Li , Wang Ping , Li Ruimeng

This study investigated the utilization of heterometals, such as Al, Fe, and Ti, inherent in fly ash in the synthesis of metal-doped MCM-41 molecular sieve for the efficient capture of low-concentration carbon dioxide (CO₂). While active Si and Al components were extracted by an acid leaching-alkali fusion pretreatment process, the adsorbent was prepared using an in situ doping method, resulting in metal-doped MCM-41 with small grain sizes and ordered mesoporous channels. The distribution of metal heteroatoms was optimized by adjusting the synthesis pH. Al atoms were concentrated on the surface of the molecular sieve to form active sites, while Fe and Ti atoms were preferably incorporated into the bulk phase to regulate the pore structure. C10.5-M41, synthesized at pH 10.5, exhibited abundant surface acid-base sites and an increased pore size of 5.4 nm. In low-concentration CO₂ adsorption tests, the material demonstrated adsorption capacities of 1.31 mmol/g at 25 °C and 1.06 mmol/g at 90 ℃. The adsorption capacity decreased by 38% at 90℃ with 8% water vapor. In addition, 90% of the adsorption capacity at 25 ℃ could be retained after ten regeneration cycles. Based on thermodynamic analysis, physical adsorption dominates at 25 ℃, while chemical adsorption is predominant at 90 ℃. The incorporation of metal ions into the framework increases the pore size of the adsorbent and reduces its internal transport resistance for CO₂ gas. This study utilized heterometals inherent in fly ash as a resource and contributed to the design of high-capacity and thermally stable CO₂ adsorbent materials.

本研究探讨了利用粉煤灰中固有的Al、Fe、Ti等异质金属合成掺杂金属的MCM-41分子筛，高效捕集低浓度二氧化碳（CO2）。采用酸浸-碱融合预处理工艺提取活性Si和Al组分，采用原位掺杂法制备吸附剂，制备出粒径小、介孔通道有序的金属掺杂MCM-41。通过调节合成ph来优化金属杂原子的分布，Al原子集中在分子筛表面形成活性位点，而Fe和Ti原子则优选掺入体相来调节孔结构。在pH 10.5下合成的C10.5-M41具有丰富的表面酸碱位点，孔径增大到5.4 nm。在低浓度CO2吸附试验中，材料在25 ℃时的吸附量为1.31 mmol/g，在90 ℃时的吸附量为1.06 mmol/g。当温度为90℃，水蒸气含量为8%时，吸附量下降38%。在25 ℃条件下，经过10次再生后，吸附量仍可保持90%。热力学分析表明，25 ℃时以物理吸附为主，90 ℃时以化学吸附为主。金属离子加入到框架中增加了吸附剂的孔径，降低了其对CO2气体的内部输送阻力。本研究利用粉煤灰中固有的异质金属作为资源，为设计高容量、热稳定的CO2吸附剂材料做出了贡献。

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