Chemical Engineering Science最新文献

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Simultaneous water sterilization and photocatalytic degradation by full-spectrum responsive Zn3In2S6/WO3−x S-scheme heterojunction: Mechanism insight and toxicity assessment 全谱响应Zn3In2S6/WO3−x S-scheme异质结同时光催化降解水：机理洞察和毒性评估

IF 4.1 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2025-04-11 DOI: 10.1016/j.ces.2025.121651

Xiaofeng Liu , Zhenbang Meng , Weirui Chen , Rui Huang , Qiaoshan Chen , Qi He , Ri Chen , Lihua Zhou , Wenxia Wang

It is crucial to develop highly efficient full-spectrum-responsive S-scheme heterojunctions for wastewater purification. Herein, an innovative Zn₃In₂S₆/WO₃₋_x heterojunction was synthesized, featuring full-spectrum responsiveness. It achieved 100 % inactivation of methicillin-resistant Staphylococcus aureus (MRSA) in 45 min and 90.34 % photocatalytic degradation of tetracycline (TC) in 120 min. Its effectiveness was mainly due to rapid charge separation via the S-scheme electron transfer pathway and near-infrared light absorption from the Localized Surface Plasmon Resonance (LSPR) effect of WO_3−x. Importantly, it showed robust photocatalytic capacity under diverse conditions. Quenching experiments and EPR analysis confirmed that ·OH and ·O₂⁻ played essential roles in photocatalytic degradation. Intermediate products were identified using LC-MS, 3D EEMs, and TOC, revealing the degradation pathway. Quantitative structure–activity relationship (QSAR) analysis suggested reduced ecotoxicity of pollutants. A potential mechanism for enhanced sterilization and photocatalytic degradation was proposed. This study provides a theoretical and experimental basis for designing novel heterojunctions for solar-assisted water purification.

开发用于废水净化的高效全谱响应 S 型异质结至关重要。本文合成了一种创新的 Zn3In2S6/WO3-x 异质结，具有全谱响应性。它在 45 分钟内实现了对耐甲氧西林金黄色葡萄球菌（MRSA）100% 的灭活，在 120 分钟内实现了对四环素（TC）90.34% 的光催化降解。其有效性主要归功于通过 S 型电子传递途径实现的快速电荷分离以及 WO3-x 的局部表面等离子体共振（LSPR）效应产生的近红外光吸收。重要的是，它在各种条件下都表现出强大的光催化能力。淬灭实验和 EPR 分析证实，-OH 和 -O2- 在光催化降解过程中发挥了重要作用。利用 LC-MS、3D EMMs 和 TOC 对中间产物进行了鉴定，从而揭示了降解途径。定量结构-活性关系（QSAR）分析表明，污染物的生态毒性有所降低。提出了增强杀菌和光催化降解的潜在机制。这项研究为设计用于太阳能辅助水净化的新型异质结提供了理论和实验基础。

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引用次数: 0

Three-phase flow through rough-walled fractures: An experimental investigation of relative permeabilities under varying saturation histories 通过粗壁裂缝的三相流动：不同饱和度历史下相对渗透率的实验研究

IF 4.1 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2025-04-11 DOI: 10.1016/j.ces.2025.121665

Mohammed Eliebid, Abdelhalim Mohamed, Maziar Arshadi, Mohammad Piri

Relative permeabilities are essential for assessing subsurface flow performance for applications such as hydrocarbon recovery, enhanced geothermal, CO₂ storage, Hydrogen geo-storage, and water resources management. This study presents a comprehensive macro-scale experimental investigation of three-phase relative permeabilities in a rough-walled fracture across a broad range of saturation histories. The findings indicate that the brine relative permeability was primarily dependent on its saturation level. In contrast, oil relative permeability exhibited a pronounced dependence on saturation history, showing a quadratic correlation at low oil saturations (dominated by layer flow) and a quartic relationship at high saturations (governed by oil-filled fracture elements). Gas relative permeability was influenced by both its own saturation and saturation history. Higher flow rates were observed to enhance the relative permeabilities of both oil and gas. These trends are linked to changes in fluid configurations and transport dynamics within the fracture aperture.

相对渗透率对于评估油气回收、强化地热、二氧化碳封存、氢气地质封存和水资源管理等应用领域的地下流动性能至关重要。本研究对粗糙壁断裂中的三相相对渗透率进行了全面的宏观尺度实验研究，涵盖了广泛的饱和历史。研究结果表明，盐水的相对渗透率主要取决于其饱和度。相比之下，石油相对渗透率对饱和度历史具有明显的依赖性，在低石油饱和度时（由油层流动主导）呈现二次相关关系，而在高饱和度时（由充满石油的裂缝元素主导）则呈现四次相关关系。气体相对渗透率受其自身饱和度和饱和度历史的影响。据观察，流速越高，石油和天然气的相对渗透率越高。这些趋势与断裂孔道内流体配置和传输动力学的变化有关。

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引用次数: 0

The growth habit of methane hydrate film at the Gas–liquid interface 气液界面甲烷水合物膜的生长习性

IF 4.1 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2025-04-11 DOI: 10.1016/j.ces.2025.121622

Hui Zhang , Jing-Chun Feng , Bin Wang , Yongming Shen , Yue Zhang , Si Zhang

Understanding the interfacial formation characteristics of methane hydrates in deep-sea environments is fundamental to isolate leaking methane (a potent greenhouse gas). We observed the three-dimensional (3-D) characteristics of methane hydrate film (HF) growth at the gas–liquid interface (GLI) under different pressures using micro-nano industrial X-ray computed tomography (X-CT). The results indicate that the primary growth mode of the HFs at the GLI after initial formation was growth through the continuous formation of cracks. This crack-induced growth enhanced the hydrate conversion rate. We compared the thickness distribution characteristics of the hydrate growth under varying pressures. While the early HF exhibited thickening, the average thickness in the later stage of hydrate growth remained relatively stable and homogeneity. This study on the growth characteristics of HFs at the GLI provides a foundation for further development of efficient and stable methods for hydrate utilization and sequestration.

了解深海环境中甲烷水合物的界面形成特征是隔离泄漏甲烷（一种强效温室气体）的基础。我们使用微纳工业 X 射线计算机断层扫描（X-CT）技术观察了不同压力下甲烷水合物膜（HF）在气液界面（GLI）生长的三维（3-D）特征。结果表明，气液界面水合物在初始形成后的主要生长模式是通过裂缝的不断形成而生长。这种裂缝诱导的生长提高了水合物的转化率。我们比较了不同压力下水合物生长的厚度分布特征。虽然早期的水合氢表现出增厚，但水合物生长后期的平均厚度保持相对稳定和均匀。这项关于 GLI 水合物生长特征的研究为进一步开发高效稳定的水合物利用和封存方法奠定了基础。

引用次数: 0

Segment anything model-based method for precise froth size determination in flotation process 基于分段模型的浮选过程泡沫粒度精确测定方法

IF 4.1 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2025-04-11 DOI: 10.1016/j.ces.2025.121657

Jinglong Wang , Runda Jia , Jun Zheng , Mengyu Zhang , Dakuo He

Automated control of the flotation process relies on indicative information from froth images, such as texture, flow rate, shape, and froth size distribution. Conventional image segmentation methods often produce errors and lack robustness when handling variations in mineral color, resolution, and contrast. Deep learning approaches, while effective, demand extensive labeled data and high training costs. This paper introduces a high-precision froth image segmentation algorithm utilizing the Segment Anything Model (SAM) visual foundation model for flotation froth image analysis. Evaluated on three diverse mineral image datasets against manual segmentation, the method demonstrates over 90 % segmentation accuracy without requiring training or fine-tuning of the SAM, significantly reducing the need for labor-intensive dataset labeling and lowering application costs. The proposed approach offers a more efficient and cost-effective solution for froth image segmentation in the mining industry, enhancing automation and process optimization.

浮选过程的自动控制依赖于泡沫图像的指示性信息，如纹理、流速、形状和气泡大小分布。传统的图像分割方法在处理矿物颜色、分辨率和对比度的变化时往往会产生误差，并且缺乏鲁棒性。深度学习方法虽然有效，但需要大量标记数据和高昂的训练成本。介绍了一种利用分段任意模型（SAM）视觉基础模型进行浮选泡沫图像分析的高精度泡沫图像分割算法。通过对三种不同的矿物图像数据集进行人工分割的评估，该方法在不需要对SAM进行训练或微调的情况下，显示出超过90%的分割准确率，显著减少了对劳动密集型数据集标记的需求，降低了应用成本。该方法为采矿业泡沫图像分割提供了一种高效、经济的解决方案，提高了自动化程度和流程优化程度。

引用次数: 0

From laboratory to outdoor: Construction of an integrated Fe3+ smart sensing platform and its agricultural applications 从实验室到户外：Fe3+集成智能传感平台建设及其农业应用

IF 4.1 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2025-04-11 DOI: 10.1016/j.ces.2025.121650

Li Sheng , Xingli Ding , Yulin Tang , Xu Cheng , Ge Zhang , Yuqiao Zhang , Min Ji , Jianming Zhang , Long Zhang

In the realm of food quality and safety monitoring, traditional on-site detection methods have faced challenges. Conventional sensors often lack the ability to provide rapid and accurate results, with limited sensitivity and selectivity. They are also bulky, making them inconvenient for portable applications. To address these limitations, we developed a smart sensing platform using 3D printing. By incorporating a fluorescent hydrogel of poly(9-aminofluorene) (P9AF) and sodium alginate (SA) as the cross-linking substrate, the platform’s P9AF-SA film has a porous network. This structure offers enhanced ion transport channels and active sites, enabling rapid and selective detection of Fe³⁺ ions among numerous anions and cations. A 3D printed smartphone-based readout device further enables portable detection. Our platform achieved a limit of detection (LOD) of 67.47 μg/L, far below the WHO safety threshold, and was successfully applied to agricultural products. This study not only provides a novel on-site detection device but also paves the way for developing highly efficient portable sensors, significantly advancing the field.

在食品质量和安全监控领域，传统的现场检测方法一直面临着挑战。传统传感器通常无法提供快速准确的结果，灵敏度和选择性也有限。它们还十分笨重，不便便携。为了解决这些局限性，我们利用 3D 打印技术开发了一种智能传感平台。通过加入聚（9-氨基芴）（P9AF）荧光水凝胶和海藻酸钠（SA）作为交联基底，该平台的 P9AF-SA 薄膜形成了多孔网络。这种结构提供了增强的离子传输通道和活性位点，能够在众多阴离子和阳离子中快速、选择性地检测 Fe3+ 离子。基于 3D 打印的智能手机读出设备进一步实现了便携式检测。我们的平台实现了 67.47 μg/L 的检测限（LOD），远远低于世界卫生组织的安全阈值，并成功应用于农产品。这项研究不仅提供了一种新颖的现场检测装置，还为开发高效便携式传感器铺平了道路，极大地推动了该领域的发展。

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引用次数: 0

Efficient dehydrogenation of ethanol to acetaldehyde over silica supported Cu catalyst prepared from microwave-assisted wet-kneading 微波辅助湿揉法制备二氧化硅负载Cu催化剂上乙醇脱氢制乙醛的研究

IF 4.1 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2025-04-11 DOI: 10.1016/j.ces.2025.121664

Zerui Su , Jian Zhang , Yang Li , Zheyu Qiao , Ziyuan Qiao , Lihang Wei , Xiaoyuan Qin , Xiaoxue Mu , Feng-Shou Xiao

Cu-based catalysts are crucial for the dehydrogenation of ethanol (EtOH) to acetaldehyde (AcH); however, their performance decreases at higher temperatures due to the low Tammann temperature of Cu species. In this study, we synthesized silica-supported Cu catalysts using microwave-assisted wet-kneading. Characterizations revealed a typical core–shell structure (Cu@SiO₂-WK), which demonstrated high activity, excellent selectivity, and superior stability for ethanol dehydrogenation. The Cu@SiO₂-WK achieved 96.2 % EtOH conversion with 99.9 % selectivity to AcH at 260 °C. After 160 h of reaction, it maintained an EtOH conversion of 90.5 % and AcH selectivity of ∼99.9 %. Following simple calcination, the catalyst’s activity was fully regenerated to 96.1 %. Model catalysts and in situ FT-IR spectra indicate that the core–shell structure significantly enhances the catalyst’s performance in the dehydrogenation of EtOH to AcH.

铜基催化剂对于乙醇（EtOH）脱氢成乙醛（AcH）至关重要；然而，由于铜的塔曼温度较低，其性能在较高温度下会降低。在本研究中，我们利用微波辅助湿法捏合合成了二氧化硅支撑的铜催化剂。表征结果表明，该催化剂具有典型的核壳结构（Cu@SiO2-WK），在乙醇脱氢过程中具有高活性、优异的选择性和卓越的稳定性。在 260 °C 下，Cu@SiO2-WK 实现了 96.2 % 的 EtOH 转化率和 99.9 % 的 AcH 选择性。反应 160 小时后，EtOH 转化率仍为 90.5%，对 AcH 的选择性为 99.9%。简单煅烧后，催化剂的活性完全再生至 96.1%。模型催化剂和原位傅立叶变换红外光谱表明，核壳结构显著提高了催化剂在将 EtOH 脱氢为 AcH 过程中的性能。

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引用次数: 0

Mixture equilibrium and kinetics of flue gas components in CALF-20 CALF-20烟气组分混合平衡及动力学

IF 4.7 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2025-04-11 DOI: 10.1016/j.ces.2025.121663

Akhil Dilipkumar, Anshu Shukla, Dan Zhao, Shamsuzzaman Farooq

Binary and ternary mixture equilibrium and kinetic data for CO₂, N₂ and H₂O in CALF-20 particles over a wide range of temperatures (25–150 ⁰C), gas concentrations and relative humidity levels (0–90%) is presented. Data is obtained from the dynamic column breakthrough (DCB) method. Proposed empirically modified extended Sips – Henry equilibrium isotherm model reliably describes mixture equilibrium. The single component isotherm parameters are retained and new parameters from the empirical modification are calibrated with binary mixture data. The mixture isotherm model correctly predict measured ternary equilibrium data for CO₂/H₂O/N₂ mixtures. The linear driving force (LDF) mass transfer model with the rate constants calculated for Knudsen controlled macropore transport mechanism and equilibrium data from the mixture model accurately predict binary and ternary mixture breakthrough responses. The isosteric heat of adsorption for H₂O in the presence of N₂, CO₂ and helium elucidate adsorbate-adsorbent and adsorbate–adsorbate interactions.

介绍了二氧化碳、N2 和 H2O 在 CALF-20 颗粒中的二元和三元混合物平衡和动力学数据，涉及温度范围（25-150 ⁰C）、气体浓度和相对湿度水平（0-90%）。数据来自动态色谱柱突破 (DCB) 方法。根据经验修正的扩展 Sips - Henry 平衡等温线模型可靠地描述了混合物平衡。保留了单组分等温线参数，并用二元混合物数据校准了经验修正后的新参数。混合物等温线模型能正确预测 CO2/H2O/N2 混合物的三元平衡测量数据。线性驱动力（LDF）传质模型利用克努森控制的大孔传输机制计算出的速率常数和混合物模型的平衡数据，准确预测了二元和三元混合物的突破反应。在 N2、CO2 和氦气存在下 H2O 的等效吸附热阐明了吸附剂-吸附剂和吸附剂-吸附剂之间的相互作用。

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引用次数: 0

Experimental study and mechanism analysis of coal spontaneous combustion inhibition based on oxidation characteristics of key coal reaction groups 基于煤关键反应基团氧化特性的煤自燃抑制实验研究及机理分析

IF 4.1 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2025-04-11 DOI: 10.1016/j.ces.2025.121656

Xun Zhang , Chen Yu , Bing Lu , Gang Bai , Huimin Liang , Jieyu Li

Based on the staged oxidation development process dominated by the temperature node of coal itself, the correlation contribution of the staged oxidation reaction of key active groups is thoroughly analyzed. The mathematical relationship between macroscopic gas characteristics and microscopic active groups of different coal samples was established. The exothermic mechanism of the self-reaction associated with the key active groups during the staged oxidation of coal was investigated using quantum chemical calculations. The performance of inhibitors is significantly diminished during the latent development stage of coal. The key temperature node accelerates the desorption of crystal water from the physical inhibitor, enabling it to act more effectively on the coal body. Meanwhile, the chemical antioxidant becomes more active in quenching and capturing key active groups, thereby inhibiting the chain reaction process and the release of heat from self-reactions. The critical temperature inhibition method ensures a more comprehensive suppression of coal oxidation at key stages. The research provides valuable insights and data support for enhancing the safety of coal storage and transportation.

基于煤自身温度节点主导的阶段氧化发育过程，深入分析了关键活性基团阶段氧化反应的相关贡献。建立了不同煤样宏观气体特征与微观活性基团之间的数学关系。利用量子化学计算方法研究了煤分阶段氧化过程中与关键活性基团相关的自反应放热机理。在煤的潜伏发育阶段，抑制剂的性能明显下降。关键温度节点加速了物理抑制剂对结晶水的解吸，使其更有效地作用于煤体。同时，化学抗氧化剂在猝灭和捕获关键活性基团方面变得更加活跃，从而抑制链式反应过程和自反应释放热量。临界温度抑制法确保在关键阶段更全面地抑制煤的氧化。该研究为提高煤炭储运安全提供了有价值的见解和数据支持。

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引用次数: 0

Experimental investigation and kinetic modeling of n-propylbenzene oxidation under high-pressure conditions 高压条件下正丙苯氧化的实验研究与动力学建模

IF 4.1 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2025-04-11 DOI: 10.1016/j.ces.2025.121653

Xu-Peng Yu , Du Wang , Xu Zhang , Xiang Gao , Ahmed E. Mansy , Jin-Hu Yang , Zhen-Yu Tian

In this study, oxidation experiments of n-propylbenzene (NPB) were conducted at 24 atm, with equivalence ratios (Φ = 0.5, 1.0, and 2.0), and temperatures ranging from 640-820 K. A total of 17 products and intermediates were qualitatively and quantitatively detected using gas chromatography (GC) and gas chromatography-mass spectrometry (GC–MS). The most important rate coefficients, H-abstraction reactions by OH at the α, β, and γ carbon sites of the side chain, were theoretically calculated at G4//wb97xd/6-311 + g(d,p) level. A comprehensive oxidation model of NPB, comprising 285 species and 1953 elementary reactions was constructed to understand the high-pressure oxidation. The model was extensively validated across a pressure range of 1–50 atm using oxidation data from JSR reactor, mole fraction data from shock tube, ignition delay time, and laminar flame speed. According to the selectivity of products analysis, high pressure promotes the complete progression of the reaction and reduces the formation of PAHs.

本研究在 24 个大气压、等效比（Φ = 0.5、1.0 和 2.0）和 640-820 K 的温度范围内进行了正丙基苯（NPB）的氧化实验。利用气相色谱（GC）和气相色谱-质谱法（GC-MS）对总共 17 种产物和中间产物进行了定性和定量检测。在 G4//wb97xd/6-311+g(d,p)水平上对侧链 α、β 和 γ 碳位点上的羟基萃取反应中最重要的速率系数进行了理论计算。为了理解 NPB 的高压氧化过程，我们构建了一个包含 285 个物种和 1953 个基本反应的 NPB 综合氧化模型。利用 JSR 反应器的氧化数据、冲击管的分子分数数据、点火延迟时间和层流火焰速度，在 1-50 atm 的压力范围内对该模型进行了广泛验证。根据产物的选择性分析，高压促进了反应的完全进行，并减少了多环芳烃的生成。

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引用次数: 0

Enhanced Long-Time prediction of Gas-Solid flows via Integrating Reduced-Order model with Cluster-Based network model 通过将降序模型与基于集群的网络模型相结合，增强气固流动的长期预测能力

IF 4.1 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science

Pub Date : 2025-04-10 DOI: 10.1016/j.ces.2025.121634

Tingting Liu , Yu Jiang , Yuanye Zhou , Sheng Chen , Luowei Cao , Xizhong Chen , Zheng-Hong Luo

Understanding gas–solid flows is crucial due to their extensive industrial processes. Integrating data-driven models into the analysis has been increasingly recognized for its ability to reduce computational costs while decoding the intricate flow behaviors. In this work, a coupling approach using Singular Value Decomposition (SVD) and Cluster-based Network Model (CNM) was developed, where SVD is employed to extract and decompose the essential information into key modes then CNM is performed for exploring the spatiotemporal correlations between modes, ultimately achieving robust long-time predictions of the system. Applied to various fluidized beds, including bubbling and spout beds, this method demonstrates stability and accuracy in predicting gas–solid flows by capturing crucial flow patterns and minimizing data redundancy. With its industrial scale running time stability, the coupling approach shows promise as a cost-effective tool for the design and optimization of real industrial processes.

由于广泛的工业过程，了解气固流动是至关重要的。将数据驱动模型集成到分析中，在解码复杂的流动行为的同时减少了计算成本，这一点越来越得到人们的认可。本文提出了一种基于奇异值分解（SVD）和聚类网络模型（CNM）的耦合方法，利用奇异值分解（SVD）提取基本信息并将其分解为关键模式，然后利用CNM探索模式之间的时空相关性，最终实现系统的鲁棒长期预测。应用于各种流化床，包括鼓泡床和喷淋床，该方法通过捕获关键流动模式和最小化数据冗余，在预测气固流动方面表现出稳定性和准确性。由于其工业规模运行时间的稳定性，耦合方法有望成为设计和优化实际工业过程的一种经济有效的工具。

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引用次数: 0

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