Pub Date : 2025-04-25DOI: 10.1016/j.ces.2025.121724
S. Atri, A. Kumar, S. Fotovati, H.V. Tafreshi, B. Pourdeyhimi
In this study, we utilized a Discrete Element Model (DEM) approach to generate fibrous media comprised of flexible fibers with different diameters. This approach allowed simulations to predict the solid volume fraction (SVF) of the resulting media, which is a unique advantage over previous models reported in the literature, where SVF was used as an input to the fiber generation algorithms. We generated realistic bimodal fibrous media in which coarse and fine fibers of different mass ratios, SVFs, and coarse-to-fine fiber diameter ratios were intimately blended. Permeability of the resulting media were predicted by numerically solving the Stokes equations in the 3-D space between the fibers. To circumvent the need to conduct excessively expensive numerical simulations, we developed a Micro-Macro simulation approach in which the fine fibers were treated as porous matrix engulfing the coarse fibers. The accuracy of our CPU-efficient Micro-Macro simulations was assessed through comparison with the more accurate Micro-Micro (CPU-intensive) simulations, where the actual geometry of both the fine and coarse fibers were resolved. The Micro-Macro simulations were then used to produce a dataset of permeability values to be used in assessing the accuracy of different methods of defining an equivalent unimodal structure that can represent a bimodal fibrous medium for permeability calculation. Our study concluded that the cube-root and area-weighted mean diameter models provide the most accurate predictions for the permeability of bimodal fibrous media. Our theoretical results were compared with experimental data and reasonable agreement was observed.
{"title":"Novel microscale-macroscale approach to predict permeability of bimodal fibrous media comprised of soft fibers","authors":"S. Atri, A. Kumar, S. Fotovati, H.V. Tafreshi, B. Pourdeyhimi","doi":"10.1016/j.ces.2025.121724","DOIUrl":"https://doi.org/10.1016/j.ces.2025.121724","url":null,"abstract":"In this study, we utilized a Discrete Element Model (DEM) approach to generate fibrous media comprised of flexible fibers with different diameters. This approach allowed simulations to predict the solid volume fraction (SVF) of the resulting media, which is a unique advantage over previous models reported in the literature, where SVF was used as an input to the fiber generation algorithms. We generated realistic bimodal fibrous media in which coarse and fine fibers of different mass ratios, SVFs, and coarse-to-fine fiber diameter ratios were intimately blended. Permeability of the resulting media were predicted by numerically solving the Stokes equations in the 3-D space between the fibers. To circumvent the need to conduct excessively expensive numerical simulations, we developed a Micro-Macro simulation approach in which the fine fibers were treated as porous matrix engulfing the coarse fibers. The accuracy of our CPU-efficient Micro-Macro simulations was assessed through comparison with the more accurate Micro-Micro (CPU-intensive) simulations, where the actual geometry of both the fine and coarse fibers were resolved. The Micro-Macro simulations were then used to produce a dataset of permeability values to be used in assessing the accuracy of different methods of defining an equivalent unimodal structure that can represent a bimodal fibrous medium for permeability calculation. Our study concluded that the cube-root and area-weighted mean diameter models provide the most accurate predictions for the permeability of bimodal fibrous media. Our theoretical results were compared with experimental data and reasonable agreement was observed.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"184 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872308","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-24DOI: 10.1016/j.ces.2025.121727
Shilin Zhao , Yuxin Qian , Yuchen Wang , Qi Liu , Hanzi Liu , Lidong Wang , Zhiqiang Sun
This work systematically studies Hg0 removal performance of CuS modified Fe2O3 or MnO2 (SaMebOz). It shows Fe2O3 has a stronger catalytic enhancement than MnO2 on Hg0 removal of SaMebOz. Increasing Fe2O3 amount leads to a volcanic change in Hg0 removal performance of SaFebOx. At the optimal molar ratio of Fe2O3 to CuS with 3:2, Hg0 removal efficiency and Hg0 adsorption rate are 93.2% and 99.3%, respectively, where 92.5% of Hg0 is removed by adsorption. S2-, adsorbed oxygen (Oads), lattice oxygen (Olat), and hollow site of MnO2 are the main active sites to adsorb or catalyze Hg0, and Oads has a stronger Hg0 adsorption capacity than Olat. Hg0 removal by SaMebOz involves the catalytic oxidation of Hg0 to HgO by active sites, followed by the stable HgS formation through the reaction of HgO with active sulfur (S2-). The findings provide important guidance for flue gas Hg0 removal in complete adsorption way.
{"title":"Catalytically enhanced adsorption of flue gas mercury by CuS modified iron or manganese oxides","authors":"Shilin Zhao , Yuxin Qian , Yuchen Wang , Qi Liu , Hanzi Liu , Lidong Wang , Zhiqiang Sun","doi":"10.1016/j.ces.2025.121727","DOIUrl":"10.1016/j.ces.2025.121727","url":null,"abstract":"<div><div>This work systematically studies Hg<sup>0</sup> removal performance of CuS modified Fe<sub>2</sub>O<sub>3</sub> or MnO<sub>2</sub> (S<sub>a</sub>Me<sub>b</sub>O<sub>z</sub>). It shows Fe<sub>2</sub>O<sub>3</sub> has a stronger catalytic enhancement than MnO<sub>2</sub> on Hg<sup>0</sup> removal of S<sub>a</sub>Me<sub>b</sub>O<sub>z</sub>. Increasing Fe<sub>2</sub>O<sub>3</sub> amount leads to a volcanic change in Hg<sup>0</sup> removal performance of S<sub>a</sub>Fe<sub>b</sub>O<sub>x</sub>. At the optimal molar ratio of Fe<sub>2</sub>O<sub>3</sub> to CuS with 3:2, Hg<sup>0</sup> removal efficiency and Hg<sup>0</sup> adsorption rate are 93.2% and 99.3%, respectively, where 92.5% of Hg<sup>0</sup> is removed by adsorption. S<sup>2-</sup>, adsorbed oxygen (O<sub>ads</sub>), lattice oxygen (O<sub>lat</sub>), and hollow site of MnO<sub>2</sub> are the main active sites to adsorb or catalyze Hg<sup>0</sup>, and O<sub>ads</sub> has a stronger Hg<sup>0</sup> adsorption capacity than O<sub>lat</sub>. Hg<sup>0</sup> removal by S<sub>a</sub>Me<sub>b</sub>O<sub>z</sub> involves the catalytic oxidation of Hg<sup>0</sup> to HgO by active sites, followed by the stable HgS formation through the reaction of HgO with active sulfur (S<sup>2-</sup>). The findings provide important guidance for flue gas Hg<sup>0</sup> removal in complete adsorption way.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"313 ","pages":"Article 121727"},"PeriodicalIF":4.1,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872312","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-24DOI: 10.1016/j.ces.2025.121726
Jonne Niemi, Roland Balint, Juho Lehmusto
A novel experimental setup was developed and tested to investigate high-temperature corrosion under temperature gradients. The setup considers simultaneous deposit formation and corrosion. The setup is composed of an air-cooled probe with an exchangeable vertically aligned steel sample, inserted into a hot tube furnace. The experiments were conducted by exposing P235GH and AISI316 steel samples to PbCl2 and KCl. The salt material was vaporized from a crucible. The salt subsequently nucleated on the cooled sample surface. Material temperatures of 350–500 °C and atmospheric temperatures of 650–750 °C were tested. PbCl2 deposition increased with higher atmospheric temperatures. In addition, the oxide layer thicknesses increased with higher material and atmospheric temperatures. The presence of KCl together with PbCl2 further enhanced corrosion. The formation of FeCl2 induced the formation of eutectic molten phases, enhancing the corrosion. This research contributes to understanding the challenges posed by high-temperature corrosion in waste-fired boilers.
{"title":"Laboratory-scale method for high-temperature gas-to-solid deposition and corrosion studies – P235GH and AISI316 exposed to PbCl2 and KCl","authors":"Jonne Niemi, Roland Balint, Juho Lehmusto","doi":"10.1016/j.ces.2025.121726","DOIUrl":"10.1016/j.ces.2025.121726","url":null,"abstract":"<div><div>A novel experimental setup was developed and tested to investigate high-temperature corrosion under temperature gradients. The setup considers simultaneous deposit formation and corrosion. The setup is composed of an air-cooled probe with an exchangeable vertically aligned steel sample, inserted into a hot tube furnace. The experiments were conducted by exposing P235GH and AISI316 steel samples to PbCl<sub>2</sub> and KCl. The salt material was vaporized from a crucible. The salt subsequently nucleated on the cooled sample surface. Material temperatures of 350–500 °C and atmospheric temperatures of 650–750 °C were tested. PbCl<sub>2</sub> deposition increased with higher atmospheric temperatures. In addition, the oxide layer thicknesses increased with higher material and atmospheric temperatures. The presence of KCl together with PbCl<sub>2</sub> further enhanced corrosion. The formation of FeCl<sub>2</sub> induced the formation of eutectic molten phases, enhancing the corrosion. This research contributes to understanding the challenges posed by high-temperature corrosion in waste-fired boilers.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"313 ","pages":"Article 121726"},"PeriodicalIF":4.1,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872311","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Soot emission reduction is critical for achieving clean and efficient coal utilization. A fundamental understanding of soot formation characteristics from different coal macerals under high-temperature conditions is essential for controlling soot generation at the source. In this study, Saimengte (SMT) coal was selected as the raw material, and its macerals were separated and enriched via density gradient centrifugation. Rapid pyrolysis of different macerals was conducted in a drop tube furnace, and the resulting soot was systematically characterized using XRD, Raman spectroscopy, TEM, and TGA. The results demonstrate that vitrinite (SMT-V) generates significantly higher soot yields compared to inertinite. SMT-V-derived soot exhibits a lower degree of aromatic condensation in the inner core, leading to higher oxidation reactivity. In contrast the outer surface develops a more ordered graphitized structure with reduced oxidation reactivity. These findings provide valuable insights into the relationship between coal macerals and their soot formation mechanisms.
{"title":"Influence of vitrinite and inertinite on the soot formation characteristics during coal rapid pyrolysis in a drop tube furnace","authors":"Donglai Ma, Hua Ma, Peng Lv, Yonghui Bai, Xudong Song, Jiaofei Wang, Weiguang Su, Juntao Wei, Guangsuo Yu","doi":"10.1016/j.ces.2025.121722","DOIUrl":"https://doi.org/10.1016/j.ces.2025.121722","url":null,"abstract":"Soot emission reduction is critical for achieving clean and efficient coal utilization. A fundamental understanding of soot formation characteristics from different coal macerals under high-temperature conditions is essential for controlling soot generation at the source. In this study, Saimengte (SMT) coal was selected as the raw material, and its macerals were separated and enriched via density gradient centrifugation. Rapid pyrolysis of different macerals was conducted in a drop tube furnace, and the resulting soot was systematically characterized using XRD, Raman spectroscopy, TEM, and TGA. The results demonstrate that vitrinite (SMT-V) generates significantly higher soot yields compared to inertinite. SMT-V-derived soot exhibits a lower degree of aromatic condensation in the inner core, leading to higher oxidation reactivity. In contrast the outer surface develops a more ordered graphitized structure with reduced oxidation reactivity. These findings provide valuable insights into the relationship between coal macerals and their soot formation mechanisms.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"25 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872314","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
We propose a dual-active-site catalytic system with an interlayer confinement effect, inducing a vertical synergistic interaction to enhance CO2 reduction reaction (CO2RR) activity and selectivity. Using density functional theory (DFT) calculations, we systematically explore how interlayer distance influences CO2 adsorption and key reaction intermediates. Our results reveal that confinement enhances electronic interactions, but excessive confinement induces steric hindrance, reducing catalytic activity. We identify two distinct carbon–carbon (CC) coupling mechanisms: a single-site adsorption pathway involving *CO desorption followed by *CO + *CO coupling and a dual-site adsorption pathway enabled by *CHO rotation and subsequent *CO + *CHO coupling. Strong confinement enhances dual-site coupling. The optimal interlayer distance for ethanol production is 6.5 Å (limiting potential: 0.7 V), while 7.5 Å favors CH4 selectivity. This study establishes a theoretical framework for confined dual-site catalysis, providing design principles of interlayer-confined-enabled vertically aligned dual-site synergy approach for next-generation CO2 electrocatalysts.
{"title":"Interlayer-confined-enabled dual-site synergy Strategy: A bilayer FeN4 catalyst for enhanced CO2 reduction and C-C coupling","authors":"Xinyi Lu, Yanyan Xia, Yihui Bao, Zhencheng Ye, Houyang Chen, Haicai Huang","doi":"10.1016/j.ces.2025.121728","DOIUrl":"https://doi.org/10.1016/j.ces.2025.121728","url":null,"abstract":"We propose a dual-active-site catalytic system with an interlayer confinement effect, inducing a vertical synergistic interaction to enhance CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) activity and selectivity. Using density functional theory (DFT) calculations, we systematically explore how interlayer distance influences CO<sub>2</sub> adsorption and key reaction intermediates. Our results reveal that confinement enhances electronic interactions, but excessive confinement induces steric hindrance, reducing catalytic activity. We identify two distinct carbon–carbon (C<img alt=\"single bond\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/sbnd.gif\" style=\"vertical-align:middle\"/>C) coupling mechanisms: a single-site adsorption pathway involving *CO desorption followed by *CO + *CO coupling and a dual-site adsorption pathway enabled by *CHO rotation and subsequent *CO + *CHO coupling. Strong confinement enhances dual-site coupling. The optimal interlayer distance for ethanol production is 6.5 Å (limiting potential: 0.7 V), while 7.5 Å favors CH<sub>4</sub> selectivity. This study establishes a theoretical framework for confined dual-site catalysis, providing design principles of interlayer-confined-enabled vertically aligned dual-site synergy approach for next-generation CO<sub>2</sub> electrocatalysts.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"73 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872313","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-23DOI: 10.1016/j.ces.2025.121719
Amaury de Hemptinne, Müge Bilgen, Quentin Galand, Ilyesse Bihi, Dominique Maes, Wim De Malsche
This study investigates the microfluidic-assisted antisolvent crystallization of miconazole nitrate (MCN). Droplets containing MCN dissolved in dimethyl sulfoxide (DMSO) and water were generated in a microfluidic device. As MCN is insoluble in water, it crystallized within the droplets as DMSO and water mixed. The droplets were formed in a flow focusing structure within a continuous phase. Two distinct crystal morphologies were observed: branched polycrystals and needle-like monocrystals. The firsts resulted from secondary nucleation under high supersaturation and migrated to the interface and into the continuous phase. The seconds originated from primary nucleation at a later stage, under lower supersaturation, and remained within the droplet’s bulk. Both types of crystals were characterized and compared to those produced under bulk industrial conditions. The study also examined the influence of droplet dimensions, flow rates, and solvent/antisolvent ratios. Additionally, internal vortices within the droplets were highlighted by observing the crystal motion during crystallization.
{"title":"Controlled antisolvent crystallization of miconazole nitrate in microfluidic droplets","authors":"Amaury de Hemptinne, Müge Bilgen, Quentin Galand, Ilyesse Bihi, Dominique Maes, Wim De Malsche","doi":"10.1016/j.ces.2025.121719","DOIUrl":"https://doi.org/10.1016/j.ces.2025.121719","url":null,"abstract":"This study investigates the microfluidic-assisted antisolvent crystallization of miconazole nitrate (MCN). Droplets containing MCN dissolved in dimethyl sulfoxide (DMSO) and water were generated in a microfluidic device. As MCN is insoluble in water, it crystallized within the droplets as DMSO and water mixed. The droplets were formed in a flow focusing structure within a continuous phase. Two distinct crystal morphologies were observed: branched polycrystals and needle-like monocrystals. The firsts resulted from secondary nucleation under high supersaturation and migrated to the interface and into the continuous phase. The seconds originated from primary nucleation at a later stage, under lower supersaturation, and remained within the droplet’s bulk. Both types of crystals were characterized and compared to those produced under bulk industrial conditions. The study also examined the influence of droplet dimensions, flow rates, and solvent/antisolvent ratios. Additionally, internal vortices within the droplets were highlighted by observing the crystal motion during crystallization.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"41 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862291","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-23DOI: 10.1016/j.ces.2025.121717
Yang Yang , Jiafu Shi , Yu Chen , Shihao Li , Han Wang , Wenping Li , Shusong Liu , Xinyu Mao , Hong Wu , Zhongyi Jiang
Rational design of immobilized enzyme catalysts based on covalent organic framework (COF) with high enzyme loading and superior robustness is highly desired. Herein, we designed an immobilized enzyme catalyst based on bifunctional COF. The quaternary ammonium-functionalized COF nanosheets adsorbed enzymes and subsequently induced the in-situ formation of silica coating without additional reagents. The ultrathin COF nanosheets guaranteed high enzyme loading of 3.4 mg mg−1. Meanwhile, quaternary ammonium groups on COF induced the formation of silica coating on the surface of COF, where the as-formed silica coating protected the fragile enzyme. The stability of the enzyme in immobilization form increased by 165 %, 113 % and 44 %, respectively, compared to the enzyme directly adsorbed on COF under different conditions (50 °C, pH 11, or after five cycles). Furthermore, given the high enzyme loading of COF nanosheets, an immobilized multi-enzyme catalytic system was constructed to convert methanol to ethylene glycol via a four-enzyme cascade reaction, which exhibited 143 % increase in catalytic activity by contrast with free enzymes system. This study provides a promising approach for enzyme immobilization and extends the application of COF in biocatalysis.
人们迫切需要基于共价有机骨架（COF）合理设计具有高酶载量和良好鲁棒性的固定化酶催化剂。本文设计了一种基于双功能COF的固定化酶催化剂。季铵功能化COF纳米片吸附酶，随后诱导原位形成二氧化硅涂层，无需额外试剂。超薄COF纳米片保证了3.4 mg mg−1的高酶载量。同时，COF上的季铵基团诱导COF表面形成二氧化硅涂层，形成的二氧化硅涂层保护脆弱的酶。在不同条件下（50 °C, pH 11，循环5次），固定化形式的酶的稳定性分别比直接吸附在COF上的酶提高了165 %，113 %和44 %。此外，考虑到COF纳米片的高酶载量，构建了固定化多酶催化体系，通过四酶级联反应将甲醇转化为乙二醇，其催化活性比自由酶体系提高了143 %。该研究为酶固定化提供了一种有前景的方法，并扩展了COF在生物催化中的应用。
{"title":"Bifunctional COF-templated synthesis of immobilized enzyme catalysts for efficient bioconversion","authors":"Yang Yang , Jiafu Shi , Yu Chen , Shihao Li , Han Wang , Wenping Li , Shusong Liu , Xinyu Mao , Hong Wu , Zhongyi Jiang","doi":"10.1016/j.ces.2025.121717","DOIUrl":"10.1016/j.ces.2025.121717","url":null,"abstract":"<div><div>Rational design of immobilized enzyme catalysts based on covalent organic framework (COF) with high enzyme loading and superior robustness is highly desired. Herein, we designed an immobilized enzyme catalyst based on bifunctional COF. The quaternary ammonium-functionalized COF nanosheets adsorbed enzymes and subsequently induced the in-situ formation of silica coating without additional reagents. The ultrathin COF nanosheets guaranteed high enzyme loading of 3.4 mg mg<sup>−1</sup>. Meanwhile, quaternary ammonium groups on COF induced the formation of silica coating on the surface of COF, where the as-formed silica coating protected the fragile enzyme. The stability of the enzyme in immobilization form increased by 165 %, 113 % and 44 %, respectively, compared to the enzyme directly adsorbed on COF under different conditions (50 °C, pH 11, or after five cycles). Furthermore, given the high enzyme loading of COF nanosheets, an immobilized multi-enzyme catalytic system was constructed to convert methanol to ethylene glycol via a four-enzyme cascade reaction, which exhibited 143 % increase in catalytic activity by contrast with free enzymes system. This study provides a promising approach for enzyme immobilization and extends the application of COF in biocatalysis.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"313 ","pages":"Article 121717"},"PeriodicalIF":4.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143867044","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-23DOI: 10.1016/j.ces.2025.121718
Xingyu Lin , Hongsheng Lu , Ruoxin Zhang , Ziteng Yang , Yingjiang Chen , Baiwen Huang
CO2 flooding offers dual benefits by enhancing oil recovery and facilitating CO2 storage. However, reservoir heterogeneity and clay swelling can significantly limit CO2 storage capacity. Here, a novel strategy for in-situ formation of particle profile control agent and clay swelling inhibitor was established by CO2-responsive ionic liquids (ILs). Two fatty acid (FA)-based ILs were synthesized by reacting N, N-dimethylcyclohexylamine (DMCHA) with myristic acid (C14) and palmitic acid (C16). After CO2 injection, FA was precipitated again as a particle profile control agent with a particle size exceeding 10.65 μm, while the protonated DMCHA in the remaining liquid phase serves as a clay swelling inhibitor. Notably, the precipitation of FA within the core increases the CO2 storage capacity by 1.96 times. This innovative approach holds great promise for enhancing the efficiency and sustainability of CO2 injection, benefiting both the petroleum industry and environmental protection.
{"title":"CO2-induced phase separation in ionic liquid aqueous solutions: enhancing CO2 storage capacity in CO2 flooding","authors":"Xingyu Lin , Hongsheng Lu , Ruoxin Zhang , Ziteng Yang , Yingjiang Chen , Baiwen Huang","doi":"10.1016/j.ces.2025.121718","DOIUrl":"10.1016/j.ces.2025.121718","url":null,"abstract":"<div><div>CO<sub>2</sub> flooding offers dual benefits by enhancing oil recovery and facilitating CO<sub>2</sub> storage. However, reservoir heterogeneity and clay swelling can significantly limit CO<sub>2</sub> storage capacity. Here, a novel strategy for in-situ formation of particle profile control agent and clay swelling inhibitor was established by CO<sub>2</sub>-responsive ionic liquids (ILs). Two fatty acid (FA)-based ILs were synthesized by reacting <em>N, N</em>-dimethylcyclohexylamine (DMCHA) with myristic acid (C14) and palmitic acid (C16). After CO<sub>2</sub> injection, FA was precipitated again as a particle profile control agent with a particle size exceeding 10.65 μm, while the protonated DMCHA in the remaining liquid phase serves as a clay swelling inhibitor. Notably, the precipitation of FA within the core increases the CO<sub>2</sub> storage capacity by 1.96 times. This innovative approach holds great promise for enhancing the efficiency and sustainability of CO<sub>2</sub> injection, benefiting both the petroleum industry and environmental protection.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"313 ","pages":"Article 121718"},"PeriodicalIF":4.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143867045","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-22DOI: 10.1016/j.ces.2025.121713
Abir Sagaama, Afef Guesmi, Noureddine ISSAOUI, Omar M. Al-Dossary, Vincent Dorcet, Thierry Roisnel, Houda Marouani
This paper reports an experimental and theoretical analysis of a novel hybrid molecule, m(CH2NH3)2C6H4(HPO4).2H2O, abbreviated as m-XDMP. The synthesis was carried out at room temperature using a slow evaporation method, by the dropwise addition of m-xylylenediamine to an ethanol solution containing diluted phosphoric acid under magnetic stirring. The X-Ray diffractionprove that m-XDMP crystallizes in the monoclinic system by mean of non-centrosymmetric space group P21.This compound was characterized by UV–vis, infrared and differential scanning calorimetry (DSC) spectroscopies. Molecular optimization analysis was performed using quantum chemical calculations based on Density Functional Theory (DFT) with the B3LYP/6–311++G(d,p) method. The nucleophilic (oxygen atoms) and electrophilic (hydrogen atoms) sites responsible for the establishment of hydrogen bonding interactions were identified through Molecular Electrostatic Potential (MEP) surface analysis. The energy gap, global softness, and chemical hardness values confirmed the chemical stability of m-XDMP. Atoms in Molecules (AIM) analysis highlighted the formation of intramolecular hydrogen bonds, including O–H···O, O–H···N, N–H···O, N–H···H, and C–H···O interactions. In contrast, Hirshfeld surface analysis confirmed the presence of N–H···O, C–H···O, O–H···O, and π–π interactions within the crystalline arrangement of m-XDMP. In addition, molecular docking simulations were conducted to investigate the pharmacological potential of the compound. Several bacterial and fungal proteins were docked with m-XDMP. The docking results were compared to those of a standard drug, indicating the inhibitory potential of the studied compound, particularly against the 8OXI enzyme. Moreover, ADMET (Absorption, Distribution, Metabolism, Excretion, and Toxicity) properties were also evaluated.
{"title":"Synthesis, Structural, Spectroscopic, Inhibitory, and biological Activity studies of a novel hybrid m-(CH2NH3)2C6H4 (HPO4)•2H2O: Experimental and quantum chemical Investigations","authors":"Abir Sagaama, Afef Guesmi, Noureddine ISSAOUI, Omar M. Al-Dossary, Vincent Dorcet, Thierry Roisnel, Houda Marouani","doi":"10.1016/j.ces.2025.121713","DOIUrl":"https://doi.org/10.1016/j.ces.2025.121713","url":null,"abstract":"This paper reports an experimental and theoretical analysis of a novel hybrid molecule, <em>m</em>(CH<sub>2</sub>NH<sub>3</sub>)<sub>2</sub>C<sub>6</sub>H<sub>4</sub>(HPO<sub>4</sub>).2H<sub>2</sub>O, abbreviated as m-XDMP. The synthesis was carried out at room temperature using a slow evaporation method, by the dropwise addition of m-xylylenediamine to an ethanol solution containing diluted phosphoric acid under magnetic stirring. The X-Ray diffractionprove that <em>m</em>-XDMP crystallizes in the monoclinic system by mean of non-centrosymmetric space group <em>P</em>2<sub>1</sub>.This compound was characterized by UV–vis, infrared and differential scanning calorimetry (DSC) spectroscopies. Molecular optimization analysis was performed using quantum chemical calculations based on Density Functional Theory (DFT) with the B3LYP/6–311++G(d,p) method. The nucleophilic (oxygen atoms) and electrophilic (hydrogen atoms) sites responsible for the establishment of hydrogen bonding interactions were identified through Molecular Electrostatic Potential (MEP) surface analysis. The energy gap, global softness, and chemical hardness values confirmed the chemical stability of m-XDMP. Atoms in Molecules (AIM) analysis highlighted the formation of intramolecular hydrogen bonds, including O–H···O, O–H···N, N–H···O, N–H···H, and C–H···O interactions. In contrast, Hirshfeld surface analysis confirmed the presence of N–H···O, C–H···O, O–H···O, and π–π interactions within the crystalline arrangement of m-XDMP. In addition, molecular docking simulations were conducted to investigate the pharmacological potential of the compound. Several bacterial and fungal proteins were docked with m-XDMP. The docking results were compared to those of a standard drug, indicating the inhibitory potential of the studied compound, particularly against the 8OXI enzyme. Moreover, ADMET (Absorption, Distribution, Metabolism, Excretion, and Toxicity) properties were also evaluated.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"7 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862292","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-22DOI: 10.1016/j.ces.2025.121708
Luis R. Barajas-Villarruel, Sergio Damián-Vázquez, Vicente Rico-Ramirez
This work presents an approach to developing high-order fractional kinetic models. Certain chemical and biological reactions exhibit atypical kinetics with non-local behavior, deviating from classical kinetic models. These deviations are associated with anomalous diffusion processes that do not follow the classical Fick’s law. To model that anomalous kinetics, fractional equations are frequently used; their implementation is not trivial, as an incorrect formulation may result in inconsistencies with mass conservation. Therefore, we propose a strategy in which nonlinear reaction rates are defined as functions of the fractional derivatives of the species, following a structure analogous to the law of mass action. This approach allows the development of models that are consistent with the mass balance. Two case studies illustrate this issue: a second-order reversible reaction and a heterogeneous catalytic reaction. Results show that the proposed models are consistent with mass conservation and can predict the non-local behavior of the reaction systems.
{"title":"A generalized approach to the development of high order fractional kinetics models","authors":"Luis R. Barajas-Villarruel, Sergio Damián-Vázquez, Vicente Rico-Ramirez","doi":"10.1016/j.ces.2025.121708","DOIUrl":"10.1016/j.ces.2025.121708","url":null,"abstract":"<div><div>This work presents an approach to developing high-order fractional kinetic models. Certain chemical and biological reactions exhibit atypical kinetics with non-local behavior, deviating from classical kinetic models. These deviations are associated with anomalous diffusion processes that do not follow the classical Fick’s law. To model that anomalous kinetics, fractional equations are frequently used; their implementation is not trivial, as an incorrect formulation may result in inconsistencies with mass conservation. Therefore, we propose a strategy in which nonlinear reaction rates are defined as functions of the fractional derivatives of the species, following a structure analogous to the law of mass action. This approach allows the development of models that are consistent with the mass balance. Two case studies illustrate this issue: a second-order reversible reaction and a heterogeneous catalytic reaction. Results show that the proposed models are consistent with mass conservation and can predict the non-local behavior of the reaction systems.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"313 ","pages":"Article 121708"},"PeriodicalIF":4.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858085","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
C) coupling mechanisms: a single-site adsorption pathway involving *CO desorption followed by *CO + *CO coupling and a dual-site adsorption pathway enabled by *CHO rotation and subsequent *CO + *CHO coupling. Strong confinement enhances dual-site coupling. The optimal interlayer distance for ethanol production is 6.5 Å (limiting potential: 0.7 V), while 7.5 Å favors CH4 selectivity. This study establishes a theoretical framework for confined dual-site catalysis, providing design principles of interlayer-confined-enabled vertically aligned dual-site synergy approach for next-generation CO2 electrocatalysts.
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