Pub Date : 2025-03-13DOI: 10.1016/j.ces.2025.121487
Yuting Yuan, Xu Zhang, Li Liu, Haofan Wang, Zhiqi Bao, Yahua Liu, Chenxiao Jiang, Bin Wu
Bipolar membrane electrodialysis (BMED) efficiently transforms salts into acids and bases, with bipolar membranes (BPMs) playing a pivotal role. This study pioneers high-performance BPMs via a layer-by-layer casting/spraying technique, incorporating sulfonated polysulfone cation-exchange layers, polydopamine-modified MXene (PDA-Ti3C2TX) interfacial layers, and quaternized polyphenylene oxide anion-exchange layers. PDA-Ti3C2TX exhibits remarkable catalytic activity, promoting water dissociation. The BPMs exhibit exceptional interfacial compatibility, alkali resistance, and long-term durability. At 80 mA · cm−2, the BPMs manifest reduced transmembrane voltages (1.54 ∼ 2.80 V) compared to control samples (Blank BPM: 7.70 V; 0.75 %-Ti3C2TX-BPM: 5.51 V). Post-BMED salt conversion, the 1.00 %-PDA-Ti3C2TX-BPM displays the lowest final voltage drop (9.9 V), akin to the commercial SSBP-1 (9.8 V). The 0.75 %-PDA-Ti3C2TX-BPM attains the highest OH– concentration (0.094 mol·L-1) and current efficiency (98.79 %), surpassing SSBP-1 (0.090 mol·L-1, 94.47 %). The BPMs demonstrate superior energy consumption (2.00 ∼ 2.49 kWh kg−1) compared to SSBP-1 (2.94 kWh kg−1). This investigation delineates efficient and stable BPMs for BMED applications.
{"title":"MXene/Polydopamine as interfacial layers for enhancing the water dissociation within bipolar membranes","authors":"Yuting Yuan, Xu Zhang, Li Liu, Haofan Wang, Zhiqi Bao, Yahua Liu, Chenxiao Jiang, Bin Wu","doi":"10.1016/j.ces.2025.121487","DOIUrl":"https://doi.org/10.1016/j.ces.2025.121487","url":null,"abstract":"Bipolar membrane electrodialysis (BMED) efficiently transforms salts into acids and bases, with bipolar membranes (BPMs) playing a pivotal role. This study pioneers high-performance BPMs <em>via</em> a layer-by-layer casting/spraying technique, incorporating sulfonated polysulfone cation-exchange layers, polydopamine-modified MXene (PDA-Ti<sub>3</sub>C<sub>2</sub>T<sub>X</sub>) interfacial layers, and quaternized polyphenylene oxide anion-exchange layers. PDA-Ti<sub>3</sub>C<sub>2</sub>T<sub>X</sub> exhibits remarkable catalytic activity, promoting water dissociation. The BPMs exhibit exceptional interfacial compatibility, alkali resistance, and long-term durability. At 80 mA · cm<sup>−2</sup>, the BPMs manifest reduced transmembrane voltages (1.54 ∼ 2.80 V) compared to control samples (Blank BPM: 7.70 V; 0.75 %-Ti<sub>3</sub>C<sub>2</sub>T<sub>X</sub>-BPM: 5.51 V). Post-BMED salt conversion, the 1.00 %-PDA-Ti<sub>3</sub>C<sub>2</sub>T<sub>X</sub>-BPM displays the lowest final voltage drop (9.9 V), akin to the commercial SSBP-1 (9.8 V). The 0.75 %-PDA-Ti<sub>3</sub>C<sub>2</sub>T<sub>X</sub>-BPM attains the highest OH<sup>–</sup> concentration (0.094 mol·L<sup>-1</sup>) and current efficiency (98.79 %), surpassing SSBP-1 (0.090 mol·L<sup>-1</sup>, 94.47 %). The BPMs demonstrate superior energy consumption (2.00 ∼ 2.49 kWh kg<sup>−1</sup>) compared to SSBP-1 (2.94 kWh kg<sup>−1</sup>). This investigation delineates efficient and stable BPMs for BMED applications.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"15 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608600","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}
Self-repairing anti-corrosion coatings are characterized by their ability to autonomously repair damage, which effectively prevents corrosion of metals by corrosive media and provides enduring protection against metal corrosion. In recent years, there appears to have been a notable increase in research focus on self-healing anti-corrosion coatings as a means of protecting metals. Nevertheless, a systematic theory and in-depth analysis of reversible reactive coatings remain elusive, impeding researchers from grasping the overall picture and research focus of the field and limiting the efficient promotion of coating performance and application potential. This article presents an analysis of the reversible reaction type self-healing anticorrosive coating, a study of its self-healing mechanism, an explanation of the function of the various reversibly bonded dynamic units in self-healing coatings, and a systematic review of the research findings in this field. This article provides a comprehensive account of the synergistic effect of multiple self-healing mechanisms, encompassing a spectrum of phenomena from a solitary dynamic bond to the orchestration of dynamic bonds, shape memory effects, and repair agents. These mechanisms collectively exert a beneficial influence on the self-healing capacity of coatings. Furthermore, the article considers the deployment of reversible reactive self-healing anti-corrosion coatings in a variety of contexts and presents an overview of the prospective trajectory of this field, with the objective of offering insights and design principles for the advancement of self-healing coatings.
{"title":"Research progress and challenges of healing mechanism, types, and applications of reversible self-healing anti-corrosion coatings","authors":"Bingfan Li, Shiyu Long, Manping Yang, Daxin Zhou, Jiang Han, Tifeng Jiao","doi":"10.1016/j.ces.2025.121498","DOIUrl":"https://doi.org/10.1016/j.ces.2025.121498","url":null,"abstract":"Self-repairing anti-corrosion coatings are characterized by their ability to autonomously repair damage, which effectively prevents corrosion of metals by corrosive media and provides enduring protection against metal corrosion. In recent years, there appears to have been a notable increase in research focus on self-healing anti-corrosion coatings as a means of protecting metals. Nevertheless, a systematic theory and in-depth analysis of reversible reactive coatings remain elusive, impeding researchers from grasping the overall picture and research focus of the field and limiting the efficient promotion of coating performance and application potential. This article presents an analysis of the reversible reaction type self-healing anticorrosive coating, a study of its self-healing mechanism, an explanation of the function of the various reversibly bonded dynamic units in self-healing coatings, and a systematic review of the research findings in this field. This article provides a comprehensive account of the synergistic effect of multiple self-healing mechanisms, encompassing a spectrum of phenomena from a solitary dynamic bond to the orchestration of dynamic bonds, shape memory effects, and repair agents. These mechanisms collectively exert a beneficial influence on the self-healing capacity of coatings. Furthermore, the article considers the deployment of reversible reactive self-healing anti-corrosion coatings in a variety of contexts and presents an overview of the prospective trajectory of this field, with the objective of offering insights and design principles for the advancement of self-healing coatings.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"19 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599141","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 : 2025-03-12DOI: 10.1016/j.ces.2025.121524
He Zhao, Chunying Zhu, Taotao Fu, Xiqun Gao, Youguang Ma
The polyethylene glycol (PEG)-rich aqueous solutions with and without nanoparticle colloidal silica as the continuous phase, and the trisodium citrate (TSC)-rich aqueous solution as the dispersed phase, the water-in-water droplets were effectively prepared through a T-junction microchannel with an internal capillary. The process of droplet generation involves three distinct stages: slow necking, fast necking, and pinch-off. The nanoparticle-stabilized droplets exhibit a slower necking rate in the slow necking stage compared with conventional droplets, and the dimensionless neck width varies linearly with dimensionless time. In the fast necking stage, the adsorption of particles on the droplet surface causes the nanoparticle-stabilized droplets to undergo more difficult interfacial deformation, which further slows down the necking rate. The dimensionless neck width and the dimensionless time have a power-law relationship in the fast necking and pinch-off stages. In general, the droplets stabilized by nanoparticles show a longer formation period and a larger droplet size.
{"title":"Breakup dynamics of water-in-water droplet generation stabilized by nanoparticles in T-junction microchannel","authors":"He Zhao, Chunying Zhu, Taotao Fu, Xiqun Gao, Youguang Ma","doi":"10.1016/j.ces.2025.121524","DOIUrl":"https://doi.org/10.1016/j.ces.2025.121524","url":null,"abstract":"The polyethylene glycol (PEG)-rich aqueous solutions with and without nanoparticle colloidal silica as the continuous phase, and the trisodium citrate (TSC)-rich aqueous solution as the dispersed phase, the water-in-water droplets were effectively prepared through a T-junction microchannel with an internal capillary. The process of droplet generation involves three distinct stages: slow necking, fast necking, and pinch-off. The nanoparticle-stabilized droplets exhibit a slower necking rate in the slow necking stage compared with conventional droplets, and the dimensionless neck width varies linearly with dimensionless time. In the fast necking stage, the adsorption of particles on the droplet surface causes the nanoparticle-stabilized droplets to undergo more difficult interfacial deformation, which further slows down the necking rate. The dimensionless neck width and the dimensionless time have a power-law relationship in the fast necking and pinch-off stages. In general, the droplets stabilized by nanoparticles show a longer formation period and a larger droplet size.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"21 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599203","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 : 2025-03-12DOI: 10.1016/j.ces.2025.121522
Jian Liu, Jie Yun, Jianyi Song, Jingyao Sun, Qiao Lan
Continuous flow catalytic system based on Pickering emulsion has extensive applications in wastewater treatment. However, the traditional method hardly prepares Pickering emulsion with uniform droplet and good stability, and the catalyst is loaded onto emulsifier difficultly. Herein, oil-in-water Pickering emulsion based on chitosan with excellent stability and uniform droplet is successfully prepared by a microfluidic chip to apply in an upflow bubbling fluidized bed reactor for the treatment of 4-NP wastewater. The catalyst can be stablely and efficiently loaded on chitosan emulsifier. And the uniform size distribution of Pickering emulsion droplet minimizes the flocculation and coalescence, guaranteeing adequate contact between the reaction solution and the catalyst. After the standing of 14 days, the diameter deviation of emulsion droplet prepared by microfluidic control method only is about 8.4 %. Remarkably, the reaction efficiency of high-concentration 4-NP wastewater for the fluidized bed reactor at 100 μL·min−1 consistently remains above 99 % for 360 h.
{"title":"Pickering emulsion based on chitosan with uniform droplet size for high-efficient and stable treatment of 4-nitrophenol wastewater","authors":"Jian Liu, Jie Yun, Jianyi Song, Jingyao Sun, Qiao Lan","doi":"10.1016/j.ces.2025.121522","DOIUrl":"https://doi.org/10.1016/j.ces.2025.121522","url":null,"abstract":"Continuous flow catalytic system based on Pickering emulsion has extensive applications in wastewater treatment. However, the traditional method hardly prepares Pickering emulsion with uniform droplet and good stability, and the catalyst is loaded onto emulsifier difficultly. Herein, oil-in-water Pickering emulsion based on chitosan with excellent stability and uniform droplet is successfully prepared by a microfluidic chip to apply in an upflow bubbling fluidized bed reactor for the treatment of 4-NP wastewater. The catalyst can be stablely and efficiently loaded on chitosan emulsifier. And the uniform size distribution of Pickering emulsion droplet minimizes the flocculation and coalescence, guaranteeing adequate contact between the reaction solution and the catalyst. After the standing of 14 days, the diameter deviation of emulsion droplet prepared by microfluidic control method only is about 8.4 %. Remarkably, the reaction efficiency of high-concentration 4-NP wastewater for the fluidized bed reactor at 100 μL·min<sup>−1</sup> consistently remains above 99 % for 360 h.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"56 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599196","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 : 2025-03-11DOI: 10.1016/j.ces.2025.121497
Margaux L’Huissier, Johan Wärnå, Tapio Salmi
Ferric sulfate is an efficient coagulant in water treatment. Ferric sulfate is produced via oxidation of ferrous sulfate. The reaction proceeds spontaneously in the absence of an added catalyst, but the rate can be enhanced by solid catalysts, such as active carbon and metal-doped active carbon. The reaction environment is a complex gas–liquid (GL) or a gas–liquid-solid (GLS) system, with a strong interaction of gas solubility, interfacial mass transfer and kinetic effects. Because of the large volumes in the water treatment, selection of continuous reactor technology is an evident option. The aim of this work was to perform model simulations for continuous stirred tank reactors and tubular reactors by using a multiscale approach, from the kinetics of catalytic surface reactions to transport phenomena and flow pattern. The kinetic equations for non-catalytic and catalytic reactions were extracted from previous studies, as well as the Henry’s constant for oxygen solubility. Mass balance equations permitted to obtain the reactor models which were solved numerically. The results showed that the non-catalytic reaction is non-negligible but not sufficient for effective oxidation. Oxygen can be introduced in excess to compensate for the oxygen remaining in gas phase during the process. The tubular reactor concept and the series of two continuous stirred tank reactors (both catalytic or one non-catalytic and one catalytic) showed very satisfactory results, enabling a high conversion of ferrous sulfate to ferric sulfate
{"title":"Modelling of gas–liquid and gas–liquid-solid reactors for water treatment chemicals – From ferrous sulfate to ferric sulfate","authors":"Margaux L’Huissier, Johan Wärnå, Tapio Salmi","doi":"10.1016/j.ces.2025.121497","DOIUrl":"https://doi.org/10.1016/j.ces.2025.121497","url":null,"abstract":"Ferric sulfate is an efficient coagulant in water treatment. Ferric sulfate is produced via oxidation of ferrous sulfate. The reaction proceeds spontaneously in the absence of an added catalyst, but the rate can be enhanced by solid catalysts, such as active carbon and metal-doped active carbon. The reaction environment is a complex gas–liquid (GL) or a gas–liquid-solid (GLS) system, with a strong interaction of gas solubility, interfacial mass transfer and kinetic effects. Because of the large volumes in the water treatment, selection of continuous reactor technology is an evident option. The aim of this work was to perform model simulations for continuous stirred tank reactors and tubular reactors by using a multiscale approach, from the kinetics of catalytic surface reactions to transport phenomena and flow pattern. The kinetic equations for non-catalytic and catalytic reactions were extracted from previous studies, as well as the Henry’s constant for oxygen solubility. Mass balance equations permitted to obtain the reactor models which were solved numerically. The results showed that the non-catalytic reaction is non-negligible but not sufficient for effective oxidation. Oxygen can be introduced in excess to compensate for the oxygen remaining in gas phase during the process. The tubular reactor concept and the series of two continuous stirred tank reactors (both catalytic or one non-catalytic and one catalytic) showed very satisfactory results, enabling a high conversion of ferrous sulfate to ferric sulfate","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"7 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143590301","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 : 2025-03-11DOI: 10.1016/j.ces.2025.121521
Dongpei Zhang, Teng Liu, Ziqi Zhou, Ze Li, Yuangao Wang, Quanxing Zhang, Wei Yu, Ning Cao, Yuanyuan Ren, Haisen Lei, Junwei Yang, Wenjuan Yan, Xin Jin, Chaohe Yang
Pt-WOx based composites have been known as critical catalysts in the energy industry, yet the electronic reconfiguration at Pt-WOx interfaces for tunable C-O bond activation and Brønsted acidity remains poorly understood. This study uncovers an unusual Pt-loading effect on electronic reconfiguration of WOx crystals, introducing an alternative H-spillover pathway that doubles C-O bond cleavage activity. Catalyst characterization (XPS, UV–Vis DRS, Raman, TEM) reveals that increasing Pt/W ratios generate additional O 2p orbital holes, promoting charge transfer from O to W sites, and forming reconfigured active centers for selective C-O bond activation. Furthermore, experiments on 2-butanol dehydration demonstrate in-situ Brønsted acid sites formation via H-spillover, involving Hδ+(WO3)nδ− centers in tandem C-O bond breaking. The Pt/W/Al catalyst achieves 56.6 % selectivity for 1,3-propanediol at 50 wt% glycerol medium. The fundamental studies on electronic coupling effect at Pt-O-W interfaces are crucial for the rational design of solid acid catalysts for future bio-refineries.
{"title":"Revealing alternative mechanism for H-spillover and C-O bond cleavage reactions over interfacial Pt-WOx catalysts during glycerol hydrogenolysis","authors":"Dongpei Zhang, Teng Liu, Ziqi Zhou, Ze Li, Yuangao Wang, Quanxing Zhang, Wei Yu, Ning Cao, Yuanyuan Ren, Haisen Lei, Junwei Yang, Wenjuan Yan, Xin Jin, Chaohe Yang","doi":"10.1016/j.ces.2025.121521","DOIUrl":"https://doi.org/10.1016/j.ces.2025.121521","url":null,"abstract":"Pt-WO<sub>x</sub> based composites have been known as critical catalysts in the energy industry, yet the electronic reconfiguration at Pt-WO<sub>x</sub> interfaces for tunable C-O bond activation and Brønsted acidity remains poorly understood. This study uncovers an unusual Pt-loading effect on electronic reconfiguration of WO<sub>x</sub> crystals, introducing an alternative H-spillover pathway that doubles C-O bond cleavage activity. Catalyst characterization (XPS, UV–Vis DRS, Raman, TEM) reveals that increasing Pt/W ratios generate additional O <em>2p</em> orbital holes, promoting charge transfer from O to W sites, and forming reconfigured active centers for selective C-O bond activation. Furthermore, experiments on 2-butanol dehydration demonstrate <em>in-situ</em> Brønsted acid sites formation <em>via</em> H-spillover, involving H<sup>δ+</sup>(WO<sub>3</sub>)<sub>n</sub><sup>δ−</sup> centers in tandem C-O bond breaking. The Pt/W/Al catalyst achieves 56.6 % selectivity for 1,3-propanediol at 50 wt% glycerol medium. The fundamental studies on electronic coupling effect at Pt-O-W interfaces are crucial for the rational design of solid acid catalysts for future bio-refineries.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"5 1 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599198","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}
This study proposes a magnetic levitation fixed bed flocculation reactor as an effective method for the removal of Cr (VI). The research examines the effects of both single and dual polymer flocculants on the efficiency of the flocculation process. Initially, a magnetic levitation layer was established using a radial magnetic field in conjunction with stainless steel balls. Subsequently, polyaluminum chloride (PAC) and a non-ionic coagulant, polyacrylamide (NPAM), were introduced into the water to create a magnetic levitation fixed bed flocculation reactor. This reactor with the objective of purifying water contaminated with simulated Cr (VI).The results indicate that the incorporation of a reducing agent, specifically FeSO4, in conjunction with PAC and NPAM respectively, can achieve Cr (VI) removal rates exceeding 97% and turbidity removal rates exceeding 96%. The interaction between the cross-flow influent and the flocculating particles promotes the formation of micro-vortex flocculation.
{"title":"Research on the performance of coagulation with dual high molecular weight flocculant PAC-NPAM for the treatment of Cr (VI) containing wastewater in a magnetic levitation fixed bed","authors":"Yunxiao Ban, Zhijie Wan, Cong Ma, Yuzhen Wu, Haoran Chen","doi":"10.1016/j.ces.2025.121518","DOIUrl":"https://doi.org/10.1016/j.ces.2025.121518","url":null,"abstract":"This study proposes a magnetic levitation fixed bed flocculation reactor as an effective method for the removal of Cr (VI). The research examines the effects of both single and dual polymer flocculants on the efficiency of the flocculation process. Initially, a magnetic levitation layer was established using a radial magnetic field in conjunction with stainless steel balls. Subsequently, polyaluminum chloride (PAC) and a non-ionic coagulant, polyacrylamide (NPAM), were introduced into the water to create a magnetic levitation fixed bed flocculation reactor. This reactor with the objective of purifying water contaminated with simulated Cr (VI).The results indicate that the incorporation of a reducing agent, specifically FeSO<sub>4</sub>, in conjunction with PAC and NPAM respectively, can achieve Cr (VI) removal rates exceeding 97% and turbidity removal rates exceeding 96%. The interaction between the cross-flow influent and the flocculating particles promotes the formation of micro-vortex flocculation.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"56 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143590175","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}
The separation of propylene (C3H6) and propane (C3H8) is vital for producing high-purity C3H6. Molecular diffusion in porous materials governs equilibrium in adsorption-based separations and affects membrane efficiency by controlling permeation rates. In molecular dynamics (MD) simulations, the framework flexibility of porous materials significantly influences diffusion but is often overlooked. This study explores how the flexibility of covalent organic frameworks (COFs) impacts the diffusion of C3H6 and C3H8 using high-throughput simulations. A classification model with perfect accuracy was developed using the sure independence screening and sparsifying operator (SISSO) algorithm to predict the effect of flexibility on gas diffusion. Descriptor analysis identified PLD and LCD as key features. Reliable regression models were constructed to predict diffusion coefficients. The interpretable SISSO models show that COFs with carbonyl or hydrogenated groups facilitate gas diffusion, while ether bonds inhibit gas diffusion, offering valuable insights for understanding C3H6 and C3H8 diffusion in COFs.
{"title":"Interpretable machine learning on C3H6 and C3H8 diffusion in covalent organic frameworks: Incorporating the effects of framework flexibility","authors":"Rongyu Pan, Xiaoli Tu, Xue Ma, Liu Liu, Tongan Yan, Minman Tong","doi":"10.1016/j.ces.2025.121520","DOIUrl":"https://doi.org/10.1016/j.ces.2025.121520","url":null,"abstract":"The separation of propylene (C<sub>3</sub>H<sub>6</sub>) and propane (C<sub>3</sub>H<sub>8</sub>) is vital for producing high-purity C<sub>3</sub>H<sub>6</sub>. Molecular diffusion in porous materials governs equilibrium in adsorption-based separations and affects membrane efficiency by controlling permeation rates. In molecular dynamics (MD) simulations, the framework flexibility of porous materials significantly influences diffusion but is often overlooked. This study explores how the flexibility of covalent organic frameworks (COFs) impacts the diffusion of C<sub>3</sub>H<sub>6</sub> and C<sub>3</sub>H<sub>8</sub> using high-throughput simulations. A classification model with perfect accuracy was developed using the sure independence screening and sparsifying operator (SISSO) algorithm to predict the effect of flexibility on gas diffusion. Descriptor analysis identified PLD and LCD as key features. Reliable regression models were constructed to predict diffusion coefficients. The interpretable SISSO models show that COFs with carbonyl or hydrogenated groups facilitate gas diffusion, while ether bonds inhibit gas diffusion, offering valuable insights for understanding C<sub>3</sub>H<sub>6</sub> and C<sub>3</sub>H<sub>8</sub> diffusion in COFs.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"32 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599197","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 : 2025-03-10DOI: 10.1016/j.ces.2025.121513
Kevin Van Droogenbroek, Christos Georgiadis, Benoit Scheid, Joris Proost
In this work, single-phase Computational Fluid Dynamics (CFD) simulations are used to extract, based on a Residence Time Distribution (RTD) analysis, two representative parameters that allow to quantify electrolyte flow uniformity and flow recirculation in water electrolysis cells. This then allows to compare different cell geometries on the same ground. The optimum cell configuration is the one that homogenises the flow without generating recirculation of the electrolyte within the cell. In that case, we can take advantage of the whole surface area of the electrodes, without the risk of gas bubbles being trapped inside the cell. In a first step, several modifications of the injection channels are considered in a reference configuration using knitted mesh-type spacers as porous transport layer (PTL). Although this indeed results in some improvement in the flow behaviour, significantly better results are obtained by the use of foams as PTL: they increase the effective cell volume covered by the electrolyte and at the same time lower the risk of flow recirculation within the cell. Furthermore, keeping the foam’s pore size sufficiently large on the order of 3000 µm allows to limit the pressure drop across the cell.
{"title":"Assessment of electrolyte flow uniformity and recirculation in a water electrolysis cell through computational fluid dynamics simulations","authors":"Kevin Van Droogenbroek, Christos Georgiadis, Benoit Scheid, Joris Proost","doi":"10.1016/j.ces.2025.121513","DOIUrl":"https://doi.org/10.1016/j.ces.2025.121513","url":null,"abstract":"In this work, single-phase Computational Fluid Dynamics (CFD) simulations are used to extract, based on a Residence Time Distribution (RTD) analysis, two representative parameters that allow to quantify electrolyte flow uniformity and flow recirculation in water electrolysis cells. This then allows to compare different cell geometries on the same ground. The optimum cell configuration is the one that homogenises the flow without generating recirculation of the electrolyte within the cell. In that case, we can take advantage of the whole surface area of the electrodes, without the risk of gas bubbles being trapped inside the cell. In a first step, several modifications of the injection channels are considered in a reference configuration using knitted mesh-type spacers as porous transport layer (PTL). Although this indeed results in some improvement in the flow behaviour, significantly better results are obtained by the use of foams as PTL: they increase the effective cell volume covered by the electrolyte and at the same time lower the risk of flow recirculation within the cell. Furthermore, keeping the foam’s pore size sufficiently large on the order of 3000 µm allows to limit the pressure drop across the cell.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"12 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143582547","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 : 2025-03-10DOI: 10.1016/j.ces.2025.121510
Ning Bi , Lixiao Sun , Meihua Hu , Wei Song , Jun Xu , Lei Jia
A novel colorimetric/surface-enhanced Raman spectroscopy (SERS) dual-signal nanozyme sensor was developed for the rapid and sensitive detection of Hg2+ based on peroxidase-like gold-platinum core–shell nanoflowers (Au@Pt NFs). Au@Pt NFs catalyzed the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to its blue oxidation product, 3,3′,5,5′-tetramethylbenzidinediamine (oxTMB), which exhibits high Raman activity. However, the presence of Hg2+ inhibited the catalytic activity of Au@Pt NFs, leading to a gradual disappearance of the blue color of oxTMB. Consequently, both the absorbance at 650 nm and the Raman intensity at 1639 cm−1 decrease with increasing Hg2+ concentration. The limits of detection (LODs) were 3.2 nM for colorimetric and 0.22 nM for SERS. The preparation method of Au@Pt NFs dual-signal nanozyme sensor was simple and allowed for naked-eye colorimetric detection as well as simultaneous SERS signal measurement. In addition, this nanozyme sensor demonstrates excellent selectivity and sensitivity, making it a promising probe for water quality monitoring.
{"title":"Highly sensitive detection of mercury(II) based on colorimetric-SERS dual signal recognition strategy","authors":"Ning Bi , Lixiao Sun , Meihua Hu , Wei Song , Jun Xu , Lei Jia","doi":"10.1016/j.ces.2025.121510","DOIUrl":"10.1016/j.ces.2025.121510","url":null,"abstract":"<div><div>A novel colorimetric/surface-enhanced Raman spectroscopy (SERS) dual-signal nanozyme sensor was developed for the rapid and sensitive detection of Hg<sup>2+</sup> based on peroxidase-like gold-platinum core–shell nanoflowers (Au@Pt NFs). Au@Pt NFs catalyzed the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to its blue oxidation product, 3,3′,5,5′-tetramethylbenzidinediamine (oxTMB), which exhibits high Raman activity. However, the presence of Hg<sup>2+</sup> inhibited the catalytic activity of Au@Pt NFs, leading to a gradual disappearance of the blue color of oxTMB. Consequently, both the absorbance at 650 nm and the Raman intensity at 1639 cm<sup>−1</sup> decrease with increasing Hg<sup>2+</sup> concentration. The limits of detection (LODs) were 3.2 nM for colorimetric and 0.22 nM for SERS. The preparation method of Au@Pt NFs dual-signal nanozyme sensor was simple and allowed for naked-eye colorimetric detection as well as simultaneous SERS signal measurement. In addition, this nanozyme sensor demonstrates excellent selectivity and sensitivity, making it a promising probe for water quality monitoring.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"309 ","pages":"Article 121510"},"PeriodicalIF":4.1,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143582548","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}
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