Pub Date : 2025-04-21DOI: 10.1016/j.ces.2025.121712
Feiyang Chen , Zhichao Zhu , Fakun Qu , Lei Ni , Juncheng Jiang , Zhiquan Chen
Microreactor technology has garnered significant attention for its efficiency and precision in chemical production. However, research on data analysis within microreactors remains limited. Fault detection and diagnosis is crucial for ensuring safety in the chemical industry. Although many fault detection algorithms based on reconstruction deep learning methods have been proposed and tested using simulated data, these simulations often fail to account for disturbances that may occur in real chemical production processes. To address this gap, this paper presents a microreactor system capable of real-time data monitoring and proposes a Transformer-based hybrid model that incorporates cross-time and cross-variable attention mechanisms. The performance of this model is evaluated using both normal and abnormal data from water test and an oxidation process in the microreactor. Compared to traditional reconstruction-based methods, our model demonstrates a higher fault detection rate when applied to real-world data containing disturbances, highlighting its significant potential for improving process safety.
{"title":"A Transformer-based fault detection method built on real-time data from microreactors","authors":"Feiyang Chen , Zhichao Zhu , Fakun Qu , Lei Ni , Juncheng Jiang , Zhiquan Chen","doi":"10.1016/j.ces.2025.121712","DOIUrl":"10.1016/j.ces.2025.121712","url":null,"abstract":"<div><div>Microreactor technology has garnered significant attention for its efficiency and precision in chemical production. However, research on data analysis within microreactors remains limited. Fault detection and diagnosis is crucial for ensuring safety in the chemical industry. Although many fault detection algorithms based on reconstruction deep learning methods have been proposed and tested using simulated data, these simulations often fail to account for disturbances that may occur in real chemical production processes. To address this gap, this paper presents a microreactor system capable of real-time data monitoring and proposes a Transformer-based hybrid model that incorporates cross-time and cross-variable attention mechanisms. The performance of this model is evaluated using both normal and abnormal data from water test and an oxidation process in the microreactor. Compared to traditional reconstruction-based methods, our model demonstrates a higher fault detection rate when applied to real-world data containing disturbances, highlighting its significant potential for improving process safety.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"312 ","pages":"Article 121712"},"PeriodicalIF":4.1,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853577","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 : 2025-04-21DOI: 10.1016/j.ces.2025.121714
Wei Chen, Wenjie Guo, Weijie Mao
Process monitoring is essential for ensuring the safety, reliability, and efficiency of industrial production processes. However, traditional process monitoring methods struggle with multi-mode processes simultaneously containing outliers, especially when the data are nonlinear and imbalanced. To address these challenges, this paper proposes a novel nonlinear process monitoring method that combines improved Connectivity Kernel based Density Peak Clustering with Outlier Filter (CKDPOF) technique and Cost-sensitive Support Vector Data Description (CSVDD). The core contributions of this study are twofold. First, we develop a CKDPOF method that integrates a connectivity kernel technique for identifying data manifolds with a local center extraction strategy aimed at clustering modes and filtering outliers. Second, we propose a CSVDD model that enhances SVDD by incorporating semi-supervised learning concepts, effectively leveraging available anomaly information to create a highly discriminative model capable of mitigating the negative impact caused by imbalanced data. It is particularly noteworthy that the collaborative relationship between CKDPOF and CSVDD can enhance the robustness of fault detection and improve the accuracy of modal identification. Extensive experimental conducted on a simulated wastewater treatment plant platform conclusively demonstrate the superiority of the proposed method in terms of various evaluation indices.
{"title":"A simultaneous multi-mode identification and outlier filtering method for imbalanced nonlinear process monitoring","authors":"Wei Chen, Wenjie Guo, Weijie Mao","doi":"10.1016/j.ces.2025.121714","DOIUrl":"10.1016/j.ces.2025.121714","url":null,"abstract":"<div><div>Process monitoring is essential for ensuring the safety, reliability, and efficiency of industrial production processes. However, traditional process monitoring methods struggle with multi-mode processes simultaneously containing outliers, especially when the data are nonlinear and imbalanced. To address these challenges, this paper proposes a novel nonlinear process monitoring method that combines improved Connectivity Kernel based Density Peak Clustering with Outlier Filter (CKDPOF) technique and Cost-sensitive Support Vector Data Description (CSVDD). The core contributions of this study are twofold. First, we develop a CKDPOF method that integrates a connectivity kernel technique for identifying data manifolds with a local center extraction strategy aimed at clustering modes and filtering outliers. Second, we propose a CSVDD model that enhances SVDD by incorporating semi-supervised learning concepts, effectively leveraging available anomaly information to create a highly discriminative model capable of mitigating the negative impact caused by imbalanced data. It is particularly noteworthy that the collaborative relationship between CKDPOF and CSVDD can enhance the robustness of fault detection and improve the accuracy of modal identification. Extensive experimental conducted on a simulated wastewater treatment plant platform conclusively demonstrate the superiority of the proposed method in terms of various evaluation indices.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"313 ","pages":"Article 121714"},"PeriodicalIF":4.1,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143857869","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}
As the non-covalent interfacial interactions of adhesive-metal bonds are inherently susceptible to disruption by water molecules, bonding structures often culminate in failure under hydrothermal conditions. Herein, we designed a novel primer composed of catechol-based epoxy adhesive containing the aniline trimer, which enhances both the adhesion properties and anti-corrosive performance for ordinary epoxy adhesive. The lap shear strength of Q235 steel coated with EP-AT-CMB increased from 8.36 MPa to 22.07 MPa compared to untreated substrates. Notably, the adhesion strength of Q235 steel coated with EP-AT-CMB remained robust at 14.16 MPa after being immersed in water for 4 days, whereas the untreated samples experienced a near-total loss of adhesion strength. The superior anti-corrosion capability of EP-AT-CMB specimens is attributed to two factors: (1) the high density of hydrogen bonds of the primer/metal interface exhibit a barrier property for water molecules; (2) the electroactivity aniline trimer, which facilitates the formation of a passive film composed of Fe2O3 and Fe3O4. The synergism between the catechol structure of the primer and the electrochemical behavior of the aniline trimer enhances the durability of the adhesive structure, offering a practical and durable primer material for a wide range of applications.
{"title":"Enhanced adhesion and corrosion resistance of steel under hygrothermal conditions through an interfacial catechol-epoxy primer containing aniline trimer","authors":"Yu Xie , Yeping Wu , Xiuli Zhao , Hanbing Ma , Ping Zhang , Yinyu Zhang","doi":"10.1016/j.ces.2025.121715","DOIUrl":"10.1016/j.ces.2025.121715","url":null,"abstract":"<div><h3>Abstract</h3><div>As the non-covalent interfacial interactions of adhesive-metal bonds are inherently susceptible to disruption by water molecules, bonding structures often culminate in failure under hydrothermal conditions. Herein, we designed a novel primer composed of catechol-based epoxy adhesive containing the aniline trimer, which enhances both the adhesion properties and anti-corrosive performance for ordinary epoxy adhesive. The lap shear strength of Q235 steel coated with EP-AT-CMB increased from 8.36 MPa to 22.07 MPa compared to untreated substrates. Notably, the adhesion strength of Q235 steel coated with EP-AT-CMB remained robust at 14.16 MPa after being immersed in water for 4 days, whereas the untreated samples experienced a near-total loss of adhesion strength. The superior anti-corrosion capability of EP-AT-CMB specimens is attributed to two factors: (1) the high density of hydrogen bonds of the primer/metal interface exhibit a barrier property for water molecules; (2) the electroactivity aniline trimer, which facilitates the formation of a passive film composed of Fe<sub>2</sub>O<sub>3</sub> and Fe<sub>3</sub>O<sub>4</sub>. The synergism between the catechol structure of the primer and the electrochemical behavior of the aniline trimer enhances the durability of the adhesive structure, offering a practical and durable primer material for a wide range of applications.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"313 ","pages":"Article 121715"},"PeriodicalIF":4.1,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143857870","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 : 2025-04-21DOI: 10.1016/j.ces.2025.121711
Yunqiao Huang , Xianguo Li , Zhongchao Tan
Liquid transport on fibers is crucial for various applications but often faces disruptions due to drop formation from Plateau-Rayleigh instability. This study reports the continuous liquid transport on ribbon-like fibers leveraging the instability. Liquid deposited on the fiber aggregates on the broad side with low curvature, triggering Plateau-Rayleigh instability with long wavelengths. The formed drops are connected by a flowing film, enabling liquid transport over centimeter-scale distances without external forces. Particle-image velocimetry analysis reveals opposing flows in the film and organized vortices in the shear layer, driven by capillary effects. Leveraging the long-wave characteristics of Plateau-Rayleigh instability, we introduce a rivulets-on-web structure that uses liquid bridges as artificial drops to enable continuous transport over a 10 cm2 fiber web. The unique transport characteristics of ribbon-like fibers and fiber webs are promising for practical applications.
{"title":"Continuous long-distance liquid transport along fibers arising from Plateau-Rayleigh instability","authors":"Yunqiao Huang , Xianguo Li , Zhongchao Tan","doi":"10.1016/j.ces.2025.121711","DOIUrl":"10.1016/j.ces.2025.121711","url":null,"abstract":"<div><div>Liquid transport on fibers is crucial for various applications but often faces disruptions due to drop formation from Plateau-Rayleigh instability. This study reports the continuous liquid transport on ribbon-like fibers leveraging the instability. Liquid deposited on the fiber aggregates on the broad side with low curvature, triggering Plateau-Rayleigh instability with long wavelengths. The formed drops are connected by a flowing film, enabling liquid transport over centimeter-scale distances without external forces. Particle-image velocimetry analysis reveals opposing flows in the film and organized vortices in the shear layer, driven by capillary effects. Leveraging the long-wave characteristics of Plateau-Rayleigh instability, we introduce a rivulets-on-web structure that uses liquid bridges as artificial drops to enable continuous transport over a 10 cm<sup>2</sup> fiber web. The unique transport characteristics of ribbon-like fibers and fiber webs are promising for practical applications.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"312 ","pages":"Article 121711"},"PeriodicalIF":4.1,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853578","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 : 2025-04-21DOI: 10.1016/j.ces.2025.121704
Manzoore Elahi M. Soudagar, Ravindra Pratap Singh, Nagabhooshanam Nagarajan, Vinayagam Mohanavel, K Karthik, Manikandan Ayyar, Manickam Ravichandran, R. Venkatesh, A.H. Seikh
Hydrogen energy is the trend and beneficial over fossil fuels, specifically in terms of zero carbon emission, eco-friendliness, and better energy efficiency. Algae are a potential source for hydrogen production, and the concentration of biomass leads to better hydrogen yield. This research aims to enhance hydrogen production from algae (using aquaculture wastewater) through a supercritical steam gasification process. The study will investigate different steam-to-biomass ratios (0.1, 0.3, 0.5, and 0.7) at a high gasification temperature of 1050 °C, under a gasification pressure of 23 MPa, and with a residence time of 30 min. During the gasification process, the potassium hydroxide (KOH) catalyst and sorbent injection are utilized to enhance the hydrogen yield. The titanium dioxide (TiO2) nanoparticles are utilized for different percentages (0, 1, 3, and 5 %), and 5 % of TiO2 favours optimum growth (0.95µ/day) microalgae, which is the feedstock for hydrogen production. The effect of steam to steam-to-biomass ratio on the functional behaviour of steam gasification for hydrogen production is evaluated. A higher steam-to-biomass ratio of 0.7 % is found to improve gasification efficiency (GE), hydrogen selectivity, and lower heating value (LHV), with KOH catalysis achieving a 54.7 % H2 gas yield and increasing GE and LHV by 12.7 % and 23.4 %, respectively. Sorbent injection further increased GE to 54.3 %, hydrogen selectivity to 81.7 %, and LHV to 14.2 MJ/Nm3. The findings demonstrate the potential of TiO2 nanoparticles and catalytic enhancements for improving biomass growth and hydrogen production efficiency.
{"title":"Featuring of in-situ carbon capturing and functional performance study of hydrogen from aquaculture wastewater algae biomass via supercritical steam gasification route","authors":"Manzoore Elahi M. Soudagar, Ravindra Pratap Singh, Nagabhooshanam Nagarajan, Vinayagam Mohanavel, K Karthik, Manikandan Ayyar, Manickam Ravichandran, R. Venkatesh, A.H. Seikh","doi":"10.1016/j.ces.2025.121704","DOIUrl":"https://doi.org/10.1016/j.ces.2025.121704","url":null,"abstract":"Hydrogen energy is the trend and beneficial over fossil fuels, specifically in terms of zero carbon emission, eco-friendliness, and better energy efficiency. Algae are a potential source for hydrogen production, and the concentration of biomass leads to better hydrogen yield. This research aims to enhance hydrogen production from algae (using aquaculture wastewater) through a supercritical steam gasification process. The study will investigate different steam-to-biomass ratios (0.1, 0.3, 0.5, and 0.7) at a high gasification temperature of 1050 °C, under a gasification pressure of 23 MPa, and with a residence time of 30 min. During the gasification process, the potassium hydroxide (KOH) catalyst and sorbent injection are utilized to enhance the hydrogen yield. The titanium dioxide (TiO<sub>2</sub>) nanoparticles are utilized for different percentages (0, 1, 3, and 5 %), and 5 % of TiO<sub>2</sub> favours optimum growth (0.95µ/day) microalgae, which is the feedstock for hydrogen production. The effect of steam to steam-to-biomass ratio on the functional behaviour of steam gasification for hydrogen production is evaluated. A higher steam-to-biomass ratio of 0.7 % is found to improve gasification efficiency (GE), hydrogen selectivity, and lower heating value (LHV), with KOH catalysis achieving a 54.7 % H<sub>2</sub> gas yield and increasing GE and LHV by 12.7 % and 23.4 %, respectively. Sorbent injection further increased GE to 54.3 %, hydrogen selectivity to 81.7 %, and LHV to 14.2 MJ/Nm<sup>3</sup>. The findings demonstrate the potential of TiO<sub>2</sub> nanoparticles and catalytic enhancements for improving biomass growth and hydrogen production efficiency.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"62 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143857874","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 : 2025-04-20DOI: 10.1016/j.ces.2025.121707
Isabel S. Fernandes, Joana Matos, Madalena M. Dias, José Carlos B. Lopes, Ricardo J. Santos
NETmix is a mesoscale static mixer comprising cylindrical chambers interconnected by prismatic channels. Efficient chaotic mixing is typically achieved above a critical Reynolds number. However, reaching this threshold requires increased flow rates, which reduce residence time, a limitation often addressed by fluid recirculation in multiple passages. This study introduces O-NETmix technology, enabling active mixing under batch operation with high mixing intensities without fluid recirculation. Using CFD models, the influence of injected volume per oscillation was analysed for four oscillatory Reynolds numbers. Tracer distribution simulations demonstrated that chaotic mixing is achievable even below the critical Reynolds, identifying optimal oscillatory parameters for each Reynolds number, where mixing occurs more rapidly. A key factor is the ratio of injected volume per oscillation to chamber volume, with an optimal value of approximately 38% for this geometry. The O-NETmix technology offers significant potential for applications requiring long residence times, such as emulsification processes and crystallisation.
{"title":"A new operating mode of NETmix for active mixing under batch operation","authors":"Isabel S. Fernandes, Joana Matos, Madalena M. Dias, José Carlos B. Lopes, Ricardo J. Santos","doi":"10.1016/j.ces.2025.121707","DOIUrl":"https://doi.org/10.1016/j.ces.2025.121707","url":null,"abstract":"NETmix is a mesoscale static mixer comprising cylindrical chambers interconnected by prismatic channels. Efficient chaotic mixing is typically achieved above a critical Reynolds number. However, reaching this threshold requires increased flow rates, which reduce residence time, a limitation often addressed by fluid recirculation in multiple passages. This study introduces O-NETmix technology, enabling active mixing under batch operation with high mixing intensities without fluid recirculation. Using CFD models, the influence of injected volume per oscillation was analysed for four oscillatory Reynolds numbers. Tracer distribution simulations demonstrated that chaotic mixing is achievable even below the critical Reynolds, identifying optimal oscillatory parameters for each Reynolds number, where mixing occurs more rapidly. A key factor is the ratio of injected volume per oscillation to chamber volume, with an optimal value of approximately 38% for this geometry. The O-NETmix technology offers significant potential for applications requiring long residence times, such as emulsification processes and crystallisation.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"1 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853579","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 : 2025-04-20DOI: 10.1016/j.ces.2025.121709
Ana Amorim, Rui M. Filipe, Henrique A. Matos
Calcium looping is a promising post-combustion CO2 capturing technology, highly compatible with the cement industry, one of the major industrial sources of CO2 emissions. Limestone, a raw material for clinker, forms lime, a calcium looping adsorbent. Thus, it is possible to maximize the synergies between a cement plant and a calcium looping unit by establishing an integrated configuration. Nevertheless, the integration of calcium looping in cement plants has not yet been thoroughly studied. This study examines different integration alternatives, developing models for the preheater and calciner using Aspen Plus, validated with operational data, alongside an entrained-flow carbonator model considering adsorbent deactivation. By combining these models, six integrated configurations are proposed and compared with the tail–end calcium looping configuration. The integrated configurations show a reduction in fuel consumption and net energy consumption for the same CO2 avoided emissions. The most promising configuration was identified and a comparative techno-economic analysis was conducted.
{"title":"Analysis of integrated calcium looping alternatives in a cement plant","authors":"Ana Amorim, Rui M. Filipe, Henrique A. Matos","doi":"10.1016/j.ces.2025.121709","DOIUrl":"https://doi.org/10.1016/j.ces.2025.121709","url":null,"abstract":"Calcium looping is a promising post-combustion CO<sub>2</sub> capturing technology, highly compatible with the cement industry, one of the major industrial sources of CO<sub>2</sub> emissions. Limestone, a raw material for clinker, forms lime, a calcium looping adsorbent. Thus, it is possible to maximize the synergies between a cement plant and a calcium looping unit by establishing an integrated configuration. Nevertheless, the integration of calcium looping in cement plants has not yet been thoroughly studied. This study examines different integration alternatives, developing models for the preheater and calciner using Aspen Plus, validated with operational data, alongside an entrained-flow carbonator model considering adsorbent deactivation. By combining these models, six integrated configurations are proposed and compared with the tail–end calcium looping configuration. The integrated configurations show a reduction in fuel consumption and net energy consumption for the same CO<sub>2</sub> avoided emissions. The most promising configuration was identified and a comparative techno-economic analysis was conducted.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"28 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853286","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 : 2025-04-19DOI: 10.1016/j.ces.2025.121706
Daping Xia , Hang Lv , Zhenhong Chen , Hao Chen , Pengfei Su
This study explores the microbial degradation mechanisms and molecular structural transitions of coal during the bioconversion process. We built macromolecular structure models of coal samples at various stages of anaerobic fermentation by analyzing its elemental makeup, carbon framework, surface groups, and pore changes, and using molecular simulation. Experimental results indicate that: the pore size of the coal sample increased from 3.04 nm to 5.0 nm, accompanied by a slight increase in the interlayer spacing d002 of the aromatic layers, with a decrease in both the microcrystalline extension La and the stacking height Lc, suggesting the disruption of the coal sample’s microcrystalline structure. During the biogas production process, the molecular structural transformations are primarily focused on the side chains, specifically characterized by a reduction in − CH2 − groups within the aliphatic chains, consumption of − OH groups, and the formation of − COOH groups. Notably, the cleavage of benzene rings occurs at the initial stage of biogas production, while the degradation of naphthalene rings takes place during the biogas production peak, indicating that the aromatic structures significantly influence the biogas production process in lignite. GC–MS analysis of the fermentation liquid revealed that benzene compounds are the main constituents, suggesting that the degradation of naphthalene rings occurs through an open-ring mechanism rather than a direct degradation pathway. During microbial fermentation, the model’s total potential energy drops significantly, making it more stable. This change increases non-six-membered rings and lattice defects, affecting the coal’s pore structure and reducing its surface fractal dimension.
{"title":"Bioconversion of coal to Biogas: Insights into the microbial degradation mechanisms and molecular structure transformations","authors":"Daping Xia , Hang Lv , Zhenhong Chen , Hao Chen , Pengfei Su","doi":"10.1016/j.ces.2025.121706","DOIUrl":"10.1016/j.ces.2025.121706","url":null,"abstract":"<div><div>This study explores the microbial degradation mechanisms and molecular structural transitions of coal during the bioconversion process. We built macromolecular structure models of coal samples at various stages of anaerobic fermentation by analyzing its elemental makeup, carbon framework, surface groups, and pore changes, and using molecular simulation. Experimental results indicate that: the pore size of the coal sample increased from 3.04 nm to 5.0 nm, accompanied by a slight increase in the interlayer spacing d<sub>002</sub> of the aromatic layers, with a decrease in both the microcrystalline extension L<sub>a</sub> and the stacking height L<sub>c</sub>, suggesting the disruption of the coal sample’s microcrystalline structure. During the biogas production process, the molecular structural transformations are primarily focused on the side chains, specifically characterized by a reduction in − CH<sub>2</sub> − groups within the aliphatic chains, consumption of − OH groups, and the formation of − COOH groups. Notably, the cleavage of benzene rings occurs at the initial stage of biogas production, while the degradation of naphthalene rings takes place during the biogas production peak, indicating that the aromatic structures significantly influence the biogas production process in lignite. GC–MS analysis of the fermentation liquid revealed that benzene compounds are the main constituents, suggesting that the degradation of naphthalene rings occurs through an open-ring mechanism rather than a direct degradation pathway. During microbial fermentation, the model’s total potential energy drops significantly, making it more stable. This change increases non-six-membered rings and lattice defects, affecting the coal’s pore structure and reducing its surface fractal dimension.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"312 ","pages":"Article 121706"},"PeriodicalIF":4.1,"publicationDate":"2025-04-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143849412","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 : 2025-04-19DOI: 10.1016/j.ces.2025.121705
Cristhian A. Fonseca Benítez, Pablo J. Luggren
ABE (acetone-butanol-ethanol) and IBE (isopropanol-butanol-ethanol) fermentation are well-established processes for producing ketones and alcohols from biomass. Using these low-carbon alcohols and acetone might improve the production of olefins.
The gas-phase synthesis of light olefins from 1-butanol, ABE and IBE was investigated on Zn-Zr mixed oxides and reference ZnO and ZrO2. Zn-Zr catalysts with different Zn/Zr molar ratios (0.11–0.43) were prepared by incipient wetness impregnation of Zn on Zr(OH)4. The 1-butanol to olefin reaction pathways operating under different reaction conditions were elucidated. This tandem process comprises dehydrogenation, ketonization, aldol condensation, C–C bond cleavage, and deoxygenation reactions. ABE and IBE mixtures conversion was also evaluated, achieving total olefin yields of ∼65 %. Isobutene and ethylene (∼91 %) were the main components of the olefin fraction, while pentenes, isohexenes, heptenes, and octenes were the remaining components. These results highlight the potential of Zn-Zr oxides to develop a sustainable production of olefins.
{"title":"One-pot gas-phase upgrading of low-carbon alcohols and acetone to C2-C8 olefins on Zn-Zr oxides","authors":"Cristhian A. Fonseca Benítez, Pablo J. Luggren","doi":"10.1016/j.ces.2025.121705","DOIUrl":"10.1016/j.ces.2025.121705","url":null,"abstract":"<div><div>ABE (acetone-butanol-ethanol) and IBE (isopropanol-butanol-ethanol) fermentation are well-established processes for producing ketones and alcohols from biomass. Using these low-carbon alcohols and acetone might improve the production of olefins.</div><div>The gas-phase synthesis of light olefins from 1-butanol, ABE and IBE was investigated on Zn-Zr mixed oxides and reference ZnO and ZrO<sub>2</sub>. Zn-Zr catalysts with different Zn/Zr molar ratios (0.11–0.43) were prepared by incipient wetness impregnation of Zn on Zr(OH)<sub>4</sub>. The 1-butanol to olefin reaction pathways operating under different reaction conditions were elucidated. This tandem process comprises dehydrogenation, ketonization, aldol condensation, C–C bond cleavage, and deoxygenation reactions. ABE and IBE mixtures conversion was also evaluated, achieving total olefin yields of ∼65 %. Isobutene and ethylene (∼91 %) were the main components of the olefin fraction, while pentenes, isohexenes, heptenes, and octenes were the remaining components. These results highlight the potential of Zn-Zr oxides to develop a sustainable production of olefins.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"312 ","pages":"Article 121705"},"PeriodicalIF":4.1,"publicationDate":"2025-04-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143849413","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 : 2025-04-19DOI: 10.1016/j.ces.2025.121693
Xiaodan Zhang , Yongjun Zhang , Hongjing Han , Yanan Zhang , Haiying Wang , Jiayu Zhang , Huiying Chen , Xinyu Liu , Yanguang Chen
Catalytic cracking of light oil to produce the ethylene and propylene has become more attractive. However, the yields of ethylene and propylene remain challenging. Herein, the bifunctional La/P/HT-ZSM-35 zeolite was prepared by the combination of hydrothermal treatment and La & P doping. Compared to La/P/H-ZSM-35 zeolite obtained by direct impregnation method, La/P/HT-ZSM-35 catalysts have higher specific surface area and higher oxide dispersion due to the introduction of La & P interacting with non-framework Al produced by hydrothermal treatment of H-ZSM-35 zeolite. The total yields of ethylene and propylene increased to 57.05%, compared to H-ZSM-35 (31.0%) and La/P/H-ZSM-35 (45.44%), in which the free radical and monomolecular cleavage reactions were promoted in the catalytic cracking process of n-heptane. For real light diesel oil, the overall selectivity of ethylene and propylene was 64.73%, which exhibited excellent generalizability.
{"title":"Modulation of framework Al distribution and acidity via the combination of hydrothermal treatment and La & P doping for catalytic cracking of n-heptane and diesel","authors":"Xiaodan Zhang , Yongjun Zhang , Hongjing Han , Yanan Zhang , Haiying Wang , Jiayu Zhang , Huiying Chen , Xinyu Liu , Yanguang Chen","doi":"10.1016/j.ces.2025.121693","DOIUrl":"10.1016/j.ces.2025.121693","url":null,"abstract":"<div><div>Catalytic cracking of light oil to produce the ethylene and propylene has become more attractive. However, the yields of ethylene and propylene remain challenging. Herein, the bifunctional La/P/HT-ZSM-35 zeolite was prepared by the combination of hydrothermal treatment and La & P doping. Compared to La/P/H-ZSM-35 zeolite obtained by direct impregnation method, La/P/HT-ZSM-35 catalysts have higher specific surface area and higher oxide dispersion due to the introduction of La & P interacting with non-framework Al produced by hydrothermal treatment of H-ZSM-35 zeolite. The total yields of ethylene and propylene increased to 57.05%, compared to H-ZSM-35 (31.0%) and La/P/H-ZSM-35 (45.44%), in which the free radical and monomolecular cleavage reactions were promoted in the catalytic cracking process of <em>n</em>-heptane. For real light diesel oil, the overall selectivity of ethylene and propylene was 64.73%, which exhibited excellent generalizability.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"313 ","pages":"Article 121693"},"PeriodicalIF":4.1,"publicationDate":"2025-04-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143849414","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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