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Experimental and simulation study of a catalytic-membrane integrated system for efficient CO2 stripping 高效二氧化碳汽提催化膜集成系统的实验和模拟研究
IF 3.8 3区 工程技术 Q3 ENERGY & FUELS Pub Date : 2025-02-13 DOI: 10.1016/j.cep.2025.110216
Muhammad Waseem, Nayef Ghasem, Mohamed Al-Marzouqi
Global warming, mainly caused by carbon dioxide (CO2) emissions, is rapidly becoming a serious concern. The Carbon Capture, Utilization, and Storage (CCUS) process, particularly the amine-based absorption process, is among the most developed industrial processes for capturing CO2 from anthropogenic and natural sources. However, the energy-intensive nature of the equipment, as well as its high capital cost, inhibits widespread application. A porous hollow fiber membrane contactor (HFMC) is considered a promising technique for solvent regeneration in CO2 capture applications. Recent research on catalyst-assisted solvent regeneration has also shown that nano catalytic materials can reduce solvent regeneration energy costs while increasing CO2 desorption. Therefore, a self-fabricated gas-liquid membrane contactor (GLMC) module integrated with catalytically promoted CO2 desorption to maximize their potential for solvent regeneration is used in this paper. A polytetrafluoroethylene (PTFE) hollow fiber membrane module combined with and without catalytic stripping is tested for CO2 stripping performance under varying gas-liquid flowrates, temperatures, and initial CO2 loading concentrations. Increasing the liquid phase temperature and liquid flowrate significantly improved CO2 stripping, whereas increasing the gas flowrate did not increase stripping flux as much. Adding nanomaterial increased the stripping efficiency of membrane modules from 53 % to 72 % at 80 °C during CO2 stripping experiments. Catalytically assisted systems exhibited improved stripping efficiency from 48 % to 65 % when liquid flow rates were increased from 20 mL/min to 100 mL/min. A mathematical model for the fabricated module is developed for CO2 stripping from rich ethanolamine (MEA) solutions and it is simulated using COMSOL. Model predictions align well with experimental data outcomes.
{"title":"Experimental and simulation study of a catalytic-membrane integrated system for efficient CO2 stripping","authors":"Muhammad Waseem,&nbsp;Nayef Ghasem,&nbsp;Mohamed Al-Marzouqi","doi":"10.1016/j.cep.2025.110216","DOIUrl":"10.1016/j.cep.2025.110216","url":null,"abstract":"<div><div>Global warming, mainly caused by carbon dioxide (CO<sub>2</sub>) emissions, is rapidly becoming a serious concern. The Carbon Capture, Utilization, and Storage (CCUS) process, particularly the amine-based absorption process, is among the most developed industrial processes for capturing CO<sub>2</sub> from anthropogenic and natural sources. However, the energy-intensive nature of the equipment, as well as its high capital cost, inhibits widespread application. A porous hollow fiber membrane contactor (HFMC) is considered a promising technique for solvent regeneration in CO<sub>2</sub> capture applications. Recent research on catalyst-assisted solvent regeneration has also shown that nano catalytic materials can reduce solvent regeneration energy costs while increasing CO<sub>2</sub> desorption. Therefore, a self-fabricated gas-liquid membrane contactor (GLMC) module integrated with catalytically promoted CO<sub>2</sub> desorption to maximize their potential for solvent regeneration is used in this paper. A polytetrafluoroethylene (PTFE) hollow fiber membrane module combined with and without catalytic stripping is tested for CO<sub>2</sub> stripping performance under varying gas-liquid flowrates, temperatures, and initial CO<sub>2</sub> loading concentrations. Increasing the liquid phase temperature and liquid flowrate significantly improved CO<sub>2</sub> stripping, whereas increasing the gas flowrate did not increase stripping flux as much. Adding nanomaterial increased the stripping efficiency of membrane modules from 53 % to 72 % at 80 °C during CO<sub>2</sub> stripping experiments. Catalytically assisted systems exhibited improved stripping efficiency from 48 % to 65 % when liquid flow rates were increased from 20 mL/min to 100 mL/min. A mathematical model for the fabricated module is developed for CO<sub>2</sub> stripping from rich ethanolamine (MEA) solutions and it is simulated using COMSOL. Model predictions align well with experimental data outcomes.</div></div>","PeriodicalId":9929,"journal":{"name":"Chemical Engineering and Processing - Process Intensification","volume":"211 ","pages":"Article 110216"},"PeriodicalIF":3.8,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143430047","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Paired electrochemical synthesis of Cl2 from alkali chloride and CO from CO2
IF 3.8 3区 工程技术 Q3 ENERGY & FUELS Pub Date : 2025-02-13 DOI: 10.1016/j.cep.2025.110209
Jan Vehrenberg , Georg Gert , Maren Grosseheide , Matthias Wessling , Robert Keller
In order to bring electrochemical CO2 reduction (eCO2R) to economical feasibility on an industrial scale, the conventional oxygen evolution reaction (OER) can be replaced with a value added reaction. In this work, we replace OER with chlorine evolution reaction (CER) in a paired synthesis with CO from CO2. Hereby, the reaction system is assessed at industrial relevant current densities with respect to electrolyte species & concentration and stability of up to 24 h. We report constant anodic FEs to Cl2 of >97% for up to 400 mA/cm2 with concurrent FEs to CO of 90% at 100 mA/cm2 and 74% at 200 mA/cm2 over 4.5 h, significantly exceeding previous studies for comparable systems. The FE for CER did not show any decline over 24 h of operation. KCl showed superior results over NaCl and CsCl in terms of cathodic FE and cell potential. CER is affected by educt limitation with FE dropping below 95% at an electrolyte concentration of 0.8 mol/L at 400 mA/cm2. By successfully pairing eCO2R and CER with stable and high FEs at industrially relevant current densities, this work marks an important step towards an industrial application.
{"title":"Paired electrochemical synthesis of Cl2 from alkali chloride and CO from CO2","authors":"Jan Vehrenberg ,&nbsp;Georg Gert ,&nbsp;Maren Grosseheide ,&nbsp;Matthias Wessling ,&nbsp;Robert Keller","doi":"10.1016/j.cep.2025.110209","DOIUrl":"10.1016/j.cep.2025.110209","url":null,"abstract":"<div><div>In order to bring electrochemical CO<sub>2</sub> reduction (eCO<sub>2</sub>R) to economical feasibility on an industrial scale, the conventional oxygen evolution reaction (OER) can be replaced with a value added reaction. In this work, we replace OER with chlorine evolution reaction (CER) in a paired synthesis with CO from CO<sub>2</sub>. Hereby, the reaction system is assessed at industrial relevant current densities with respect to electrolyte species &amp; concentration and stability of up to 24 h. We report constant anodic FEs to Cl<sub>2</sub> of <span><math><mo>&gt;</mo></math></span>97<span><math><mtext>%</mtext></math></span> for up to 400 <span><math><mrow><mi>mA</mi><mo>/</mo><msup><mrow><mi>cm</mi></mrow><mrow><mn>2</mn></mrow></msup></mrow></math></span> with concurrent FEs to CO of 90<span><math><mtext>%</mtext></math></span> at 100 <span><math><mrow><mi>mA</mi><mo>/</mo><msup><mrow><mi>cm</mi></mrow><mrow><mn>2</mn></mrow></msup></mrow></math></span> and 74<span><math><mtext>%</mtext></math></span> at 200 <span><math><mrow><mi>mA</mi><mo>/</mo><msup><mrow><mi>cm</mi></mrow><mrow><mn>2</mn></mrow></msup></mrow></math></span> over 4.5 h, significantly exceeding previous studies for comparable systems. The FE for CER did not show any decline over 24 h of operation. KCl showed superior results over NaCl and CsCl in terms of cathodic FE and cell potential. CER is affected by educt limitation with FE dropping below 95<span><math><mtext>%</mtext></math></span> at an electrolyte concentration of 0.8 mol/L at 400 <span><math><mrow><mi>mA</mi><mo>/</mo><msup><mrow><mi>cm</mi></mrow><mrow><mn>2</mn></mrow></msup></mrow></math></span>. By successfully pairing eCO<sub>2</sub>R and CER with stable and high FEs at industrially relevant current densities, this work marks an important step towards an industrial application.</div></div>","PeriodicalId":9929,"journal":{"name":"Chemical Engineering and Processing - Process Intensification","volume":"211 ","pages":"Article 110209"},"PeriodicalIF":3.8,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143452880","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Intensified rotary drum bioreactor for cellulase production from agro-industrial residues by solid-state cultivation
IF 3.8 3区 工程技术 Q3 ENERGY & FUELS Pub Date : 2025-02-12 DOI: 10.1016/j.cep.2025.110223
Lina María Grajales , Hailei Wang , Fernanda Perpétua Casciatori , João Claúdio Thoméo
Cellulolytic enzymes are vital for converting cellulosic residues into biofuels, yet large-scale production through solid-state cultivation (SSC) remains challenging due to the lack of suitable bioreactors. This study addresses this issue by developing a rotary drum bioreactor to produce cellulases from the thermophilic fungus Myceliophthora thermophila I-1D3b, using sugarcane bagasse and wheat bran as substrates. The bioreactor integrates upstream, fermentation, and downstream processes, streamlining production and enhancing efficiency. The study explored enzymatic activity (EA) at varying substrate loadings and drum rotation conditions. Although statistically similar, at 50 % loading, drum rotation slightly improved EA (49.12 U/mL ± 6.56 U/mL) compared to static conditions (47.78 U/mL ± 8.25 U/mL). Conversely, at 40 % loading, rotation reduced EA significantly (23.57 U/mL ± 3.17 U/mL) compared to static conditions (46.91 U/mL ± 8.17 U/mL). At 60 % loading, EA was similar under both static and rotated conditions. The design effectively supports fermentation, facilitates enzymatic extract recovery, and minimizes temperature and moisture gradients. These results demonstrate the rotary drum bioreactor's potential for scaling up cellulase production, offering a promising solution for industrial SSC processes.
{"title":"Intensified rotary drum bioreactor for cellulase production from agro-industrial residues by solid-state cultivation","authors":"Lina María Grajales ,&nbsp;Hailei Wang ,&nbsp;Fernanda Perpétua Casciatori ,&nbsp;João Claúdio Thoméo","doi":"10.1016/j.cep.2025.110223","DOIUrl":"10.1016/j.cep.2025.110223","url":null,"abstract":"<div><div>Cellulolytic enzymes are vital for converting cellulosic residues into biofuels, yet large-scale production through solid-state cultivation (SSC) remains challenging due to the lack of suitable bioreactors. This study addresses this issue by developing a rotary drum bioreactor to produce cellulases from the thermophilic fungus <em>Myceliophthora thermophila</em> I-1D3b, using sugarcane bagasse and wheat bran as substrates. The bioreactor integrates upstream, fermentation, and downstream processes, streamlining production and enhancing efficiency. The study explored enzymatic activity (EA) at varying substrate loadings and drum rotation conditions. Although statistically similar, at 50 % loading, drum rotation slightly improved EA (49.12 U/mL ± 6.56 U/mL) compared to static conditions (47.78 U/mL ± 8.25 U/mL). Conversely, at 40 % loading, rotation reduced EA significantly (23.57 U/mL ± 3.17 U/mL) compared to static conditions (46.91 U/mL ± 8.17 U/mL). At 60 % loading, EA was similar under both static and rotated conditions. The design effectively supports fermentation, facilitates enzymatic extract recovery, and minimizes temperature and moisture gradients. These results demonstrate the rotary drum bioreactor's potential for scaling up cellulase production, offering a promising solution for industrial SSC processes.</div></div>","PeriodicalId":9929,"journal":{"name":"Chemical Engineering and Processing - Process Intensification","volume":"210 ","pages":"Article 110223"},"PeriodicalIF":3.8,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143420091","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Assessment of the sustainability of intensified CO2 capture schemes
IF 3.8 3区 工程技术 Q3 ENERGY & FUELS Pub Date : 2025-02-12 DOI: 10.1016/j.cep.2025.110222
Melanie Coronel-Muñoz , Ana Gabriela Romero-García , Brenda Huerta-Rosas , Eduardo Sánchez-Ramírez , Juan José Quiroz-Ramírez , Juan Gabriel Segovia-Hernández
The SDGs do address climate-related goals that are interconnected with the need to reduce greenhouse gas emissions. CO2 capture involves the use of solvents such as Monoethanolamine (MEA), whose use, advantages, and disadvantages are well reported. Currently, there are alternative solvents that are theoretically more sustainable such as deep eutectic solvents (DES), however, a direct comparative with sustainable indicators is not always available. In this work, two schemes for the CO2 capture process are evaluated and compared in a sustainable framework. Both schemes capture CO2 from a combustion process to generate electricity. The first scheme considers Monoethanolamine (MEA) and the second scheme considers a DES (ChCl/ urea (1:2), considering in both schemes the use of natural gas, biogas, and coal as fuels that originate the CO2 flux. The evaluation of both alternatives must be approached in a weighted manner and within a framework of sustainability. The results indicate that there is no single solution as the optimal solvent for CO2 capture. It was observed that the choice of solvent is predominantly influenced by the type of fuel used in the combustion zone for electricity generation.
可持续发展目标确实涉及与气候相关的目标,这些目标与减少温室气体排放的需要相互关联。二氧化碳捕获需要使用单乙醇胺(MEA)等溶剂,其使用、优点和缺点已被广泛报道。目前,理论上有一些替代溶剂更具可持续性,如深共晶溶剂 (DES),但并不总能与可持续指标进行直接比较。在这项工作中,我们在可持续框架内对两种二氧化碳捕集工艺方案进行了评估和比较。这两种方案都是从燃烧过程中捕获二氧化碳来发电。第一个方案考虑的是单乙醇胺(MEA),第二个方案考虑的是 DES(氯化氢/尿素(1:2)),两个方案都考虑使用天然气、沼气和煤作为产生二氧化碳通量的燃料。必须在可持续发展的框架内以加权方式对这两种替代方案进行评估。结果表明,二氧化碳捕获的最佳溶剂并不是单一的解决方案。据观察,溶剂的选择主要受发电燃烧区所用燃料类型的影响。
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引用次数: 0
Experimental study of acoustically induced hydroxyl radicals in hydrogen peroxide systems based on fluorescence analysis
IF 3.8 3区 工程技术 Q3 ENERGY & FUELS Pub Date : 2025-02-11 DOI: 10.1016/j.cep.2025.110219
Wenlong Li , Linzheng Ye , XiJing Zhu , Yao Liu , Jialong Wu , Shida Chuai , Zexiao Wang
The hydroxyl radical (·OH), an extremely reactive oxidizing agent, can interact with both brittle and hard materials, such as single-crystal silicon carbide (SiC), facilitating material removal via ultrasonic-assisted chemical mechanical polishing (UCMP). It is crucial to explore the generation mechanism of acoustically induced ·OH radicals within the UCMP process. This study investigated the influence of ultrasonic duration, initial solution temperature, frequency, power, and initial hydrogen peroxide (H2O2) concentration on the ·OH radical yield in the H2O2 system based on fluorescence analysis. Furthermore, it elucidates the quantitative relationships between the parameters and ·OH radical generation. The experimental data showed that ultrasonic vibrations significantly enhanced the decomposition of H2O2, with the ultrasonic duration being key to ·OH radical production, increasing 32.42 times in 30 min without a water-bath. Water-bath conditions reduce the thermal effects, yielding ·OH at a rate of 0.1826. The initial temperature had little impact within a specific range, and the peaking ·OH yield increased at 0.0662 from 20 to 50 °C. Lower frequencies and higher powers enhanced the ·OH yield by 5.37 to 10.126 times. Low H2O2 concentrations produced high ·OH radicals, peaking at 3.753 μmol/L at 1.5 wt%. These results are vital for improving UCMP efficiency and surface quality.
{"title":"Experimental study of acoustically induced hydroxyl radicals in hydrogen peroxide systems based on fluorescence analysis","authors":"Wenlong Li ,&nbsp;Linzheng Ye ,&nbsp;XiJing Zhu ,&nbsp;Yao Liu ,&nbsp;Jialong Wu ,&nbsp;Shida Chuai ,&nbsp;Zexiao Wang","doi":"10.1016/j.cep.2025.110219","DOIUrl":"10.1016/j.cep.2025.110219","url":null,"abstract":"<div><div>The hydroxyl radical (·OH), an extremely reactive oxidizing agent, can interact with both brittle and hard materials, such as single-crystal silicon carbide (SiC), facilitating material removal via ultrasonic-assisted chemical mechanical polishing (UCMP). It is crucial to explore the generation mechanism of acoustically induced ·OH radicals within the UCMP process. This study investigated the influence of ultrasonic duration, initial solution temperature, frequency, power, and initial hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) concentration on the ·OH radical yield in the H<sub>2</sub>O<sub>2</sub> system based on fluorescence analysis. Furthermore, it elucidates the quantitative relationships between the parameters and ·OH radical generation. The experimental data showed that ultrasonic vibrations significantly enhanced the decomposition of H<sub>2</sub>O<sub>2</sub>, with the ultrasonic duration being key to ·OH radical production, increasing 32.42 times in 30 min without a water-bath. Water-bath conditions reduce the thermal effects, yielding ·OH at a rate of 0.1826. The initial temperature had little impact within a specific range, and the peaking ·OH yield increased at 0.0662 from 20 to 50 °C. Lower frequencies and higher powers enhanced the ·OH yield by 5.37 to 10.126 times. Low H<sub>2</sub>O<sub>2</sub> concentrations produced high ·OH radicals, peaking at 3.753 μmol/L at 1.5 wt%. These results are vital for improving UCMP efficiency and surface quality.</div></div>","PeriodicalId":9929,"journal":{"name":"Chemical Engineering and Processing - Process Intensification","volume":"210 ","pages":"Article 110219"},"PeriodicalIF":3.8,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143403057","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Optimizing the microchannel geometry for effective control of analyte band dispersion
IF 3.8 3区 工程技术 Q3 ENERGY & FUELS Pub Date : 2025-02-11 DOI: 10.1016/j.cep.2025.110221
Iman Aslani, Mahdi Khatibi, Seyed Nezameddin Ashrafizadeh
Managing analyte band dispersion is a critical challenge in diagnostic systems, medical spectroscopy, chromatography, and drug delivery devices. Effective dispersion control ensures reliable measurements, enhanced resolution, heightened sensitivity, and improved system performance. This study emphasizes the importance of optimizing microchannel geometries, particularly curvature sections, to effectively control analyte band dispersion. To achieve this, four microchannel geometries, namely Type I to Type IV, each with distinct curvature differences, were analyzed to identify the optimal geometry with the lowest dispersion. Key parameters, including wall zeta potential, applied voltage, and the internal-to-external curvature radius ratio, were examined for their influence on dispersion. The finite element method was employed to solve the Laplace and Navier-Stokes equations for electric field and velocity distributions, while the unsteady-state diffusion-convection equation determined analyte concentration profiles. Results showed that dispersion reductions after optimization were 60 % for Type II, 48 % for Type III, and 32 % for Type IV microchannels, nevertheless for Type I microchannel dispersion remain constant after and before optimization about 70 %. Increasing the zeta potential from ζ = -0.1 V to ζ = -0.5 V led to a significant rise in dispersion from 25 % to 90 % post-optimization. Conversely, adjusting the curvature ratio Rr from 0.1 to 0.5 decreased dispersion from 42 % to 15 %. These findings underscore the importance of precise dispersion control in advancing analytical systems such as lab-on-disk and lab-on-chip technologies. This research provides valuable insights for optimizing microchannel designs to enhance the performance and reliability of various analytical and diagnostic applications.
{"title":"Optimizing the microchannel geometry for effective control of analyte band dispersion","authors":"Iman Aslani,&nbsp;Mahdi Khatibi,&nbsp;Seyed Nezameddin Ashrafizadeh","doi":"10.1016/j.cep.2025.110221","DOIUrl":"10.1016/j.cep.2025.110221","url":null,"abstract":"<div><div>Managing analyte band dispersion is a critical challenge in diagnostic systems, medical spectroscopy, chromatography, and drug delivery devices. Effective dispersion control ensures reliable measurements, enhanced resolution, heightened sensitivity, and improved system performance. This study emphasizes the importance of optimizing microchannel geometries, particularly curvature sections, to effectively control analyte band dispersion. To achieve this, four microchannel geometries, namely Type I to Type IV, each with distinct curvature differences, were analyzed to identify the optimal geometry with the lowest dispersion. Key parameters, including wall zeta potential, applied voltage, and the internal-to-external curvature radius ratio, were examined for their influence on dispersion. The finite element method was employed to solve the Laplace and Navier-Stokes equations for electric field and velocity distributions, while the unsteady-state diffusion-convection equation determined analyte concentration profiles. Results showed that dispersion reductions after optimization were 60 % for Type II, 48 % for Type III, and 32 % for Type IV microchannels, nevertheless for Type I microchannel dispersion remain constant after and before optimization about 70 %. Increasing the zeta potential from ζ = -0.1 V to ζ = -0.5 V led to a significant rise in dispersion from 25 % to 90 % post-optimization. Conversely, adjusting the curvature ratio R<sub>r</sub> from 0.1 to 0.5 decreased dispersion from 42 % to 15 %. These findings underscore the importance of precise dispersion control in advancing analytical systems such as lab-on-disk and lab-on-chip technologies. This research provides valuable insights for optimizing microchannel designs to enhance the performance and reliability of various analytical and diagnostic applications.</div></div>","PeriodicalId":9929,"journal":{"name":"Chemical Engineering and Processing - Process Intensification","volume":"210 ","pages":"Article 110221"},"PeriodicalIF":3.8,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143420089","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Biocatalytic kinetics of the reaction between CO2 and tertiary amine using carbonic anhydrase
IF 3.8 3区 工程技术 Q3 ENERGY & FUELS Pub Date : 2025-02-10 DOI: 10.1016/j.cep.2025.110218
Meng-Meng Du , Yuan-Cheng Wang , Bao-Chang Sun , Yong Luo , Liang-Liang Zhang , Guang-Wen Chu , Hai-Kui Zou
Carbonic anhydrase (CA) is a high-efficiency biocatalyst that significantly improves the absorption of CO2 by tertiary amine. This work aims to investigate kinetics behaviors from the perspective of enzymatic reaction mechanism. The influences of the CA concentration, type of tertiary amines, pH, and temperature on the reaction rate between CO2 and tertiary amine (ν) and catalytic activity of CA (φ) were first investigated in a stopped-flow device. Adding 50 g∙m⁻³ CA enhanced ν in tertiary amine solutions by a factor ranging from 22 to 42 at 298 K and pH=9.5, demonstrating its excellent catalytic performance. The ν increased with increasing CA concentration, pH, temperature, and tertiary amine's pKa. φ increased with the increase of CA concentration, as well as the decrease of temperature, pH, and tertiary amine's pKa. Proteomics analysis further revealed that conformational changes of the CA's secondary structure induced by high pH and temperature altered the expressions of the local active-site region and deactivated CA, ultimately leading to a decrease in φ. Additionally, the CA-catalysis kinetics equation accorded with the Michaelis-Menten model, with catalytic second-order rate constants on the magnitude of 107. Overall, this work provides a guideline for its industrial application in the CO2 capture process.
{"title":"Biocatalytic kinetics of the reaction between CO2 and tertiary amine using carbonic anhydrase","authors":"Meng-Meng Du ,&nbsp;Yuan-Cheng Wang ,&nbsp;Bao-Chang Sun ,&nbsp;Yong Luo ,&nbsp;Liang-Liang Zhang ,&nbsp;Guang-Wen Chu ,&nbsp;Hai-Kui Zou","doi":"10.1016/j.cep.2025.110218","DOIUrl":"10.1016/j.cep.2025.110218","url":null,"abstract":"<div><div>Carbonic anhydrase (CA) is a high-efficiency biocatalyst that significantly improves the absorption of CO<sub>2</sub> by tertiary amine. This work aims to investigate kinetics behaviors from the perspective of enzymatic reaction mechanism. The influences of the CA concentration, type of tertiary amines, pH, and temperature on the reaction rate between CO<sub>2</sub> and tertiary amine (<em>ν</em>) and catalytic activity of CA (<em>φ</em>) were first investigated in a stopped-flow device. Adding 50 g∙m⁻³ CA enhanced <em>ν</em> in tertiary amine solutions by a factor ranging from 22 to 42 at 298 K and pH=9.5, demonstrating its excellent catalytic performance. The <em>ν</em> increased with increasing CA concentration, pH, temperature, and tertiary amine's <em>pK</em>a. <em>φ</em> increased with the increase of CA concentration, as well as the decrease of temperature, pH, and tertiary amine's <em>pK</em>a. Proteomics analysis further revealed that conformational changes of the CA's secondary structure induced by high pH and temperature altered the expressions of the local active-site region and deactivated CA, ultimately leading to a decrease in <em>φ</em>. Additionally, the CA-catalysis kinetics equation accorded with the Michaelis-Menten model, with catalytic second-order rate constants on the magnitude of 10<sup>7</sup>. Overall, this work provides a guideline for its industrial application in the CO<sub>2</sub> capture process.</div></div>","PeriodicalId":9929,"journal":{"name":"Chemical Engineering and Processing - Process Intensification","volume":"211 ","pages":"Article 110218"},"PeriodicalIF":3.8,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143437454","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Development of a novel rotary kiln-type reactor for intensified gas-solid reactions: Performance evaluation for solid fuels processing
IF 3.8 3区 工程技术 Q3 ENERGY & FUELS Pub Date : 2025-02-10 DOI: 10.1016/j.cep.2025.110217
Konstantinos S. Hatzilyberis , Constantinos E. Salmas , Georgios D. Stefanidis , Georgios P. Androutsopoulos
Rotary kiln-type reactors have been investigated at bench, pilot and demonstration scale for a broad range of processes involving solids thermal conversion and gas-solid chemical reactions, such as (among others) lignite drying and lignite/biomass pyrolysis and gasification by means of either indirect heating (gas or electricity), or direct heating through a chemical looping energy carrier. This work focuses on the evolutionary development of a novel reactor of rotary kiln-type for intensified gas-solid reactions. Design and performance highlights are reported, while relevant processes serve herein as benchmarks for reactor evaluation. In the context of the latter class of processes, which constitute an example of a promising energy technology, we evaluated a pair of advanced rotary kiln-type reactors, that is, a gasifier to produce synthesis gas rich in H2 and a calciner for the regeneration of the solid energy carrier (CaCO3) and the production of clean CO2 for chemical exploitation. The novel reactors feature intensified mass and heat transfer rates enabling in this example up to 80 % LHV gasification efficiency and 96 % overall energy efficiency at 0.36 kg/h/LR solids throughput and 10–12 MJsyngasLHV/Nm3 fuel gas energy density with up to 80 % v/v H2 content when operating in Calcium-chemical looping gasification mode.
{"title":"Development of a novel rotary kiln-type reactor for intensified gas-solid reactions: Performance evaluation for solid fuels processing","authors":"Konstantinos S. Hatzilyberis ,&nbsp;Constantinos E. Salmas ,&nbsp;Georgios D. Stefanidis ,&nbsp;Georgios P. Androutsopoulos","doi":"10.1016/j.cep.2025.110217","DOIUrl":"10.1016/j.cep.2025.110217","url":null,"abstract":"<div><div>Rotary kiln-type reactors have been investigated at bench, pilot and demonstration scale for a broad range of processes involving solids thermal conversion and gas-solid chemical reactions, such as (among others) lignite drying and lignite/biomass pyrolysis and gasification by means of either indirect heating (gas or electricity), or direct heating through a chemical looping energy carrier. This work focuses on the evolutionary development of a novel reactor of rotary kiln-type for intensified gas-solid reactions. Design and performance highlights are reported, while relevant processes serve herein as benchmarks for reactor evaluation. In the context of the latter class of processes, which constitute an example of a promising energy technology, we evaluated a pair of advanced rotary kiln-type reactors, that is, a gasifier to produce synthesis gas rich in H<sub>2</sub> and a calciner for the regeneration of the solid energy carrier (CaCO<sub>3</sub>) and the production of clean CO<sub>2</sub> for chemical exploitation. The novel reactors feature intensified mass and heat transfer rates enabling in this example up to 80 % LHV gasification efficiency and 96 % overall energy efficiency at 0.36 kg/h/L<sub>R</sub> solids throughput and 10–12 MJ<sub>syngasLHV</sub>/Nm<sup>3</sup> fuel gas energy density with up to 80 % v/v H<sub>2</sub> content when operating in Calcium-chemical looping gasification mode.</div></div>","PeriodicalId":9929,"journal":{"name":"Chemical Engineering and Processing - Process Intensification","volume":"211 ","pages":"Article 110217"},"PeriodicalIF":3.8,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143437457","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Chemical looping gasification of microalgae biomass with Fe-based oxygen carrier for gas production and kinetic behavior
IF 3.8 3区 工程技术 Q3 ENERGY & FUELS Pub Date : 2025-02-10 DOI: 10.1016/j.cep.2025.110215
Yijie Wang , Yi Xing , Chen Hong
Chemical looping gasification (CLG) is an efficient method for energy conversion and utilization. It is an emerging technology to convert bioenergy into high value gas through redox of oxygen carriers (OCs). In this paper, the pyrolysis process of Chlorella vulgaris(CV) with OCs was mainly divided into three stages by TG-FTIR-MS test. Using iron ore as OCs and quartz sand as blank experiment. The addition of OCs increases the reaction rate and exhibits a catalytic effect on tar cracking. The kinetic equations for Stage 2 and Stage 3 are /dt=3.12(1-α)3·exp(-1.62 × 104/T) and /dt=5.49[(1-α)2/3/(1-(1-α)1/3)]·exp(-4.86 × 104/T), respectively. The most probable mechanism functions are the reaction order models (O3) and the diffusion models (D3), respectively. The average activation energy E0 and pre-exponential factor A0 were 134.44 kJ/mol, 3.12 min-1 and 404.18 kJ/mol, 3.66 min-1 for Stage 2 and Stage 3, respectively. The CLG process of CV&OCs showed that the yields of CO2, H2 and CO were increase by the addition of OCs. The CO yield increased most significantly from 0.097 Nm3/kg to 0.313 Nm3/kg. The carbon conversion and gasification efficiency increased from 41.7 % and 43.4 % to 78.3 % and 54.9 %, respectively. Moreover, appropriately increasing the temperature can promote the deep pyrolysis gasification of CV and generate more pyrolysis gas with high value. The microalgae CLG power generation system was found to have less negative effects on the environment through LAC and is a worthwhile gasification technology.
{"title":"Chemical looping gasification of microalgae biomass with Fe-based oxygen carrier for gas production and kinetic behavior","authors":"Yijie Wang ,&nbsp;Yi Xing ,&nbsp;Chen Hong","doi":"10.1016/j.cep.2025.110215","DOIUrl":"10.1016/j.cep.2025.110215","url":null,"abstract":"<div><div>Chemical looping gasification (CLG) is an efficient method for energy conversion and utilization. It is an emerging technology to convert bioenergy into high value gas through redox of oxygen carriers (OCs). In this paper, the pyrolysis process of <em>Chlorella vulgaris</em>(CV) with OCs was mainly divided into three stages by TG-FTIR-MS test. Using iron ore as OCs and quartz sand as blank experiment. The addition of OCs increases the reaction rate and exhibits a catalytic effect on tar cracking. The kinetic equations for Stage 2 and Stage 3 are <em>dα</em>/<em>dt</em>=3.12(1-<em>α</em>)<sup>3</sup>·exp(-1.62 × 10<sup>4</sup>/T) and <em>dα</em>/<em>dt</em>=5.49[(1-<em>α</em>)<sup>2/3</sup>/(1-(1-<em>α</em>)<sup>1/3</sup>)]·exp(-4.86 × 10<sup>4</sup>/T), respectively. The most probable mechanism functions are the reaction order models (O3) and the diffusion models (D3), respectively. The average activation energy <em>E</em><sub>0</sub> and pre-exponential factor <em>A</em><sub>0</sub> were 134.44 kJ/mol, 3.12 min<sup>-1</sup> and 404.18 kJ/mol, 3.66 min<sup>-1</sup> for Stage 2 and Stage 3, respectively. The CLG process of CV&amp;OCs showed that the yields of CO<sub>2</sub>, H<sub>2</sub> and CO were increase by the addition of OCs. The CO yield increased most significantly from 0.097 Nm<sup>3</sup>/kg to 0.313 Nm<sup>3</sup>/kg. The carbon conversion and gasification efficiency increased from 41.7 % and 43.4 % to 78.3 % and 54.9 %, respectively. Moreover, appropriately increasing the temperature can promote the deep pyrolysis gasification of CV and generate more pyrolysis gas with high value. The microalgae CLG power generation system was found to have less negative effects on the environment through LAC and is a worthwhile gasification technology.</div></div>","PeriodicalId":9929,"journal":{"name":"Chemical Engineering and Processing - Process Intensification","volume":"210 ","pages":"Article 110215"},"PeriodicalIF":3.8,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143386544","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A novel approach to heat removal and temperature control in fed-batch extractive ethanol fermentation using CO2
IF 3.8 3区 工程技术 Q3 ENERGY & FUELS Pub Date : 2025-02-09 DOI: 10.1016/j.cep.2025.110212
Brenda G. Campos , Ivan I.K. Veloso , Maíra M. da Silva , Alberto C. Badino , Antonio J.G. Cruz
This study proposes a novel approach to remove heat and maintain the broth temperature constant during fed-batch ethanol extractive fermentations by using a carbon dioxide (CO2) flow rate. The method offers an alternative to traditional cooling methods, such as water-based plate heat exchangers, which can be inefficient in distilleries located in hot regions. A mathematical model was developed and used to find the optimal CO2 flow rate to maintain constant the broth temperature in simulated fermentations at 30, 32, and 34 °C. The results showed that using multiple CO2 flow rates over an 8-hour stripping period could effectively reduce temperature deviations from the set-point while minimizing the total amount of CO2 used. However, finding the optimal combination of flow rates becomes computationally expensive as the stripping period is split in a greater number of time subintervals. A comprehensive study was carried out to assess the adequate number of time subintervals to keep the broth temperature constant. Experimental fermentation carried out at 34 °C using eight-time subintervals confirmed the accuracy of the model's predictions. A temperature deviation of less than 0.5 °C from the set-point highlights the potential of extractive fermentation for controlling temperature and offers insights to enhance process efficiency.
{"title":"A novel approach to heat removal and temperature control in fed-batch extractive ethanol fermentation using CO2","authors":"Brenda G. Campos ,&nbsp;Ivan I.K. Veloso ,&nbsp;Maíra M. da Silva ,&nbsp;Alberto C. Badino ,&nbsp;Antonio J.G. Cruz","doi":"10.1016/j.cep.2025.110212","DOIUrl":"10.1016/j.cep.2025.110212","url":null,"abstract":"<div><div>This study proposes a novel approach to remove heat and maintain the broth temperature constant during fed-batch ethanol extractive fermentations by using a carbon dioxide (CO<sub>2</sub>) flow rate. The method offers an alternative to traditional cooling methods, such as water-based plate heat exchangers, which can be inefficient in distilleries located in hot regions. A mathematical model was developed and used to find the optimal CO<sub>2</sub> flow rate to maintain constant the broth temperature in simulated fermentations at 30, 32, and 34 °C. The results showed that using multiple CO<sub>2</sub> flow rates over an 8-hour stripping period could effectively reduce temperature deviations from the set-point while minimizing the total amount of CO<sub>2</sub> used. However, finding the optimal combination of flow rates becomes computationally expensive as the stripping period is split in a greater number of time subintervals. A comprehensive study was carried out to assess the adequate number of time subintervals to keep the broth temperature constant. Experimental fermentation carried out at 34 °C using eight-time subintervals confirmed the accuracy of the model's predictions. A temperature deviation of less than 0.5 °C from the set-point highlights the potential of extractive fermentation for controlling temperature and offers insights to enhance process efficiency.</div></div>","PeriodicalId":9929,"journal":{"name":"Chemical Engineering and Processing - Process Intensification","volume":"210 ","pages":"Article 110212"},"PeriodicalIF":3.8,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143420090","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
期刊
Chemical Engineering and Processing - Process Intensification
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