Pub Date : 2024-12-02DOI: 10.1021/acs.iecr.4c02417
Utkarsh Shah, Joel A. Paulson, Bhavik R. Bakshi
Engineering design and operations have traditionally favored steady-state optimization, often overlooking the dynamic and intermittent nature of ecosystems. This has led to environmental degradation and unsustainable practices. Techno-Ecological Synergy (TES) offers an alternative framework that seeks to harmonize technological systems with ecological processes, but previous TES studies have relied on retrospective models that assume perfect foresight of ecosystem behavior. This work presents a novel framework called TES-IDC (Techno-Ecological Synergy - integrated design and control) that addresses the limitations of retrospective TES models by incorporating adaptive recourse decisions. The framework extends the IDC methodology to TES models, utilizing a simulation-optimization approach to separate design and operational problems. The operational problem is modeled as a closed-loop model predictive controller (MPC) simulation, while Bayesian optimization is employed to identify design conditions that minimize both capital and operational costs. A key innovation of TES-IDC is the use of an infinite-horizon MPC policy to account for both short- and long-term impacts at a reasonable computational cost. The effectiveness of the TES-IDC framework is demonstrated through an air quality regulation case study, where it determines the optimal size of a reforestation area and a policy for technological operations, considering the environment’s dynamic capacity. The derived operational policy successfully meets short-term air quality constraints while optimizing long-term economic and ecological objectives. This research highlights the potential of TES-IDC in designing sustainable systems that adapt to the dynamic nature of ecosystems, paving the way for a more harmonious coexistence between human activities and the environment.
{"title":"Real-Time Synergies between Homeostatic Technological and Homeorhetic Ecological Systems by Multiscale MPC and Bayesian Optimization","authors":"Utkarsh Shah, Joel A. Paulson, Bhavik R. Bakshi","doi":"10.1021/acs.iecr.4c02417","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c02417","url":null,"abstract":"Engineering design and operations have traditionally favored steady-state optimization, often overlooking the dynamic and intermittent nature of ecosystems. This has led to environmental degradation and unsustainable practices. Techno-Ecological Synergy (TES) offers an alternative framework that seeks to harmonize technological systems with ecological processes, but previous TES studies have relied on retrospective models that assume perfect foresight of ecosystem behavior. This work presents a novel framework called TES-IDC (Techno-Ecological Synergy - integrated design and control) that addresses the limitations of retrospective TES models by incorporating adaptive recourse decisions. The framework extends the IDC methodology to TES models, utilizing a simulation-optimization approach to separate design and operational problems. The operational problem is modeled as a closed-loop model predictive controller (MPC) simulation, while Bayesian optimization is employed to identify design conditions that minimize both capital and operational costs. A key innovation of TES-IDC is the use of an infinite-horizon MPC policy to account for both short- and long-term impacts at a reasonable computational cost. The effectiveness of the TES-IDC framework is demonstrated through an air quality regulation case study, where it determines the optimal size of a reforestation area and a policy for technological operations, considering the environment’s dynamic capacity. The derived operational policy successfully meets short-term air quality constraints while optimizing long-term economic and ecological objectives. This research highlights the potential of TES-IDC in designing sustainable systems that adapt to the dynamic nature of ecosystems, paving the way for a more harmonious coexistence between human activities and the environment.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"26 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758376","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}
Pub Date : 2024-12-02DOI: 10.1021/acs.iecr.4c02765
Bipasha Banerjee, Pekham Chakrabortty, Avik Chowdhury, Nasir A. Siddiqui, Sk. Manirul Islam
A proficient heterogeneous catalytic system for the photocatalytic N-formylation reaction of amines and cyclic carbonate synthesis from epoxides using CO2 as a carbon source under ambient reaction conditions has been documented. A sophisticated approach has been established for the current photocatalytic process, aiming for the successful production of formamides and cyclic carbonates with high levels of selectivity and efficiency by adjusting several variables such as the solvent, time, as well as light source involved in the reaction. We have synthesized two distinct catalysts, T-COF and N-COF, along with the g-C3N4 heterojunction, demonstrating outstanding photocatalytic performance. Compared to g-C3N4@N-COF, the g-C3N4@T-COF photocatalyst showed significantly better catalytic efficiency in the light-driven formation of cyclic carbonates and formamides using CO2 under other suitable reaction conditions at room temperature. The g-C3N4@COF photocatalysts can be recycled and used multiple times without any noticeable decrease in the efficiency.
{"title":"Photochemical N-Formylation of Amines and Cyclic Carbonate Synthesis from Epoxides by the Use of Light-Mediated Fixation of Carbon Dioxide Using Covalent Organic Framework/g-C3N4 Composites","authors":"Bipasha Banerjee, Pekham Chakrabortty, Avik Chowdhury, Nasir A. Siddiqui, Sk. Manirul Islam","doi":"10.1021/acs.iecr.4c02765","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c02765","url":null,"abstract":"A proficient heterogeneous catalytic system for the photocatalytic N-formylation reaction of amines and cyclic carbonate synthesis from epoxides using CO<sub>2</sub> as a carbon source under ambient reaction conditions has been documented. A sophisticated approach has been established for the current photocatalytic process, aiming for the successful production of formamides and cyclic carbonates with high levels of selectivity and efficiency by adjusting several variables such as the solvent, time, as well as light source involved in the reaction. We have synthesized two distinct catalysts, T-COF and N-COF, along with the g-C<sub>3</sub>N<sub>4</sub> heterojunction, demonstrating outstanding photocatalytic performance. Compared to g-C<sub>3</sub>N<sub>4</sub>@N-COF, the g-C<sub>3</sub>N<sub>4</sub>@T-COF photocatalyst showed significantly better catalytic efficiency in the light-driven formation of cyclic carbonates and formamides using CO<sub>2</sub> under other suitable reaction conditions at room temperature. The g-C<sub>3</sub>N<sub>4</sub>@COF photocatalysts can be recycled and used multiple times without any noticeable decrease in the efficiency.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"12 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758236","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}
Phosgene is a highly toxic gas that is widely used in various industries, making its rapid detection essential for safety. To address this need, we developed a smartphone-based technique using convolutional neural networks (CNNs) for real-time, portable phosgene detection. Unlike traditional fluorescence spectroscopy, which requires specialized equipment and expertise, this CNN-based approach is accessible and affordable and offers quick analysis, making it ideal for on-the-spot detection. We employed this method to identify phosgene toxicity in solutions ranging from 0 to 10 ppm by analyzing images of the solutions. Specifically, we used intramolecular charge transfer (ICT)-based TPAOD and SAHY probes to detect phosgene through turn-off and turn-on fluorescence, with detection limits of 19.44 nM (0.00759 ppm) and 34.89 nM (0.00817 ppm), respectively. A lifetime study of TPAOD confirmed that the quenching mechanism operates through static quenching. The SAHY probe was utilized for the CNN model and was also tested for cell imaging studies in HeLa cells.
{"title":"Next-Generation Phosgene Detection: Convolutional Neural Network with Triphenylamine and N-Salicylaldehyde Probes for Enhanced Sensitivity and Bioimaging","authors":"Ramakrishnan AbhijnaKrishna, Adarsh Valoor, Shu-Pao Wu, Sivan Velmathi","doi":"10.1021/acs.iecr.4c03836","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c03836","url":null,"abstract":"Phosgene is a highly toxic gas that is widely used in various industries, making its rapid detection essential for safety. To address this need, we developed a smartphone-based technique using convolutional neural networks (CNNs) for real-time, portable phosgene detection. Unlike traditional fluorescence spectroscopy, which requires specialized equipment and expertise, this CNN-based approach is accessible and affordable and offers quick analysis, making it ideal for on-the-spot detection. We employed this method to identify phosgene toxicity in solutions ranging from 0 to 10 ppm by analyzing images of the solutions. Specifically, we used intramolecular charge transfer (ICT)-based TPAOD and SAHY probes to detect phosgene through turn-off and turn-on fluorescence, with detection limits of 19.44 nM (0.00759 ppm) and 34.89 nM (0.00817 ppm), respectively. A lifetime study of TPAOD confirmed that the quenching mechanism operates through static quenching. The SAHY probe was utilized for the CNN model and was also tested for cell imaging studies in HeLa cells.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"9 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758237","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}
The real-time and full concentration analysis of ethanol during the fermentation reaction could reduce product inhibition, thereby promoting productivity. However, only a few techniques can directly detect the fermentation broth without pretreatment. To address this issue, we proposed an ultrasensitive biosensing microchip to realize the precise determination of ethanol concentrations in the original fermentation broth, which relied on the construction of a Prussian blue (PB)/Au nanoflower architecture as the recognition probe. Since the in situ growth of the nanoflowers, a biosensing microchip was functionalized to accurately recognize the ethanol within only 9 s. Using this biosensor to monitor and control the ethanol concentration in the whole 109 h fermentation production, the ethanol yield has been increased from 47.1% to 50.09%, and the average fermentation time has been reduced from 44 to 27.25 h to successfully cut down the product inhibition during the whole industrial fermentation process.
{"title":"Ultrasensitive Biosensing Microchips to Control Ethanol Fermentation for Effectively Reducing Product Inhibition","authors":"Shaoqi Zhang, Meiyue Wang, Ying Xie, Shuhan Li, Ying Chen, Hao Wu, Donghao Cheng, Zhenyu Chu, Wanqin Jin","doi":"10.1021/acs.iecr.4c02595","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c02595","url":null,"abstract":"The real-time and full concentration analysis of ethanol during the fermentation reaction could reduce product inhibition, thereby promoting productivity. However, only a few techniques can directly detect the fermentation broth without pretreatment. To address this issue, we proposed an ultrasensitive biosensing microchip to realize the precise determination of ethanol concentrations in the original fermentation broth, which relied on the construction of a Prussian blue (PB)/Au nanoflower architecture as the recognition probe. Since the in situ growth of the nanoflowers, a biosensing microchip was functionalized to accurately recognize the ethanol within only 9 s. Using this biosensor to monitor and control the ethanol concentration in the whole 109 h fermentation production, the ethanol yield has been increased from 47.1% to 50.09%, and the average fermentation time has been reduced from 44 to 27.25 h to successfully cut down the product inhibition during the whole industrial fermentation process.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"205 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758288","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}
Pub Date : 2024-12-02DOI: 10.1021/acs.iecr.4c01213
Aditya Singh, Karan Singh, Ram Ji Dixit, Biswajit Samir De, Suddhasatwa Basu
Among all the available resources, biomass is the key renewable resource to capture carbon dioxide from the atmosphere and produce fuels, chemicals, and other value-added products. This work uses an electrochemical process to generate value-added chemicals and hydrogen simultaneously from a biomass-derived platform chemical. A 3D-printed flow electrolyzer is used to study the generation of hydrogen and FDCA (2,5-furandicarboxylic acid) from HMF (5-(hydroxymethyl)furan-2-carbaldehyde) using an alkaline electrolyte based on the principles of electrochemical oxidation. A 3D-printed electrolytic cell is designed with a channel size of 55 mm × 55 mm × 6 mm and an electrocatalyst area of 6.25 cm2 in the form of an anode and cathode. In this work, gold-sputtered nickel foam is used as an anode, while platinum-sputtered nickel foam is used as a cathode. A single pass through the electrolyzer yields 130 μmol/(h cm2) of hydrogen gas at ambient temperature and pressure, along with 46 μmol/(h cm2) of FDCA. A maximum value of 80% conversion of HMF is obtained at a flow rate of 0.5 mL/min in a single pass with a potential bias of 3.5 V. This work opens the pathways for incorporating a microflow electrolyzer to coproduce FDCA and hydrogen from biomass-derived HMF.
{"title":"Co-Generation of Hydrogen and FDCA from Biomass-Based HMF in a 3D-Printed Flow Electrolyzer","authors":"Aditya Singh, Karan Singh, Ram Ji Dixit, Biswajit Samir De, Suddhasatwa Basu","doi":"10.1021/acs.iecr.4c01213","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c01213","url":null,"abstract":"Among all the available resources, biomass is the key renewable resource to capture carbon dioxide from the atmosphere and produce fuels, chemicals, and other value-added products. This work uses an electrochemical process to generate value-added chemicals and hydrogen simultaneously from a biomass-derived platform chemical. A 3D-printed flow electrolyzer is used to study the generation of hydrogen and FDCA (2,5-furandicarboxylic acid) from HMF (5-(hydroxymethyl)furan-2-carbaldehyde) using an alkaline electrolyte based on the principles of electrochemical oxidation. A 3D-printed electrolytic cell is designed with a channel size of 55 mm × 55 mm × 6 mm and an electrocatalyst area of 6.25 cm<sup>2</sup> in the form of an anode and cathode. In this work, gold-sputtered nickel foam is used as an anode, while platinum-sputtered nickel foam is used as a cathode. A single pass through the electrolyzer yields 130 μmol/(h cm<sup>2</sup>) of hydrogen gas at ambient temperature and pressure, along with 46 μmol/(h cm<sup>2</sup>) of FDCA. A maximum value of 80% conversion of HMF is obtained at a flow rate of 0.5 mL/min in a single pass with a potential bias of 3.5 V. This work opens the pathways for incorporating a microflow electrolyzer to coproduce FDCA and hydrogen from biomass-derived HMF.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"18 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758483","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}
Pub Date : 2024-11-30DOI: 10.1021/acs.iecr.4c02591
P Thamarai, S. Karishma, V.C. Deivayanai, A. Saravanan, P R Yaashikaa
The critical issue of lead pollution in wastewater, which, even in low quantities, presents serious health risks, is the focus of this investigation. The study investigates the adsorption capacities of Physically Modified Seaweed Biosorbent (PMSB) and Chemically Modified Seaweed Biosorbent (CMSB) for Pb (II) ion removal. SEM, EDX, FTIR, and XRD techniques were used to analyze surface morphology, elemental composition, functional groups, and crystallographic structure. Furthermore, it assesses the effect of pH, biosorbent dosage, temperature, initial Pb (II) ion concentration, and contact time on adsorption efficiency. The results indicated that the optimal parameters were 303 K in temperature, 5.0 in pH, and 1 g/L and 2.5 g/L of biosorbent for CMSB and PMSB, respectively, with contact durations of 40 and 80 min. The Freundlich isotherm model indicated adsorption on heterogeneous surfaces, with maximum adsorption capacities of 149.8 mg/g for PMSB and 175.5 mg/g for CMSB, demonstrating efficient Pb (II) ion removal. Higher R2 values from kinetic investigations indicate that the pseudo-first-order model fits PMSB and CMSB better for the adsorption of Pb (II) ions. The thermodynamic analysis found negative ΔH° and ΔG° values, indicating an exothermic and spontaneous adsorption mechanism, respectively. Desorption tests showed that CMSB retains greater efficiency across several cycles, demonstrating its durability and adaptability for long-term use. According to the studies, chemical modifications significantly enhance CMSB’s adsorption stability and effectiveness, which makes it a viable option for eliminating Pb (II) ions from wastewater and improving water quality.
{"title":"Theoretical and Experimental Analysis of Pb (II) Ion Adsorption Using Surface Modified Macroalgal Biosorbents: Modelling and Desorption Study","authors":"P Thamarai, S. Karishma, V.C. Deivayanai, A. Saravanan, P R Yaashikaa","doi":"10.1021/acs.iecr.4c02591","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c02591","url":null,"abstract":"The critical issue of lead pollution in wastewater, which, even in low quantities, presents serious health risks, is the focus of this investigation. The study investigates the adsorption capacities of Physically Modified Seaweed Biosorbent (PMSB) and Chemically Modified Seaweed Biosorbent (CMSB) for Pb (II) ion removal. SEM, EDX, FTIR, and XRD techniques were used to analyze surface morphology, elemental composition, functional groups, and crystallographic structure. Furthermore, it assesses the effect of pH, biosorbent dosage, temperature, initial Pb (II) ion concentration, and contact time on adsorption efficiency. The results indicated that the optimal parameters were 303 K in temperature, 5.0 in pH, and 1 g/L and 2.5 g/L of biosorbent for CMSB and PMSB, respectively, with contact durations of 40 and 80 min. The Freundlich isotherm model indicated adsorption on heterogeneous surfaces, with maximum adsorption capacities of 149.8 mg/g for PMSB and 175.5 mg/g for CMSB, demonstrating efficient Pb (II) ion removal. Higher <i>R</i><sup>2</sup> values from kinetic investigations indicate that the pseudo-first-order model fits PMSB and CMSB better for the adsorption of Pb (II) ions. The thermodynamic analysis found negative Δ<i>H</i>° and Δ<i>G</i>° values, indicating an exothermic and spontaneous adsorption mechanism, respectively. Desorption tests showed that CMSB retains greater efficiency across several cycles, demonstrating its durability and adaptability for long-term use. According to the studies, chemical modifications significantly enhance CMSB’s adsorption stability and effectiveness, which makes it a viable option for eliminating Pb (II) ions from wastewater and improving water quality.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"25 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2024-11-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142753340","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}
Pub Date : 2024-11-30DOI: 10.1021/acs.iecr.4c03319
Huihui Wang, Li Sun, Zhen Liu, Zuoxiang Zeng
The effects of water molecules on the chemical structure, microstructure, molecular kinematics, and relaxation behavior of polyvinyl butyral (PVB) films were investigated. The 2D ATR-FTIR results demonstrated that water molecules initially interacted with free O–H and C═O, subsequently with hydrogen-bonded O–H and C═O between the hard and soft segments, and ultimately with hydrogen-bonded O–H and C═O in the hard segments. The SEM, AFM, DSC, and SAXS-WAXS results indicated that the microphase separation structure of PVB was formed by soft and hard domains, and the entry of water molecules disrupted the original structural regularity of the hard segments of the PVB films, resulting in a decrease in microphase separation degree. The BDRS results showed that water absorption had a significant effect on the molecular kinematics of the soft segments and the hard–soft interface. The results of the stress relaxation behavior showed that the relaxation properties of PVB films deteriorated after water absorption.
{"title":"Understanding the Effect of Water Absorption on the Microstructure, Molecular Kinematics, and Relaxation Behavior of Polyvinyl Butyral Films","authors":"Huihui Wang, Li Sun, Zhen Liu, Zuoxiang Zeng","doi":"10.1021/acs.iecr.4c03319","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c03319","url":null,"abstract":"The effects of water molecules on the chemical structure, microstructure, molecular kinematics, and relaxation behavior of polyvinyl butyral (PVB) films were investigated. The 2D ATR-FTIR results demonstrated that water molecules initially interacted with free O–H and C═O, subsequently with hydrogen-bonded O–H and C═O between the hard and soft segments, and ultimately with hydrogen-bonded O–H and C═O in the hard segments. The SEM, AFM, DSC, and SAXS-WAXS results indicated that the microphase separation structure of PVB was formed by soft and hard domains, and the entry of water molecules disrupted the original structural regularity of the hard segments of the PVB films, resulting in a decrease in microphase separation degree. The BDRS results showed that water absorption had a significant effect on the molecular kinematics of the soft segments and the hard–soft interface. The results of the stress relaxation behavior showed that the relaxation properties of PVB films deteriorated after water absorption.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"30 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2024-11-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142756120","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}
Pub Date : 2024-11-28DOI: 10.1021/acs.iecr.4c02534
Junjie Wang, Lin Sheng, Jian Deng, Guangsheng Luo
Current methods for determining gas–liquid mass transfer or reaction performance in micropacked bed reactors (μPBRs) are inefficient and complex, hindering their application in high throughput screening, process optimization, and online monitoring. New fast determining technology is highly required. This study introduced an innovative soft measurement technology for reliable determining of gas–liquid mass transfer by directly correlating pressure drop with mass transfer coefficients through online measurement. We systematically analyzed the effect of various factors, including two-phase flow rate, packing particle size, front-end predispersion, gas composition, and liquid concentration on gas–liquid flow pressure drop and mass transfer in μPBRs. A predictive mathematical model for mass transfer coefficients was successfully established, and its capacity was successfully validated in the hydrogenation experiments within the Riedl–Pfleiderer process. This technology offers a fast, reliable, and real-time online approach for process monitoring, process optimization, and rapid catalyst screening within μPBRs.
{"title":"Fast Reliable Determination of Gas–Liquid Mass Transfer in Micropacked Beds via In-line Direct Measuring of Pressure Drop","authors":"Junjie Wang, Lin Sheng, Jian Deng, Guangsheng Luo","doi":"10.1021/acs.iecr.4c02534","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c02534","url":null,"abstract":"Current methods for determining gas–liquid mass transfer or reaction performance in micropacked bed reactors (μPBRs) are inefficient and complex, hindering their application in high throughput screening, process optimization, and online monitoring. New fast determining technology is highly required. This study introduced an innovative soft measurement technology for reliable determining of gas–liquid mass transfer by directly correlating pressure drop with mass transfer coefficients through online measurement. We systematically analyzed the effect of various factors, including two-phase flow rate, packing particle size, front-end predispersion, gas composition, and liquid concentration on gas–liquid flow pressure drop and mass transfer in μPBRs. A predictive mathematical model for mass transfer coefficients was successfully established, and its capacity was successfully validated in the hydrogenation experiments within the Riedl–Pfleiderer process. This technology offers a fast, reliable, and real-time online approach for process monitoring, process optimization, and rapid catalyst screening within μPBRs.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"9 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2024-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142742474","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}
Pub Date : 2024-11-28DOI: 10.1021/acs.iecr.4c02850
Tommaso Cogliano, Angie Desgouliere, Wander Y. Perez-Sena, Kari Eränen, Antonio D’Angelo, Atte Aho, Narendra N. Kumar, Laurence Pirault-Roy, Dmitry Yu. Murzin, Tapio Salmi
Catalytic epoxidation of tall oil, a Scandinavian raw material originating from the Kraft pulping process, was studied in this work. Conversely from the industrial process, the reaction was carried out via the hydroperoxide pathway, where the epoxidation of the double bonds takes place by hydrogen peroxide without the need for a reaction carrier. Metal oxide-modified SBA-15 catalysts were screened in the experiments performed in a laboratory-scale reactor where the operating conditions, such as the reaction temperature, the reaction time, and the reactant molar ratio, were kept constant. The main aim was to identify the best catalyst among those synthesized that would give promising results, in terms of activity and selectivity, in the epoxidation reaction. For this purpose, the relationship between the physicochemical properties of the selected catalysts and the obtained performances in the reaction system were studied in depth. Characterization analysis showed that almost all of the catalysts exhibited an organized mesoporous structure typical of SBA-15 without any morphological deformation after the metal introduction, which is present for all of them as oxide. Good activity was shown by most of the catalysts, with almost complete double bond conversion after 24 h reaction. However, selectivity to the target product was not as remarkable as the actvity. Among the tested catalysts, promising results were obtained in the presence of Mn-SBA-15 with a conversion and selectivity of 25 and 23% after 8 h of reaction, respectively.
{"title":"Tall Oil Epoxidation in the Presence of Non-Noble Metal Oxide-Modified Heterogeneous Catalysts","authors":"Tommaso Cogliano, Angie Desgouliere, Wander Y. Perez-Sena, Kari Eränen, Antonio D’Angelo, Atte Aho, Narendra N. Kumar, Laurence Pirault-Roy, Dmitry Yu. Murzin, Tapio Salmi","doi":"10.1021/acs.iecr.4c02850","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c02850","url":null,"abstract":"Catalytic epoxidation of tall oil, a Scandinavian raw material originating from the Kraft pulping process, was studied in this work. Conversely from the industrial process, the reaction was carried out via the hydroperoxide pathway, where the epoxidation of the double bonds takes place by hydrogen peroxide without the need for a reaction carrier. Metal oxide-modified SBA-15 catalysts were screened in the experiments performed in a laboratory-scale reactor where the operating conditions, such as the reaction temperature, the reaction time, and the reactant molar ratio, were kept constant. The main aim was to identify the best catalyst among those synthesized that would give promising results, in terms of activity and selectivity, in the epoxidation reaction. For this purpose, the relationship between the physicochemical properties of the selected catalysts and the obtained performances in the reaction system were studied in depth. Characterization analysis showed that almost all of the catalysts exhibited an organized mesoporous structure typical of SBA-15 without any morphological deformation after the metal introduction, which is present for all of them as oxide. Good activity was shown by most of the catalysts, with almost complete double bond conversion after 24 h reaction. However, selectivity to the target product was not as remarkable as the actvity. Among the tested catalysts, promising results were obtained in the presence of Mn-SBA-15 with a conversion and selectivity of 25 and 23% after 8 h of reaction, respectively.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"22 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2024-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142742475","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}
Pub Date : 2024-11-28DOI: 10.1021/acs.iecr.4c03318
Lei Pan, Changhui Zhang, Chengna Dai, Ning Liu, Ning Wang, Gangqiang Yu, Biaohua Chen, Ruinian Xu
Efficient and economical purification of nitrous oxide (N2O), one of the most abundant greenhouse gases, is urgently needed to prevent global warming, especially from exhaust emissions produced during adipic acid production. This study investigates the N2O thermal decomposition process via high-temperature incineration (800–1400 °C), as well as the effects of oxygen (O2) and methane (CH4) on deN2O efficiency and nitrogen selectivity. Under sufficient reaction conditions, deN2O efficiency reached 100% at ∼1000 °C. The introduction of CH4 was found to significantly enhance deN2O efficiency, with the addition of 5% CH4 resulting in complete N2O removal at <900 °C. Additionally, the influences of O2 and CH4 on the products nitric oxide and nitrogen dioxide (NO2) were analyzed via temperature-programmed reaction monitoring. Combined with the energy barriers obtained from density functional theory calculations, the reaction pathway network of N2O decomposition with and without CH4 was established. Moreover, the reaction rate equation for the crucial byproduct NO2 was derived from the elementary steps in the reaction network.
{"title":"Purification of Nitrous Oxide via Thermal Decomposition with the Assistance of Methane: Mechanistic Study of By-Reactions","authors":"Lei Pan, Changhui Zhang, Chengna Dai, Ning Liu, Ning Wang, Gangqiang Yu, Biaohua Chen, Ruinian Xu","doi":"10.1021/acs.iecr.4c03318","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c03318","url":null,"abstract":"Efficient and economical purification of nitrous oxide (N<sub>2</sub>O), one of the most abundant greenhouse gases, is urgently needed to prevent global warming, especially from exhaust emissions produced during adipic acid production. This study investigates the N<sub>2</sub>O thermal decomposition process via high-temperature incineration (800–1400 °C), as well as the effects of oxygen (O<sub>2</sub>) and methane (CH<sub>4</sub>) on <i>de</i>N<sub>2</sub>O efficiency and nitrogen selectivity. Under sufficient reaction conditions, <i>de</i>N<sub>2</sub>O efficiency reached 100% at ∼1000 °C. The introduction of CH<sub>4</sub> was found to significantly enhance <i>de</i>N<sub>2</sub>O efficiency, with the addition of 5% CH<sub>4</sub> resulting in complete N<sub>2</sub>O removal at <900 °C. Additionally, the influences of O<sub>2</sub> and CH<sub>4</sub> on the products nitric oxide and nitrogen dioxide (NO<sub>2</sub>) were analyzed via temperature-programmed reaction monitoring. Combined with the energy barriers obtained from density functional theory calculations, the reaction pathway network of N<sub>2</sub>O decomposition with and without CH<sub>4</sub> was established. Moreover, the reaction rate equation for the crucial byproduct NO<sub>2</sub> was derived from the elementary steps in the reaction network.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"116 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2024-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142756119","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}
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