Utilizing N₂ from the air and water for the electrocatalytic nitrogen reduction reaction shows promise for NH₃ synthesis under mild conditions. However, the chemical stability of N₂ and the thermodynamic limitations of NH₃ synthesis hinder its effectiveness. Herein, we integrated a specially designed Cu nanowire catalyst with a five-fold twin structure (T-CuNW) into an electrocatalytic system, combining electrocatalytic nitrogen reduction with nonthermal plasma-assisted N₂ activation. This work achieved an NH₃ yield of 45 mg·mgcat.−1·h−1 and a Faradaic efficiency of over 95% at −0.5 V versus RHE after a 90-h stability test. In situ characterization revealed that the T-CuNW's twin structure plays a crucial role for the generation of a large quantity of Hads, essential for the hydrogenation of nitrate intermediates, particularly nitrite (NO₂−). This enhanced hydrogenation process significantly contributes to the high performance of the ammonia synthesis system.
{"title":"A five-fold twin structure copper for enhanced electrocatalytic nitrogen reduction to sustainable ammonia","authors":"Xiaoqing Yan, Ying Zhao, Yuzhe Zhang, Bowen Wang, Hanhong Fan, Honghui Ou, Xuelan Hou, Qizhong Huang, Huagui Hu, Guidong Yang","doi":"10.1002/aic.18654","DOIUrl":"https://doi.org/10.1002/aic.18654","url":null,"abstract":"Utilizing N₂ from the air and water for the electrocatalytic nitrogen reduction reaction shows promise for NH₃ synthesis under mild conditions. However, the chemical stability of N₂ and the thermodynamic limitations of NH₃ synthesis hinder its effectiveness. Herein, we integrated a specially designed Cu nanowire catalyst with a five-fold twin structure (T-CuNW) into an electrocatalytic system, combining electrocatalytic nitrogen reduction with nonthermal plasma-assisted N₂ activation. This work achieved an NH₃ yield of 45 mg·mg<sub>cat.</sub><sup>−1</sup>·h<sup>−1</sup> and a Faradaic efficiency of over 95% at −0.5 V versus RHE after a 90-h stability test. In situ characterization revealed that the T-CuNW's twin structure plays a crucial role for the generation of a large quantity of H<sub>ads</sub>, essential for the hydrogenation of nitrate intermediates, particularly nitrite (NO₂<sup>−</sup>). This enhanced hydrogenation process significantly contributes to the high performance of the ammonia synthesis system.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"34 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142788761","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}
Matthew Lee Manion, Joshua Doctor, Albert Tianxiang Liu
Accurate mapping of chemical concentrations in reactor networks remains an obstacle to establish complete systems-level insight and control. This issue extends beyond traditional reactor design to biological and other inaccessible systems of interest. Recent developments in novel materials with non-volatile memory allow autonomous sensor nodes to record information with minimal external supervision. Integrating these materials in solution suspended particles demonstrates the unique potential for diffuse measurements of chemical data at the microscale. In this study, we establish a generalized workflow for the simulated deployment of time aware particle sensors (TAPS) in ideal reactor systems to measure analyte profiles, using Gillespie kinetic Monte Carlo algorithms (KMC). Our results show that computationally-limited, chemically sensitive tracer particles capable of timestamping an analyte detection event can provide accurate analyte profiles throughout multistage reactors in an ensemble fashion.
{"title":"Temporally resolved concentration profiling via computationally limited, distributed sensor nodes","authors":"Matthew Lee Manion, Joshua Doctor, Albert Tianxiang Liu","doi":"10.1002/aic.18691","DOIUrl":"https://doi.org/10.1002/aic.18691","url":null,"abstract":"Accurate mapping of chemical concentrations in reactor networks remains an obstacle to establish complete systems-level insight and control. This issue extends beyond traditional reactor design to biological and other inaccessible systems of interest. Recent developments in novel materials with non-volatile memory allow autonomous sensor nodes to record information with minimal external supervision. Integrating these materials in solution suspended particles demonstrates the unique potential for diffuse measurements of chemical data at the microscale. In this study, we establish a generalized workflow for the simulated deployment of time aware particle sensors (TAPS) in ideal reactor systems to measure analyte profiles, using Gillespie kinetic Monte Carlo algorithms (KMC). Our results show that computationally-limited, chemically sensitive tracer particles capable of timestamping an analyte detection event can provide accurate analyte profiles throughout multistage reactors in an ensemble fashion.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"47 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142788673","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}
Achieving rapid synthesis alongside efficient shaping without sacrificing high porosity and crystallinity poses significant challenges for metal–organic frameworks (MOFs) in practical applications. Here, we report an ultrafast, scalable method for preparing an ultramicroporous MOF at room temperature. This method achieves a space–time yield significantly higher than conventional MOF synthesis by orders of magnitude. As a result of strongly promoted crystal nucleation by careful selection of solvent and metal source, the MOF material is produced in a gel state offering both high crystallinity and processability. This allows for the binder-free fabrication of monolithic adsorbents with predesigned macro shapes and sizes. Owing to its narrowly distributed pore size and high-density open metal sites, the monolithic adsorbent demonstrates top-tier selectivity for CO2/N2 (>200) and CO2/CH4 separations. The performance sets a new benchmark among current MOF xero- or aerogel monoliths. Breakthrough experiments further verify its robust ability for carbon capture under dynamic conditions.
{"title":"Ultrafast synthesis and binder-free fabrication of a monolithic metal–organic framework for efficient carbon capture","authors":"Qi Ding, Yulong Liu, Jia Liu, Jingyue Cheng, Zhaoqiang Zhang, Kungang Chai, Sui Zhang","doi":"10.1002/aic.18673","DOIUrl":"https://doi.org/10.1002/aic.18673","url":null,"abstract":"Achieving rapid synthesis alongside efficient shaping without sacrificing high porosity and crystallinity poses significant challenges for metal–organic frameworks (MOFs) in practical applications. Here, we report an ultrafast, scalable method for preparing an ultramicroporous MOF at room temperature. This method achieves a space–time yield significantly higher than conventional MOF synthesis by orders of magnitude. As a result of strongly promoted crystal nucleation by careful selection of solvent and metal source, the MOF material is produced in a gel state offering both high crystallinity and processability. This allows for the binder-free fabrication of monolithic adsorbents with predesigned macro shapes and sizes. Owing to its narrowly distributed pore size and high-density open metal sites, the monolithic adsorbent demonstrates top-tier selectivity for CO<sub>2</sub>/N<sub>2</sub> (>200) and CO<sub>2</sub>/CH<sub>4</sub> separations. The performance sets a new benchmark among current MOF xero- or aerogel monoliths. Breakthrough experiments further verify its robust ability for carbon capture under dynamic conditions.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"60 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142788671","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 influences of temperature and water−graphite interaction energy on the contact angle (<i>θ</i>) and structure of water on the graphite-like substrate have been investigated using the classical density functional theory. We find that the temperature-dependent behavior of cos<i>θ</i> is contingent upon the water−graphite interaction energy, manifesting in three distinct patterns: increasing, decreasing, or remaining nearly invariant with temperature within the examined range (273.16–640K). Furthermore, a novel simple equation has been derived to describe the temperature-dependent variation of cos<i>θ</i> at constant water−graphite interaction energy, that is, <span data-altimg="/cms/asset/2c57eb43-b526-412d-84e2-2636c4abe0e9/aic18697-math-0001.png"></span><mjx-container ctxtmenu_counter="4" ctxtmenu_oldtabindex="1" jax="CHTML" role="application" sre-explorer- style="font-size: 103%; position: relative;" tabindex="0"><mjx-math aria-hidden="true" location="graphic/aic18697-math-0001.png"><mjx-semantics><mjx-mrow data-semantic-children="21,22" data-semantic-content="6" data-semantic- data-semantic-role="equality" data-semantic-speech="partial differential cosine theta slash partial differential upper T equals lamda divided by left parenthesis gamma Superscript l v Baseline right parenthesis squared" data-semantic-type="relseq"><mjx-mrow data-semantic-children="20,5" data-semantic-content="4" data-semantic- data-semantic-parent="23" data-semantic-role="prefix operator" data-semantic-type="infixop"><mjx-mrow data-semantic-children="19" data-semantic-content="0" data-semantic- data-semantic-parent="21" data-semantic-role="prefix operator" data-semantic-type="prefixop"><mjx-mi data-semantic- data-semantic-operator="prefixop,∂" data-semantic-parent="20" data-semantic-role="prefix operator" data-semantic-type="operator"><mjx-c></mjx-c></mjx-mi><mjx-mrow data-semantic-children="1,17" data-semantic-content="18,1" data-semantic- data-semantic-parent="20" data-semantic-role="prefix function" data-semantic-type="appl"><mjx-mi data-semantic-font="normal" data-semantic- data-semantic-operator="appl" data-semantic-parent="19" data-semantic-role="prefix function" data-semantic-type="function"><mjx-c></mjx-c><mjx-c></mjx-c><mjx-c></mjx-c></mjx-mi><mjx-mo data-semantic-added="true" data-semantic- data-semantic-operator="appl" data-semantic-parent="19" data-semantic-role="application" data-semantic-type="punctuation" style="margin-left: 0.056em; margin-right: 0.056em;"><mjx-c></mjx-c></mjx-mo><mjx-mrow data-semantic-children="2" data-semantic-content="3" data-semantic- data-semantic-parent="19" data-semantic-role="division" data-semantic-type="postfixop"><mjx-mi data-semantic-annotation="clearspeak:simple" data-semantic-font="italic" data-semantic- data-semantic-parent="17" data-semantic-role="greekletter" data-semantic-type="identifier"><mjx-c></mjx-c></mjx-mi><mjx-mo data-semantic- data-semantic-operator="postfixop,/" data-semantic-parent="17" data-semantic-role=
{"title":"The contact angle and structure of water on the graphite-like substrate: A classical density functional approach","authors":"Jiarong Sang, Feng Wei, Junsu Jin","doi":"10.1002/aic.18697","DOIUrl":"https://doi.org/10.1002/aic.18697","url":null,"abstract":"The influences of temperature and water−graphite interaction energy on the contact angle (<i>θ</i>) and structure of water on the graphite-like substrate have been investigated using the classical density functional theory. We find that the temperature-dependent behavior of cos<i>θ</i> is contingent upon the water−graphite interaction energy, manifesting in three distinct patterns: increasing, decreasing, or remaining nearly invariant with temperature within the examined range (273.16–640K). Furthermore, a novel simple equation has been derived to describe the temperature-dependent variation of cos<i>θ</i> at constant water−graphite interaction energy, that is, <span data-altimg=\"/cms/asset/2c57eb43-b526-412d-84e2-2636c4abe0e9/aic18697-math-0001.png\"></span><mjx-container ctxtmenu_counter=\"4\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" role=\"application\" sre-explorer- style=\"font-size: 103%; position: relative;\" tabindex=\"0\"><mjx-math aria-hidden=\"true\" location=\"graphic/aic18697-math-0001.png\"><mjx-semantics><mjx-mrow data-semantic-children=\"21,22\" data-semantic-content=\"6\" data-semantic- data-semantic-role=\"equality\" data-semantic-speech=\"partial differential cosine theta slash partial differential upper T equals lamda divided by left parenthesis gamma Superscript l v Baseline right parenthesis squared\" data-semantic-type=\"relseq\"><mjx-mrow data-semantic-children=\"20,5\" data-semantic-content=\"4\" data-semantic- data-semantic-parent=\"23\" data-semantic-role=\"prefix operator\" data-semantic-type=\"infixop\"><mjx-mrow data-semantic-children=\"19\" data-semantic-content=\"0\" data-semantic- data-semantic-parent=\"21\" data-semantic-role=\"prefix operator\" data-semantic-type=\"prefixop\"><mjx-mi data-semantic- data-semantic-operator=\"prefixop,∂\" data-semantic-parent=\"20\" data-semantic-role=\"prefix operator\" data-semantic-type=\"operator\"><mjx-c></mjx-c></mjx-mi><mjx-mrow data-semantic-children=\"1,17\" data-semantic-content=\"18,1\" data-semantic- data-semantic-parent=\"20\" data-semantic-role=\"prefix function\" data-semantic-type=\"appl\"><mjx-mi data-semantic-font=\"normal\" data-semantic- data-semantic-operator=\"appl\" data-semantic-parent=\"19\" data-semantic-role=\"prefix function\" data-semantic-type=\"function\"><mjx-c></mjx-c><mjx-c></mjx-c><mjx-c></mjx-c></mjx-mi><mjx-mo data-semantic-added=\"true\" data-semantic- data-semantic-operator=\"appl\" data-semantic-parent=\"19\" data-semantic-role=\"application\" data-semantic-type=\"punctuation\" style=\"margin-left: 0.056em; margin-right: 0.056em;\"><mjx-c></mjx-c></mjx-mo><mjx-mrow data-semantic-children=\"2\" data-semantic-content=\"3\" data-semantic- data-semantic-parent=\"19\" data-semantic-role=\"division\" data-semantic-type=\"postfixop\"><mjx-mi data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"italic\" data-semantic- data-semantic-parent=\"17\" data-semantic-role=\"greekletter\" data-semantic-type=\"identifier\"><mjx-c></mjx-c></mjx-mi><mjx-mo data-semantic- data-semantic-operator=\"postfixop,/\" data-semantic-parent=\"17\" data-semantic-role=","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"17 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142788675","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}
Le Zhou, Xin Zhang, Yu Han, Xin Li, Ze-Quan Zeng, Hai-Kui Zou, Yong Luo
The Co@NC catalyst exhibits significant protic solvent preference for hydrogenation of nitriles to primary amines. However, the effect of mixed protic solvents on catalytic hydrogenation has received little attention. Herein, the synergetic solvent effect has been proposed to accelerate the hydrogenation of adiponitrile (ADN) to hexamethylenediamine through H2O-ethanol hydrogen bond networks on Co@NC catalyst. Experimental screenings on solvents showed that ADN conversion in H2O-ethanol was 1.6 ~ 5.1 times greater than in single solvents. Kinetic models in H2O/ethanol (vW = 0.6), H2O, and ethanol showed that the solvents effected on H2 transformation dominated the reaction. Isotope labelling and kinetic experiments revealed that H2O and ethanol acted as co-catalysts through exchanging and transferring hydrogen via hydroxyl groups. Density functional theory calculations confirmed that the energy barrier for proton transfer mediated by H₂O–ethanol was reduced by 0.18 eV compared to proton transfer mediated by H₂O–H₂O dimers.
{"title":"Insight into the synergetic solvent effect of H2O-ethanol on the adiponitrile hydrogenation","authors":"Le Zhou, Xin Zhang, Yu Han, Xin Li, Ze-Quan Zeng, Hai-Kui Zou, Yong Luo","doi":"10.1002/aic.18677","DOIUrl":"https://doi.org/10.1002/aic.18677","url":null,"abstract":"The Co@NC catalyst exhibits significant protic solvent preference for hydrogenation of nitriles to primary amines. However, the effect of mixed protic solvents on catalytic hydrogenation has received little attention. Herein, the synergetic solvent effect has been proposed to accelerate the hydrogenation of adiponitrile (ADN) to hexamethylenediamine through H<sub>2</sub>O-ethanol hydrogen bond networks on Co@NC catalyst. Experimental screenings on solvents showed that ADN conversion in H<sub>2</sub>O-ethanol was 1.6 ~ 5.1 times greater than in single solvents. Kinetic models in H<sub>2</sub>O/ethanol (<i>v</i><sub>W</sub> = 0.6), H<sub>2</sub>O, and ethanol showed that the solvents effected on H<sub>2</sub> transformation dominated the reaction. Isotope labelling and kinetic experiments revealed that H<sub>2</sub>O and ethanol acted as co-catalysts through exchanging and transferring hydrogen via hydroxyl groups. Density functional theory calculations confirmed that the energy barrier for proton transfer mediated by H₂O–ethanol was reduced by 0.18 eV compared to proton transfer mediated by H₂O–H₂O dimers.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"10 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142782909","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}
Junfeng Lu, Tinglan Sun, Yumiao Lu, Hongyan He, Yanlei Wang
Hydrogen bonds (HBs) widely exist in applications ranging from biology to electrochemistry, where quantifying HB at the electrochemical interface poses significant challenges. Herein, we propose an approach to quantitatively decouple the electrostatic and van der Waals interactions of HBs in ionic liquids (ILs) by injecting electrons into the electrode interface. The charging process showed that the order of obtaining electrons is molybdenum disulfide > graphene > IL > boron nitride. Interestingly, the preferentially charged cations would lead to a direct reduction of coulombic interactions in HBs; in contrast, the charged substrate would repel the anion and weaken HBs indirectly. Infrared (IR) spectrum and covalent change analysis verified the charging-induced direct and indirect decoupling processes. Moreover, the energy analysis indicates that the electrostatic terms account for ~50% of HBs. These results on the weakening origin of HBs can guide the molecular design of ILs toward high-performance electrochemical applications.
{"title":"Weakening origin of hydrogen bond in ionic liquid at the electrified interface","authors":"Junfeng Lu, Tinglan Sun, Yumiao Lu, Hongyan He, Yanlei Wang","doi":"10.1002/aic.18660","DOIUrl":"https://doi.org/10.1002/aic.18660","url":null,"abstract":"Hydrogen bonds (HBs) widely exist in applications ranging from biology to electrochemistry, where quantifying HB at the electrochemical interface poses significant challenges. Herein, we propose an approach to quantitatively decouple the electrostatic and van der Waals interactions of HBs in ionic liquids (ILs) by injecting electrons into the electrode interface. The charging process showed that the order of obtaining electrons is molybdenum disulfide > graphene > IL > boron nitride. Interestingly, the preferentially charged cations would lead to a direct reduction of coulombic interactions in HBs; in contrast, the charged substrate would repel the anion and weaken HBs indirectly. Infrared (IR) spectrum and covalent change analysis verified the charging-induced direct and indirect decoupling processes. Moreover, the energy analysis indicates that the electrostatic terms account for ~50% of HBs. These results on the weakening origin of HBs can guide the molecular design of ILs toward high-performance electrochemical applications.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"216 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142782982","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}
Zishuai Wang, Yaoqiang Wang, Gang Xiao, Zequn Tang, Shaojie Wang, Yu Jin, Haijia Su
Upcycling of waste poly(ethylene terephthalate) (PET) into valuable products represents a promising avenue for advancing carbon neutrality and circular economy. Here, we demonstrate a modular strategy for converting waste PET into glycolic acid (GA) and 2,4-pyridine dicarboxylic acid (2,4-PDCA), achieving an upcycling process and 45% reduction in greenhouse gas emissions. We conducted comprehensive studies on PET hydrolysis, PET-derived ethylene glycol (EG) photooxidation, and PET-derived terephthalic acid (TPA) bioconversion. Utilizing a plasmon-active CuPt nanoalloy, EG oxidation proceeds at mild conditions with impressive EG conversion (94.78%) and GA yield (71.98%). Two Escherichia coli strains were employed to convert TPA into 2,4-PDCA, achieved a 91.03% molar yield. This work successfully accomplishes the comprehensive utilization of waste PET through an environmentally friendly and economically viable strategy, leading to a significant reduction in PET plastic pollution while simultaneously generating substantial economic benefits.
{"title":"Modular chem-bio upcycling of waste poly(ethylene terephthalate) to glycolic acid and 2,4-pyridine dicarboxylic acid","authors":"Zishuai Wang, Yaoqiang Wang, Gang Xiao, Zequn Tang, Shaojie Wang, Yu Jin, Haijia Su","doi":"10.1002/aic.18686","DOIUrl":"https://doi.org/10.1002/aic.18686","url":null,"abstract":"Upcycling of waste poly(ethylene terephthalate) (PET) into valuable products represents a promising avenue for advancing carbon neutrality and circular economy. Here, we demonstrate a modular strategy for converting waste PET into glycolic acid (GA) and 2,4-pyridine dicarboxylic acid (2,4-PDCA), achieving an upcycling process and 45% reduction in greenhouse gas emissions. We conducted comprehensive studies on PET hydrolysis, PET-derived ethylene glycol (EG) photooxidation, and PET-derived terephthalic acid (TPA) bioconversion. Utilizing a plasmon-active CuPt nanoalloy, EG oxidation proceeds at mild conditions with impressive EG conversion (94.78%) and GA yield (71.98%). Two <i>Escherichia coli</i> strains were employed to convert TPA into 2,4-PDCA, achieved a 91.03% molar yield. This work successfully accomplishes the comprehensive utilization of waste PET through an environmentally friendly and economically viable strategy, leading to a significant reduction in PET plastic pollution while simultaneously generating substantial economic benefits.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"2 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142783036","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}
Hanyang Liu, Ning Yang, Junan Jiang, Zundong Xiao, Chenfeng Wang, Beili Lu, Rijie Wang, Lirong Tang
Flow chemistry is widely valued for its enhanced transport properties and safety, but scaling up while maintaining the advantages of the microenvironment in small-scale systems remains challenging. We addressed this by developing a novel tube-in-tube millireactor with a multi-hole jet inlet and deflectors, designed to maintain consistent flow regimes and optimize micromixing, residence time distribution (RTD), and heat transfer at various scales. The reactor increases flux by enlarging tube diameters and incorporating micro-holes and deflectors, all while maintaining a constant annular space. This design, validated through both CFD modeling and experimental results, maintains consistent fluid flow and excellent transfer properties, achieving micromixing time below 2 ms at Reh > 2000, a plug-flow-like RTD profile, and a heat transfer capacity up to 12.4 times greater than conventional designs. This study presents a simple, scalable approach to millireactor design, combining “number-up” and “size-up” strategies, offering a cost-effective solution for industrial applications.
{"title":"Seamless scale-up of tube-in-tube millireactors by annular structure and feed method design: Micromixing, residence time distribution and heat transfer","authors":"Hanyang Liu, Ning Yang, Junan Jiang, Zundong Xiao, Chenfeng Wang, Beili Lu, Rijie Wang, Lirong Tang","doi":"10.1002/aic.18695","DOIUrl":"https://doi.org/10.1002/aic.18695","url":null,"abstract":"Flow chemistry is widely valued for its enhanced transport properties and safety, but scaling up while maintaining the advantages of the microenvironment in small-scale systems remains challenging. We addressed this by developing a novel tube-in-tube millireactor with a multi-hole jet inlet and deflectors, designed to maintain consistent flow regimes and optimize micromixing, residence time distribution (<i>RTD</i>), and heat transfer at various scales. The reactor increases flux by enlarging tube diameters and incorporating micro-holes and deflectors, all while maintaining a constant annular space. This design, validated through both CFD modeling and experimental results, maintains consistent fluid flow and excellent transfer properties, achieving micromixing time below 2 ms at <i>Re</i><sub><i>h</i></sub> > 2000, a plug-flow-like <i>RTD</i> profile, and a heat transfer capacity up to 12.4 times greater than conventional designs. This study presents a simple, scalable approach to millireactor design, combining “number-up” and “size-up” strategies, offering a cost-effective solution for industrial applications.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"17 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142782984","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}
Arie H. Huijgen, P. M. Durubal, Cristina García Llamas, Kay A. Buist, J. A. M. (Hans) Kuipers, Maike W. Baltussen
This study focuses on the dynamics of two equal-sized droplets of non-Newtonian liquids with simulations using the volume of fluid method and the local front reconstruction method. The non-Newtonian behavior is implement via a power-law model. The droplet interactions are performed for Weber numbers ranging from 20 to 300 and impact parameters from 0 to 0.6. Both methods produce similar results at low Weber numbers, while the disintegration of the droplets at high Weber numbers occurs via different mechanisms. Our results demonstrate that the boundaries of the collision maps are highly dependent on the power-law index. Additionally, the diameter of the ring for head-on collisions is increased with increasing Weber number and decreasing power-law index, while the critical ligament length in off-center collisions increases with Weber number and power-law index.
{"title":"Characterizing binary droplet collisions of power-law fluids","authors":"Arie H. Huijgen, P. M. Durubal, Cristina García Llamas, Kay A. Buist, J. A. M. (Hans) Kuipers, Maike W. Baltussen","doi":"10.1002/aic.18667","DOIUrl":"https://doi.org/10.1002/aic.18667","url":null,"abstract":"This study focuses on the dynamics of two equal-sized droplets of non-Newtonian liquids with simulations using the volume of fluid method and the local front reconstruction method. The non-Newtonian behavior is implement via a power-law model. The droplet interactions are performed for Weber numbers ranging from 20 to 300 and impact parameters from 0 to 0.6. Both methods produce similar results at low Weber numbers, while the disintegration of the droplets at high Weber numbers occurs via different mechanisms. Our results demonstrate that the boundaries of the collision maps are highly dependent on the power-law index. Additionally, the diameter of the ring for head-on collisions is increased with increasing Weber number and decreasing power-law index, while the critical ligament length in off-center collisions increases with Weber number and power-law index.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"27 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142788676","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}
This work investigates the bubble breakup process with and without particles in turbulent conditions using the image‐based method. A binocular high‐speed camera was employed to capture breakup events. A deep learning‐based image identification software (Large Deformation Dispersed Phase Analysis in Multiphase Flows) and a highly deformed bubble volume/surface area quantification method (Dense Adaptive Segmentation Method) are proposed. An energy barrier is found during the bubble breakup process, with the maximum increase in surface area (ΔSmax) being two to three times the final increase after breakup (ΔSfinal). This indicates that the critical energy required for bubble breakup is underestimated in most breakup models. The presence of suspended particles raises this energy barrier, thus reducing the breakup probability. The daughter bubble size distribution follows an M‐type distribution in water, while the addition of particles leads to a tendency towards equal‐size breakup. This work provides a reliable technology and the experimental data for further clarifying the bubble breakup mechanism.
{"title":"Experimental study of bubble breakup in water and solid suspension by using the image‐based method","authors":"Haozheng Wang, Xiaoxia Duan, Wenjuan Wu, Xin Feng, Dingwang Huang, Weipeng Zhang, Zheng Li, Runci Song, Junya Cao, Chao Yang","doi":"10.1002/aic.18689","DOIUrl":"https://doi.org/10.1002/aic.18689","url":null,"abstract":"This work investigates the bubble breakup process with and without particles in turbulent conditions using the image‐based method. A binocular high‐speed camera was employed to capture breakup events. A deep learning‐based image identification software (Large Deformation Dispersed Phase Analysis in Multiphase Flows) and a highly deformed bubble volume/surface area quantification method (Dense Adaptive Segmentation Method) are proposed. An energy barrier is found during the bubble breakup process, with the maximum increase in surface area (Δ<jats:italic>S</jats:italic><jats:sub>max</jats:sub>) being two to three times the final increase after breakup (Δ<jats:italic>S</jats:italic><jats:sub>final</jats:sub>). This indicates that the critical energy required for bubble breakup is underestimated in most breakup models. The presence of suspended particles raises this energy barrier, thus reducing the breakup probability. The daughter bubble size distribution follows an M‐type distribution in water, while the addition of particles leads to a tendency towards equal‐size breakup. This work provides a reliable technology and the experimental data for further clarifying the bubble breakup mechanism.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"81 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142782983","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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