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Modular chem-bio upcycling of waste poly(ethylene terephthalate) to glycolic acid and 2,4-pyridine dicarboxylic acid
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2024-12-06 DOI: 10.1002/aic.18686
Zishuai Wang, Yaoqiang Wang, Gang Xiao, Zequn Tang, Shaojie Wang, Yu Jin, Haijia Su
{"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}
引用次数: 0
Characterizing binary droplet collisions of power-law fluids
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2024-12-06 DOI: 10.1002/aic.18667
Arie H. Huijgen, P. M. Durubal, Cristina García Llamas, Kay A. Buist, J. A. M. (Hans) Kuipers, Maike W. Baltussen
{"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}
引用次数: 0
Seamless scale-up of tube-in-tube millireactors by annular structure and feed method design: Micromixing, residence time distribution and heat transfer
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2024-12-06 DOI: 10.1002/aic.18695
Hanyang Liu, Ning Yang, Junan Jiang, Zundong Xiao, Chenfeng Wang, Beili Lu, Rijie Wang, Lirong Tang
{"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> &gt; 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}
引用次数: 0
Experimental study of bubble breakup in water and solid suspension by using the image‐based method
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2024-12-06 DOI: 10.1002/aic.18689
Haozheng Wang, Xiaoxia Duan, Wenjuan Wu, Xin Feng, Dingwang Huang, Weipeng Zhang, Zheng Li, Runci Song, Junya Cao, Chao Yang
{"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}
引用次数: 0
Screening of metal–organic frameworks for efficient electrocatalytic nitrogen reduction
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2024-12-05 DOI: 10.1002/aic.18652
Jiawei Lin, Yuhang Li, Hongping Yan, Tingting Qi, Shijing Liang, Lilong Jiang
{"title":"Screening of metal–organic frameworks for efficient electrocatalytic nitrogen reduction","authors":"Jiawei Lin, Yuhang Li, Hongping Yan, Tingting Qi, Shijing Liang, Lilong Jiang","doi":"10.1002/aic.18652","DOIUrl":"https://doi.org/10.1002/aic.18652","url":null,"abstract":"In this work, 44 metal–organic frameworks (MOFs) are screened for efficient electrocatalytic nitrogen reduction reaction (eNRR). The isosteric heats of N<sub>2</sub> adsorption on the 44 metal active centers of MOFs are calculated by the grand canonical Monte Carlo method. It is found that p-block-elements exhibit the highest N<sub>2</sub> affinity among all screened elements, implying their excellent catalytic potentials for eNRR. Furthermore, the Al element is preferentially chosen as the metal center of MOFs (MIL-53 (Al)) owing to its relatively low toxicity and cost. Combined <i>in situ</i> Diffuse Reflectance Infrared Fourier Transform (DRIFT) analysis with theoretical calculation, we found that N<sub>2</sub> is mainly attracted by the bridging oxygen of Al-O-Al structure in the MIL-53 (Al). The optimized MIL-53 (Al) shows a superior activity with the NH<sub>3</sub> yield rate of 74.55 ± 1 μg h<sup>−1</sup> mg<sub>cat</sub><sup>−1</sup> at −0.3 V vs. Reversible Hydrogen Electrode (RHE), to our best knowledge, which is currently the highest activity of MOF-based catalyst for eNRR reported in the literature.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"1 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142777449","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
Dynamics of two bubbles colliding at high Reynolds numbers in water: Bubble rebound behavior study
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2024-12-02 DOI: 10.1002/aic.18682
Runci Song, Kefeng Fang, Bing Xiang, Luchang Han, Xin Feng, Jie Chen, Chao Yang
{"title":"Dynamics of two bubbles colliding at high Reynolds numbers in water: Bubble rebound behavior study","authors":"Runci Song, Kefeng Fang, Bing Xiang, Luchang Han, Xin Feng, Jie Chen, Chao Yang","doi":"10.1002/aic.18682","DOIUrl":"https://doi.org/10.1002/aic.18682","url":null,"abstract":"The collision between bubbles is essential to gas–liquid dispersion systems. When bubbles encounter each other, they may either rebound or coalesce. Yet, little is known about the rebound dynamics immediately after two bubbles collide. This work investigates such collision dynamics of two bubbles at high Reynolds numbers in water through experiment and simulation. The moving velocity, deformation, contact time during collision and restitution coefficient of bubbles are analyzed. Simulations reproduced quantitatively the bubble rebound behavior, revealing the evolution of various energies involved in collision. Simulation results show that over 70% of the system's initial mechanical energy (SME) could be converted into bubble surface energy (BSE) during the approach. In turn, the excess BSE is converted back into SME driving bubbles to rebound with significant dissipation. A mass-spring-damper model is developed, which describes the dynamic of bubble rebound well. This contribution enhances the understanding of bubble interactions in multiphase flow.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"21 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142760822","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
Producing battery grade lithium carbonate from salt-lake brine via bipolar membrane carbon dioxide mineralization
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2024-12-02 DOI: 10.1002/aic.18675
Weixiang Shan, Guangzhong Cao, Tianle Gu, Xiao Liu, Dongyue Sun, Rongqiang Fu, Zhaoming Liu, Chenxiao Jiang, Tongwen Xu
{"title":"Producing battery grade lithium carbonate from salt-lake brine via bipolar membrane carbon dioxide mineralization","authors":"Weixiang Shan, Guangzhong Cao, Tianle Gu, Xiao Liu, Dongyue Sun, Rongqiang Fu, Zhaoming Liu, Chenxiao Jiang, Tongwen Xu","doi":"10.1002/aic.18675","DOIUrl":"https://doi.org/10.1002/aic.18675","url":null,"abstract":"Producing battery-grade Li<sub>2</sub>CO<sub>3</sub> product from salt-lake brine is a critical issue for meeting the growing demand of the lithium-ion battery industry. Traditional procedures include Na<sub>2</sub>CO<sub>3</sub> precipitation and multi-stage crystallization for refining, resulting in significant lithium loss and undesired lithium product quality. Herein, we first proposed a bipolar membrane CO<sub>2</sub> mineralization technique for directly producing battery-grade Li<sub>2</sub>CO<sub>3</sub> from lake brine that enriches alkali metals (Na<sup>+</sup>, K<sup>+</sup>). Results indicate the process can successfully separate Li<sup>+</sup> from contaminants and present a selectivity above 900 for Li<sup>+</sup> through the CO<sub>2</sub> mineralization reaction, while prevent electro-oxidating Cl<sup>−</sup> to Cl<sub>2</sub> pollution. The obtained Li<sub>2</sub>CO<sub>3</sub> production purity is above 99.75% with lithium recovery rate of 86%. Carbon dioxide was captured in the form of Li<sub>2</sub>CO<sub>3</sub>, with a capacity of 595 g of CO<sub>2</sub> for1 kg of Li<sub>2</sub>CO<sub>3</sub>. The technology provides a sustainable and cost-effective path for producing battery-grade Li<sub>2</sub>CO<sub>3</sub> from the lake brine.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"388 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142760823","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
Do large language models “understand” their knowledge?
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2024-11-30 DOI: 10.1002/aic.18661
Venkat Venkatasubramanian
{"title":"Do large language models “understand” their knowledge?","authors":"Venkat Venkatasubramanian","doi":"10.1002/aic.18661","DOIUrl":"https://doi.org/10.1002/aic.18661","url":null,"abstract":"Large language models (LLMs) are often criticized for lacking true “understanding” and the ability to “reason” with their knowledge, being seen merely as autocomplete engines. I suggest that this assessment might be missing a nuanced insight. LLMs do develop a kind of empirical “understanding” that is “geometry”-like, which is adequate for many applications. However, this “geometric” understanding, built from incomplete and noisy data, makes them unreliable, difficult to generalize, and lacking in inference capabilities and explanations. To overcome these limitations, LLMs should be integrated with an “algebraic” representation of knowledge that includes symbolic AI elements used in expert systems. This integration aims to create large knowledge models (LKMs) grounded in first principles that can reason and explain, mimicking human expert capabilities. Furthermore, we need a conceptual breakthrough, such as the transformation from Newtonian mechanics to statistical mechanics, to create a new science of LLMs.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"18 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-11-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142756266","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
Hydrodynamics and mass transfer performance of gas–liquid two-phase flow in a high-throughput chaotic microreactor
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2024-11-30 DOI: 10.1002/aic.18657
Jia-Ni Zhang, Hao-Tian Tong, Zu-Chun Shi, Ting-Liang Xie, Qiang Liu, Shi-Xiao Wei, Shuang-Feng Yin
{"title":"Hydrodynamics and mass transfer performance of gas–liquid two-phase flow in a high-throughput chaotic microreactor","authors":"Jia-Ni Zhang, Hao-Tian Tong, Zu-Chun Shi, Ting-Liang Xie, Qiang Liu, Shi-Xiao Wei, Shuang-Feng Yin","doi":"10.1002/aic.18657","DOIUrl":"https://doi.org/10.1002/aic.18657","url":null,"abstract":"Microbubbles have been widely applied in various fields. Here, an oscillating feedback microreactor (OFM) was designed to produce microbubbles at high throughput (5–80 mL/min), where the hydrodynamics and mass transfer performance of gas–liquid two-phase system were investigated. The hydrodynamics results showed that three secondary flows (oscillation, vortex, and feedback) could be effectively generated for inducing chaotic flow in the OFM, and the gas phase could be effectively broken up into small microbubbles. The bubble size was more sensitive to the liquid phase flow rate than the gas phase. Two dimensionless prediction formulas for bubble Sauter size were proposed based on gas–liquid flow ratio and Reynolds number at different liquid flow rates. The mass transfer experiments showed that the volumetric average mass transfer coefficient <i>k</i><sub>L</sub><i>a</i> was 1–3 orders of magnitude higher than those of conventional reactors.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"12 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-11-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142756267","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
Direct conversion of syngas into methyl acetate by relay catalysis: From fabrication of active sites to process control
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2024-11-30 DOI: 10.1002/aic.18664
Suhan Liu, Gongli Wu, Yuqing Chen, Yaoyao Han, Mingchao Zhang, Jincan Kang, Min Tang, Krijn P. de Jong, Qinghong Zhang, Ye Wang, Kang Cheng
{"title":"Direct conversion of syngas into methyl acetate by relay catalysis: From fabrication of active sites to process control","authors":"Suhan Liu, Gongli Wu, Yuqing Chen, Yaoyao Han, Mingchao Zhang, Jincan Kang, Min Tang, Krijn P. de Jong, Qinghong Zhang, Ye Wang, Kang Cheng","doi":"10.1002/aic.18664","DOIUrl":"https://doi.org/10.1002/aic.18664","url":null,"abstract":"The direct and selective conversion of syngas into C<sub>2+</sub> oxygenates is challenging due to the complex reaction network. Here, we report a robust relay system for the direct synthesis of methyl acetate (MA) from syngas, which combines CuZnAlO<sub><i>x</i></sub>/H-ZSM-5 for syngas to dimethyl ether (DME) with modified H-MOR for DME carbonylation. The dehydration of methanol to DME on H-ZSM-5 significantly enhanced the hydrogenation of CO on CuZnAlO<sub><i>x</i></sub>, because of high DME equilibrium yields. Blocking of Brönsted acid sites with basic molecules or selective dealumination of 12-membered rings in H-MOR suppressed the zeolite coking. Besides, reaction temperatures above 240°C avoided H<sub>2</sub>O poisoning of carbonylation sites inside 8-MR side pockets of H-MOR, further benefiting the catalytic stability. Eventually, this relay system provided a high MA selectivity of 75% and an acetic acid selectivity of 13% at a CO conversion of 65%, outperforming reported catalysts.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"26 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-11-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142756268","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
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