AIChE Journal最新文献_第10页

Ultrafast synthesis and binder-free fabrication of a monolithic metal–organic framework for efficient carbon capture 用于高效碳捕获的单片金属有机框架的超快合成和无粘结剂制造

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2024-12-07 DOI: 10.1002/aic.18673

Qi Ding, Yulong Liu, Jia Liu, Jingyue Cheng, Zhaoqiang Zhang, Kungang Chai, Sui Zhang

{"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":"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 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.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 3","pages":""},"PeriodicalIF":3.5,"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}

引用次数: 0

The contact angle and structure of water on the graphite-like substrate: A classical density functional approach 石墨基板上水的接触角和结构：一个经典的密度泛函方法

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2024-12-07 DOI: 10.1002/aic.18697

Jiarong Sang, Feng Wei, Junsu Jin

{"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":"10.1002/aic.18697","url":null,"abstract":"The influences of temperature and water−graphite interaction energy on the contact angle (θ) 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 cosθ 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 cosθ at constant water−graphite interaction energy, that is, <math>\u0000 <mi>∂</mi>\u0000 <mi>cos</mi>\u0000 <mi>θ</mi>\u0000 <mo>/</mo>\u0000 <mi>∂</mi>\u0000 <mi>T</mi>\u0000 <mo>=</mo>\u0000 <mi>λ</mi>\u0000 <mo>/</mo>\u0000 <msup>\u0000 <mfenced>\u0000 <msup>\u0000 <mi>γ</mi>\u0000 <mi>lv</mi>\u0000 </msup>\u0000 </mfenced>\u0000 <mn>2</mn>\u0000 </msup></math>, where <math>\u0000 <msup>\u0000 <mi>γ</mi>\u0000 <mi>lv</mi>\u0000 </msup></math> is the water−vapor interfacial tension, and the value of <math>\u0000 <mi>λ</mi></math> depends on the water−graphite interaction energy. According to different values of <math>\u0000 <mi>λ</mi></math>, this equation is able to successfully represent the three aforementioned patterns. At last, the density profile and hydrogen bonding structure of water near the substrate have been analyzed to offer microscopic insights.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 3","pages":""},"PeriodicalIF":3.5,"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}

引用次数: 0

Solvent-enabled intensification of liquid–liquid heterogeneous catalysis exemplified by direct hydration of cyclohexene

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2024-12-06 DOI: 10.1002/aic.18698

Zhixiang Zhang, Xiang Zhang, Ke Wang, Kunchi Xie, Shu Wang, Zhen Song, Hongye Cheng, Lifang Chen, Zhiwen Qi

{"title":"Solvent-enabled intensification of liquid–liquid heterogeneous catalysis exemplified by direct hydration of cyclohexene","authors":"Zhixiang Zhang, Xiang Zhang, Ke Wang, Kunchi Xie, Shu Wang, Zhen Song, Hongye Cheng, Lifang Chen, Zhiwen Qi","doi":"10.1002/aic.18698","DOIUrl":"https://doi.org/10.1002/aic.18698","url":null,"abstract":"A strategy of adding solvents to adjust liquid–liquid equilibrium for intensifying liquid–liquid heterogeneous catalytic reactions is presented. A systematic framework involving computational and experimental procedures is proposed for solvent screening and exemplified by the direct hydration of cyclohexene. The solvents that are stable, nonreactive, inert to catalyst, and easily recovered are first filtered out. Besides, two tailored key performance indicators are defined and computed to find the solvents that can promote mutual solubility of reactants and reaction conversion. Potential solvents are sent to test their effects on product yield via experiment. m-Cresol is found to have the highest cyclohexanol yield of 47.5% and its explicit roles for enhancing the reaction is revealed by rigorous liquid–liquid equilibrium. The mechanism of why the resulted solvents can intensify the reaction is theoretically explored. By a comparative study, an additional heuristic is found to serve for expediting solvent screening.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 3","pages":""},"PeriodicalIF":3.5,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143362342","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

Insight into the synergetic solvent effect of H2O-ethanol on the adiponitrile hydrogenation 水-乙醇在己二腈加氢反应中的协同溶剂效应

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2024-12-06 DOI: 10.1002/aic.18677

Le Zhou, Xin Zhang, Yu Han, Xin Li, Ze-Quan Zeng, Hai-Kui Zou, Yong Luo

{"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":"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 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.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 3","pages":""},"PeriodicalIF":3.5,"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}

引用次数: 0

Weakening origin of hydrogen bond in ionic liquid at the electrified interface 离子液体中带电界面处氢键的弱化成因

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2024-12-06 DOI: 10.1002/aic.18660

Junfeng Lu, Tinglan Sun, Yumiao Lu, Hongyan He, Yanlei Wang

引用次数: 0

Modular chem-bio upcycling of waste poly(ethylene terephthalate) to glycolic acid and 2,4-pyridine dicarboxylic acid 废弃聚对苯二甲酸乙酯的模块化化学生物升级回收制乙醇酸和2,4-吡啶二羧酸

IF 3.5 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

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 采用环形结构和进料法设计的管中管微反应器无缝放大：微混合、停留时间分布和传热

IF 3.5 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":"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 (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.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 3","pages":""},"PeriodicalIF":3.5,"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

Characterizing binary droplet collisions of power-law fluids 幂律流体二元液滴碰撞的表征

IF 3.5 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

引用次数: 0

Experimental study of bubble breakup in water and solid suspension by using the image-based method 基于图像方法的水和固体悬浮液中气泡破碎实验研究

IF 3.5 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":"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 (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.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 3","pages":""},"PeriodicalIF":3.5,"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 高效电催化氮还原金属有机框架的筛选

IF 3.5 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":"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 N2 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 N2 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 in situ Diffuse Reflectance Infrared Fourier Transform (DRIFT) analysis with theoretical calculation, we found that N2 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 NH3 yield rate of 74.55 ± 1 μg h−1 mgcat−1 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":"71 3","pages":""},"PeriodicalIF":3.5,"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