AIChE Journal最新文献

{"title":"Mechanistically guided kinetic analysis of G3-catalyzed ROMP for the precision synthesis of cyclic olefin polymers","authors":"Tian-Tian Wang, Jiang Wang, Yu-Cai Cao, Zheng-Hong Luo, Yin-Ning Zhou","doi":"10.1002/aic.18794","DOIUrl":"https://doi.org/10.1002/aic.18794","url":null,"abstract":"Grubbs third-generation catalyst (G3) in ring-opening metathesis polymerization (ROMP) shows unique kinetic behaviors and ligand-addition enabled metathesis activity regulation, while several kinetic features have not been fully revealed. In this work, a thorough kinetic analysis of G3-catalyzed ROMP, for the first time, is carried out via method-of-moments-based numerical simulation and experiments. A generalized kinetic model considering possible metathesis reactions is developed and a stable-deviation-analysis strategy is proposed to estimate the rate coefficient for cyclic monomer propagation. Simulation results confirm that the number of active sites for propagation is independent of the G3 concentration, resulting in the zeroth-order kinetic dependence. Adding external pyridine ligand accelerates the consumption of G3 through a coordination competition, and a positive relation between external ligand concentration and the rate for reaching the steady-state condition is disclosed. The interchain metathesis reaction increases molar mass dispersity by increasing the weight-average molar mass, which can be effectively mitigated by adding a strongly coordinating external ligand. Analysis of ring-chain competition in intrachain backbiting suggests that increasing the initial concentration of reactants can enhance the selectivity for producing linear polymers. This study provides a comprehensive understanding of the mechanism-governed ROMP kinetic behaviors and aids in the precision synthesis of cyclic olefin polymers.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"1 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143495190","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}

{"title":"Coalescence dynamics of nanofluid droplets in an expansion chamber structure microchannel","authors":"Daofan Ma, Yanjun Deng, Guangwei Wang, Youguang Ma, Chunying Zhu, Xiangyang Tang","doi":"10.1002/aic.18796","DOIUrl":"https://doi.org/10.1002/aic.18796","url":null,"abstract":"Nanofluid droplets have considerable applications in industry. In this study, the coalescence dynamics of nanofluid droplets in an expansion chamber structure microchannel were visually investigated; the shape and liquid bridge evolutions of droplets were studied systematically. Five droplet coalescence flow patterns were observed: non-contact, double coalescence, cascade coalescence, compact slug flow, and jetting flow regimes. Due to the adsorption of nanoparticles on the fluid interface, a solidified layer is formed, which restrains the curvature change of the liquid bridge, slowing down the shrinkage of the liquid bridge. The evolution of the liquid bridge neck width with time could be divided into two stages: the dispersed phase control stage and the continuous phase control stage. The nanoparticles could affect markedly the dispersed phase control stage, while having less effect on the continuous control stage.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"10 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486049","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}

{"title":"Isobutylene polymerization in gas-liquid-solid circulating mini-fluidized bed","authors":"Yan Sun, Yongli Ma, Taiji Wang, Hao Guo, Mingyan Liu","doi":"10.1002/aic.18806","DOIUrl":"https://doi.org/10.1002/aic.18806","url":null,"abstract":"The polymerization of isobutylene is an important chemical reaction process. In order to overcome the shortcomings of existing industrial fixed-bed reactors in application, a new gas-liquid-solid circulating mini-fluidized bed reactor with an inner diameter of 10 mm is developed. The influences of operating conditions, solvents, and reactant properties on isobutylene conversion, selectivity, and yield of di-isobutylene were investigated. Compared with fixed-bed reactor, the performance of the reactor was evaluated. The experimental results showed that the highest yield of di-isobutylene was 83.4%. Under the same operating conditions, the conversion rate of isobutylene in the circulating mini-fluidized bed is twice that of the fixed-bed reactor. The reaction time to achieve the same conversion rate is reduced by 2.5 times. The solid particles and bubbles in the circulating mini-fluidized bed not only provide a higher specific surface area but also cause hydrodynamic changes and effectively improve the reactor performance.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"232 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486050","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}

{"title":"Reduction in adsorbent granule dimensionality to strengthen lithium adsorption in low-grade salt lakes","authors":"Jun Chen, Jianguo Yu, Sen Lin","doi":"10.1002/aic.18795","DOIUrl":"https://doi.org/10.1002/aic.18795","url":null,"abstract":"Sluggish internal mass transfer within granulated adsorbents constrains the efficiency of Li⁺ extraction from low-grade salt lakes. In this study, Li⁺ diffusion behavior simulations using finite element analysis indicated that reducing the granule dimensionality enhanced Li⁺ transfer in aluminum-based lithium adsorbents, with ionic strength as the driving force. Hence, low-dimensional aluminum-based adsorbent granules (LD-LDHs) with fast transport channels and highly accessible adsorption sites were directionally prepared via a wet-spinning method. Adsorption kinetics suggested LD-LDHs with reduced internal diffusion resistance achieved equilibrium in less than 30 min, which was significantly shorter than the 36 h required for larger granules prepared by conventional extrusion molding, while maintaining the performance of the encapsulated active components. During continuous lithium extraction from low-grade Qarhan old brine, LD-LDHs reached adsorption saturation in 60 min, with a 1.8-fold increased working capacity, and the desorption solution was of higher quality, favorable for subsequent lithium carbonate production processes.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"14 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486052","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}

{"title":"Hierarchical porous carbon membranes for lean-helium extraction from high-pressure natural gas","authors":"Chi Zhang, Guanran Zhao, Zhi Li, Linfeng Lei, Zhi Xu","doi":"10.1002/aic.18790","DOIUrl":"https://doi.org/10.1002/aic.18790","url":null,"abstract":"Given the scarcity of helium (He) resources, the application of scalable and energy-efficient membrane-mediated separation techniques for helium extraction holds substantial potential; however, few membrane materials have been reported for lean-helium extraction from natural gas feeds (<1000 ppm). Herein, we present a facile strategy for fabricating the carbon molecular sieve (CMS) hollow fiber membranes with a hierarchical porous structure by tailoring the phase inversion behaviors of blend polymeric precursors and engineering the pyrolysis protocol. The CMS membranes composed of highly homogenized and inconsecutive macropores and size-constrained ultramicropores in synergy exhibited superior separation performance in the separation of He/CH₄. For instance, CA-3-700 membranes showed a He/CH₄ ideal selectivity of 1427 and He permeability of 521 barrer. In addition, the membrane presented superior mixed gas separation performances under simulated helium-contained high-pressure natural gas at hundred ppm levels (400–1300 ppm), while demonstrating long-term continuous stability (from a quinary mixture of He/CH₄/N₂/C₂H₆/CO₂) over 120 h.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"31 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477875","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}

{"title":"Machine learning knowledge-driven Pt-based catalyst design library development for selective oxidation of  polyalcohol","authors":"Xin Zhou, Honghua Qin, Zhibo Zhang, Mengzhen Zhu, Hao Yan, Xiang Feng, Lianying Wu, Chaohe Yang, De Chen","doi":"10.1002/aic.18793","DOIUrl":"https://doi.org/10.1002/aic.18793","url":null,"abstract":"Laborious first-principles calculations and trial-and-error experimentation often fail to meet the demands of rational and efficient catalyst development. This paper introduces an approach that integrates costly labeled data with process reaction mechanisms for catalyst formulation in the high-value conversion of glycerol. We developed an innovative system framework, POCOM, which simultaneously generates the optimal process superstructure and operating conditions to achieve peak conversion rates and desired product specifications. We synergistically combined reaction mechanisms, machine learning, process optimization, and data generation techniques, encapsulating them into a cutting-edge software system specifically designed for catalyst formulation in glycerol selective oxidation. In this process, we identified a previously unreported Pt-ZnO catalyst formulation. The catalyst, with 1.8 wt% Pt and 0.4 wt% ZnO, demonstrated exceptional performance, achieving a glycerol conversion rate of 88% and a glyceric acid selectivity of 80%. This study offers groundbreaking insights and robust data support for the rational design of glycerol oxidation catalysts.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"5 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477873","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}

{"title":"CoN4 active sites coupled with low-loading Pt as advanced oxygen electrocatalyst for proton exchange membrane fuel cells","authors":"Chunzhu Bao, Bolong Yang, Lingling Zhai, Zhonghua Xiang","doi":"10.1002/aic.18763","DOIUrl":"https://doi.org/10.1002/aic.18763","url":null,"abstract":"Proton exchange membrane fuel cells (PEMFCs) are regarded as a cornerstone of next-generation energy conversion technologies due to zero emission and high energy efficiency. However, the high cost and scarcity of conventional Pt-based electrocatalysts hinder its commercialization. Herein, we successfully developed a platinum and cobalt bimetallic covalent organic polymer (Pt-CoNC) electrocatalyst with low Pt loading (0.96 wt%) for the oxygen reduction reaction (ORR) by integrating Pt sites with carbon materials featuring Co-N₄ active centers. This unique structural design not only effectively mitigates the high cost associated with Pt-based catalysts but also notably boosts the activity and stability of non-precious metal catalysts. The results verified that the half-wave potential of Pt-CoNC in the acidic ORR was increased by 105 mV as compared with pure cobalt phthalocyanine-based covalent organic polymer (COP-Co). Furthermore, the as-assembled PEMFC device achieved a peak power density of 1.14 W cm⁻² under an H₂-O₂ atmosphere, which is comparable to commercialized 20% Pt/C catalysts.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"8 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486083","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}

{"title":"Carbon matrix anchored Rh1Co single-atom alloy catalyst for robust hydroformylation with wide substrate generality","authors":"Xin Zhang, Xuelu Ma, Hsiao-Chien Chen, Shu Tao, Da Yang, Yingying Liu, Wenwen Gao, Guangxun Sun, Tingyu Chang, Zhidong Wang, Bin Liu, Yongming Chai, Zhi Liu, Yuan Pan","doi":"10.1002/aic.18798","DOIUrl":"https://doi.org/10.1002/aic.18798","url":null,"abstract":"A novel Rh₁Co single-atom alloy (SAA) catalyst, in which Rh species are atomically dispersed on Co nanoparticles that are anchored by N-doped carbon (N-C) matrix for hydroformylation of olefins. The Rh₁Co SAA/N-C catalyst exhibits high activity towards the hydroformylation of 1-hexene, achieving both nearly 100% conversion and selectivity as well as good cycle stability. It also shows extremely wide substrate generality for at least 17 different types of olefins. A synergistic catalytic mechanism of the Rh₁Co SAA/N-C catalyst was discovered that H₂ is dissociated on Co sites and Co-H species are facilitated to be generated, CO is also adsorbed and inserted on Co sites that promote the C-C coupling, while the Rh-Co dual sites are beneficial to the co-adsorption of 1-hexene. Theoretical calculations reveal the Rh₁Co SAA/N-C catalyst shows a lower rate-determining energy barrier of CO insertion due to the optimized charge distribution of the precursor of CO insertion at Co sites.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"35 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477872","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}

{"title":"A functionalized zwitterionic PAN fiber membrane with enhanced antifouling for stable emulsion separation","authors":"Hao Chen, Haonan Wu, Yuting Dai, Dongfan Liu, Dongya Yang, Fengxian Qiu, Tao Zhang","doi":"10.1002/aic.18791","DOIUrl":"https://doi.org/10.1002/aic.18791","url":null,"abstract":"Membrane fouling significantly hinders the efficacy of membrane separation engineering in treating oily wastewater. Here, a combined internal and external modification strategy was presented to fabricate a functionalized zwitterionic polyacrylonitrile (PAN) fiber membrane with enhanced antifouling properties for stable emulsion separation. Internally, a zwitterionic polymer betaine methacrylate sulfonate (SBMA) was incorporated into the PAN fiber network to improve hydration, establishing hydration layer barriers to confer fouling resistance. Externally, fluorocarbon small molecules were grafted to create low-surface-energy microregions, imparting the “fouling-release” properties. Due to its fouling resistance and release properties, the resulting membrane (F-PAN@SBMA M) exhibited excellent underwater oil repellency, ultra-low oil adhesion, achieving high separation fluxes (>2000 L m⁻² h⁻¹) and efficiencies (>99.1%) for multiple oil-in-water emulsions. Enhanced antifouling properties and high flux recovery rates promoted stable separation performance and membrane regeneration. This modification strategy offers a promising pathway for developing effective membrane separation materials in industrial wastewater treatment.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"34 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477874","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}

{"title":"Classical density functional theory as a fast and accurate method for adsorption property prediction of porous materials","authors":"Vincent Dufour-Décieux, Philipp Rehner, Johannes Schilling, Elias Moubarak, Joachim Gross, André Bardow","doi":"10.1002/aic.18779","DOIUrl":"https://doi.org/10.1002/aic.18779","url":null,"abstract":"Physical adsorption is crucial in many industrial processes, prompting researchers to develop new materials for energy-efficient processes. Porous adsorbents are particularly promising due to their design flexibility, and computational screening has accelerated the search for optimal materials. Recently, classical density functional theory (cDFT) has emerged as a faster screening alternative to state-of-the-art computational methods. However, its predictions have not been extensively validated, especially for materials involving strong Coulombic interactions. This article validates cDFT by calculating adsorption properties for over 500 Metal-Organic Frameworks with three adsorbates <span data-altimg=\"/cms/asset/2b4ac214-7081-4b58-89b7-95daa2eeb1ba/aic18779-math-0001.png\"></span><mjx-container ctxtmenu_counter=\"24\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" role=\"application\" sre-explorer- style=\"font-size: 103%; position: relative;\" tabindex=\"0\"><mjx-math aria-hidden=\"true\" location=\"graphic/aic18779-math-0001.png\"><mjx-semantics><mjx-mrow data-semantic-children=\"0,3\" data-semantic-content=\"0\" data-semantic- data-semantic-role=\"startpunct\" data-semantic-speech=\"left parenthesis CH Subscript 4 Baseline\" data-semantic-type=\"punctuated\"><mjx-mo data-semantic- data-semantic-operator=\"punctuated\" data-semantic-parent=\"4\" data-semantic-role=\"openfence\" data-semantic-type=\"punctuation\" style=\"margin-left: 0.056em; margin-right: 0.056em;\"><mjx-c></mjx-c></mjx-mo><mjx-msub data-semantic-children=\"1,2\" data-semantic- data-semantic-parent=\"4\" data-semantic-role=\"unknown\" data-semantic-type=\"subscript\"><mjx-mrow><mjx-mtext data-semantic-annotation=\"clearspeak:unit\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"3\" data-semantic-role=\"unknown\" data-semantic-type=\"text\"><mjx-c></mjx-c><mjx-c></mjx-c></mjx-mtext></mjx-mrow><mjx-script style=\"vertical-align: -0.15em;\"><mjx-mrow size=\"s\"><mjx-mn data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"3\" data-semantic-role=\"integer\" data-semantic-type=\"number\"><mjx-c></mjx-c></mjx-mn></mjx-mrow></mjx-script></mjx-msub></mjx-mrow></mjx-semantics></mjx-math><mjx-assistive-mml display=\"inline\" unselectable=\"on\"><math altimg=\"urn:x-wiley:00011541:media:aic18779:aic18779-math-0001\" display=\"inline\" location=\"graphic/aic18779-math-0001.png\" overflow=\"scroll\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><semantics><mrow data-semantic-=\"\" data-semantic-children=\"0,3\" data-semantic-content=\"0\" data-semantic-role=\"startpunct\" data-semantic-speech=\"left parenthesis CH Subscript 4 Baseline\" data-semantic-type=\"punctuated\"><mo data-semantic-=\"\" data-semantic-operator=\"punctuated\" data-semantic-parent=\"4\" data-semantic-role=\"openfence\" data-semantic-type=\"punctuation\" stretchy=\"false\">(</mo><msub data-semantic-=\"\" data-semantic-children=\"1,2\" data-semantic-parent=\"4\" data-semantic-role=\"unknown\" data-semantic-type=\"subscript\"><mrow><mtext data-semantic-=\"\" data-sem","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"62 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143462946","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}