AIChE Journal最新文献

{"title":"Enhancing HER catalyst screening of modified MXenes through DFT and machine learning integration","authors":"Hui Xu, Wenhao Lv, Shaojie Yang, Shuna Yang, Yawei Liu, Feng Huo","doi":"10.1002/aic.18618","DOIUrl":"https://doi.org/10.1002/aic.18618","url":null,"abstract":"MXenes doped with non-metallic and transition metal elements exhibit remarkable potential as catalysts in the hydrogen energy. Nonetheless, efficiently identifying viable materials from a vast array of candidates remains a formidable challenge. Here, we conducted density functional theory (DFT) calculations to obtain the hydrogen adsorption free energy (<span data-altimg=\"/cms/asset/55280795-4fbc-497a-95da-89a1c82bc57a/aic18618-math-0001.png\"></span><mjx-container ctxtmenu_counter=\"3\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" role=\"application\" sre-explorer- style=\"font-size: 103%; position: relative;\" tabindex=\"0\"><mjx-math aria-hidden=\"true\" location=\"graphic/aic18618-math-0001.png\"><mjx-semantics><mjx-mrow data-semantic-children=\"3\" data-semantic-content=\"0\" data-semantic- data-semantic-role=\"prefix operator\" data-semantic-speech=\"increment upper G Subscript normal upper H\" data-semantic-type=\"prefixop\"><mjx-mo data-semantic- data-semantic-operator=\"prefixop,∆\" data-semantic-parent=\"4\" data-semantic-role=\"prefix operator\" data-semantic-type=\"operator\" rspace=\"3\" space=\"3\"><mjx-c></mjx-c></mjx-mo><mjx-msub data-semantic-children=\"1,2\" data-semantic- data-semantic-parent=\"4\" data-semantic-role=\"latinletter\" data-semantic-type=\"subscript\"><mjx-mi data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"italic\" data-semantic- data-semantic-parent=\"3\" data-semantic-role=\"latinletter\" data-semantic-type=\"identifier\"><mjx-c></mjx-c></mjx-mi><mjx-script style=\"vertical-align: -0.15em;\"><mjx-mi data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"3\" data-semantic-role=\"latinletter\" data-semantic-type=\"identifier\" size=\"s\"><mjx-c></mjx-c></mjx-mi></mjx-script></mjx-msub></mjx-mrow></mjx-semantics></mjx-math><mjx-assistive-mml display=\"inline\" unselectable=\"on\"><math altimg=\"urn:x-wiley:00011541:media:aic18618:aic18618-math-0001\" display=\"inline\" location=\"graphic/aic18618-math-0001.png\" overflow=\"scroll\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><semantics><mrow data-semantic-=\"\" data-semantic-children=\"3\" data-semantic-content=\"0\" data-semantic-role=\"prefix operator\" data-semantic-speech=\"increment upper G Subscript normal upper H\" data-semantic-type=\"prefixop\"><mo data-semantic-=\"\" data-semantic-operator=\"prefixop,∆\" data-semantic-parent=\"4\" data-semantic-role=\"prefix operator\" data-semantic-type=\"operator\">∆</mo><msub data-semantic-=\"\" data-semantic-children=\"1,2\" data-semantic-parent=\"4\" data-semantic-role=\"latinletter\" data-semantic-type=\"subscript\"><mi data-semantic-=\"\" data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"italic\" data-semantic-parent=\"3\" data-semantic-role=\"latinletter\" data-semantic-type=\"identifier\">G</mi><mi data-semantic-=\"\" data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"normal\" data-semantic-parent=\"3\" data-semantic-role=\"latinletter\" data-semantic-type=\"identifier\" mathvariant=\"normal\">H</mi></msub></mrow>$$ Delta {G}_{mathrm{H}} $$</a","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"57 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329719","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":"Charged layered double hydroxides with sub-nanometer channel for efficient monovalent cation sieving","authors":"Xin Zhang, Wanjie Song, Lixuan Sun, Cui Yang, Mingyue Wu, Bin Wu, Xiaolin Ge, Rongqiang Fu, Zhaoming Liu, Tongwen Xu","doi":"10.1002/aic.18571","DOIUrl":"https://doi.org/10.1002/aic.18571","url":null,"abstract":"The design of monovalent cation selective membranes for precise separation requires a comprehensive understanding of the geometry and chemical environment of the transport channels. Here, a charged cation transfer channel with sub-1-nanometer is constructed by layer-by-layer self-assembly of layered double hydroxides. To effectively improve the separation performance, the thickness of the membrane and the separation performance test temperature are explored. The enhanced size confinement effect and wall Coulomb interaction lead to better migration of K⁺/Na⁺ than of Li⁺, which allows the selectivity of K⁺/Li⁺ or Na⁺/Li⁺ as 5.7 and 4.0 for 3 μm thickness at 293 K, respectively. Molecular dynamics simulation and density functional theory calculation further illustrate the root cause of different transfer rates and high selectivity due to the different Coulomb effects between various cations and channel walls. These results provide insight into the ion transfer behavior and separation mechanism in a charged confinement regime.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"27 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325815","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":"Activity of bimetallic PdIn/CeO2 catalysts tuned by thermal reduction for improving methanol synthesis via CO2 hydrogenation","authors":"Yan Shao, Bohong Wu, Boya Qiu, Rongsheng Cai, Cui Quan, Ningbo Gao, Feng Zeng, Xiaolei Fan, Huanhao Chen","doi":"10.1002/aic.18617","DOIUrl":"https://doi.org/10.1002/aic.18617","url":null,"abstract":"Synergistic Pd–In₂O₃ catalysts are promising candidates for producing methanol via CO₂ hydrogenation, and the metal phases in them can be tuned by thermal reduction treatment affecting the catalytic activity significantly. This work presents a comprehensive investigation to gain an insight into the effect of thermal reduction temperature on the variation and interaction of Pd and In₂O₃ phases supported on CeO₂ (viz., PdIn/CeO₂) and their correlations with CO₂ hydrogenation toward methanol synthesis. The findings show that Pd/In-rich PdIn alloys and In₂O₃ with relatively strong interaction are key phases (by reducing the PdIn/CeO₂ at 300°C) for promoting methanol formation, leading to a high selectivity to methanol at 78.9% and space–time yield (STY) of 3.6 g_CH3OH g_PdIn⁻¹ h⁻¹. A further increase in reduction temperature (from 300 to 500°C) promoted the formation of homogenized PdIn intermetallic alloys with significantly poor ability for H₂ dissociation and CO₂ activation, and hence poor methanol yield.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"51 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142317767","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":"VOF-DEM numerical study of mesoscale bubble dynamics in the gas-liquid-solid three-phase flow system","authors":"Hongshi Yu,&nbsp;Shiliang Yang,&nbsp;Hua Wang","doi":"10.1002/aic.18614","DOIUrl":"10.1002/aic.18614","url":null,"abstract":"<p>Mesoscale bubble dynamics play a critical role in governing the overall performance of gas-liquid-solid systems. In this study, the volume of fluid method coupled with a discrete element method is utilized to scrutinize the mesoscale bubble dynamics within a gas-liquid-solid system featuring a dense particle bed. The results reveal that the squeezing effect of the particle bed induces a bubble pairs regime, which causes the bubble collision, coalescence and breakup, thereby generating daughter bubbles. Additionally, the combined influence of large size, flattened shape, off-center collisions and the exists of particles facilitate bubble wakes to transform from closed into asymmetrical open patterns, further causing particles released from bubble wakes. Finally, the high-speed region is predominantly confined to the bubble wake area, resulting in a diminished overall stirring capability compared with two-phase system. The insights obtained from this study shed valuable light on bubble behaviors within gas-liquid-solid systems, offering implications for further study in this field.</p>","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"70 12","pages":""},"PeriodicalIF":3.5,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321397","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":"Adaptive safe reinforcement learning-enabled optimization of battery fast-charging protocols","authors":"Myisha A. Chowdhury, Saif S.S. Al-Wahaibi, Qiugang Lu","doi":"10.1002/aic.18605","DOIUrl":"https://doi.org/10.1002/aic.18605","url":null,"abstract":"Optimizing charging protocols is critical for reducing battery charging time and decelerating battery degradation in applications such as electric vehicles. Recently, reinforcement learning (RL) methods have been adopted for such purposes. However, RL-based methods may not ensure system (safety) constraints, which can cause irreversible damages to batteries and reduce their lifetime. To this end, this article proposes an adaptive and safe RL framework to optimize fast charging strategies while respecting safety constraints with a high probability. In our method, any unsafe action that the RL agent decides will be projected into a safety region by solving a constrained optimization problem. The safety region is constructed using adaptive Gaussian process (GP) models, consisting of static and dynamic GPs, that learn from online experience to adaptively account for any changes in battery dynamics. Simulation results show that our method can charge the batteries rapidly with constraint satisfaction under varying operating conditions.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"216 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142317794","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 CFD-PBM-ANN framework to simulate the liquid–liquid two-phase flow in a pulsed column","authors":"Bo Wang, Siyuan Ma, Han Zhou, Qiang Zheng, Wenjie Lan, Shan Jing, Shaowei Li","doi":"10.1002/aic.18612","DOIUrl":"https://doi.org/10.1002/aic.18612","url":null,"abstract":"CFD-PBM numerical simulation is a powerful tool in the research of droplet swarm behavior. In this work, an artificial neural network (ANN) based droplet breakage frequency function is established based on the directly measured data from our previous studies. Then, the weights and biases of ANN are embedded into the CFD-PBM code in the form of matrices and vectors. For the first time, a CFD-PBM-ANN simulation framework is established. Simulation results are in good agreement with the experimental data under different operation conditions. The cumulative droplet size distribution decreases with the increase of interfacial tension and pulse intensity. It is also found by the simulation that the droplet breakage frequency is relatively high at the edge of disc and doughnut plate, which is accordant with the distribution of turbulent energy dissipation and velocity gradient.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"31 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142317765","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":"Cracking the physical insight of power law models: Bridging the gap between macroscopic kinetics and surface coverages","authors":"Fernando Vega‐Ramon, Alexander W. Rogers, Christopher Hardacre, Dongda Zhang","doi":"10.1002/aic.18616","DOIUrl":"https://doi.org/10.1002/aic.18616","url":null,"abstract":"We propose a methodological framework to quantify the relative abundance of key surface intermediates via analysis of the macroscopic intrinsic kinetic characteristics of gas‐phase data. At the core of this approach is the development of analytical expressions, which link reaction orders and activation energies in macroscopic power law models to the fractional coverage of the non‐observable intermediates. Through the design of an advanced parameter estimation methodology, these relationships were further exploited to develop thermodynamically consistent and mechanistic‐based power law models which could capture the evolution of surface occupancy profiles along the reactor length. The developed framework was tested through in‐silico water gas shift reaction case‐studies; the results indicate the robustness of the approach and the mechanistic insight that can be gained from its application. The methodology proposed in this study could thus be of general value to assist in reaction mechanism analysis, identification of key surface intermediates, and reactor optimization.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"1 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142276742","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":"Molecular layer deposition of polyhydroquinone thin films for Li-ion battery applications","authors":"Nikhila C. Paranamana,&nbsp;Amit K. Datta,&nbsp;Quinton K. Wyatt,&nbsp;Ryan C. Gettler,&nbsp;Andreas Werbrouck,&nbsp;Matthias J. Young","doi":"10.1002/aic.18613","DOIUrl":"10.1002/aic.18613","url":null,"abstract":"<p>Many next-generation materials for Li-ion batteries are limited by material instabilities. To stabilize these materials, ultrathin, protective coatings are needed that conduct both lithium ions and electrons. Here, we demonstrate a hybrid chemistry combining molecular layer deposition (MLD) of trimethylaluminum (TMA) and p-hydroquinone (HQ) with oxidative molecular layer deposition (oMLD) of molybdenum pentachloride (MoCl₅) and HQ to enable vapor-phase molecular layer growth of poly(p-hydroquinone) (PHQ)—a mixed electron and lithium ion conducting polymer. We employ quartz crystal microbalance (QCM) studies to understand the chemical mechanism and demonstrate controlled linear growth with a 0.5 nm/cycle growth rate. Spectroscopic characterization indicates that this hybrid MLD/oMLD chemistry polymerizes surface HQ monomers from the TMA-HQ chemistry to produce PHQ. The polymerization to PHQ improves air stability over MLD TMA-HQ films without crosslinking. Electrochemical measurements on hybrid MLD/oMLD films indicate electronic conductivity of ~10⁻⁹ S/cm and a Li-ion conductivity of ~10⁻⁴ S/cm. While these coatings show promise for Li-ion battery applications, this work focuses on establishing the coating chemistry and future studies are needed to examine the stability, structure, and cycling performance of these coatings in full Li-ion cells.</p>","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"70 12","pages":""},"PeriodicalIF":3.5,"publicationDate":"2024-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142276743","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":"Sol–gel pore-confined strategy to synthesize atomically dispersed metal sites for enhanced CO2 electroreduction","authors":"Youzhi Li, Dashuai Wang, Hualong Liu, Yanran Bao, Xuesong Zhao, Chen Sun, Zhongjian Li, Lecheng Lei, Yang Hou, Bin Yang","doi":"10.1002/aic.18587","DOIUrl":"https://doi.org/10.1002/aic.18587","url":null,"abstract":"Excavating highly efficient and cost-effective non-noble metal single-atom catalysts for electrocatalytic CO₂ reduction reaction (CO₂RR) is of paramount significance. However, the general and universal strategy for designing atomically dispersed metals as accessible active sites is still in its infancy. Herein, we reported a general sol–gel pore-confined strategy for preparing a series of isolated transition metal single atoms (Fe/Co/Ni/Cu) anchored on nitrogen-doped carbon matrix. Benefiting from synergistic effect of M-N₄ coordination and neighboring N doping, the Fe-N₄-C catalyst exhibited superior capability with a Faradaic efficiency of 96.9%, achieving highly stable electrocatalytic activity for more than 20 h. Density functional theory (DFT) calculations further revealed the changes in the d_xz orbital of Fe, with a decrease in the out-of-plane component. Thus, a lower free energy barrier (ΔG) in thermodynamic pathway and the accelerated proton transfer to *COOH in kinetic pathway both enhanced electrocatalytic process.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"6 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142247062","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":"Why insulin aspart and insulin degludec exhibit distinct release mechanisms","authors":"Zhuo Lin Li, Yun Hao Feng, Jie Jiao, Xin Yu Ju, Lingyun Yu, Guo Liang Zhang, Ruixing Yu, Bo Zhi Chen, Xin Dong Guo","doi":"10.1002/aic.18609","DOIUrl":"https://doi.org/10.1002/aic.18609","url":null,"abstract":"Exploring the molecular mechanisms underlying insulin analogs is important for protein engineering to design innovative drug proteins. Insulin aspart (IAsp) and insulin degludec (IDeg) are representative examples of insulin analogs with distinct release profiles synthesized by targeted mutagenesis in protein engineering. Despite their importance in diabetes treatment, there remains a gap in our understanding of the molecular basis for their differential release mechanisms. In this study, ordinary molecular dynamics simulation and steered molecular dynamics are utilized to investigate the structural stability, solubility analysis, and monomer interactions of these insulins, with the aim to explain the mesoscale differences between the two insulin release mechanisms. Simulation findings have further been validated through experimental verification, shedding light on the intricate mechanisms underlying insulin release and providing valuable insights into pharmaceutical implications and potential advancements in the design of insulin therapy.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"23 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142247057","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}