AIChE Journal最新文献

{"title":"Photoreforming of waste plastic by B-doped carbon nitride nanotube: Atomic-level modulation and mechanism insights","authors":"Zongyang Ya, Lei Tang, Dong Xu, Hua Wang, Shengbo Zhang","doi":"10.1002/aic.18740","DOIUrl":"https://doi.org/10.1002/aic.18740","url":null,"abstract":"Photoreforming waste plastics into valuable products is a promising approach, but it requires efficient, eco-friendly photocatalysts and a deeper understanding of catalytic mechanism. We have developed a B-doped g-C₃N₄ nanotube catalyst with well-defined structure for photoreforming poly(ethylene terephthalate) (PET) into valuable chemicals and H₂. This catalyst achieved a H₂ evolution rate of 3240 μmol g_catal⁻¹ h⁻¹, outperforming previous cadmium-free catalysts. It also oxidized PET to higher-value organic acids via a hole oxidation mechanism. Experimental and theoretical calculations showed that B atom doping not only greatly increased the catalyst's active sites, but also significantly accelerated the electron–hole separation and transfer rate, optimized the adsorption and activation behavior of the substrate. Using concentrated sunlight, we achieved a H₂ evolution rate of 475 μmol g_catal⁻¹ h⁻¹ for real-world PET in seawater. Techno-economic analysis suggests processing 50,000 tons of waste plastic annually could yield a profit of $7.45 million.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"60 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143021067","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":"Robust bilayer Ni–Sb–SnO2 combined with continuous flow stacked electrolyzer for electrochemical ozone production","authors":"Xiaosa Wang, Zaixiang Xu, Mengmeng Lu, Lei Ding, Huaijie Shi, Jiahui He, Haoqiang Cao, Yunyi Cao, Xing Zhong, Jianguo Wang","doi":"10.1002/aic.18711","DOIUrl":"https://doi.org/10.1002/aic.18711","url":null,"abstract":"Ni–Sb–SnO₂ (NATO) has demonstrated significant practical advantages for electrochemical ozone production (EOP) and wastewater treatment. However, its limited lifetime poses challenges for environmental applications. In this study, bilayer electrocatalysts (NATO/C-ATO) with an inner layer doped with carbon material were synthesized by electrodeposition combined with multiple quenching processes. It exhibited excellent EOP activity and stability under acidic conditions, achieving a current efficiency of 34.4% and an accelerated lifetime of 121 h. Additionally, a continuous flow stacked electrolyzer was designed via a combination of flow field simulation and experimental validation. Compared to conventional batch reactors, this design intensifies the mass and heat transfer processes in operation, enabling the production of ozonated water at a high concentration of 36.6 mg h⁻¹ and the rapid degradation of organic pollutants. This work provides new insights into the design of efficient electrocatalysts and application equipment for advanced oxidation processes.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"82 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143020932","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":"Brownian bridges for contained random walks","authors":"George Curtis, Doraiswami Ramkrishna, Vivek Narsimhan","doi":"10.1002/aic.18658","DOIUrl":"https://doi.org/10.1002/aic.18658","url":null,"abstract":"Using linear operator techniques, we demonstrate an efficient method for investigating rare events in stochastic processes. Specifically, we examine contained trajectories, which are continuous random walks that only leave a specified region of phase space after a set period of time <span data-altimg=\"/cms/asset/a0469ccf-17af-4b97-93c8-3c46f35fdc73/aic18658-math-0001.png\"></span><mjx-container ctxtmenu_counter=\"250\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" role=\"application\" sre-explorer- style=\"font-size: 103%; position: relative;\" tabindex=\"0\"><mjx-math aria-hidden=\"true\" location=\"graphic/aic18658-math-0001.png\"><mjx-semantics><mjx-mrow><mjx-mi data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"italic\" data-semantic- data-semantic-role=\"latinletter\" data-semantic-speech=\"upper T\" data-semantic-type=\"identifier\"><mjx-c></mjx-c></mjx-mi></mjx-mrow></mjx-semantics></mjx-math><mjx-assistive-mml display=\"inline\" unselectable=\"on\"><math altimg=\"urn:x-wiley:00011541:media:aic18658:aic18658-math-0001\" display=\"inline\" location=\"graphic/aic18658-math-0001.png\" overflow=\"scroll\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><semantics><mrow><mi data-semantic-=\"\" data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"italic\" data-semantic-role=\"latinletter\" data-semantic-speech=\"upper T\" data-semantic-type=\"identifier\">T</mi></mrow>$$ T $$</annotation></semantics></math></mjx-assistive-mml></mjx-container>. We show that such trajectories can be efficiently generated through the use of a Brownian Bridge, derived via the solution to the Backward Fokker–Planck (BFP) equation. Using linear operator techniques, we place the BFP operator in self-adjoint form and show that in the asymptotic limit <span data-altimg=\"/cms/asset/128708a3-6ffd-4c86-b14d-78bdfa6190b3/aic18658-math-0002.png\"></span><mjx-container ctxtmenu_counter=\"251\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" role=\"application\" sre-explorer- style=\"font-size: 103%; position: relative;\" tabindex=\"0\"><mjx-math aria-hidden=\"true\" location=\"graphic/aic18658-math-0002.png\"><mjx-semantics><mjx-mrow data-semantic-children=\"0,2\" data-semantic-content=\"1\" data-semantic- data-semantic-role=\"inequality\" data-semantic-speech=\"upper T much greater than 1\" data-semantic-type=\"relseq\"><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-mo data-semantic- data-semantic-operator=\"relseq,≫\" data-semantic-parent=\"3\" data-semantic-role=\"inequality\" data-semantic-type=\"relation\" rspace=\"5\" space=\"5\"><mjx-c></mjx-c></mjx-mo><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-semantics></mjx-math><mjx-assistive-mml display=\"inline\" unselectable=\"on\"><math altimg=\"urn:x-wiley:00011541:med","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"5 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142990523","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":"Unveiling the role of mixing in [Fe(CN)6]4− defects and Na content for preparing NaxMn[Fe(CN)6]y · nH2O via microreactor","authors":"Hao‐Tian Tong, Shi‐Xiao Wei, Yan‐Jiang Liu, Ting‐Liang Xie, Shuang‐Feng Yin","doi":"10.1002/aic.18735","DOIUrl":"https://doi.org/10.1002/aic.18735","url":null,"abstract":"Taking advantage of strong mixing performance in oscillating feedback microreactor (OFM), the manganese hexacyanoferrates (Na<jats:sub><jats:italic>x</jats:italic></jats:sub>Mn[Fe(CN)<jats:sub>6</jats:sub>]<jats:sub><jats:italic>y</jats:italic></jats:sub> · <jats:italic>n</jats:italic>H<jats:sub>2</jats:sub>O, MnHCFs) with low defects and high sodium content were controllably prepared. First, fluid mixing performance in OFM was investigated via dye‐tracer and Villermaux‐Dushman experiments, and the fluid mixing mechanism in OFM was investigated through CFD simulations. Then, MnHCFs were prepared using OFM at different flow rates, and the role of mixing in [Fe(CN)<jats:sub>6</jats:sub>]<jats:sup>4−</jats:sup> vacancies and sodium content during co‐precipitation synthesis of MnHCFs was discussed. The results indicate that an increase in flow rates can increase fluid chaos strength, enhancing the mass transfer process to match the extremely fast reaction rate of MnHCFs, thus preparing MnHCFs with high sodium content and low defects. Relevant electrochemical tests indicate that the MnHCF prepared at the largest throughput (180 mL/min) has the highest initial specific capacity (132 mAh/g at 15 mA/g), minimum electrochemical impedance, and fastest sodium ion transport rate.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"36 3 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142989788","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":"An experimental flow regime map to dynamically structure gas–solid bubbling fluidized beds","authors":"Kaiqiao Wu, Victor Francia, Shuxian Jiang, Marc-Olivier Coppens","doi":"10.1002/aic.18681","DOIUrl":"https://doi.org/10.1002/aic.18681","url":null,"abstract":"Employing oscillatory gas flows to create ordered bubble dynamics in fluidized beds represents a promising approach in reactor design, enhancing efficiency, scalability, and control. This study reports an extensive experimental campaign that identifies the operational regime for structuring Geldart B fluidized beds, introducing a novel pattern recognition algorithm to quantify flow stability and distinguish between “structured” and “unstructured” oscillating beds. The analysis reveals the characteristic features of structured units, including enhanced scalability, homogeneity with narrower bubble size and separation distributions, controlled bubble dynamics, and compartmentalized solid mixing. A nondimensional bubble size, derived from natural frequency and two-phase theory, is proposed to describe the relationship between oscillation characteristics and bubble nucleation. This allows the formulation of a general map to fine-tune oscillating bed operations. The study provides the first comprehensive framework for real-time control of structured beds and sets the stage for further exploration in process intensification and scaling.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"30 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987253","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":"Highly selective lithium extraction by forming ion pairs using 2,9-Dialkyl-1,10-Phenanthrolines and a hydrophobic anion","authors":"Xiao Geng, Jianfeng Zhang, Benzheng Xia, Yuqiu Guan, Qiyu Meng, Zhuojun Jiang, Yifan Zhang, Bharat Prasad Sharma, Yufeng Liang, Liangrong Yang, Zheng Li","doi":"10.1002/aic.18704","DOIUrl":"https://doi.org/10.1002/aic.18704","url":null,"abstract":"Lithium is becoming increasingly important due to its indispensable role in lithium-ion batteries. The direct extraction of lithium from salt lakes, which are a main source of lithium, is challenging due to the coexistence of many interfering alkali and alkaline earth metals. In this work, we report that a synergistic solvent extraction (SSX) system containing 2,9-dialkyl-1,10-phenanthroline and a hydrophobic anion ([NTf₂]⁻) could extract lithium selectively with a high lithium loading capacity from solutions containing both alkali (sodium, potassium) and alkaline earth metals (magnesium, calcium), enabling the direct recovery of lithium from complex salt lakes. The outstanding lithium extraction performance of the SSX system is unprecedented, to the best knowledge of the authors. Through various characterizations and X-ray diffraction of the complex crystals, the extraction mechanism has been revealed. This SSX system will potentially promote more efficient recovery of lithium from salt lakes.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"55 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987642","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":"Integrated learning-based estimation and nonlinear predictive control of an ammonia synthesis reactor","authors":"Amirsalar Bagheri, Thiago Oliveira Cabral, Davood B. Pourkargar","doi":"10.1002/aic.18732","DOIUrl":"https://doi.org/10.1002/aic.18732","url":null,"abstract":"This paper presents an advanced machine learning-based framework designed for predictive modeling, state estimation, and feedback control of ammonia synthesis reactor dynamics. A high-fidelity two-dimensional multiphysics model is employed to generate a comprehensive dataset that captures variable dynamics under various operational conditions. Surrogate long short-term memory neural networks are trained to enable real-time predictions and model-based control. Additionally, a feedforward neural network is developed to estimate the outlet ammonia concentration and hotspot temperature using spatially distributed temperature readings, thereby addressing the challenges associated with real-time concentration and maximum temperature measurements. The machine learning-based predictive modeling and state estimation methods are integrated into a model predictive control architecture to regulate ammonia synthesis. Simulation results demonstrate that the machine learning surrogates accurately represent the nonlinear process dynamics with minimal discrepancy while reducing optimization costs compared to the high-fidelity model, ensuring adaptability and effective guidance of the reactor to desired set points.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"87 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968595","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":"Experimental and molecular thermodynamics insights into separating bicyclic aromatics from diesel oil with ionic liquids","authors":"Qinghua Liu, Minghao Song, Fei Zhao, Chengmin Gui, Jichang Liu, Zhigang Lei, Guoxuan Li","doi":"10.1002/aic.18729","DOIUrl":"https://doi.org/10.1002/aic.18729","url":null,"abstract":"The presence of aromatics in diesel oil significantly reduces its overall quality. Ionic liquids (ILs) combined with extraction technology were proposed to separate three typical bicyclic aromatics and two monocyclic aromatics from diesel oils. The solubility of IL in raffinate phase was introduced as a crucial factor in IL screening process. The accuracy of COSMO-RS model was evaluated using 2942 LLE data points. 1,3-dimethylimidazolium methylsulfate was considered a suitable extractive solvent. The optimal operating conditions were identified by varying the extraction temperatures, solvent ratios, and stages. Heptane was used as a back-extractive solvent to recover IL; the regenerative and humidity stability of selected IL were proven. The separation mechanisms were explored through molecular dynamic simulation and quantum chemistry calculation. Cation plays a more critical role in the extraction process than anion. The extraction performance mainly depends on the π–π stacking and C–H···O H-bond formed between BAHs molecules and IL.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"86 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142961943","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":"Selection of solvents for integrated CO2 absorption and electrochemical reduction systems","authors":"Fragkiskos Tzirakis, Luis A. Diaz, Ioannis Chararas, Daniel Molina Montes de Oca, Zeyu Zhao, Panos Seferlis, Ioannis Tsivintzelis, Athanasios I. Papadopoulos","doi":"10.1002/aic.18734","DOIUrl":"https://doi.org/10.1002/aic.18734","url":null,"abstract":"Solvent-based electrochemical CO₂ reduction (CO₂R) enables the production of chemicals or fuels using CO₂ from a preceding absorption process. Employing previously tested CO₂ capture solvents does not ensure their suitability for either CO₂R or integrated CO₂ absorption-reduction. We propose solvent selection criteria that include the CO₂ solubility, kinetic constant, ionic conductivity, concentration of the bicarbonate, carbamate, and solvent cation in the CO₂-loaded solution, and sustainability indicators. They are implemented for solvent selection (a) from novel, aqueous mixtures of <i>N</i>-methylcyclohexylamine (MCA) with piperazine (PZ), 2-amino-2-methyl-1-propanol (AMP), potassium hydroxide (KOH), and potassium chloride (KCl) and (b) from aqueous monoethanolamine (MEA), AMP, KOH, MCA, and PZ solutions. Versions of a modified Kent-Eisenberg model for strong bases, carbamate, and non-carbamate-forming amine solutions are developed and parameterized through experimental equilibrium measurements. CO₂R experimental results are presented for solutions of KOH and MCA + KOH, as these indicate desired trade-offs for CO₂ absorption and reduction.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"3 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142940176","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":"Deep extractive denitrogenation with Cu-based ionic liquids and mechanistic insights","authors":"Peiwen Wu, Bangzhu Wang, Hongping Li, Shaojie Ma, Linlin Chen, Jixing Liu, Yanhong Chao, Wenshuai Zhu, Chunming Xu","doi":"10.1002/aic.18739","DOIUrl":"https://doi.org/10.1002/aic.18739","url":null,"abstract":"A major challenge in the extractive denitrogenation (EDN) of fuel oils lies in achieving high nitrogen removal efficiency with minimal extractant usage. To address this, a series of Cu-based ionic liquids (ILs) ([Bmim]Cl/CuCl₂-<i>X</i>) with different cation-to-anion ratios were synthesized and characterized. The cation-to-anion ratio was found to be crucial in determining the predominant anions present in the ILs. Among the synthesized Cu-based ILs, [Bmim]Cl/CuCl₂-1 exhibited outstanding EDN performance, achieving 100% nitrogen removal with minimal ionic liquid consumption. The anion [CuCl₃]⁻ was identified as playing a key role in the EDN process, where the unoccupied orbitals of Cu and the chloridion in [CuCl₃]⁻ facilitate effective coordination with nitrogen atoms in organic nitrogen compounds. This coordination forms Lewis acid–base interactions, which are essential for deep EDN. The study not only introduces an efficient Cu-based ionic liquid but also provides insights into optimizing ionic liquid design for better extraction performance.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"58 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142937793","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}