{"title":"Integrated catalyst‐reactor design for benzylic C‐H oxidation: NiCo2O4 nanoarrays on metal foam in continuous flow","authors":"Xiaohui Zhang, Xude Yu, Zhuo Chen, Jian Chen, Jianhong Xu","doi":"10.1002/aic.18942","DOIUrl":"https://doi.org/10.1002/aic.18942","url":null,"abstract":"The selective oxidation of benzylic C‐H bonds to aryl ketones and alcohols holds significant importance in fine chemical synthesis. This study introduces a continuous‐flow aerobic oxidation strategy employing nickel foam‐supported NiCo<jats:sub>2</jats:sub>O<jats:sub>4</jats:sub> spinel oxides as highly efficient heterogeneous catalysts. Prepared via electrodeposition, the catalysts feature nanosheet arrays (~5 nm thick), enabling efficient diffusion of liquid‐phase substrates into the solid catalyst. In a micro‐packed bed reactor, the open‐cell nickel foam, with (~160 μm pores), enhances gas–liquid mass transfer. This strategy achieved >96% fluorene oxidation conversion and >98% selectivity within a short residence time (48 min), with stable performance over 130 h. The method was successfully applied to 13 diverse benzylic C–H substrates. Mechanistic studies indicate a radical‐based pathway, with oxygen adsorption following the Langmuir–Hinshelwood model. Cobalt sites promote oxygen activation, while nickel sites enhance substrate adsorption. This work presents a safe and efficient approach, offering prospects for industrial applications.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"11 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144547305","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}
AIChE JournalPub Date : 2025-07-02DOI: 10.1002/aic.18937
Yuxin Chen, Qian Zhang, Shizhen Wang
{"title":"Mechanistic study for catalytic promiscuity of phenylalanine dehydrogenase induced by amino acid deep eutectic solvents","authors":"Yuxin Chen, Qian Zhang, Shizhen Wang","doi":"10.1002/aic.18937","DOIUrl":"https://doi.org/10.1002/aic.18937","url":null,"abstract":"Catalytic promiscuity of phenylalanine dehydrogenase (NTAaDH) induced by the amino acid deep eutectic solvents (AA‐DES) was studied. The activity of NTAaDH with the L‐Phe‐DES as substrate was 71.7‐fold that of the buffer system, while it was 24.4‐fold for L‐Lys‐DES. The half‐life of NTAaDH was enhanced by threefold of that of buffer at 50°C. Mechanism of catalytic promiscuity induced by AA‐DES was studied. AA‐DES can biomimetic intracellular environment with a crowding effect and provide a protective layer of enzyme. Analysis of the conformation change of NTAaDH indicated the shrinkage of the substrate channel. This study provided a new strategy for the solvent engineering for the oxidoreductases and further for industrial production.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"18 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144532957","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}
AIChE JournalPub Date : 2025-07-01DOI: 10.1002/aic.18935
Meili Ding, Wei Rong, Yang Wang, Jianfeng Yao
{"title":"Surface structure modulation of biochar enables high‐efficiency photodriven CO2 fixation","authors":"Meili Ding, Wei Rong, Yang Wang, Jianfeng Yao","doi":"10.1002/aic.18935","DOIUrl":"https://doi.org/10.1002/aic.18935","url":null,"abstract":"Reforming desirable photocatalytic platforms for efficient carbon dioxide (CO<jats:sub>2</jats:sub>) utilization is highly desirable but represents a great challenge. In this study, we report a facile surface structure modulation strategy to fabricate functional biochars (BCs) with different surface oxygen functional groups. The mild oxidation of sodium hypochlorite endows BC with abundant surface oxygen species without significantly compromising its inherent morphology. Under Xe lamp irradiation (400 mW/cm<jats:sup>2</jats:sup>) and 1 bar CO<jats:sub>2</jats:sub>, the catalytic activity toward the coupling of CO<jats:sub>2</jats:sub> and epichlorohydrin based on BC‐NaClO reached 100% yield, which was 3.8, 2.6, and 1.5 times greater than that of pristine BC, functional BC‐HNO<jats:sub>3</jats:sub>, and BC‐NaOH, respectively. Further investigations revealed the contributions of both holes and electrons to the photocatalytic activity of BC‐NaClO and the synergistic effects of photocatalysis and photothermal catalysis. This work demonstrates a rational pathway toward high‐efficiency biomass‐derived photocatalysts for targeted CO<jats:sub>2</jats:sub> conversion.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"19 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144533050","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}
AIChE JournalPub Date : 2025-06-25DOI: 10.1002/aic.18932
David S. Sholl
{"title":"Correction to “Could The Chemical Industry Mitigate Rapid Global Cooling From A Catastrophic Volcanic Eruption?”","authors":"David S. Sholl","doi":"10.1002/aic.18932","DOIUrl":"https://doi.org/10.1002/aic.18932","url":null,"abstract":"","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"26 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144479008","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}
AIChE JournalPub Date : 2025-06-17DOI: 10.1002/aic.18931
Yiming Ma, Wei Li, Jiaxu Liu, Gao Shang, Huaiyu Yang, Junbo Gong, Zoltan K. Nagy, Brahim Benyahia
{"title":"Digital design and optimization of the integrated synthesis and crystallization process using data-driven approaches","authors":"Yiming Ma, Wei Li, Jiaxu Liu, Gao Shang, Huaiyu Yang, Junbo Gong, Zoltan K. Nagy, Brahim Benyahia","doi":"10.1002/aic.18931","DOIUrl":"https://doi.org/10.1002/aic.18931","url":null,"abstract":"This study presents a data-driven modeling and multi-objective optimization framework for an integrated section of continuous pharmaceutical manufacturing, focusing on flow synthesis and continuous crystallization. To address data scarcity and trade-offs among product quality, efficiency, and environmental impact, the framework combines generative adversarial networks (GANs), artificial neural networks (ANNs), and genetic algorithms (GAs). An integrated dual-GAN (ID-GAN) generates data under physicochemical constraints, which are merged with real data to train an ANN with 15%–20% mean absolute errors for particle size, productivity, and a sustainability throughput index. The ANN is then coupled with a GA to identify Pareto-optimal solutions based on user-defined objectives and constraints. Case studies validate the framework's capability to facilitate process design decisions by systematically exploring trade-offs among competing objectives, underscoring its potential utility in the digitalization of critical units within continuous manufacturing systems.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"24 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144311948","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}
AIChE JournalPub Date : 2025-06-11DOI: 10.1002/aic.18930
Huijie Chen, Menglu Cai, Jianbo Shao, Ting Lin, Yan Liu, Yiming Mo
{"title":"A tandem electro-thermocatalysis platform for practical hydrogen peroxide-mediated oxygenation reactions at high rates","authors":"Huijie Chen, Menglu Cai, Jianbo Shao, Ting Lin, Yan Liu, Yiming Mo","doi":"10.1002/aic.18930","DOIUrl":"https://doi.org/10.1002/aic.18930","url":null,"abstract":"Hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) is a platform green oxidant for high-value chemical synthesis, but its centralized production hinders its widespread use in a safe manner. Here, we describe a practical tandem electro-thermochemical H<sub>2</sub>O<sub>2</sub>-mediated oxygenation platform for the synthesis of various high-value oxygen-containing compounds. The integration of solid-electrolyte H<sub>2</sub>O<sub>2</sub> electrosynthesis with heterogeneous zeolite thermocatalysis enables atom-efficient oxygenations without the need for downstream electrolytes or catalysts separation. A spatially decoupled tandem system integrating aqueous H<sub>2</sub>O<sub>2</sub> electrosynthesis with nonaqueous thermocatalysis offers independent optimization capabilities, thus maximizing the overall space–time yield (STY). With microfluidic packed-bed intensification for heterogeneous thermocatalysis, this tandem system achieved H<sub>2</sub>O<sub>2</sub>-mediated oxygenation of thioesters to sulfoxide at a high current density (300 mA cm<sup>−2</sup>) and STY (7.07 mmol cm<sup>−3</sup> h<sup>−1</sup>). Furthermore, the platform's broad applicability was showcased with titanium-silicalite-1 zeolite catalyzed olefin epoxidation and cyclohexanone oxime synthesis, underscoring its potential for diverse catalytic oxygenation applications.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"41 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144260261","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":"Probing bimodal sub-nanopores in carbon for ideal fast sieving separation of propylene/propane","authors":"Xinxin Li, Jiawu Huang, Cuiting Yang, Xingjie Wang, Xuan Wei, Xiaoying Zhou, Hao Tang, Jing Xiao","doi":"10.1002/aic.18926","DOIUrl":"https://doi.org/10.1002/aic.18926","url":null,"abstract":"Rigid molecular sieve is highly desirable in industrial gas separation, but persistently challenged by sluggish adsorption within inherent rigidity-confined narrow sieving pores. Herein, we report a rigid carbon-based molecular sieve featuring ink-bottle bimodal sub-nanopores for the ideal fast sieving separation of propylene/propane mixture. The tailor-made narrow pore entrance, centered at 5.0 Å, affords precise sieving capacity for propylene over propane with a high selectivity exceeding 200. Concurrently, the larger cavity located at 6.4 Å allows the exceptional fast adsorption kinetics of propylene. The measured diffusion coefficient of propylene (4.2 × 10–3 s<sup>−1</sup>) is one to two orders of magnitude higher than state-of-the-art rigid molecular sieves and comparable to the non-steric diffusion observed in mesoporous zeolite. High-purity C<sub>3</sub>H<sub>6</sub> production (>99.2%) is achieved in breakthrough experiments through a single adsorption–desorption cycle. This study paves an avenue to unlock rigid molecular sieves toward advanced separation of challenging gas analogues.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"585 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144260262","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}
AIChE JournalPub Date : 2025-06-09DOI: 10.1002/aic.18929
Lin Wang, Xiaohe Zheng, Zhengfei Chen, Jiadong Wu, Qiang Zhou, Zhongjian Li, Bin Yang, Cheng Lian, Jianguo Lu, Yuanyuan Li, Lecheng Lei, Yang Hou
{"title":"Chloride-resistant NiFe oxyhydroxides via dual-atom doping for industrial-grade alkaline seawater electrolysis","authors":"Lin Wang, Xiaohe Zheng, Zhengfei Chen, Jiadong Wu, Qiang Zhou, Zhongjian Li, Bin Yang, Cheng Lian, Jianguo Lu, Yuanyuan Li, Lecheng Lei, Yang Hou","doi":"10.1002/aic.18929","DOIUrl":"https://doi.org/10.1002/aic.18929","url":null,"abstract":"Developing efficient and stable electrocatalysts for seawater splitting remains a huge challenge because of low catalytic selectivity and poor resistance to chlorine-induced corrosion. Here, we developed a nickel-iron layered double hydroxide nanosheets doped with chromium and sulfur dual atoms (Cr,S-NiFe LDH). Cr,S-NiFe LDH exhibited low overpotentials of 321 and 406 mV at industrial current densities of 500 and 1000 mA cm<sup>−2</sup>, respectively. An anion exchange membrane electrolyzer based on Cr,S-NiFe LDH anode can maintain 2000 mA cm<sup>−2</sup>@1.764 V for 100 h. Electronic structure analysis revealed that the sulfur doping facilitates electron transfer from nickel to sulfur sites, while chromium incorporation strengthens the electronic interactions between iron and chromium sites. This modification induced the formation of high-valence nickel and chromium species, which favor seawater electrolysis. Mechanistic studies revealed that dual heteroatom doping modifies the local electronic environment of nickel/iron sites, repelling chlorine ions and optimizing the adsorption of oxygenated intermediates.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"60 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144237913","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":"Novel microannular rotating bed: Hydrodynamics and liquid–liquid dispersion study","authors":"Zhiliang Zhang, Qiao Chen, Hui Xue, Guo Yang, Gongtao Wu, Wei Liu, Dongting Wang, Jianbing Ji","doi":"10.1002/aic.18928","DOIUrl":"https://doi.org/10.1002/aic.18928","url":null,"abstract":"Microannular rotating bed (MARB) is a newly designed reactor that integrates high-gravity fields and microscale effects to enable efficient liquid mixing. This study systematically investigated the hydrodynamic and liquid–liquid dispersion characteristics of the MARB, including residence time distribution, liquid holdup, energy dissipation rate, and Sauter mean diameter (<i>d</i><sub>32</sub>). Mathematical correlations for predicting these parameters were established. The results showed that the MARB operates with a flow pattern similar to that of a continuous stirred-tank reactor. Liquid holdup increased linearly with flow rate and decreased with rotational speed, while energy dissipation rate was primarily governed by rotational speed. Notably, the MARB demonstrated excellent liquid–liquid dispersion performance, attaining a minimum <i>d</i><sub>32</sub> of 4.9 μm at a flow rate of 5 L/min, along with improved energy efficiency compared to conventional reactors. With its simple, high-throughput, and effective design, the MARB offers a highly promising solution for efficient liquid–liquid dispersion in industrial applications.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"17 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144252861","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}
AIChE JournalPub Date : 2025-06-06DOI: 10.1002/aic.18922
Ittisak Promma, Marc G. Aucoin, Nasser Mohieddin Abukhdeir, Hector Budman
{"title":"Modeling heterogeneity in large-scale bioreactors using the method of moments with a truncated normal distribution","authors":"Ittisak Promma, Marc G. Aucoin, Nasser Mohieddin Abukhdeir, Hector Budman","doi":"10.1002/aic.18922","DOIUrl":"https://doi.org/10.1002/aic.18922","url":null,"abstract":"Large-scale bioreactors in industrial bioprocesses pose challenges due to extracellular concentration gradients and intracellular heterogeneity. This study introduces a novel approach integrating the method of moments with truncated normal distributions (MM-TND) to model intracellular heterogeneity while maintaining computational feasibility compared to continuum simulations. The MM-TND framework reconstructs intracellular state distributions while respecting physical constraints, which previous methods could not ensure. Validation against experimental data confirms that MM-TND effectively captures microbial population dynamics, particularly in large-scale systems where convection and metabolic adaptation timescales are comparable. The results underscore the importance of intracellular heterogeneity in bioprocess modeling and highlight computational advantages of the MM-TND approach. This approach offers valuable insights into microbial behavior under industrially relevant conditions.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"59 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-06-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144228810","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}