Zhiheng Wang, Ningning Wu, Jiali Huang, Tuo Ji, Han Lin, Liwen Mu, Xiaohua Lu, Jiahua Zhu
Direct synthesis of hydrogen peroxide (DSHP) from H 2 and O 2 is indeed a promising sustainable alternative to the conventional anthraquinone oxidation process, yet achieving high H 2 O 2 productivity and selectivity simultaneously remains a significant challenge. Herein, we designed a diode‐inspired interfacial microenvironment to address this challenge by synchronizing the kinetic relay of the key transport and reaction steps in DSHP. Specifically, this microenvironment was fabricated by grafting hydrophobic silane molecules onto the carbon surface followed by loading palladium nanoparticles. Results indicate that the interfacial microenvironment enables an efficient relay of H 2 dissociation, H 2 O 2 formation and desorption, shutting down the reverse path of the side reaction. Benefiting from this diode‐inspired interfacial design, high H 2 O 2 productivity of 21,647.1 mol kg Pd−1 h −1 and H 2 O 2 selectivity of 93.3% were successfully achieved under ambient conditions. This work demonstrated the critical role of the interfacial microenvironment in regulating the synergy between mass transfer and reaction in heterogeneous reaction.
从h22和o2直接合成过氧化氢（DSHP）确实是传统蒽醌氧化工艺的一种有前途的可持续替代方法，但同时实现高h2o2生产率和选择性仍然是一个重大挑战。在此，我们设计了一个二极管启发的界面微环境，通过同步DSHP中关键传输和反应步骤的动力学继电器来解决这一挑战。具体来说，这种微环境是通过将疏水性硅烷分子接枝到碳表面，然后加载钯纳米粒子来制备的。结果表明，该界面微环境能够有效地实现h2解离、h2o2生成和解吸，关闭副反应的反向路径。得益于这种二极管启发的界面设计，在环境条件下成功地获得了21,647.1 mol kg Pd−1 H−1的高h2o2生产率和93.3%的h2o2选择性。这项工作证明了界面微环境在调节非均相反应中传质与反应协同作用中的关键作用。
{"title":"A diode‐inspired microenvironment enables efficient direct H 2 O 2 synthesis from H 2 and O 2 at ambient conditions","authors":"Zhiheng Wang, Ningning Wu, Jiali Huang, Tuo Ji, Han Lin, Liwen Mu, Xiaohua Lu, Jiahua Zhu","doi":"10.1002/aic.70274","DOIUrl":"https://doi.org/10.1002/aic.70274","url":null,"abstract":"Direct synthesis of hydrogen peroxide (DSHP) from H <jats:sub>2</jats:sub> and O <jats:sub>2</jats:sub> is indeed a promising sustainable alternative to the conventional anthraquinone oxidation process, yet achieving high H <jats:sub>2</jats:sub> O <jats:sub>2</jats:sub> productivity and selectivity simultaneously remains a significant challenge. Herein, we designed a diode‐inspired interfacial microenvironment to address this challenge by synchronizing the kinetic relay of the key transport and reaction steps in DSHP. Specifically, this microenvironment was fabricated by grafting hydrophobic silane molecules onto the carbon surface followed by loading palladium nanoparticles. Results indicate that the interfacial microenvironment enables an efficient relay of H <jats:sub>2</jats:sub> dissociation, H <jats:sub>2</jats:sub> O <jats:sub>2</jats:sub> formation and desorption, shutting down the reverse path of the side reaction. Benefiting from this diode‐inspired interfacial design, high H <jats:sub>2</jats:sub> O <jats:sub>2</jats:sub> productivity of 21,647.1 mol kg <jats:sub>Pd</jats:sub> <jats:sup>−1</jats:sup> h <jats:sup>−1</jats:sup> and H <jats:sub>2</jats:sub> O <jats:sub>2</jats:sub> selectivity of 93.3% were successfully achieved under ambient conditions. This work demonstrated the critical role of the interfacial microenvironment in regulating the synergy between mass transfer and reaction in heterogeneous reaction.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"388 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146071900","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}
Oxygen‐coordinated single atom catalysts (SACs) hold promise for enhancing electrocatalytic performance in oxygen evolution reactions (OER). However, their synthesis remains challenging due to the instability of metal‐oxygen bonds under traditional high‐temperature methods. This difficulty is compounded by the lack of model SACs with well‐defined oxygen coordination, hindering the study of structural evolution during catalysis. Herein we propose a stepwise electrochemical oxidation strategy to synthesize nickel SACs on graphite foil with precisely controlled oxygen coordination numbers. The initial oxygen coordination number significantly influences the structural evolution of these SACs during OER, with partial Ni‐O 5 configurations undergoing reconstruction into clusters, while others maintain atomic dispersion. By establishing a direct correlation between the initial coordination environment and the SACs' dynamic behavior under operational conditions, this study provides a comprehensive framework for understanding and designing adaptive and active OER catalysts.
氧配位单原子催化剂（SACs）有望提高析氧反应（OER）的电催化性能。然而，由于传统高温方法下金属-氧键的不稳定性，它们的合成仍然具有挑战性。由于缺乏具有明确氧配位的SACs模型，这一困难变得更加复杂，阻碍了催化过程中结构演化的研究。本文提出了一种在精确控制氧配位数的石墨箔上合成镍SACs的分步电化学氧化策略。在OER过程中，初始氧配位数显著影响这些SACs的结构演变，部分Ni - O - 5构型重建成簇，而其他的则保持原子弥散。通过建立初始配位环境与sac在操作条件下的动态行为之间的直接关系，本研究为理解和设计自适应和活性OER催化剂提供了一个全面的框架。
{"title":"Electrochemical oxygen coordination engineering of nickel single atoms for enhanced oxygen evolution reactions","authors":"Yuanyuan Li, Huawei Huang, Xiaotong Han, Xinyi Tan, Jianren Wang, Shaofeng Li, Zhibin Liu","doi":"10.1002/aic.70272","DOIUrl":"https://doi.org/10.1002/aic.70272","url":null,"abstract":"Oxygen‐coordinated single atom catalysts (SACs) hold promise for enhancing electrocatalytic performance in oxygen evolution reactions (OER). However, their synthesis remains challenging due to the instability of metal‐oxygen bonds under traditional high‐temperature methods. This difficulty is compounded by the lack of model SACs with well‐defined oxygen coordination, hindering the study of structural evolution during catalysis. Herein we propose a stepwise electrochemical oxidation strategy to synthesize nickel SACs on graphite foil with precisely controlled oxygen coordination numbers. The initial oxygen coordination number significantly influences the structural evolution of these SACs during OER, with partial Ni‐O <jats:sub>5</jats:sub> configurations undergoing reconstruction into clusters, while others maintain atomic dispersion. By establishing a direct correlation between the initial coordination environment and the SACs' dynamic behavior under operational conditions, this study provides a comprehensive framework for understanding and designing adaptive and active OER catalysts.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"7 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146071885","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}
Bastian Oldach, Konrad E. R. Boettcher, Alexander S. Sommer‐Behr, Norbert Kockmann
In porous beds, physical boundaries restrict particle arrangement, leading to inhomogeneous porosity. This paper reports on the porosity profiles that are the result of geometric effects on monodisperse packed beds in cylindrical and cubic arrangements. Special focus is given to the influence of edges and corners in cubic geometries. Three‐dimensional (3D) imaging results show that due to the arrangement of the spherical particles in corners and edges, where adjacent walls meet, maxima and minima in the porosity profile are more pronounced, and that peaks are less frequent than in systems with curved walls. For the porosity profile imposed by edges and corners, there are no notable global maxima or minima, but they show an increased bulk porosity, indicating anisotropic structural effects. To capture these geometric influences, a mathematical model based on an exponential approach is proposed, offering new insights for predicting porosity in systems bounded by both curved and planar walls.
{"title":"3D investigation and modeling of the geometric effects on porosity in packed beds","authors":"Bastian Oldach, Konrad E. R. Boettcher, Alexander S. Sommer‐Behr, Norbert Kockmann","doi":"10.1002/aic.70240","DOIUrl":"https://doi.org/10.1002/aic.70240","url":null,"abstract":"In porous beds, physical boundaries restrict particle arrangement, leading to inhomogeneous porosity. This paper reports on the porosity profiles that are the result of geometric effects on monodisperse packed beds in cylindrical and cubic arrangements. Special focus is given to the influence of edges and corners in cubic geometries. Three‐dimensional (3D) imaging results show that due to the arrangement of the spherical particles in corners and edges, where adjacent walls meet, maxima and minima in the porosity profile are more pronounced, and that peaks are less frequent than in systems with curved walls. For the porosity profile imposed by edges and corners, there are no notable global maxima or minima, but they show an increased bulk porosity, indicating anisotropic structural effects. To capture these geometric influences, a mathematical model based on an exponential approach is proposed, offering new insights for predicting porosity in systems bounded by both curved and planar walls.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"55 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146070562","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}
Yang Ding, Zhenyang Dong, Hailiang Zhou, Kai Li, Wei Guo, Yuhang Wang, Lihao Liu, Zujiang Yi, Zhengbin Zhang, Xing Zhong, Jianguo Wang
Ozonolysis offers a clean and selective route for CC bond cleavage, but conventional processes suffer from ozonide explosion hazards and poor mass transfer. Here, we integrate electrochemical ozone production (EOP) with continuous‐flow microchannel ozonolysis for the safe conversion of steroid substrates. A dual surfactant modified β‐PbO 2 electrocatalyst (β‐PbO 2 ‐CP) in a self‐developed ozone electrolyzer achieved high ozone generation efficiency with over 750 h stability. Precision‐engineered microchannel reactor intensified gas–liquid transfer via microscale bubble dynamics, affording 91.3% conversion and 98.1% selectivity for 17α‐methyltestosterone, which achieved a 33.7‐fold increase in space–time yield vs. batch reactor. Computational fluid dynamics (CFD) simulations revealed electrothermal flow modeling showed 42.6% lower peak temperature with 98.9% prediction accuracy in the ozone electrolyzer and elucidated gas–liquid behavior in microchannel reactor. This integrated platform demonstrates a controlled continuous‐flow approach suitable for pharmaceutical manufacturing, highlighting the potential of coupling EOP with flow chemistry for industrial oxidative processes.
{"title":"Efficient ozonolysis of steroids via electrochemical ozone production coupled with microchannel reactor","authors":"Yang Ding, Zhenyang Dong, Hailiang Zhou, Kai Li, Wei Guo, Yuhang Wang, Lihao Liu, Zujiang Yi, Zhengbin Zhang, Xing Zhong, Jianguo Wang","doi":"10.1002/aic.70230","DOIUrl":"https://doi.org/10.1002/aic.70230","url":null,"abstract":"Ozonolysis offers a clean and selective route for CC bond cleavage, but conventional processes suffer from ozonide explosion hazards and poor mass transfer. Here, we integrate electrochemical ozone production (EOP) with continuous‐flow microchannel ozonolysis for the safe conversion of steroid substrates. A dual surfactant modified β‐PbO <jats:sub>2</jats:sub> electrocatalyst (β‐PbO <jats:sub>2</jats:sub> ‐CP) in a self‐developed ozone electrolyzer achieved high ozone generation efficiency with over 750 h stability. Precision‐engineered microchannel reactor intensified gas–liquid transfer via microscale bubble dynamics, affording 91.3% conversion and 98.1% selectivity for 17α‐methyltestosterone, which achieved a 33.7‐fold increase in space–time yield vs. batch reactor. Computational fluid dynamics (CFD) simulations revealed electrothermal flow modeling showed 42.6% lower peak temperature with 98.9% prediction accuracy in the ozone electrolyzer and elucidated gas–liquid behavior in microchannel reactor. This integrated platform demonstrates a controlled continuous‐flow approach suitable for pharmaceutical manufacturing, highlighting the potential of coupling EOP with flow chemistry for industrial oxidative processes.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"33 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146070560","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}
Ziming Zhao, Yuhan Mei, Shuai Zhao, Yuping Liu, Huan Li
Aqueous dual‐ion batteries (ADIBs) are promising for large‐scale storage but face challenges in a lack of in‐depth understanding of anion intercalation behavior and the difficulty in formulating aqueous electrolytes with a wide electrochemical stability window. Here, we regulate the anion intercalation behavior in graphite cathodes by designing high‐concentration aqueous electrolytes using organic lithium salts (LiTFSI, LiFSI, and LiOTf). A combined experimental and theoretical calculation reveals that the intercalation behavior, including intercalation energy and diffusion barrier, is highly anion‐dependent, identifying TFSI − and FSI − as the anions with the most favorable kinetics and reversibility. Electrolyte optimization, particularly a mixed‐salt system (37m 9LiFSI‐1LiTFSI), expands the electrochemical window beyond 3.1 V and enhances cycling stability. Furthermore, partial water substitution by 12‐crown‐4 ether effectively suppresses hydrogen evolution, boosting the Coulombic efficiency to 90%. This work provides fundamental insights into anion intercalation mechanisms in aqueous media and offers a viable electrolyte design strategy toward high‐voltage ADIBs.
{"title":"Tailoring high‐concentration aqueous electrolytes for enhanced anion intercalation behavior in dual‐ion batteries","authors":"Ziming Zhao, Yuhan Mei, Shuai Zhao, Yuping Liu, Huan Li","doi":"10.1002/aic.70267","DOIUrl":"https://doi.org/10.1002/aic.70267","url":null,"abstract":"Aqueous dual‐ion batteries (ADIBs) are promising for large‐scale storage but face challenges in a lack of in‐depth understanding of anion intercalation behavior and the difficulty in formulating aqueous electrolytes with a wide electrochemical stability window. Here, we regulate the anion intercalation behavior in graphite cathodes by designing high‐concentration aqueous electrolytes using organic lithium salts (LiTFSI, LiFSI, and LiOTf). A combined experimental and theoretical calculation reveals that the intercalation behavior, including intercalation energy and diffusion barrier, is highly anion‐dependent, identifying TFSI <jats:sup>−</jats:sup> and FSI <jats:sup>−</jats:sup> as the anions with the most favorable kinetics and reversibility. Electrolyte optimization, particularly a mixed‐salt system (37m 9LiFSI‐1LiTFSI), expands the electrochemical window beyond 3.1 V and enhances cycling stability. Furthermore, partial water substitution by 12‐crown‐4 ether effectively suppresses hydrogen evolution, boosting the Coulombic efficiency to 90%. This work provides fundamental insights into anion intercalation mechanisms in aqueous media and offers a viable electrolyte design strategy toward high‐voltage ADIBs.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"85 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146070563","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}
Congyou Yang, Zhiyong Xu, Ning Zhao, Bo Wang, Wenbo Zhao
To address the high energy consumption, insufficient thermal stability, and lack of systematic optimization strategies of conventional aqueous alkanolamine CO 2 absorbents, this study developed a blended monoethanolamine/ethylene glycol (EG) absorbent system by replacing water with EG. The CO 2 absorption performance was systematically investigated. Validated kinetic and thermodynamic models were integrated into a robust coupled model to simulate absorption behavior. Based on the coupled model, two optimization strategies for the CO 2 absorption process were proposed: determining the optimal absorption temperature to maximize absorption capacity under fixed CO 2 partial pressure and absorption time; identifying the optimal temperature to minimize absorption time under fixed CO 2 partial pressure and absorption capacity. The research results indicate that both optimization strategies exhibit significant optimization effects under a variety of absorption conditions. This study provides a vital theoretical framework and experimental foundation for the design of industrial CO 2 capture absorbents and the optimization of process parameters.
{"title":"Absorption capacity and time optimization of CO 2 capture in MEA–EG system based on kinetic‐thermodynamic coupled model","authors":"Congyou Yang, Zhiyong Xu, Ning Zhao, Bo Wang, Wenbo Zhao","doi":"10.1002/aic.70264","DOIUrl":"https://doi.org/10.1002/aic.70264","url":null,"abstract":"To address the high energy consumption, insufficient thermal stability, and lack of systematic optimization strategies of conventional aqueous alkanolamine CO <jats:sub>2</jats:sub> absorbents, this study developed a blended monoethanolamine/ethylene glycol (EG) absorbent system by replacing water with EG. The CO <jats:sub>2</jats:sub> absorption performance was systematically investigated. Validated kinetic and thermodynamic models were integrated into a robust coupled model to simulate absorption behavior. Based on the coupled model, two optimization strategies for the CO <jats:sub>2</jats:sub> absorption process were proposed: determining the optimal absorption temperature to maximize absorption capacity under fixed CO <jats:sub>2</jats:sub> partial pressure and absorption time; identifying the optimal temperature to minimize absorption time under fixed CO <jats:sub>2</jats:sub> partial pressure and absorption capacity. The research results indicate that both optimization strategies exhibit significant optimization effects under a variety of absorption conditions. This study provides a vital theoretical framework and experimental foundation for the design of industrial CO <jats:sub>2</jats:sub> capture absorbents and the optimization of process parameters.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"30 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146070561","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}
High‐entropy oxides (HEOs) are promising heterogeneous catalysts due to their multiple active sites and structural stability, but their application is limited by complex synthesis and nanoparticle sintering. Here, we present a defect‐induced strategy to construct strong metal‐support interactions (SMSI) between MnCeNiCuCo HEO nanoparticles and defect‐rich hexagonal boron nitride nanosheets (h‐BNNS), forming HEO/h‐BNNS. Contrary to classical H 2 ‐induced SMSI, the inherent N/B vacancies in h‐BNNS anchor the HEO and induce spontaneous B‐atom migration over the HEO surface under N 2 , forming a permeable B–O encapsulation. This encapsulation not only inhibits sintering but also induces electronic coupling with the HEO lattice, modulating local charge density and generating abundant oxygen vacancies. Using aerobic oxidative desulfurization as a model reaction, HEO/h‐BNNS achieves a 99.9% desulfurization efficiency. This work demonstrates a defect‐driven pathway to engineer supported high‐entropy catalysts and provides a rational framework for designing efficient, durable, and scalable catalytic systems for energy and environmental applications.
{"title":"Defect‐driven electronic coupling and oxygen vacancy engineering in supported high‐entropy oxides for desulfurization","authors":"Chang Deng, Zhendong Yu, Xueyan Ju, Feng Liu, Mingfeng Li, Benlin Dai, Feihu Mu, Xiaozhong Chu, Peiwen Wu, Wenshuai Zhu","doi":"10.1002/aic.70273","DOIUrl":"https://doi.org/10.1002/aic.70273","url":null,"abstract":"High‐entropy oxides (HEOs) are promising heterogeneous catalysts due to their multiple active sites and structural stability, but their application is limited by complex synthesis and nanoparticle sintering. Here, we present a defect‐induced strategy to construct strong metal‐support interactions (SMSI) between MnCeNiCuCo HEO nanoparticles and defect‐rich hexagonal boron nitride nanosheets (h‐BNNS), forming HEO/h‐BNNS. Contrary to classical H <jats:sub>2</jats:sub> ‐induced SMSI, the inherent N/B vacancies in h‐BNNS anchor the HEO and induce spontaneous B‐atom migration over the HEO surface under N <jats:sub>2</jats:sub> , forming a permeable B–O encapsulation. This encapsulation not only inhibits sintering but also induces electronic coupling with the HEO lattice, modulating local charge density and generating abundant oxygen vacancies. Using aerobic oxidative desulfurization as a model reaction, HEO/h‐BNNS achieves a 99.9% desulfurization efficiency. This work demonstrates a defect‐driven pathway to engineer supported high‐entropy catalysts and provides a rational framework for designing efficient, durable, and scalable catalytic systems for energy and environmental applications.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"30 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146056002","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}
Precise sieving of structurally similar solutes in organic solvents is crucial for chemical industries such as pharmaceutical synthesis and petroleum refining. However, it remains technically challenging due to their similar physicochemical properties. Achieving this with organic solvent nanofiltration (OSN) requires membranes with narrow pore‐size distribution and tailored surface chemistry. Herein, we report an additive‐free strategy to prepare ultrathin, structurally homogeneous polyamide (PA) nanofilms via alkyl chain engineering during interfacial polymerization (IP). Alkyl chains synergistically regulate the diffusion kinetics and the reaction process: they enable rapid, uniform amine supply while introducing steric hindrance that moderates polycondensation. This dual regulation yields a structurally homogeneous PA layer with sub‐nanometer pores. The optimized membrane shows a sharp rejection curve and effectively separates antibiotics, demonstrating promise for pharmaceutical purification. This work advances the understanding of diffusion‐reaction synergy in IP and offers a facile strategy for precision separation membranes.
{"title":"Polyamide membranes with structural homogeneity regulated by alkyl chain engineering for precise molecular sieving","authors":"Hui Yang, Dan Wang, Shuyun Gu, Linlong Zhou, Siyao Li, Zhi Xu","doi":"10.1002/aic.70250","DOIUrl":"https://doi.org/10.1002/aic.70250","url":null,"abstract":"Precise sieving of structurally similar solutes in organic solvents is crucial for chemical industries such as pharmaceutical synthesis and petroleum refining. However, it remains technically challenging due to their similar physicochemical properties. Achieving this with organic solvent nanofiltration (OSN) requires membranes with narrow pore‐size distribution and tailored surface chemistry. Herein, we report an additive‐free strategy to prepare ultrathin, structurally homogeneous polyamide (PA) nanofilms via alkyl chain engineering during interfacial polymerization (IP). Alkyl chains synergistically regulate the diffusion kinetics and the reaction process: they enable rapid, uniform amine supply while introducing steric hindrance that moderates polycondensation. This dual regulation yields a structurally homogeneous PA layer with sub‐nanometer pores. The optimized membrane shows a sharp rejection curve and effectively separates antibiotics, demonstrating promise for pharmaceutical purification. This work advances the understanding of diffusion‐reaction synergy in IP and offers a facile strategy for precision separation membranes.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"504 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146056003","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}
Xiaoling Liu, Mingzhen Wang, Ting Li, Jiao Wei, Tian Rong, Qiqi Liu, Yajie Wang, Yu Zhou, Jun Wang
Efficient removal of trace acetylene (C 2 H 2 ) from ethylene (C 2 H 4 ) is crucial for polymer production, yet remains challenging for physisorption separation owing to their molecular similarity. Herein, we synthesized a series of LTL zeolites with varied Si/Al ratios via an acid co‐hydrolysis route. The optimal adsorbent LTL(2.3) with a low Si/Al ratio of 2.3 exhibited both high C 2 H 2 uptake (2.79 mmol g −1 ) and C 2 H 2 /C 2 H 4 (1/99, v / v ) selectivity of 26.84 at 1 bar and 298 K, as well as superior dynamic separation efficiency. Structural refinement based on high‐resolution powder X‐ray diffraction (PXRD) patterns illustrates that reducing Si/Al ratio provides more K + cation that serves as the strong C 2 H 2 binding sites, thereby promoting the C 2 H 2 /C 2 H 4 separation. Moreover, the optimal LTL zeolite also demonstrates favorable separation efficiency towards other gas mixtures (e.g., CO 2 /N 2 , CO 2 /CH 4 , C 2 H 4 /C 2 H 6 , and C 3 H 6 /C 3 H 8 ), showing the promising potential as a versatile adsorbent for gas separation and purification.
{"title":"Regulating silica/alumina ratio of LTL zeolites for acetylene/ethylene separation","authors":"Xiaoling Liu, Mingzhen Wang, Ting Li, Jiao Wei, Tian Rong, Qiqi Liu, Yajie Wang, Yu Zhou, Jun Wang","doi":"10.1002/aic.70255","DOIUrl":"https://doi.org/10.1002/aic.70255","url":null,"abstract":"Efficient removal of trace acetylene (C <jats:sub>2</jats:sub> H <jats:sub>2</jats:sub> ) from ethylene (C <jats:sub>2</jats:sub> H <jats:sub>4</jats:sub> ) is crucial for polymer production, yet remains challenging for physisorption separation owing to their molecular similarity. Herein, we synthesized a series of LTL zeolites with varied Si/Al ratios via an acid co‐hydrolysis route. The optimal adsorbent LTL(2.3) with a low Si/Al ratio of 2.3 exhibited both high C <jats:sub>2</jats:sub> H <jats:sub>2</jats:sub> uptake (2.79 mmol g <jats:sup>−1</jats:sup> ) and C <jats:sub>2</jats:sub> H <jats:sub>2</jats:sub> /C <jats:sub>2</jats:sub> H <jats:sub>4</jats:sub> (1/99, <jats:italic>v</jats:italic> / <jats:italic>v</jats:italic> ) selectivity of 26.84 at 1 bar and 298 K, as well as superior dynamic separation efficiency. Structural refinement based on high‐resolution powder X‐ray diffraction (PXRD) patterns illustrates that reducing Si/Al ratio provides more K <jats:sup>+</jats:sup> cation that serves as the strong C <jats:sub>2</jats:sub> H <jats:sub>2</jats:sub> binding sites, thereby promoting the C <jats:sub>2</jats:sub> H <jats:sub>2</jats:sub> /C <jats:sub>2</jats:sub> H <jats:sub>4</jats:sub> separation. Moreover, the optimal LTL zeolite also demonstrates favorable separation efficiency towards other gas mixtures (e.g., CO <jats:sub>2</jats:sub> /N <jats:sub>2</jats:sub> , CO <jats:sub>2</jats:sub> /CH <jats:sub>4</jats:sub> , C <jats:sub>2</jats:sub> H <jats:sub>4</jats:sub> /C <jats:sub>2</jats:sub> H <jats:sub>6</jats:sub> , and C <jats:sub>3</jats:sub> H <jats:sub>6</jats:sub> /C <jats:sub>3</jats:sub> H <jats:sub>8</jats:sub> ), showing the promising potential as a versatile adsorbent for gas separation and purification.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"40 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146056004","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}
Long Qian, Gaoyuan Gu, Yao Zhu, Yuhao Yin, Songlin Xue, Yuting Dai, Tao Zhang, Dongya Yang, Toshiharu Teranishi, Fengxian Qiu
Activating the lattice oxygen mechanism (LOM) is an effective strategy to enhance the oxygen evolution reaction (OER) activity of catalysts, thereby further promoting overall water splitting for hydrogen production. In this work, a dual modulation electrocatalyst (donated as S, Mo–RuCoO x ) was prepared by ion‐exchange and sulfurization methods. The optimized S, Mo–RuCoO x catalyst demonstrated exceptional OER activity in the alkaline environment with an overpotential of only 222 mV to reach 10 mA cm −2 , as well as an electrolytic cell voltage of 1.62 V at 100 mA cm −2 . The experimental results and theoretical calculations proved that the dual modulation enables the d ‐band center of the RuCo composite to be close to the Fermi energy level ( EF ), which activated the LOM pathway and lowers the reaction energy barrier, thereby enhancing the OER performance. This work presents a facile approach to activate LOM and achieve efficient hydrogen production from water electrolysis.
激活晶格氧机制（LOM）是提高催化剂析氧反应（OER）活性的有效策略，从而进一步促进整体水裂解制氢。本文采用离子交换和硫化法制备了双调制电催化剂S， Mo-RuCoO x。优化后的S， Mo-RuCoO x催化剂在碱性环境中表现出优异的OER活性，过电位仅为222 mV，达到10 mA cm - 2，电解池电压为1.62 V，为100 mA cm - 2。实验结果和理论计算证明，双调制使RuCo复合材料的d波段中心接近费米能级（E F），激活了LOM途径，降低了反应能垒，从而提高了OER性能。这项工作提出了一种简便的方法来激活LOM并实现水电解高效制氢。
{"title":"Lattice oxygen mechanism enhanced alkaline oxygen evolution and water splitting","authors":"Long Qian, Gaoyuan Gu, Yao Zhu, Yuhao Yin, Songlin Xue, Yuting Dai, Tao Zhang, Dongya Yang, Toshiharu Teranishi, Fengxian Qiu","doi":"10.1002/aic.70270","DOIUrl":"https://doi.org/10.1002/aic.70270","url":null,"abstract":"Activating the lattice oxygen mechanism (LOM) is an effective strategy to enhance the oxygen evolution reaction (OER) activity of catalysts, thereby further promoting overall water splitting for hydrogen production. In this work, a dual modulation electrocatalyst (donated as S, Mo–RuCoO <jats:sub> <jats:italic>x</jats:italic> </jats:sub> ) was prepared by ion‐exchange and sulfurization methods. The optimized S, Mo–RuCoO <jats:sub> <jats:italic>x</jats:italic> </jats:sub> catalyst demonstrated exceptional OER activity in the alkaline environment with an overpotential of only 222 mV to reach 10 mA cm <jats:sup>−2</jats:sup> , as well as an electrolytic cell voltage of 1.62 V at 100 mA cm <jats:sup>−2</jats:sup> . The experimental results and theoretical calculations proved that the dual modulation enables the <jats:italic>d</jats:italic> ‐band center of the RuCo composite to be close to the Fermi energy level ( <jats:italic>E</jats:italic> <jats:sub>F</jats:sub> ), which activated the LOM pathway and lowers the reaction energy barrier, thereby enhancing the OER performance. This work presents a facile approach to activate LOM and achieve efficient hydrogen production from water electrolysis.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"88 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146056273","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}
京公网安备 11010802042870号
京ICP备2023020795号-1
扫码关注我们
求助内容：
应助结果提醒方式：