Xue-Li Cao, Tian Tian, Yong Bai, Chun Cui, Cong Luo, Jiang-Shan Xing, Chuan-Yu Chen, Lili Zhao, Shi-Peng Sun
Traditional nanofiltration membranes often struggle to maintain stability in harsh environments due to issues like swelling, chemical bond dissociation, and polymer chain creep. Fluoropolymers like poly(ethylene-chlorotrifluoroethylene) (ECTFE) are promising substrate candidates for broad-spectrum corrosion-resistant nanofiltration (CRNF) membranes, but their solvent insolubility and hydrophobicity present significant processing challenges. This study harnesses the electrospinnability and abundant reactive sites of polyvinyl alcohol to create a reactive site-bridged nanofibrous network. This network provides reactive sites to decorate the hydrophobic ECTFE substrate and bridges the molecular selective layer through aldolization, Schiff base reactions, and esterification. The resulting robust thin-film nanofibrous composite membranes exhibit high rejection rates for small molecular dyes under a variety of harsh conditions, including exposure to 10 wt% H2SO4, 1 M NaOH, ethanol, N,N-dimethylformamide, N-methylpyrrolidone, and 80°C solutions. This work paves the way for designing next-generation broad-spectrum CRNF membranes, enhancing their applicability in diverse harsh environments.
{"title":"Broad-spectrum corrosion-resistant nanofiltration membranes via reactive site-bridged nanofibrous network","authors":"Xue-Li Cao, Tian Tian, Yong Bai, Chun Cui, Cong Luo, Jiang-Shan Xing, Chuan-Yu Chen, Lili Zhao, Shi-Peng Sun","doi":"10.1002/aic.18699","DOIUrl":"https://doi.org/10.1002/aic.18699","url":null,"abstract":"Traditional nanofiltration membranes often struggle to maintain stability in harsh environments due to issues like swelling, chemical bond dissociation, and polymer chain creep. Fluoropolymers like poly(ethylene-chlorotrifluoroethylene) (ECTFE) are promising substrate candidates for broad-spectrum corrosion-resistant nanofiltration (CRNF) membranes, but their solvent insolubility and hydrophobicity present significant processing challenges. This study harnesses the electrospinnability and abundant reactive sites of polyvinyl alcohol to create a reactive site-bridged nanofibrous network. This network provides reactive sites to decorate the hydrophobic ECTFE substrate and bridges the molecular selective layer through aldolization, Schiff base reactions, and esterification. The resulting robust thin-film nanofibrous composite membranes exhibit high rejection rates for small molecular dyes under a variety of harsh conditions, including exposure to 10 wt% H<sub>2</sub>SO<sub>4</sub>, 1 M NaOH, ethanol, <i>N</i>,<i>N</i>-dimethylformamide, <i>N</i>-methylpyrrolidone, and 80°C solutions. This work paves the way for designing next-generation broad-spectrum CRNF membranes, enhancing their applicability in diverse harsh environments.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"28 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841893","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}
Solvent extraction of lithium by β-diketones from alkaline brine has been known to be an efficient process. However, its relatively high working pH, consequently the high alkaline consumption and substantial dissolution loss in raffinate, limit its industrial application. Herein, a novel lithium extractant, i.e., 2-hydroxy-5-nitro-4-n-octoxy-benzophenone (referred to as N531), was proposed, which can extract lithium at relatively lower pH with remarkable low alkaline consumption and dissolution loss. Exactly, the pH corresponding to half lithium extraction is 8.5, and the Li/Na separation factor is ~500. The extractant concentration in the raffinate varied from 0.8 to 9.3 mg L−1, depending on the pH and salinity. An application case was given to extract lithium from the raw brine of Zabuye salt lake, indicating that N531 is a commercially prospective extractant to extract lithium from alkaline brine.
{"title":"Lithium solvent extraction from weak alkaline brine by 2-hydroxy-5-nitro-4-alkoxy-benzophenone and TRPO","authors":"Guimei Zhou, Wenjun Yan, Shufan Yan, Dandan Gao, Debin Zeng, Dongdong Li, Dewen Zeng","doi":"10.1002/aic.18703","DOIUrl":"https://doi.org/10.1002/aic.18703","url":null,"abstract":"Solvent extraction of lithium by β-diketones from alkaline brine has been known to be an efficient process. However, its relatively high working pH, consequently the high alkaline consumption and substantial dissolution loss in raffinate, limit its industrial application. Herein, a novel lithium extractant, i.e., 2-hydroxy-5-nitro-4-<i>n</i>-octoxy-benzophenone (referred to as N531), was proposed, which can extract lithium at relatively lower pH with remarkable low alkaline consumption and dissolution loss. Exactly, the pH corresponding to half lithium extraction is 8.5, and the Li/Na separation factor is ~500. The extractant concentration in the raffinate varied from 0.8 to 9.3 mg L<sup>−1</sup>, depending on the pH and salinity. An application case was given to extract lithium from the raw brine of Zabuye salt lake, indicating that N531 is a commercially prospective extractant to extract lithium from alkaline brine.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"30 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841856","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}
The understanding of thermocapillary convection is important in both fundamental and industrial aspects. However, efficient tools that can provide dynamic details of the convective flows are still lacking. Here, we discovered a unique phenomenon of photoinduced fluorogenic shift of HDPI derivatives in chloroform and utilized this trait to map the temperature field and capillary flow on the surface of or inside volatile chloroform with a high spatial resolution and a long observation window. By inducing a proper co-imaging agent that enhanced the fluorescence contrast via generating more distinguishable chromaticity, the fluorescence-based method exhibited further enhanced imaging resolution and elongated observation time, facilitating the continuous monitoring of temperature field and capillary flow. This work presents a powerful tool to study the behaviors of fluid (thermo-)dynamics.
{"title":"Fluorescent imaging agents for mapping temperature field and capillary flow on the surface of volatile solvent","authors":"Hao Gu, Sibo Wan, Sheng Lu, Yahui Chen, Fang Wang, Shiyue Zheng, Yourong Li, Xiaoqiang Chen","doi":"10.1002/aic.18696","DOIUrl":"https://doi.org/10.1002/aic.18696","url":null,"abstract":"The understanding of thermocapillary convection is important in both fundamental and industrial aspects. However, efficient tools that can provide dynamic details of the convective flows are still lacking. Here, we discovered a unique phenomenon of photoinduced fluorogenic shift of <b>HDPI</b> derivatives in chloroform and utilized this trait to map the temperature field and capillary flow on the surface of or inside volatile chloroform with a high spatial resolution and a long observation window. By inducing a proper co-imaging agent that enhanced the fluorescence contrast via generating more distinguishable chromaticity, the fluorescence-based method exhibited further enhanced imaging resolution and elongated observation time, facilitating the continuous monitoring of temperature field and capillary flow. This work presents a powerful tool to study the behaviors of fluid (thermo-)dynamics.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"28 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841853","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}
This perspectives article outlines and discusses the future of supply chains. The existing challenges and flaws in supply chains design and management are described, motivating the need for the next-generation supply chains. We present a holistic paradigm for viewing and analyzing supply chains as networks of networks with various dimensions, hierarchies, and players with their various forms of decision-making. Cyber-Physical Systems is offered as a key enabler to obtain a digital supply chain exhibiting the features of heterogeneity, interoperability, modularity, customizability, decentralization, autonomy, and cooperativity. The role of virtual assistants is described, along with research directions to create the technology for establishing true digital supply chains. The role of Process Systems Engineering (PSE) is outlined with the hope that the ideas discussed will motivate the PSE community to become active participants in attaining the next-generation supply chains.
本视角文章概述并讨论了供应链的未来。文章描述了供应链设计和管理中现有的挑战和缺陷，从而激发了对下一代供应链的需求。我们提出了一个整体范式，将供应链视为具有不同维度、层级和参与者及其各种决策形式的网络之网，并对其进行分析。网络物理系统是实现数字化供应链的关键因素，它具有异构性、互操作性、模块化、可定制性、分散性、自主性和合作性等特点。本文介绍了虚拟助手的作用，以及为建立真正的数字供应链创造技术的研究方向。此外，还概述了流程系统工程（PSE）的作用，希望所讨论的观点能激励 PSE 社区成为实现下一代供应链的积极参与者。
{"title":"Digital supply chain: An industrial perspective","authors":"John M. Wassick, Hector D. Perez","doi":"10.1002/aic.18688","DOIUrl":"https://doi.org/10.1002/aic.18688","url":null,"abstract":"This perspectives article outlines and discusses the future of supply chains. The existing challenges and flaws in supply chains design and management are described, motivating the need for the next-generation supply chains. We present a holistic paradigm for viewing and analyzing supply chains as networks of networks with various dimensions, hierarchies, and players with their various forms of decision-making. Cyber-Physical Systems is offered as a key enabler to obtain a digital supply chain exhibiting the features of heterogeneity, interoperability, modularity, customizability, decentralization, autonomy, and cooperativity. The role of virtual assistants is described, along with research directions to create the technology for establishing true digital supply chains. The role of Process Systems Engineering (PSE) is outlined with the hope that the ideas discussed will motivate the PSE community to become active participants in attaining the next-generation supply chains.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"87 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832670","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}
Louis Kontschak, Oliver Gruschke, Lena Trapp, Hatice Nur Baser, Neil MacKinnon, Philippe Rychen, Hermann Nirschl, Gisela Guthausen
Ion exchange resins were studied on different length scales by magnetic resonance imaging (MRI) with the focus on their interactions with nanoparticles (NP) and molecular clusters. On the length scale of resin beds (bed diameters <20 mm), the behavior of NP and of molecular clusters was shown to depend on the kind of ion exchange resin and nanoscale moiety. The kinetics of absorption and penetration into the resin beads was quantified on a smaller length scale of a stack of resin beads (sample with an outer diameter of 1.7 mm). Finally, using an MRI μ-coil (3D spatial resolution ≥8 μm), adsorption of superparamagnetic NP on individual resin beads was observed via the magnetic field disturbance characteristic for magnetic dipoles. As a result, this allows the detection of NP (diameter ≤100 nm) by MRI on much larger length scales of several micrometers.
{"title":"MRI on ion exchange resins at different length scales","authors":"Louis Kontschak, Oliver Gruschke, Lena Trapp, Hatice Nur Baser, Neil MacKinnon, Philippe Rychen, Hermann Nirschl, Gisela Guthausen","doi":"10.1002/aic.18659","DOIUrl":"https://doi.org/10.1002/aic.18659","url":null,"abstract":"Ion exchange resins were studied on different length scales by magnetic resonance imaging (MRI) with the focus on their interactions with nanoparticles (NP) and molecular clusters. On the length scale of resin beds (bed diameters <20 mm), the behavior of NP and of molecular clusters was shown to depend on the kind of ion exchange resin and nanoscale moiety. The kinetics of absorption and penetration into the resin beads was quantified on a smaller length scale of a stack of resin beads (sample with an outer diameter of 1.7 mm). Finally, using an MRI μ-coil (3D spatial resolution ≥8 μm), adsorption of superparamagnetic NP on individual resin beads was observed via the magnetic field disturbance characteristic for magnetic dipoles. As a result, this allows the detection of NP (diameter ≤100 nm) by MRI on much larger length scales of several micrometers.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"86 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841848","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}
Aqueous amine solution is a promising absorbent for CO2 capture, yet irreversible reaction, that is, degradation can happen for amine and leads to performance decrease and many operating difficulties. Despite numerous research on reaction between amine and CO2 for absorption, the reaction of amine degradation is not fully understood, especially for tertiary amine which is a vital component in constructing high-performance CO2 absorbent. Considering the variety of tertiary amines, this article studied the thermal stability of five tertiary amine solutions at different temperatures to mimic the regeneration condition. The density functional theory (DFT) calculation was applied to reveal the degradation mechanism. The alkylation reaction that triggered the degradation of tertiary amine was deemed as the limiting step. Then the molecular simulation method was extended to 12 tertiary amines, aiming to further illustrate the influence of molecular structure on the alkylation reaction. These results provide basic data and theoretical guidance for developing the anti-degradation CO2 absorbent.
{"title":"Thermal degradation of tertiary amine for CO2 capture: Structure–activity relationships and density functional theory calculations","authors":"Tong Luo, Qi Liu, Min Xiao, Hongxia Gao, Teerawat Sema, Zhiwu Liang","doi":"10.1002/aic.18702","DOIUrl":"https://doi.org/10.1002/aic.18702","url":null,"abstract":"Aqueous amine solution is a promising absorbent for CO<sub>2</sub> capture, yet irreversible reaction, that is, degradation can happen for amine and leads to performance decrease and many operating difficulties. Despite numerous research on reaction between amine and CO<sub>2</sub> for absorption, the reaction of amine degradation is not fully understood, especially for tertiary amine which is a vital component in constructing high-performance CO<sub>2</sub> absorbent. Considering the variety of tertiary amines, this article studied the thermal stability of five tertiary amine solutions at different temperatures to mimic the regeneration condition. The density functional theory (DFT) calculation was applied to reveal the degradation mechanism. The alkylation reaction that triggered the degradation of tertiary amine was deemed as the limiting step. Then the molecular simulation method was extended to 12 tertiary amines, aiming to further illustrate the influence of molecular structure on the alkylation reaction. These results provide basic data and theoretical guidance for developing the anti-degradation CO<sub>2</sub> absorbent.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"52 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841874","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}
Sirui Ding, Jianfeng Wu, Zhen Huang, Sen Chang, Baoliang Zhang
For protein imprinting, template molecule anchoring and imprinting site recognition are very important processes. Herein, we have proposed for the first time to use photo-switchable host–guest interactions between α-cyclodextrin (α-CD)-modified bovine serum albumin (BSA) and azobenzene coated organic covalent framework (COF) to immobilize and elute proteins. A novel surface labeled polymer microspheres (COF-MIPs) were constructed, which could reduce the mass transfer resistance and accelerate the adsorption process, resulting in the adsorption equilibrium reaching 60 min and the saturated adsorption amount of 563.86 mg/g. Additionally, using guest molecules (azobenzene) to label the imprinted sites allows the correlation of the relationship between the fluorescence intensity and the protein adsorption process. The fluorescence analyses show that the material exhibits excellent adsorption specificity, with imprinting factors greater than 4. This work extended the application of the host–guest interaction between cyclodextrin and azobenzene and provides a new approach for developing protein-imprinting materials.
{"title":"Exploration of BSA imprinting mechanism by fluorescence anchoring and host–guest interactions","authors":"Sirui Ding, Jianfeng Wu, Zhen Huang, Sen Chang, Baoliang Zhang","doi":"10.1002/aic.18680","DOIUrl":"https://doi.org/10.1002/aic.18680","url":null,"abstract":"For protein imprinting, template molecule anchoring and imprinting site recognition are very important processes. Herein, we have proposed for the first time to use photo-switchable host–guest interactions between α-cyclodextrin (α-CD)-modified bovine serum albumin (BSA) and azobenzene coated organic covalent framework (COF) to immobilize and elute proteins. A novel surface labeled polymer microspheres (COF-MIPs) were constructed, which could reduce the mass transfer resistance and accelerate the adsorption process, resulting in the adsorption equilibrium reaching 60 min and the saturated adsorption amount of 563.86 mg/g. Additionally, using guest molecules (azobenzene) to label the imprinted sites allows the correlation of the relationship between the fluorescence intensity and the protein adsorption process. The fluorescence analyses show that the material exhibits excellent adsorption specificity, with imprinting factors greater than 4. This work extended the application of the host–guest interaction between cyclodextrin and azobenzene and provides a new approach for developing protein-imprinting materials.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"256 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841854","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}
In the context of achieving continuous synthesis of acyl peroxides using microreactors, continuous preparation of alkaline hydrogen peroxide (AHP) solution is required. However, two key issues, Na2O2 precipitation and H2O2 decomposition, need to be considered or addressed. For the precipitation of Na2O2 during NaOH and H2O2 mixing, experiments revealed that precipitation could be avoided by appropriate selection of operation window. For the risk of violent H2O2 decomposition when NaOH and H2O2 solutions are one-step mixed, theoretical approaches were adopted. Simulation-derived mixing time is combined with decomposition kinetics to find a direct relationship between operation-structure parameters and percentage of decomposed H2O2. This percentage is estimated to be in the order of 10−4 for micromixing devices, which indicates that micromixing devices can be used to one-step mix NaOH and H2O2 solution without causing violent H2O2 decomposition. This work provides insights into the preparation of AHP solution and facilitates its continuous preparation.
{"title":"Continuous preparation of alkaline hydrogen peroxide solution by micromixing device: Experiment and theoretical analysis","authors":"Shunkai Xia, Xude Yu, Zhuo Chen, Jianhong Xu","doi":"10.1002/aic.18668","DOIUrl":"https://doi.org/10.1002/aic.18668","url":null,"abstract":"In the context of achieving continuous synthesis of acyl peroxides using microreactors, continuous preparation of alkaline hydrogen peroxide (AHP) solution is required. However, two key issues, Na<sub>2</sub>O<sub>2</sub> precipitation and H<sub>2</sub>O<sub>2</sub> decomposition, need to be considered or addressed. For the precipitation of Na<sub>2</sub>O<sub>2</sub> during NaOH and H<sub>2</sub>O<sub>2</sub> mixing, experiments revealed that precipitation could be avoided by appropriate selection of operation window. For the risk of violent H<sub>2</sub>O<sub>2</sub> decomposition when NaOH and H<sub>2</sub>O<sub>2</sub> solutions are one-step mixed, theoretical approaches were adopted. Simulation-derived mixing time is combined with decomposition kinetics to find a direct relationship between operation-structure parameters and percentage of decomposed H<sub>2</sub>O<sub>2</sub>. This percentage is estimated to be in the order of 10<sup>−4</sup> for micromixing devices, which indicates that micromixing devices can be used to one-step mix NaOH and H<sub>2</sub>O<sub>2</sub> solution without causing violent H<sub>2</sub>O<sub>2</sub> decomposition. This work provides insights into the preparation of AHP solution and facilitates its continuous preparation.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"30 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825603","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}
Exploring efficient Pt‐based catalysts for the selective oxidation of polyol is still a challenge due to the lack of a mechanism‐driven approach. Here, low‐Pt content PdM3 were systematically investigated for glycerol oxidation to glyceric acid (GLYA) by density functional theory (DFT) linear synchronous transit and quadratic synchronous transit (LST/QST) assisted descriptor‐based micro‐kinetic modeling. Results revealed that the PdM3 surface induces the dissociation of O2 and H2O to form a polarized PdM3‐OH* surface, participating in the subsequent adsorption and activation of glycerol and oxygen‐containing intermediates. Moreover, the binding energy of O and H on the PdM3 could be labeled as descriptors describing catalytic selectivity and activity. On this basis, a strong electron reconstruction effect described by EO (−4.5 to −3.0 eV) and appropriate dehydrogenation ability described by EH (−3.5 to −2.5 eV) contribute to the improvement of catalytic performance for the selective oxidation of glycerol to GLYA. This study may give insights into the rational design of high‐efficient Pt‐based catalysts for polyol oxidation.
{"title":"General descriptors for glycerol oxidation to glyceric acid over PtM3‐derived bimetallic catalysts in base‐free medium","authors":"Hao Yan, Jiarong Lu, Yaqian Li, Xiang Feng, Xin Zhou, Hui Zhao, Chaohe Yang","doi":"10.1002/aic.18683","DOIUrl":"https://doi.org/10.1002/aic.18683","url":null,"abstract":"Exploring efficient Pt‐based catalysts for the selective oxidation of polyol is still a challenge due to the lack of a mechanism‐driven approach. Here, low‐Pt content PdM<jats:sub>3</jats:sub> were systematically investigated for glycerol oxidation to glyceric acid (GLYA) by density functional theory (DFT) linear synchronous transit and quadratic synchronous transit (LST/QST) assisted descriptor‐based micro‐kinetic modeling. Results revealed that the PdM<jats:sub>3</jats:sub> surface induces the dissociation of O<jats:sub>2</jats:sub> and H<jats:sub>2</jats:sub>O to form a polarized PdM<jats:sub>3</jats:sub>‐OH* surface, participating in the subsequent adsorption and activation of glycerol and oxygen‐containing intermediates. Moreover, the binding energy of O and H on the PdM<jats:sub>3</jats:sub> could be labeled as descriptors describing catalytic selectivity and activity. On this basis, a strong electron reconstruction effect described by <jats:italic>E</jats:italic><jats:sub>O</jats:sub> (−4.5 to −3.0 eV) and appropriate dehydrogenation ability described by <jats:italic>E</jats:italic><jats:sub>H</jats:sub> (−3.5 to −2.5 eV) contribute to the improvement of catalytic performance for the selective oxidation of glycerol to GLYA. This study may give insights into the rational design of high‐efficient Pt‐based catalysts for polyol oxidation.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"3 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825183","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}
Electrified methanol steam reforming (MSR) assisted by nonthermal plasma (NTP) is a pivotal enabler for clean hydrogen production at ambient conditions with several advantages. This study optimizes the NTP-assisted MSR by catalyst engineering, as well as membrane technology (via a 2D MXene nanosheet membrane reactor). Our findings reveal that active-phase engineering in catalyst design is crucial in regulating MSR pathways under NTP conditions with the bimetallic Ni–Cu alloys enhancing the H2 production via surface water–gas shift reaction (WGSR). Additionally, integrating a MXene membrane within a dielectric barrier discharge (DBD) NTP reactor enabled the reactive-separation process, improving methanol conversion, H2 formation rate with higher purity, as well as showing a good stability.
{"title":"Enhancing H2 production from plasma-assisted methanol steam reforming by catalyst engineering in a MXene membrane reactor","authors":"Shaowei Chen, Zong Lu, Jiangqi Niu, Yan Shao, Yi Chen, Yaru Ni, Xiaoying Liu, Xiaoyang Wei, Xiaoxia Ou, Xiaolei Fan, Yanying Wei, Huanhao Chen","doi":"10.1002/aic.18685","DOIUrl":"https://doi.org/10.1002/aic.18685","url":null,"abstract":"Electrified methanol steam reforming (MSR) assisted by nonthermal plasma (NTP) is a pivotal enabler for clean hydrogen production at ambient conditions with several advantages. This study optimizes the NTP-assisted MSR by catalyst engineering, as well as membrane technology (via a 2D MXene nanosheet membrane reactor). Our findings reveal that active-phase engineering in catalyst design is crucial in regulating MSR pathways under NTP conditions with the bimetallic Ni–Cu alloys enhancing the H<sub>2</sub> production via surface water–gas shift reaction (WGSR). Additionally, integrating a MXene membrane within a dielectric barrier discharge (DBD) NTP reactor enabled the reactive-separation process, improving methanol conversion, H<sub>2</sub> formation rate with higher purity, as well as showing a good stability.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"06 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142820956","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}
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