Plasmonic photochemical N2 fixation has received widespread attention owing to the attractive plasmonic enhancement effects in improving solar-to-NH3 conversion efficiency. However, the weak N2 adsorption affinity in metallic plasmonic photocatalysts and insurmountable interfacial barriers in metal–semiconductor plasmonic photocatalysts lead to rapid charge carrier recombination instead of participating in N2-to-NH3 conversion. Herein, a photothermal catalyst Fe-dispersed MoO3−x/MXene with synergistic plasmon resonance hybridization structure is fabricated for photothermal N2 fixation. The hybrid plasmon resonance effects derived from MXene and MoO3−x induce a strong optical response across the ultraviolet–visible-near-infrared range and generation of energetic charge carriers, and the induced photothermal effect further accelerates electron extraction, transport, and surface reaction kinetics. Moreover, the abundant oxygen vacancies and Fe sites can intensify the N2 adsorption and donate the energetic electrons into the anti-bonding system for the stimulative NH coupling process. A high NH3 formation rate of 87.1 μmol g−1 h−1 is achieved under solar-level illumination.
{"title":"Synergistic plasmon resonance hybridization of iron-dispersed MoO3−x/MXene for enhanced nitrogen photothermal reduction","authors":"Ying Tang, Dongsheng Xie, Xiaomin Guo, Lining Fang, Hui Zeng, Zebao Rui","doi":"10.1002/aic.18745","DOIUrl":"https://doi.org/10.1002/aic.18745","url":null,"abstract":"Plasmonic photochemical N<sub>2</sub> fixation has received widespread attention owing to the attractive plasmonic enhancement effects in improving solar-to-NH<sub>3</sub> conversion efficiency. However, the weak N<sub>2</sub> adsorption affinity in metallic plasmonic photocatalysts and insurmountable interfacial barriers in metal–semiconductor plasmonic photocatalysts lead to rapid charge carrier recombination instead of participating in N<sub>2</sub>-to-NH<sub>3</sub> conversion. Herein, a photothermal catalyst Fe-dispersed MoO<sub>3−<i>x</i></sub>/MXene with synergistic plasmon resonance hybridization structure is fabricated for photothermal N<sub>2</sub> fixation. The hybrid plasmon resonance effects derived from MXene and MoO<sub>3−<i>x</i></sub> induce a strong optical response across the ultraviolet–visible-near-infrared range and generation of energetic charge carriers, and the induced photothermal effect further accelerates electron extraction, transport, and surface reaction kinetics. Moreover, the abundant oxygen vacancies and Fe sites can intensify the N<sub>2</sub> adsorption and donate the energetic electrons into the anti-bonding system for the stimulative N<span></span>H coupling process. A high NH<sub>3</sub> formation rate of 87.1 μmol g<sup>−1</sup> h<sup>−1</sup> is achieved under solar-level illumination.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"9 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055391","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}
Marko Tesanovic, J. Pedro de Souza, Martin Z. Bazant, Sonja Berensmeier
High-gradient magnetic separation (HGMS) has traditionally been used in mineral processing, with many effective models developed for typically employed rod-wire shaped matrices. However, its potential in bioprocessing, especially for high-value products, introduces new demands on plant and matrix design. This study presents a multi-scale model for HGMS that simulates new complex geometries, which enhance particle recovery. We have developed microscopic models to accurately simulate the trajectories of magnetic particles within the fluid flow and magnetic fields of HGMS systems. A pivotal aspect of our work is the effective translation of microscopic relationships into macroscopic transport models. The model is validated experimentally using a rotor-stator HGMS system tailored for bioprocessing, with magnetic particle concentration measurements showing strong alignment with the model's predictions. The model's flexibility enables its application across various matrix shapes, overcoming the limitations of traditional rod-wire models, and providing a robust framework for improved HGMS in-silico process understanding and optimization.
{"title":"Magnetic particle capture in high-gradient magnetic separation: A theoretical and experimental study","authors":"Marko Tesanovic, J. Pedro de Souza, Martin Z. Bazant, Sonja Berensmeier","doi":"10.1002/aic.18733","DOIUrl":"https://doi.org/10.1002/aic.18733","url":null,"abstract":"High-gradient magnetic separation (HGMS) has traditionally been used in mineral processing, with many effective models developed for typically employed rod-wire shaped matrices. However, its potential in bioprocessing, especially for high-value products, introduces new demands on plant and matrix design. This study presents a multi-scale model for HGMS that simulates new complex geometries, which enhance particle recovery. We have developed microscopic models to accurately simulate the trajectories of magnetic particles within the fluid flow and magnetic fields of HGMS systems. A pivotal aspect of our work is the effective translation of microscopic relationships into macroscopic transport models. The model is validated experimentally using a rotor-stator HGMS system tailored for bioprocessing, with magnetic particle concentration measurements showing strong alignment with the model's predictions. The model's flexibility enables its application across various matrix shapes, overcoming the limitations of traditional rod-wire models, and providing a robust framework for improved HGMS in-silico process understanding and optimization.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"4 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055173","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}
Lizhi Wu, Ying Zhang, Caixin Zou, Qin Sun, Baozhen Li, Wenchun Zheng, Jiamin Liu, Juncheng He, Yu Tang, Li Tan
Ethane dehydrogenation to aromatics (EDA) is one of the most promising routes to produce aromatics. Herein, the tandem of dehydrogenation component and acidic zeolite are prepared and investigated for EDA. Pt/Fe-S-1 coupled with ZSM-5 of Si/Al of 14 via mixing homogeneously shows excellent EDA performance with 54.0% ethane conversion, 61.5% aromatics selectivity as well as a deactivation rate constant of 0.00010 h−1. According to catalysts characterizations and controlled experiments, it is confirmed the highly dispersed positive Ptδ+ species around Fe species over Pt/Fe-S-1 is the active sites for ethane dehydrogenation to ethylene and subsequent naphthenes dehydrogenation to aromatics, Brønsted acid sites of ZSM-5 and MFI pore are responsible for ethylene oligomerization and cyclization to naphthenes and further naphthenes dehydrogenation to aromatics. The short spatial space between dehydrogenation active sites and acid sites is beneficial for EDA. And the ethylene generation rate is the rate-determining step of EDA.
{"title":"Integration of Pt/Fe-silicalite-1 and acidic zeolite as a bifunctional catalyst for boosting ethane dehydroaromatization","authors":"Lizhi Wu, Ying Zhang, Caixin Zou, Qin Sun, Baozhen Li, Wenchun Zheng, Jiamin Liu, Juncheng He, Yu Tang, Li Tan","doi":"10.1002/aic.18747","DOIUrl":"https://doi.org/10.1002/aic.18747","url":null,"abstract":"Ethane dehydrogenation to aromatics (EDA) is one of the most promising routes to produce aromatics. Herein, the tandem of dehydrogenation component and acidic zeolite are prepared and investigated for EDA. Pt/Fe-S-1 coupled with ZSM-5 of Si/Al of 14 via mixing homogeneously shows excellent EDA performance with 54.0% ethane conversion, 61.5% aromatics selectivity as well as a deactivation rate constant of 0.00010 h<sup>−1</sup>. According to catalysts characterizations and controlled experiments, it is confirmed the highly dispersed positive Pt<sup><i>δ</i>+</sup> species around Fe species over Pt/Fe-S-1 is the active sites for ethane dehydrogenation to ethylene and subsequent naphthenes dehydrogenation to aromatics, Brønsted acid sites of ZSM-5 and MFI pore are responsible for ethylene oligomerization and cyclization to naphthenes and further naphthenes dehydrogenation to aromatics. The short spatial space between dehydrogenation active sites and acid sites is beneficial for EDA. And the ethylene generation rate is the rate-determining step of EDA.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"52 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055172","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 this study, an innovative strategy is proposed to design porous ionic liquids (PILs) using lipophilicity differences, defined as type III-B PIL, which overcomes the traditional size-effect limitations in PIL design. An SBA-15 confined high-entropy single-atom catalyst (HESAC@SBA-15) with an oleophobic internal surface was engineered as the porous framework and oleaginous 1-butyl-3-methylimidazolium tetrafluoroborate as the organic guest for constructing a novel type PIL (PILS-B). This type of PILS-B combines the exceptional gas storage capacity of PILs with the high catalytic activity of HESAC@SBA-15. Additionally, the mesoporous structure of SBA-15 enhances mass transfer during reactions, thereby improving catalytic efficiency. Using the aerobic oxidation of aromatic sulfur compounds in fuel oils as a model reaction, PILS-B achieved a desulfurization efficiency of >99%. This strategy expands the variety of porous frameworks and organic guests for PIL design, showcasing the potential of PILs as effective and stable catalysts with broader applications in catalysis.
{"title":"Type III porous ionic liquids via lipophilicity differences for enhanced oxidation catalysis","authors":"Ruoyu Liu, Chang Deng, Linlin Chen, Yanhong Chao, Peiwen Wu, Wenshuai Zhu, Chunming Xu","doi":"10.1002/aic.18751","DOIUrl":"https://doi.org/10.1002/aic.18751","url":null,"abstract":"In this study, an innovative strategy is proposed to design porous ionic liquids (PILs) using lipophilicity differences, defined as type III-B PIL, which overcomes the traditional size-effect limitations in PIL design. An SBA-15 confined high-entropy single-atom catalyst (HESAC@SBA-15) with an oleophobic internal surface was engineered as the porous framework and oleaginous 1-butyl-3-methylimidazolium tetrafluoroborate as the organic guest for constructing a novel type PIL (PILS-B). This type of PILS-B combines the exceptional gas storage capacity of PILs with the high catalytic activity of HESAC@SBA-15. Additionally, the mesoporous structure of SBA-15 enhances mass transfer during reactions, thereby improving catalytic efficiency. Using the aerobic oxidation of aromatic sulfur compounds in fuel oils as a model reaction, PILS-B achieved a desulfurization efficiency of >99%. This strategy expands the variety of porous frameworks and organic guests for PIL design, showcasing the potential of PILs as effective and stable catalysts with broader applications in catalysis.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"29 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050889","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}
Longyun Zheng, Ao Qi, Kai Guo, Chunjiang Liu, Xin Wen
In this study, a Coanda-swept fluidic oscillator is used to generate oscillating microbubbly flows. Flow behavior measurements show that the generated microbubbly flows have periodic sweep characteristics. Massive microbubbles are generated by shear-off-induced breakup, dynamic erosion breakup, and wall-fluid-shear-induced breakup within the fluidic oscillator. Mass transfer measurements show that the generated microbubbly flows have a higher interfacial area (a) and volumetric liquid-side mass transfer coefficients (kL) than the other comparison groups. Furthermore, the energy efficiency is assessed in terms of kL per energy consumption (η) and energy consumption per a (ξ). For the fluidic oscillator group, the highest kLa is 0.089 s−1, corresponding to (η = 0.63 m3/(kW·s), ξ = 2.6 J/m2, a = 785 m2/m3). Although it has been reported that higher kLa is typically associated with lower energy efficiency, the results indicate that the fluidic oscillator is a promising microbubble generator.
{"title":"Oscillating microbubbly flows generated by a fluidic oscillator: Flow behavior and mass transfer characteristics","authors":"Longyun Zheng, Ao Qi, Kai Guo, Chunjiang Liu, Xin Wen","doi":"10.1002/aic.18736","DOIUrl":"https://doi.org/10.1002/aic.18736","url":null,"abstract":"In this study, a Coanda-swept fluidic oscillator is used to generate oscillating microbubbly flows. Flow behavior measurements show that the generated microbubbly flows have periodic sweep characteristics. Massive microbubbles are generated by shear-off-induced breakup, dynamic erosion breakup, and wall-fluid-shear-induced breakup within the fluidic oscillator. Mass transfer measurements show that the generated microbubbly flows have a higher interfacial area (<i>a</i>) and volumetric liquid-side mass transfer coefficients (<i>k</i><sub>L</sub>) than the other comparison groups. Furthermore, the energy efficiency is assessed in terms of <i>k</i><sub>L</sub> per energy consumption (<b><i>η</i></b>) and energy consumption per <i>a</i> (<b><i>ξ</i></b>). For the fluidic oscillator group, the highest <i>k</i><sub>L</sub><i>a</i> is 0.089 s<sup>−1</sup>, corresponding to (<b><i>η</i></b> = 0.63 m<sup>3</sup>/(kW·s), <b><i>ξ</i></b> = 2.6 J/m<sup>2</sup>, <i>a =</i> 785 m<sup>2</sup>/m<sup>3</sup>). Although it has been reported that higher <i>k</i><sub>L</sub><i>a</i> is typically associated with lower energy efficiency, the results indicate that the fluidic oscillator is a promising microbubble generator.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"118 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050890","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}
Guoxin Wu, Yujing Zhao, Lei Zhang, Jian Du, Qingwei Meng, Qilei Liu
Quantum chemistry (QC) calculations have significantly advanced the development of materials, drugs, and other molecular products. Molecular geometry optimization is an indispensable step for QC calculations. However, its computational cost increases dramatically with increasing molecular system complexity, hindering the large-scale molecule screening. This work proposes a deep learning-based molecular potential energy surface prediction tool (DeePEST) to significantly accelerate geometry optimizations. The key of DeePEST involves the development of a novel machine learning potential model for accurate and fast predictions of molecular energy and atomic forces. These predictions enable efficient molecular geometry optimizations for subsequent predictions of QC properties (single-point energy, dipole moment, HOMO/LUMO, and 13C chemical shifts) and COSMO-SAC-based thermodynamic properties (activity coefficient). Moreover, DeePEST facilitates efficient computer-aided molecular designs that involve QC-based geometry optimizations. The utilization of DeePEST in geometry optimizations achieves high prediction accuracy approaching to rigorous QC methods while maintaining the computational efficiency of molecular mechanics methods.
{"title":"Machine learning potential model for accelerating quantum chemistry-driven property prediction and molecular design","authors":"Guoxin Wu, Yujing Zhao, Lei Zhang, Jian Du, Qingwei Meng, Qilei Liu","doi":"10.1002/aic.18741","DOIUrl":"https://doi.org/10.1002/aic.18741","url":null,"abstract":"Quantum chemistry (QC) calculations have significantly advanced the development of materials, drugs, and other molecular products. Molecular geometry optimization is an indispensable step for QC calculations. However, its computational cost increases dramatically with increasing molecular system complexity, hindering the large-scale molecule screening. This work proposes a deep learning-based molecular potential energy surface prediction tool (DeePEST) to significantly accelerate geometry optimizations. The key of DeePEST involves the development of a novel machine learning potential model for accurate and fast predictions of molecular energy and atomic forces. These predictions enable efficient molecular geometry optimizations for subsequent predictions of QC properties (single-point energy, dipole moment, HOMO/LUMO, and <sup>13</sup>C chemical shifts) and COSMO-SAC-based thermodynamic properties (activity coefficient). Moreover, DeePEST facilitates efficient computer-aided molecular designs that involve QC-based geometry optimizations. The utilization of DeePEST in geometry optimizations achieves high prediction accuracy approaching to rigorous QC methods while maintaining the computational efficiency of molecular mechanics methods.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"24 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050809","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}
Lingjun Pei, Xiaoyu Liu, Xihong He, Wenfeng Li, Dongfeng Sun, Huidong Xie, Hu Liu
High-entropy oxide aerogels (HEOs), combining the advantages of polymetallic oxides and aerogels, are novel materials with great prospect for catalytic applications. However, the preparation of single-phase HEOs remains a great challenge. Herein, we report a general strategy for the preparation of ultralight 3D porous HEOs by combining a gelation strategy and a high-temperature calcination process. The resulting CuFeCoAgPdOx has the structural and morphological advantages of a HEO and an aerogel and exhibits excellent selectivity (100%), full conversion (>99% yield) in the selective hydrogenation of 4-nitrostyrene. In situ Fourier transform infrared spectroscopy (FT-IR) and gas chromatography confirm that the synergistic effect of the HEOs can preferentially reduce the NO2 group rather than the CC bonds in 4-nitrostyrene. The synergistic effect of CuFeCoAgPdOx and the hydrogenation mechanism were revealed. This study provides a new idea for the design of efficient nitroaromatic hydrogenation catalysts.
{"title":"Copper-based high-entropy oxide aerogel for chemoselective hydrogenation reaction","authors":"Lingjun Pei, Xiaoyu Liu, Xihong He, Wenfeng Li, Dongfeng Sun, Huidong Xie, Hu Liu","doi":"10.1002/aic.18748","DOIUrl":"https://doi.org/10.1002/aic.18748","url":null,"abstract":"High-entropy oxide aerogels (HEOs), combining the advantages of polymetallic oxides and aerogels, are novel materials with great prospect for catalytic applications. However, the preparation of single-phase HEOs remains a great challenge. Herein, we report a general strategy for the preparation of ultralight 3D porous HEOs by combining a gelation strategy and a high-temperature calcination process. The resulting CuFeCoAgPdO<sub><i>x</i></sub> has the structural and morphological advantages of a HEO and an aerogel and exhibits excellent selectivity (100%), full conversion (>99% yield) in the selective hydrogenation of 4-nitrostyrene. <i>In situ</i> Fourier transform infrared spectroscopy (FT-IR) and gas chromatography confirm that the synergistic effect of the HEOs can preferentially reduce the <span></span>NO<sub>2</sub> group rather than the CC bonds in 4-nitrostyrene. The synergistic effect of CuFeCoAgPdO<sub><i>x</i></sub> and the hydrogenation mechanism were revealed. This study provides a new idea for the design of efficient nitroaromatic hydrogenation catalysts.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"19 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050886","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}
Zinc-based flow batteries (ZFBs) are promising for large-scale energy storage applications. However, the formation of Zn dendrites and the limited areal capacity of ZFBs hinder their further development. In this study, we designed a digital light-processed 3D-printed pillar array pore ceramic membrane (3DPC) to construct ZFBs with high areal capacity and long cycle life. The pillar array pore design reduces the transmembrane resistance by ~60% and facilitates K+ and Na+ transport. The pore arrays serve as electrolyte reservoirs to regulate interfacial ion distribution and provide sufficient space for Zn deposition. Moreover, the surface hardness of the ceramics up to 1.46 GPa provides resistance against zinc dendrite damage. Furthermore, the cell based on the designed 3DPC exhibits a stable energy efficiency exceeding 79% during operation for over 950 h at an areal capacity of 280 mAh cm−2. This study demonstrates the promising potential of 3D-printed ceramic membranes for metal-based flow batteries.
{"title":"3D-printed pillar array pore ceramic membrane for high areal capacity zinc-based flow battery","authors":"Xin Liu, Kenan Xu, Jingyi Ding, Ting Chen, Xiaoxuan Hou, Hongyan Cao, Yu Xia, Yuqin Lu, Yixing Wang, Su Fan, Kang Huang, Zhi Xu","doi":"10.1002/aic.18728","DOIUrl":"https://doi.org/10.1002/aic.18728","url":null,"abstract":"Zinc-based flow batteries (ZFBs) are promising for large-scale energy storage applications. However, the formation of Zn dendrites and the limited areal capacity of ZFBs hinder their further development. In this study, we designed a digital light-processed 3D-printed pillar array pore ceramic membrane (3DPC) to construct ZFBs with high areal capacity and long cycle life. The pillar array pore design reduces the transmembrane resistance by ~60% and facilitates K<sup>+</sup> and Na<sup>+</sup> transport. The pore arrays serve as electrolyte reservoirs to regulate interfacial ion distribution and provide sufficient space for Zn deposition. Moreover, the surface hardness of the ceramics up to 1.46 GPa provides resistance against zinc dendrite damage. Furthermore, the cell based on the designed 3DPC exhibits a stable energy efficiency exceeding 79% during operation for over 950 h at an areal capacity of 280 mAh cm<sup>−2</sup>. This study demonstrates the promising potential of 3D-printed ceramic membranes for metal-based flow batteries.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"139 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143031376","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}
Fei Zhao, Yongqiang Cheng, Ruisong Zhu, Qinghua Liu, Shuqing Liu, Minghao Song, Qingzhi Lv, Bin Jiang, Zhigang Lei
In the process of butyl rubber production, excessive water content in chloromethane has a significant impact on the conversion and molecular weight distribution of the products. In this work, a computer-aided ionic liquids design method was used for solvent design in the chloromethane dehydration process. The generate-and-test method was utilized to solve the mixed-integer nonlinear programming problem formed in the design process. A multilayer perceptron was trained to predict the surface tension of ionic liquids. Quantum chemical calculations and molecular dynamics simulations were employed to test the dehydration performance of several designed ionic liquids. A candidate was selected for experimental synthesis and characterization. The impact of different ionic liquids on the vapor–liquid equilibrium of water was measured to confirm the feasibility, which indicates that the designed ILs exhibit a better dehydration potential compared to the basement solvent, 1-Ethyl-3-methylimidazolium tetrafluoroborate. Anions play a leading role in the dehydration process.
{"title":"Computer-aided ionic liquids design and molecular insight for chloromethane dehydration","authors":"Fei Zhao, Yongqiang Cheng, Ruisong Zhu, Qinghua Liu, Shuqing Liu, Minghao Song, Qingzhi Lv, Bin Jiang, Zhigang Lei","doi":"10.1002/aic.18737","DOIUrl":"https://doi.org/10.1002/aic.18737","url":null,"abstract":"In the process of butyl rubber production, excessive water content in chloromethane has a significant impact on the conversion and molecular weight distribution of the products. In this work, a computer-aided ionic liquids design method was used for solvent design in the chloromethane dehydration process. The generate-and-test method was utilized to solve the mixed-integer nonlinear programming problem formed in the design process. A multilayer perceptron was trained to predict the surface tension of ionic liquids. Quantum chemical calculations and molecular dynamics simulations were employed to test the dehydration performance of several designed ionic liquids. A candidate was selected for experimental synthesis and characterization. The impact of different ionic liquids on the vapor–liquid equilibrium of water was measured to confirm the feasibility, which indicates that the designed ILs exhibit a better dehydration potential compared to the basement solvent, 1-Ethyl-3-methylimidazolium tetrafluoroborate. Anions play a leading role in the dehydration process.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"58 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143026676","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}
Zongyang Ya, Lei Tang, Dong Xu, Hua Wang, Shengbo Zhang
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 gcatal−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 gcatal−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.
{"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-C<sub>3</sub>N<sub>4</sub> nanotube catalyst with well-defined structure for photoreforming poly(ethylene terephthalate) (PET) into valuable chemicals and H<sub>2</sub>. This catalyst achieved a H<sub>2</sub> evolution rate of 3240 μmol g<sub>catal</sub><sup>−1</sup> h<sup>−1</sup>, 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 H<sub>2</sub> evolution rate of 475 μmol g<sub>catal</sub><sup>−1</sup> h<sup>−1</sup> 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}
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