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Challenges in Developing MOF-Based Membranes for Gas Separation

Langmuir 2023年第8期39卷 2871-2880页

作者： Kang, Dun-Yen Lee, Jong Suk Department of Chemical Engineering National Taiwan University No. 1 Sec. 4 Roosevelt Road Taipei10617 Taiwan International Graduate Program of Molecular Science and Technology National Taiwan University No. 1 Sec. 4 Roosevelt Road Taipei10617 Taiwan Center of Atomic Initiative for New Materials National Taiwan University No. 1 Sec. 4 Roosevelt Road Taipei10617 Taiwan Department of Chemical and Biomolecular Engineering Sogang University Baekbeom-ro 35 Seoul4107 Korea Republic of Institute of Emergent Materials Sogang University 35 Baekbeom-ro Seoul4107 Korea Republic of

Metal-organic frameworks (MOFs) are promising candidates for membrane gas separation. MOF-based membranes include pure MOF membranes and MOF-based mixed matrix membranes (MMMs). This Perspective discusses the challenges for the next stage of the development of MOF-based membranes based on research conducted in the past decade. We focused on three major issues associated with pure MOF membranes. First, some MOF compounds have been overstudied, despite the availability of numerous MOFs. Second, gas adsorption and diffusion in MOFs are often independently investigated. The correlation between adsorption and diffusion has seldom been discussed. Third, we identify the importance of characterizing the gas distribution in MOFs to understand the structure-property relationships for gas adsorption and diffusion in MOF membranes. For MOF-based MMMs, engineering the MOF-polymer interface is essential for achieving the desired separation performance. Various approaches to modify the MOF surface or polymer molecular structure have been proposed to improve the MOF-polymer interface. Herein, we present defect engineering as a facile and efficient approach for engineering the MOF-polymer interfacial morphology and its extended application for various gas separations. © 2023 American chemical Society.

关键词： Organometallics

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Molecular insight of dissolved organic matter and chlorinated disinfection by-products in reclaimed water during chlorination with permanganate preoxidation

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Chemosphere 2024年 349卷 140807页

作者： Hu, Wei Niu, Xi-Zhi Chen, Huan Ye, Bei Liang, Jun-Kun Guan, Yun-Tao Wu, Qian-Yuan Environmental Protection Key Laboratory of Microorganism Application and Risk Control Guangdong Provincial Engineering Research Center for Urban Water Recycling and Environmental Safety Institute of Environment and Ecology Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen518055 China Environmental Engineering and Science Program Department of Chemical and Environmental Engineering University of Cincinnati CincinnatiOH45221 United States Department of Environmental Engineering and Earth Science Clemson University SC29634 United States

Permanganate is a common preoxidant applied in water treatment to remove organic pollutants and to reduce the formation of disinfection by-products. However, the effect of permanganate preoxidation on the transformation of dissolved effluent organic matter (dEfOM) and on the formation of unknown chlorinated disinfection by-products (Cl-DBPs) during chlorination remains unknown at molecular level. In this work, the molecular changes of dEfOM during permanganate preoxidation and subsequent chlorination were characterized using Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS). Permanganate preoxidation was found to decrease the DBE (double bond equivalent) and AImod (modified aromaticity index) of the dEfOM. The identity and fate of over 400 unknown Cl-DBPs during KMnO4-chlorine treatment were investigated. Most Cl-DBPs and the precursors were found to be highly unsaturated aliphatic and phenolic compounds. The Cl-DBPs precursors with lower H/C and lower O/C were preferentially removed by permanganate preoxidation. Additionally, permanganate preoxidation decreased the number of unknown Cl-DBPs by 30% and intensity of unknown Cl-DBPs by 25%. One-chlorine-containing DBPs were the major Cl-DBPs and had more CH2 groups and higher DBEw than Cl-DBPs containing two and three chlorine atoms. 60% of the Cl-DBPs formation was attributed to substitution reactions (i.e., +Cl–H, +2Cl–2H, +3Cl–3H, +ClO–H, +Cl2O3–2H). This work provides detailed molecular level information on the efficacy of permanganate preoxidation on the control of overall Cl-DBPs formation during chlorination. © 2023 Elsevier Ltd

关键词： Chlorination

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Waste-battery-derived multifunctional zinc catalysts for glycolysis and decolorization of polyethylene terephthalate

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Applied Catalysis B: Environmental 2023年第1期325卷

作者： Chiao, Yu-Wen Liao, Weisheng Krisbiantoro, Philip Anggo Yu, Bor-Yih Wu, Kevin C.-W. Department of Chemical Engineering National Taiwan University Taipei10617 Taiwan Molecular Science and Technology Program Taiwan International Graduate Program Academia Sinica Taipei11529 Taiwan International Graduate Program of Molecular Science and Technology National Taiwan University Taipei10617 Taiwan

In this study, novel and easily recyclable catalysts were prepared from waste batteries for efficient glycolysis and decolorization of polyethylene terephthalate (PET) to obtain bis(2-hydroxyethyl) terephthalate (BHET). At 190 °C and 5 h, the PET conversion and BHET yield reach 89.7 and 77.7%, respectively, which are comparable to the values obtained for the commonly used catalyst zinc acetate. Species generated from the reaction between ethylene glycol (EG) and zinc plates (e.g., Zn-glycolate, ZnO, and other metal species on zinc plates) demonstrate excellent catalytic performance. Furthermore, dye molecules released from several commercial-colored PET bottles during glycolysis can be degraded to colorless molecules using zinc plates, thereby facilitating BHET purification. The exposed zero-valent zinc from the zinc plates in EG is responsible for degrading the dye molecules. Finally, the scaled-up PET glycolysis process is conceptually designed using Aspen Plus software. The simulation results suggest that reducing the energy requirement in distillation is necessary for further improvement. © 2022 Elsevier B.V.

关键词： Polyethylene terephthalates

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Discovery of Ni Activated Sintering of MoNbTaW Predicted by a Computed Grain Boundary Diagram

SSRN

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SSRN 2023年

作者： Shivakumar, Sashank Song, Keqi Wang, Chunyang Lei, Tianjiao Xin, Huolin L. Rupert, Timothy J. Luo, Jian Department of Nano and Chemical Engineering Program of Materials Science and Engineering University of California San Diego La Jolla CA92093 United States Department of Physics and Astronomy University of California IrvineCA92697 United States Department of Materials Science and Engineering Department of Mechanical and Aerospace Engineering University of California IrvineCA92697 United States

Activated sintering of refractory metals represents a classical phenomenon in powder metallurgy. This study discovers that Ni addition can enhance sintering of MoNbTaW both above and below the bulk solidus composition at 1800 °C, thereby demonstrating the first example of activated sintering of a high-entropy alloy. To probe the underlying mechanism, experiments reveal complete grain boundary (GB) wetting above the bulk solidus composition, which logically infers the stabilization of a liquid-like interfacial phase (GB complexion) in a prewetting region below the bulk solidus composition. Furthermore, bulk CALPHAD (calculation of phase diagram) methods have been extended to model GBs in Ni-doped MoNbTaW to compute a GB "phase" diagram to forecast high-temperature GB disordering in the prewetting region and rationalize the observed Ni activated sintering of MoNbTaW. Only weak GB segregation of Ni is found in furnace-cooled specimens, which suggests GB "drying" during cooling, consistent with the observed nanoscale precipitates along GBs. © 2023, The Authors. All rights reserved.

关键词： Grain boundaries

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Design of an Array Transducer for Localizing Microbubble Activity Through the Skull

Design of an Array Transducer for Localizing Microbubble Act...

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IEEE International Symposium on Applications of Ferroelectrics (ISAF)

作者： Malachy Newman Jiro Kusunose M. Anthony Phipps Allison Dockum Ainsley McDonald-Boyer Charles Caskey Department of Biomedical Engineering Vanderbilt University Nashville USA Department of Radiology Vanderbilt Institute of Imaging Science Vanderbilt University Nashville USA Program in Chemical and Physical Biology Vanderbilt University Nashville USA

ISBN: (数字)9798350371901

ISBN: (纸本)9798350371918

Transcranial focused ultrasound is an important tool for opening the blood brain barrier (BBB), which is typically performed by focusing ultrasonic energy through the skull into regions that have been perfused with microbubbles (MB). When sonicated, these MB oscillate and temporarily disrupt the local BBB. The procedure can be monitored for effectiveness and safety by analyzing the spectral content of echoes, and by using multiple receivers, where the active MB’s position can be triangulated, allowing for the localization of the BBB opening. The monitoring and localization of MB has been performed in rodents but translating into larger animals is a major challenge due to attenuation at the skull. Here, we used acoustic simulations to design a multi-element transmit array with multiple receivers and characterized its ability to generate a focus through the non-human primate (NHP) skull and assessed its performance in localizing MB activity while varying number and spatial arrangement of receivers, optimizing the focal gain, focal spot size, and ability to localize a MB. The resultant transducer allows for the delivery of high pressure at brain-region sized targets and can localize MB signals.

关键词： Location awareness Transducers Ultrasonic imaging Rodents Receivers Acoustics Safety In vitro Monitoring Frequency control

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Optimal Planning of Hybrid Energy Storage Systems Using Curtailed Renewable Energy Through Deep Reinforcement Learning

SSRN

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SSRN 2023年

作者： Kang, Dongju Kang, Doeun Hwangbo, Sumin Niaz, Haider Lee, Won Bo Liu, J. Jay Na, Jonggeol School of Chemical and Biological Engineering Seoul National University Gwanak-ro 1 Gwanak-gu Seoul08826 Korea Republic of Department of Chemical Engineering and Materials Science Ewha Womans University Seoul03760 Korea Republic of Graduate Program in System Health Science and Engineering Ewha Womans University Seoul03760 Korea Republic of Department of Chemical Engineering Pukyong National University Busan48513 Korea Republic of

Energy management systems (EMS) are becoming increasingly important in order to utilize the continuously growing curtailed renewable energy. Promising energy storage systems (ESS), such as batteries and green hydrogen should be employed to maximize the efficiency of energy stakeholders. However, optimal decision-making, i.e., planning the leveraging between different strategies, is confronted with the complexity and uncertainties of large-scale problems. Here, we propose a sophisticated deep reinforcement learning (DRL) methodology with a policy-based algorithm to realize the real-time optimal ESS planning under the curtailed renewable energy uncertainty. A quantitative performance comparison proved that the DRL agent outperforms the scenario-based stochastic optimization (SO) algorithm, even with a wide action and observation space. Owing to the uncertainty rejection capability of the DRL, we could confirm a robust performance, under a large uncertainty of the curtailed renewable energy, with a maximizing net profit and stable system. Action-mapping was performed for visually assessing the action taken by the DRL agent according to the state. The corresponding results confirmed that the DRL agent learns the way like what a human expert would do, suggesting reliable application of the proposed methodology. © 2023, The Authors. All rights reserved.

关键词： Reinforcement learning

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Machine Learning for Identifying Grain Boundaries in Scanning Electron Microscopy (SEM) Images of Nanoparticle Superlattices

arXiv

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arXiv 2025年

作者： Paruchuri, Aanish Thrasher, Carl Hart, A.J. Macfarlane, Robert Jayaraman, Arthi Science in Data Science Program University of Delaware NewarkDE19713 United States Department of Materials Science and Engineering Massachusetts Institute of Technology CambridgeMA02139 United States Department of Mechanical Engineering Massachusetts Institute of Technology CambridgeMA02139 United States Department of Chemical and Biomolecular Engineering University of Delaware 150 Academy St NewarkDE19713 United States Department of Materials Science and Engineering University of Delaware NewarkDE19713 United States Data Science Institute University of Delaware NewarkDE19713 United States

Nanoparticle superlattices consisting of ordered arrangements of nanoparticles exhibit unique optical, magnetic, and electronic properties arising from nanoparticle characteristics as well as their collective behaviors. Understanding how processing conditions influence the nanoscale arrangement and microstructure is critical for engineering materials with desired macroscopic properties. Microstructural features such as grain boundaries, lattice defects, and pores significantly affect these properties but are challenging to quantify using traditional manual analyses as they are labor-intensive and prone to errors. In this work, we present a machine learning workflow for automating grain segmentation in scanning electron microscopy (SEM) images of nanoparticle superlattices. This workflow integrates signal processing techniques, such as Radon transforms, with unsupervised learning methods like agglomerative hierarchical clustering to identify and segment grains without requiring manually annotated data. In the workflow we transform the raw pixel data into explainable numerical representation of superlattice orientations for clustering. Benchmarking results demonstrate the workflow's robustness against noisy images and edge cases, with a processing speed of four images per minute on standard computational hardware. This efficiency makes the workflow scalable to large datasets and makes it a valuable tool for integrating data-driven models into decision-making processes for material design and analysis. For example, one can use this workflow to quantify grain size distributions at varying processing conditions like temperature and pressure and using that knowledge adjust processing conditions to achieve desired superlattice orientations and grain sizes. © 2025, CC BY.

关键词： Grain boundaries

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Alternative photothermal/electrothermal hierarchical membrane for hypersaline water treatment

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SusMat 2022年第6期2卷 679-688页

作者： Miao Wang Wen He Yuhui Hua Xinwen Xie Shiyan Chen Lei Zhou Yunmao Zhang Yaqi Hou Shihong Lin Haiping Xia Jing Zheng Xu Hou State Key Laboratory of Physical Chemistry of Solid Surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamenChina College of Materials Xiamen UniversityXiamenChina Research Institute for Biomimetics and Soft Matter Fujian Provincial Key Laboratory for Soft Functional Materials ResearchJiujiang Research InstituteCollege of Physical Science and TechnologyXiamen UniversityXiamenChina Shenzhen Grubbs Institute and Guangdong Provincial Key Laboratory of Catalysis Department of ChemistrySouthern University of Science and TechnologyShenzhenChina Collaborative Innovation Center of Chemistry for Energy Materials(iChEM) Xiamen UniversityXiamenChina Department of Civil and Environmental Engineering Vanderbilt UniversityNashvilleTennesseeUSA Interdisciplinary Material Science Program Vanderbilt UniversityNashvilleTennesseeUSA Tan Kah Kee Innovation Laboratory Xiamen UniversityXiamenChina Engineering Research Center of Electrochemical Technologies of Ministry of Education Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamenChina

Over the last decades,the treatment of the large quantities of hypersaline wastewater generated by conventional industries,inland desalination,and fossil-fueled power plants has been an important economic issue and also an inescapable green ***,we developed a versatile interfacial heating membrane with alternating utilization of electricity or solar energy for hypersaline water *** hierarchical membrane functions both as a separation membrane and an interface heater,which can quickly(<0.1 s)convert electricity or solar energy into heat to evaporate the outermost layer of hypersaline *** 10wt% hyper-saline water,the freshwater production rate can reach 16.8kg/m^(2)⋅h by applying a voltage of 10 V and 1.36 kg/m^(2)⋅h under 1-sun ***,it exhibits high electrochemical resistance to corrosion and therefore remains stable tack-ling hypersaline water(>5 wt%),with a high salt rejection rate of 99.99%.This system shows an efficient desalination strategy that can provide fresh water from brines for agriculture and industry,and even for daily life.

关键词： carbon nanotubes electrothermal hypersaline water treatment interface evaporate pho-tothermal

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Carbon nitride- and graphene-based materials for the photocatalytic degradation of emerging water pollutants

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Materials Advances 2024年第7期5卷 2668-2688页

作者： Indra Jaya Budiarso Valentinus Alphano Dabur Riska Rachmantyo Hermawan Judawisastra Chechia Hu Arie Wibowo Master Program in Materials Science and Engineering Faculty of Mechanical and Aerospace Engineering Institut Teknologi Bandung Ganesha 10 Bandung 40132 West Java Indonesia Doctoral Program in Materials Science and Engineering Faculty of Mechanical and Aerospace Engineering Institut Teknologi Bandung Ganesha 10 Bandung 40132 West Java Indonesia Materials Science and Engineering Faculty of Mechanical and Aerospace Engineering Institut Teknologi Bandung Ganesha 10 Bandung 40132 West Java Indonesia ariewibowo@itb.ac.id Department of Chemical Engineering National Taiwan University of Science and Technology Taipei 106 Taiwan R&D Center for Membrane Technology Chung Yuan Christian University Taoyuan 320 Taiwan Research Center for Nanoscience and Nanotechnology Institut Teknolgi Bandung Ganesha 10 Bandung 40132 West Java Indonesia

Photocatalytic degradation is a promising way to treat emerging pollutants in wastewater. Recently, metal-free photocatalysts such as carbon nitride- and graphene-based materials have attracted much interest in the photocatalytic degradation of emerging water pollutants owing to their visible light activity and unique electrical properties, respectively. Graphitic carbon nitride (GCN) is considered a superior visible light–active photocatalyst because of its suitable bandgap (2.7 eV). Moreover, the facile synthesis process and the high chemical and thermal stability of GCN make it one of the research hotspots in photocatalytic wastewater treatment. Besides GCN, graphene and its derivatives are utilized to support main photocatalysts by enhancing their light absorption, pollutant adsorption, and photogenerated charge separation. Furthermore, the vast modification of these materials has promoted various outstanding performances in carbon nitride- and graphene-based photocatalysts in the application of pollutant degradation. In this review, we highlight recent developments in carbon nitride- and graphene-based photocatalysts (2018–2023), focusing on the strategies to improve the activity of GCN as a visible light–active photocatalyst and the role of graphene and its derivatives as supporting materials in wastewater pollutant remediation applications.

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Coral-Inspired Hierarchical Structure Promotes a Win-Win on Mass Loading and Rate Capability: Nickel-Cobalt-Zinc-Sulfide@Nickel-Cobalt Layered Double Hydroxide Electrode for High-Performance Supercapacitor

SSRN

引用

SSRN 2022年

作者： Hu, Wenxuan Chen, Lu Geng, Biao Wu, Xing Du, Miao Shan, Guorong Song, Yihu Wu, Ziliang Zheng, Qiang MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou310027 China State Key Laboratory of Chemical Engineering College of Chemical and Biological Engineering Zhejiang University Hangzhou310027 China

Hierarchical structure, defined as structural features occurring on different levels of scale, is widely used in the rational design of composite electrodes for its superiorities in abundant electrochemical active sites and functional differentiation for various components. Herein, we in situ prepared nickel-cobalt layered double hydroxides (NiCo-LDH) nanosheet network on ultrathin nickel-cobalt-zinc-sulfide (NiCoZnSx) microplate arrays to construct a special, coral-inspired hierarchical structure. In this structure, NiCoZnSx microplate arrays not only provide plenty of rooms for nanosheet growing, but also improve the ion diffusion, charge transfer and structural stability of the composite electrode. The NiCo-LDH nanosheet network paved through the microplate surface offer high specific surface area and capacitance. The composite electrode delivers a high areal capacitance of 8.1 F cm-2 at a mass loading of 4.2 mg cm-2, outstanding rate capability (63% capacitance retention, 50 mA cm-2) and cycling stability (80% capacitance retention, 10000 cycles). Furthermore, asymmetric supercapacitor assembled by the composite electrode and active carbon exhibits a maximal power density of 80.3 mW cm-2 at an energy density of 270 μWh cm-2 with good rate capability and long-term cycling stability. This work reveals the significance and practical potential of rational design in electrode’s hierarchical structure for high-performance supercapacitor. © 2022, The Authors. All rights reserved.

关键词： Supercapacitor

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