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Microscopic picture of paraelectric perovskites from structural prototypes

Physical Review Research 2022年第1期4卷 L012042-L012042页

作者： Michele Kotiuga Samed Halilov Boris Kozinsky Marco Fornari Nicola Marzari Giovanni Pizzi Theory and Simulation of Materials (THEOS) National Centre for Computational Design and Discovery of Novel Materials (MARVEL) École Polytechnique Fédérale de Lausanne CH-1015 Lausanne Switzerland Designed Material Technologies LLC P.O. Box 14548 Richmond Virginia 23221-9998 USA John A. Paulson School of Engineering and Applied Sciences Harvard University 29 Oxford Street Cambridge Massachusetts 02138 USA Robert Bosch LLC Research and Technology Center Cambridge Massachusetts 02139 USA Department of Physics and Science of Advanced Materials Program Central Michigan University Mt. Pleasant Michigan 48859 USA

We highlight with first-principles molecular dynamics the persistence of intrinsic 〈111〉 Ti off-centerings for BaTiO3 in its cubic paraelectric phase. Intriguingly, these are inconsistent with the Pm3¯m space group often used to atomistically model this phase using density-functional theory or similar methods. Therefore, we deploy a systematic symmetry analysis to construct representative structural models in the form of supercells that satisfy a desired point symmetry but are built from the combination of lower-symmetry primitive cells. We define as structural prototypes the smallest of these that are both energetically and dynamically stable. Remarkably, two 40-atom prototypes can be identified for paraelectric BaTiO3; these are also common to many other ABO3 perovskites. These prototypes can offer structural models of paraelectric phases that can be used for the computational engineering of functional materials. Last, we show that the emergence of B-cation off-centerings and the primitive-cell phonon instabilities is controlled by the equilibrium volume, in turn, dictated by the filler A cation.

关键词： Crystal symmetry Ferroelectricity Structural order parameter Paraelectrics

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Isolated Pt atoms tethered to N-doped MoSx as highly efficient and sustainable hydrogen evolution reaction electrocatalyst

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Applied Surface science 2023年 614卷

作者： Lee, Ting-Wei Lo, Ying-Chen Wu, Chia-Hua Ho, Cheng-Yuan Alamani, Bryan G. Chen, Jeng-Lung Chen, Chiaying Department of Environmental Engineering National Chung Hsing University Taichung City402 Taiwan Department of Materials Science and Engineering National Yang Ming Chiao Tung University Hsinchu300 Taiwan Department of Chemical Engineering College of Engineering University of the Philippines Diliman Quezon City1101 Philippines Environmental Engineering Program College of Engineering University of the Philippines Diliman Quezon City1101 Philippines National Synchrotron Radiation Research Center Hsinchu30076 Taiwan

In this work, synergistic NH4+ intercalation and nitrogen-containing molecule doping realize a crystalline-to-amorphous (i.e., MoSx) structure transition with enhanced HER reactivity and superior stability obtained via structural distortion and abundant active sites. The applied N dopants partially replace the bridging S22− and form Mo-N bonds, where the alkyl N-dopant tetramethylammonium chloride (TEA) achieves the most effective doping. The HER activity increases with an increasing number of bridging S22− and MoⅤ species, both of which contribute to advance electrocatalytic performance. Furthermore, N-doped MoSx is identified as an exceptional stabilizing platform to anchor single Pt atoms (PtSA) through Pt-S bonding, rendering MoSx/TEA/PtSA a highly promising electrocatalyst. MoSx/TEA/PtSA achieved comparable performance to that of the benchmark Pt/C catalyst (i.e., a cathodic current density of 10 mA·cm−2 at overpotential of 97 mV) with much lower loading of Pt (0.67 wt%). Theoretical calculations based on density functional theory indicate that Pt atoms and Pt-adjacent sulfur atoms act as active sites. The superior interfacial electron transfer and thus HER performance of MoSx/TEA/PtSA arises from (1) boosted electronic metal-support interaction through Pt-S bonds and (2) enhanced H adsorption ability of Pt-adjacent sulfur atoms due to Pt coordination. © 2022 Elsevier B.V.

关键词： Doping (additives)

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Introducing self-healing properties to polyethersulfone (PES) membrane via poly(vinyl alcohol)/ polyacrylic acid (PVA/PAA) surface coating

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Chemosphere 2024年 349卷 140772页

作者： Lim, Yi Heng Wong, Eng Cheong Chong, Woon Chan Mohammad, Abdul Wahab Koo, Chai Hoon Lau, Woei Jye Department of Chemical Engineering Lee Kong Chian Faculty of Engineering and Science Universiti Tunku Abdul Rahman Sungai Long Campus Jalan Sungai Long Cheras Selangor Kajang43000 Malaysia Centre for Advanced and Sustainable Materials Research Universiti Tunku Abdul Rahman Sungai Long Campus Jalan Sungai Long Cheras Selangor Kajang43000 Malaysia Chemical and Water Desalination Program College of Engineering University of Sharjah Sharjah27272 United Arab Emirates Chemical Engineering Programme Faculty of Engineering and Built Environment Universiti Kebangsaan Malaysia Selangor Bangi43600 Malaysia Faculty of Chemical and Energy Engineering Universiti Teknologi Malaysia Johor Johor Bahru81310 Malaysia

During membrane filtration, it is inevitable that a membrane will experience physical damage, leading to a loss of its integrity and a decrease in separation efficiency. Hence, the development of a water-responsive membrane capable of healing itself autonomously after physical damage is significantly important in the field of water filtration. Herein, a water-enabled self-healing composite polyethersulfone (PES) membrane was synthesized by coating the membrane surface using a mixed solution composed of poly (vinyl alcohol) and polyacrylic acid (PVA-PAA). The self-healing efficiency of the coated PES membrane was examined based on the changes in water flux at three stages which are pre-damaged, post-damaged, and post-healing. The self-healing process was initiated by the swelling of the water-responsive PVA and PAA, followed by the formation of reversible hydrogen bonds, completing the self-healing process. The coated PES membrane with three layers of PVA-PAA coatings (at 3:1 ratio) demonstrated high water flux and remarkable self-healing efficiency of up to 98.3%. The self-healing capability was evidenced by the morphology of the membrane observed via scanning electron microscope (SEM). The findings of this investigation present a novel architecture approach for fabricating self-healing membranes using PVA-PAA, in addition to other relevant parameters as reported. © 2023 Elsevier Ltd

关键词： Membranes

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Hyaluronic acid-coated iron oxide nanoparticles for magnetic fluid hyperthermia and methylene blue dye removal: Preparation, physicochemical characterization, and enhancing the heating efficiency

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Journal of Molecular Liquids 2024年 415卷

作者： Mahendravada, Srujana Lahiri, B.B. Jayakumar, Sangeetha Sathyanarayana, A.T. Vetrivendan, E. Khan, Fouzia Vidya, R. Philip, John Dasgupta, Arup Smart Materials Section Physical Metallurgy Division Materials Characterization Group Metallurgy and Materials Group Indira Gandhi Centre for Atomic Research Kalpakkam Tamil Nadu 603102 India Low Temperature Studies Section Condensed Matter Physics Division Materials Science Group Indira Gandhi Centre for Atomic Research Kalpakkam Tamil Nadu 603102 India Corrosion Engineering and Protection Section Corrosion Science and Technology Division Materials Characterization Group Metallurgy and Materials Group Indira Gandhi Centre for Atomic Research Kalpakkam Tamil Nadu 603102 India Homi Bhabha National Institute Training School Complex Anushaktinagar Mumbai400094 India Vellore Institute of Technology Tamil Nadu Vellore632014 India

We report here the magnetic fluid hyperthermia properties of water-dispersible hyaluronic acid-coated superparamagnetic iron oxide nanoparticles (HA-MNPs), prepared using the coprecipitation technique followed by ligand exchange. The presence of the hyaluronic acid coating is confirmed using Fourier transform infrared spectroscopy. Magneto-calorimetric studies show good field-induced heating efficiency of the HA-MNPs, where a high specific absorption rate (SAR) of ∼ 315 W/gFe is obtained for ∼ 5 wt% MNP concentration when exposed to an alternating magnetic field amplitude of ∼ 33.1 kA/m at ∼ 126 kHz. The heating efficiency is found to decrease by ∼ 33.8 % after immobilization of the MNPs within an agar matrix, which is attributed to the abrogation of Brownian relaxation. When subjected to an external DC magnetic field, the MNPs form linear chain-like structures, which causes the effective anisotropy energy density to increase. Magneto-calorimetric studies on agar-based oriented samples reveal a ∼ 19.5 % enhancement in SAR, thereby partly compensating for the loss in heating efficiency due to an increase in medium viscosity. The orientational ordering-induced enhancement in SAR is also verified using sweeping rate modified Stoner-Wohlfarth model-based calculations. In vitro cyto-toxicity studies on the HeLa cell lines reveal good cyto-compatibility of the MNPs. The negative charge on the surface of HA-coated MNPs is exploited to remove the cationic methylene blue dye from the aqueous medium, where the dye molecules are found to be physisorbed on the surface of the MNPs. The experimental findings clearly show the high induction heating efficiency, cyto-compatibility, and cationic dye-adsorption efficiency of the prepared HA-MNPs, thereby indicating the suitability of these MNPs for multi-functional applications like magnetic fluid hyperthermia and waste-water purification. © 2024 Elsevier B.V.

关键词： Fourier transform infrared spectroscopy

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Urban heat mitigation by green and blue infrastructure:Drivers,effectiveness,and future needs

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The Innovation 2024年第2期5卷 145-166页

作者： Prashant Kumar Sisay E.Debele Soheila Khalili Christos H.Halios Jeetendra Sahani Nasrin Aghamohammadi Maria de Fatima Andrade Maria Athanassiadou Kamaldeep Bhui Nerea Calvillo Shi-Jie Cao Frederic Coulon Jill L.Edmondson David Fletcher Edmilson Dias de Freitas Hai Guo Matthew C.Hort Madhusudan Katti Thomas Rodding Kjeldsen Steffen Lehmann Giuliano Maselli Locosselli Shelagh K.Malham Lidia Morawska Rajan Parajuli Christopher D.F.Rogers Runming Yao Fang Wang Jannis Wenk Laurence Jones Global Centre for Clean Air Research(GCARE) School of SustainabilityCivil and Environmental EngineeringFaculty of Engineering and Physical SciencesUniversity of SurreyGuildford GU27XHUK Institute for Sustainability University of SurreyGuildford GU27XHSurreyUK School of Built Environment University of ReadingWhiteknightsReading RG66BUUK School Design and the Built Environment Curtin University Sustainability Policy InstituteKent StBentley 6102Western Australia Harry Butler Institute Murdoch UniversityMurdoch 6150Western Australia Atmospheric Sciences Department Institute of AstronomyGeophysics and Atmospheric SciencesUniversity of Sao PauloSao Paulo 05508-090Brazil Met Office FitzRoy RoadExeter EX13PBUK Department of Psychiatry and Nuffield Department of Primary Care Health Sciences Wadham CollegeUniversity of OxfordOxfordUK Centre for Interdisciplinary Methodologies University of WarwickWarwickUK School of Architecture Southeast University2 SipailouNanjing 210096China Cranfield University School of WaterEnvironment and EnergyCranfield MK430ALUK Plants PhotosynthesisSoil ClusterSchool of BiosciencesUniversity of SheffieldSheffield S102TNUK UK Centre for Ecology&Hydrology Environment Centre WalesDeiniol RoadBangor LL572UWUK Air Quality Studies Department of Civil and Environmental EngineeringThe Hong Kong Polytechnic UniversityHong KongChina Department of Forestry and Environmental Resources Faculty Excellence Program for Leadership in Public ScienceNorth Carolina State UniversityChancellorRaleighNC 27695USA Departments of Architecture&Civil Engineering and Chemical EngineeringUniversity of BathBath BA27AYUK School of Architecture University of NevadaLas VegasNV 89154USA Department of Tropical Ecosystems Functioning Center of Nuclear Energy in AgricultureUniversity of São PauloPiracicaba 13416-000Sao PauloBrazil School of Ocean Sciences Bangor UniversityMenai BridgeAnglesey LL595 ABUK International Laboratory for Air Quality and Health Science and Engine

The combination of urbanization and global warming leads to urban overheating and compounds the frequency and intensity of extreme heat events due to climate ***,the risk of urban overheating can be mitigated by urban green-blue-grey infrastructure(GBGI),such as parks,wetlands,and engineered greening,which have the potential to effectively reduce summer air *** many reviews,the evidence bases on quantified GBGI cooling benefits remains partial and the practical recommendations for implementation are *** systematic literature review synthesizes the evidence base for heat mitigation and related co-benefits,identifies knowledge gaps,and proposes recommendations for their implementation to maximize their *** screening 27,486 papers,202 were reviewed,based on 51 GBGI types categorized under 10 main *** GBGI(green walls,parks,street trees)have been well researched for their urban cooling ***,several other GBGI have received negligible(zoological garden,golf course,estuary)or minimal(private garden,allotment)*** most efficient air cooling was observed in botanical gardens(5.0±3.5℃),wetlands(4.9±3.2℃),green walls(4.1±4.2℃),street trees(3.8±3.1℃),and vegetated balconies(3.8±2.7℃).Under changing climate conditions(2070–2100)with consideration of RCP8.5,there is a shift in climate subtypes,either within the same climate zone(e.g.,Dfa to Dfb and Cfb to Cfa)or across other climate zones(e.g.,Dfb[continental warm-summer humid]to BSk[dry,cold semi-arid]and Cwa[temperate]to Am[tropical]).These shifts may result in lower efficiency for the current GBGI in the *** the importance of multiple services,it is crucial to balance their functionality,cooling performance,and other related co-benefits when planning for the future *** global GBGI heat mitigation inventory can assist policymakers and urban planners in prioritizing effective interventions to reduce the risk of urban overheating,fi

关键词： estuary walls extreme

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An application of conjugate gradient technique for determination of thermal conductivity as an inverse engineering problem

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materials Today: Proceedings 2021年 47卷 3082-3087页

作者： Vivek Pandey Addisu Bekele Gulam Mohammed Sayeed Ahmed Nand Jee Kanu Gyanendra Kumar Singh Department of Thermal and Aerospace Engineering School of Mechanical Chemical and Materials Engineering Adama Science and Technology University Adama Ethiopia Centre of Excellence for Advanced Manufacturing Engineering Program of Mechanical Design and Manufacturing Engineering School of Mechanical Chemical and Materials Engineering Adama Science and Technology University Adama Ethiopia Department of Mechanical Engineering S. V. National Institute of Technology Surat India Department of Mechanical Design and Manufacturing Engineering School of Mechanical Chemical and Materials Engineering Adama Science and Technology University Adama Ethiopia

Inverse problems frequently occur when boundary conditions/thermal properties of a material are unknown, and are determined from known internal temperature measurements. A direct problem is the opposite of an inverse problem. For example, it would be the task of determining the temperature field within a material body, given boundary conditions and thermal properties. In an ill-posed, inverse problem, small variations in internal temperature measurement cause large variations in the estimated quantity such as boundary heat flux. Measured temperature variations may be due to noise, measurement error and instrumentation error, among other factors. There are various methods for solving inverse problems in materials engineering. In the paper, an inverse problem of estimating boundary heat flux for one-dimensional heat conduction is solved using the classical method of Beck and temperature dependent thermal conductivity is estimated using the more recent and advanced Conjugate Gradient method (CGM). The temperature values from the finite difference application to a direct heat transfer problem are used along with noise added to the data, in order to simulate real world, experimental conditions. The data is applied to the inverse problem of finding boundary heat flux and thermal conductivity. It is seen that Conjugate Gradient Method (CGM) along with sequential function specification method recovers the boundary heat flux and thermal conductivity quite accurately for noise levels of 1% and 2%. It is further observed that addition of future time steps stabilize the algorithm and increase accuracy of the desired results. It is also observed that CGM can recover the temperature dependent thermal conductivity quickly within few iterations, for different values of thermal conductivity function coefficients, k 0 and k 1 . CGM is found to be fast and robust when applied to one-dimensional case and can be extended to complex geometries.

关键词： Inverse problem Thermal conductivity Conjugate gradient

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Deformation twin traces on gold surfaces: A pathway to tailored epitaxial growth of 1D semiconductors

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Proceedings of the National Academy of sciences of the United States of America 2023年第50期120卷 e2314192120页

作者： Portal, Lotan Polishchuk, Iryna Zilberberg, Rotem Levi, Mor Koifman-Khristosov, Maria Katsman, Alexander Pokroy, Boaz Department of Materials Science and Engineering Technion Israel Institute of Technology Haifa 32000 Israel The Nancy and Stephen Grand Technion Energy Program Technion − Israel Institute of Technology Haifa 3200003 Israel

The field of one-dimensional semiconducting materials holds a wide variety of captivating applications, such as photovoltaic cells, electronic devices, catalysis cells, lasers, and more. The tunability of electrical, mechanical, or optical attributes of a semiconductor crystal relies on the ability to control and pattern the crystal’s growth direction, orientation, and dimensions. In this study, we harvest the unique properties of crystallographic defects in Au substrates, specifically twin boundaries, to fabricate selective epitaxial growth of semiconducting nanocrystals. Different crystallographic defects were previously shown to enhance materials properties, such as, screw dislocations providing spiral crystal growth, dislocation outcrops, and vacancies increasing their catalytic activity, dislocation strengthening, and atomic doping changing the crystal’s electrical properties. Here, we present a unique phenomenon of directed growth of semiconductor crystals of gold(I)-cyanide (AuCN) on the surface of thin Au layers, using traces of deformation twins on the surface. We show that emergence of deformation twins to the {111} Au surface leads to the formation of ledges, exposing new {001} and {111} facets on the surface. We propose that this phenomenon leads to epitaxial growth of AuCN on the freshly exposed {111} facets of the twin boundary trace ledges. Specific orientations of the twin boundaries with respect to the Au surface allow for patterned growth of AuCN in the <110> orientations. Nano-scale patterning of AuCN semiconductors may provide an avenue for property tuning, particularly the band gap acquired. © 2023 National Academy of sciences. All rights reserved.

关键词： epitaxial growth thin films crystal growth gold deformation twins

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Bulk Photovoltaic Effect in Ferroelectric Liquid Crystals Comprising of Quinquethiophene and Lactic Ester Units

SSRN

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SSRN 2023年

作者： Funahashi, Masahiro Program in Advanced Materials Science Faculty of Engineering and Design Kagawa University 2217-20 Hayashi-cho Kagawa Takamatsu761-0396 Japan Health and Medical Research Institute National Institute of Advances Industrial Science and Technology 2217-14 Hayashi-cho Kagawa Takamatsu761-0395 Japan

Carrier-transporting ferroelectric liquid crystals consisting of quinquethiophene and lactic ester units were synthesized. One compound exhibited a chiral smectic C (SmC*) phase, and another compound exhibited a chiral smectic crystal phase at room temperature below the SmC* phase. The bulk photovoltaic effect was observed in the polarized chiral smectic crystal phase. The absorption edge was shifted to 570 nm from 500 nm of a terthiophene analogue, due to the extension of the π-conjugated unit. In the polarized smectic crystal phase doped with PCBM, the open circuit voltage and short circuit voltage was 0.72 V and 270 μAcm-2, respectively. The fill factor was improved to 0.63 and the power conversion efficiency was 0.5%. The spectral sensitivity was extended to 700 nm, due to the absorption of PCBM as well as compound 1. Since compound 1 exhibits the SmC* phase above the chiral smectic crystal phase, the voltage for the poling treatment was remarkably reduced to 5 V from 40 V in the terthiophene analogue. © 2023, The Authors. All rights reserved.

关键词： Photovoltaic effects

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Indian bael mediated eco-friendly synthesis and performance evaluation of zirconium oxide nanoparticles: An efficient anti-microbial agent

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materials Today: Proceedings 2022年 62卷 5067-5070页

作者： Lakshmi Ranganatha, V. Nagaraju, G. Vidya, J.S. Deepakumari, H.N. Gurudutt, D.M. Mallikarjunaswamy, C. Department of Chemistry The National Institute of Engineering Manandavadi Road MysuruKarnataka570008 India Energy Materials Research Laboratory Department of Chemistry Siddaganga Institute of Technology Karnataka Tumakuru572103 India Department of Chemistry JSS College of Arts Commerce and Science Ooty Road MysuruKarnataka570025 India Department of Chemistry Bharathi College Bharathinagara MandyaKarnataka571422 India Department of Studies in Organic Chemistry University of Mysore Manasagangotri MysuruKarnataka570006 India Postgraduate Department of Chemistry JSS College of Arts Commerce and Science Ooty Road MysuruKarnataka570025 India

In this study, we have synthesized zirconium oxide nanoparticles by green, cost-effective solution combustion method using Indian bael extract as a fuel. The zirconium oxide nanoparticles are confirmed by spectroscopic techniques. The phase and crystalline property of the material was confirmed by powder X-ray diffraction analysis, surface morphology was checked by scanning electron microscope, and the energy dispersive X-ray spectrum confirmed the purity and elemental composition of zirconium oxide nanoparticles. Further, the zirconium oxide nanoparticles were subjected for antimicrobial activity against different bacterial strains, the biogenic zirconium oxide nanoparticles showed good activity against all tested bacterial and fungal strains. Overall, this study confirms that the biogenic zirconium oxide nanoparticles could be used as a possible antimicrobial agent. © 2022

关键词： Zirconium compounds

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Connecting polymer collapse and the onset of jamming

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Physical Review E 2024年第3期109卷 034406-034406页

作者： Alex T. Grigas Aliza Fisher Mark D. Shattuck Corey S. O'Hern Graduate Program in Computational Biology and Bioinformatics Yale University New Haven Connecticut 06520 USA Integrated Graduate Program in Physical and Engineering Biology Yale University New Haven Connecticut 06520 USA Department of Mechanical Engineering and Materials Science Yale University New Haven Connecticut 06520 USA Benjamin Levich Institute and Physics Department The City College of New York New York New York 10031 USA Department of Physics Yale University New Haven Connecticut 06520 USA Department of Applied Physics Yale University New Haven Connecticut 06520 USA

Previous studies have shown that the interiors of proteins are densely packed, reaching packing fractions that are as large as those found for static packings of individual amino-acid-shaped particles. How can the interiors of proteins take on such high packing fractions given that amino acids are connected by peptide bonds and many amino acids are hydrophobic with attractive interactions? We investigate this question by comparing the structural and mechanical properties of collapsed attractive disk-shaped bead-spring polymers to those of three reference systems: static packings of repulsive disks, of attractive disks, and of repulsive disk-shaped bead-spring polymers. We show that the attractive systems quenched to temperatures below the glass transition T≪Tg and static packings of both repulsive disks and bead-spring polymers possess similar interior packing fractions. Previous studies have shown that static packings of repulsive disks are isostatic at jamming onset, i.e., the number of interparticle contacts Nc matches the number of degrees of freedom, which strongly influences their mechanical properties. We find that repulsive polymer packings are hypostatic at jamming onset (i.e., with fewer contacts than degrees of freedom) but are effectively isostatic when including stabilizing quartic modes, which give rise to quartic scaling of the potential energy with displacements along these modes. While attractive disk and polymer packings are often considered hyperstatic with excess contacts over the isostatic number, we identify a definition for interparticle contacts for which they can also be considered as effectively isostatic. As a result, we show that the mechanical properties (e.g., scaling of the potential energy with excess contact number and low-frequency contribution to the density of vibrational modes) of weakly attractive disk and polymer packings are similar to those of isostatic repulsive disk and polymer packings. Our results demonstrate that static

关键词： Jamming Polymer folding Protein folding Single polymer chains

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