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Optimization for epitaxial fabrication of infinite-layer nickelate superconductors

Frontiers of physics 2024年第3期19卷 61-69页

作者： Minghui Xu Yan Zhao Xiang Ding Huaqian Leng Shu Zhang Jie Gong Haiyan Xiao Xiaotao Zu Huiqian Luo Ke-Jin Zhou Bing Huang Liang Qiao School of Physics University of Electronic Science and Technology of ChinaChengdu 610054China Beijing Computational Science research Center Beijing 100193China Diamond Light Source Harwell CampusDidcot OX110DEUnited Kingdom Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China Songshan Lake Materials Laboratory Dongguan 523808China

The discovery of nickelates superconductor creates exciting opportunities to unconventional superconductivity. However, its synthesis is challenging and only a few groups worldwide can obtain samples with zero-resistance. This problem becomes the major barrier for this field. From plume dynamics perspective, we found the synthesis of superconducting nickelates is a complex process and the challenge is twofold, i.e., how to stabilize an ideal infinite-layer structure Nd_(0.8)Sr_(0.2)NiO_(2), and then how to make Nd_(0.8)Sr_(0.2)NiO_(2) superconducting? The competition between perovskite Nd_(0.8)Sr_(0.2)NiO_(3) and Ruddlesden−Popper defect phase is crucial for obtaining infinite-layer structure. Due to inequivalent angular distributions of condensate during laser ablation, the laser energy density is critical to obtain phase-pure Nd_(0.8)Sr_(0.2)NiO_(3). However, for obtaining superconductivity, both laser energy density and substrate temperature are very important. We also demonstrate the superconducting Nd_(0.8)Sr_(0.2)NiO_(2) epitaxial film is very stable in ambient conditions up to 512 days. Our results provide important insights for fabrication of superconducting infinite-layer nickelates towards future device applications.

关键词： nickelate superconductivity infinite-layer plasma condensate plume dynamics

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A Workflow Demonstrator for Processing Catalysis research Data

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Data Intelligence 2022年第2期4卷 455-470页

作者： Abraham Nieva de la Hidalga Donato Decarolis Shaojun Xu Santhosh Matam Willinton Yesid Hernandez Enciso Josephine Goodall Brian Matthews C.Richard A.Catlow UK Catalysis Hub Research Complex at HarwellRutherford Appleton LaboratoryR92 HarwellOxfordshire OX11 OFAUK School of Chemistry Cardif UniversityMain BuildingPark PlaceCardiffCF103ATUK Scientific Computing Department STFC Rutherford Appleton LaboratoryHarwell CampusDidcotOX110QxUK Department of Chemistry University College LondonLondon WC1E6BTUK

The UK Catalysis Hub(UKCH)is designing a virtual research environment to support data processing and analysis,the Catalysis research Workbench(CRW).The development of this platform requires identifying the processing and analysis needs of the UKCH members and mapping them to potential *** paper presents a proposal for a demonstrator to analyse the use of scientific workflows for large scale data *** demonstrator provides a concrete target to promote further discussion of the processing and analysis needs of the UKCH *** this paper,we will discuss the main requirements for data processing elicited and the proposed adaptations that will be incorporated in the design of the CRW and how to integrate the proposed solutions with existing practices of the *** demonstrator has been used in discussion with researchers and in presentations to the UKCH community,generating increased interest and motivating furtherdevelopment.

关键词： Workflow demonstrator Prototyping Scientific workflow Management Catalysis research data High-throughput processing and analysis

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Monitoring dynamics of defects and single Fe atoms in N-functionalized few-layer graphene by in situ temperature programmed scanning transmission electron microscopy

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Journal of Energy Chemistry 2022年第1期31卷 520-530,I0014页

作者： Rosa Arrigo Takeo Sasaki June Callison Diego Gianolio Manfred Erwin Schuster School of Science Engineering and EnvironmentUniversity of SalfordManchester M54WTUK Diamond Light Source Harwell Science and Innovation CampusDidcot 0X1/ODEUK JEOL UK Ltd.JEOL House 1-2 Silver CourtWatchmeadWelwyn Garden CityHerts AL71LTUK Department of Chemistry University College London20 Gordon StreetLondon WC1H OAJUK UK Catalysis Hub Research Complex at Harwell(RCaH)Rutherford Appleton LaboratoryHarwell Oxon 0X11 OFAUK Johnson Matthey Technology Centre Reading RG49NH.UK

In this study,we aim to contribute an understanding of the pathway of formation of Fe species during top-down synthesis of dispersed Fe on N-functionalized few layer graphene,widely used in *** use X-ray absorption spectroscopy to determine the electronic structure and coordination geometry of the Fe species and in situ high angle annular dark field scanning transmission electron microscopy combined with atomic resolved electron energy loss spectroscopy to localize these,identify their chemical configuration and monitor their dynamics during thermal *** show the high mobility of peripheral Fe atoms,first diffusing rapidly at the trims of the graphene layers and at temperatures as high as 573 K,diffusing from the edge planes towards in-plane locations of the graphene layers forming three-,four-coordinated metal sites and more complexes polynuclear Fe *** process occurs via bond C-C breaking which partially reduces the extension of the graphene ***,the vast majority of Fe is segregated as a metal *** dynamic interconversion depends on the structural details of the surrounding graphitic environment in which these are formed as well as the Fe loading.N species appear stabilizing isolated and polynuclear Fe species even at temperatures as high as 873 *** significance of our results lies on the fact that single Fe atoms in graphene are highly mobile and therefore a structural description of the electroactive sites as such is insufficient and more complex species might be more relevant,especially in the case of multielectron transfer *** we provide the experimental evidence of the formation of these polynuclear Fe-N sites and their structural characteristics.

关键词： HAADF-STEM Single Fe atom sites N-doped Few-layer graphene Dinuclear Fe species

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The W3C Data Catalog Vocabulary,Version 2:Rationale,Design Principles,and Uptake

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Data Intelligence 2024年第2期6卷 457-487页

作者： Riccardo Albertoni David Browning Simon Cox Alejandra N.Gonzalez-Beltran Andrea Perego Peter Winstanley Istituto di Matematica Applicata e Tecnologie Informatiche"Enrico Magenes" Consiglio Nazionale delle Ricerche(IMATI-CNR)GenoaItaly Independent Consultant United Kingdom LandandWater CSiROMelbourneAustralia Scientific Computing Rutherford Appleton LaboratoryScience and Technology Facilities CouncilHarwell Cam-pusOx110QXUnited Kingdom European Parliament Luxembourg Semantic Arts Fort CollinsCO80524USA

DCAT is an RDF vocabulary designed to facilitate interoperability between data catalogs published on the *** its first release in 2014 as a W3C Recommendation,DCAT has seen a wide adoption across communities and domains,particularly in conjunction with implementing the FAIR data principles(forfindable,accessible,interoperable and reusable data).These implementation experiences,besides demonstrating the fitness of DCAT to meet its intended purpose,helped identify existing issues and ***,over the last few years,additional requirements emerged in data catalogs,given the increasing practice of documenting not only datasets but also data services and *** paper illustrates the new version of DCAT,explaining the rationale behind its main revisions and extensions,based on the collected use cases and requirements,and outlines the issues yet to be addressed in future versions of DCAT.

关键词： Data Catalogs Interoperability Discoverability FAIR data

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Recent advances in non-thermal plasma(NTP)catalysis towards C1 chemistry

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Chinese Journal of Chemical Engineering 2020年第8期28卷 2010-2021页

作者： Huanhao Chen Yibing Mu Shanshan Xu Shaojun Xu Christopher Hardacre Xiaolei Fan State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 210009China Department of Chemical Engineering and Analytical Science School of EngineeringThe University of ManchesterM139PLUnited Kingdom School of Chemistry Cardiff UniversityMain BuildingPark PlaceCardiff CF103ATUnited Kingdom UK Catalysis Hub Research Complex at HarwellRutherford Appleton LaboratoryHarwellOxon OX110FAUnited Kingdom

C1 chemistrymainly involves the catalytic transformation of C1molecules(i.e.,CO,CO2,CH4 and CH3OH),which usually encounters thermodynamic and/or kinetic *** address these limitations,non-thermal plasma(NTP)activated heterogeneous catalysis offers a number of advantages,such as relatively mild reaction conditions and energy efficiency,in comparison to the conventional thermal *** review presents the state-of-the-art for the application of NTP-catalysis towards C1 chemistry,including the CO2 hydrogenation,reforming of CH4 and CH3OH,and water-gas shift(WGS)*** the hybrid NTP-catalyst system,the plasma-catalyst interactions ***,this reviewalso includes a brief discussion on the fundamental research into themechanisms of NTP activated catalytic C1 chemistry,such as the advanced characterisation methods(e.g.,in situ diffuse reflectance infrared Fourier transform spectroscopy,DRIFTS),temperatureprogrammed plasma surface reaction(TPPSR),kinetic ***,prospects for the future research on the development of tailor-made catalysts for NTP-catalysis systems(which will enable the further understanding of its mechanism)and the translation of the hybrid technique to practical applications of catalytic C1 chemistry are discussed.

关键词： Non-thermal plasma(NTP) Heterogeneous catalysis C1 chemistry Mechanism In situ characterisation

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Renewable hydrogen production from steam reforming of glycerol(SRG)over ceria-modified Y-alumina supported Ni catalyst

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Chinese Journal of Chemical Engineering 2020年第9期28卷 2328-2336页

作者： Ammaru Ismaila Huanhao Chen Yan Shao Shaojun Xu Yilai Jiao Xueli Chen Xin Gao Xiaolei Fan Department of Chemical Engineering and Analytical Science School of EngineeringThe University of ManchesterOxford RoadManchester M139PLUnited Kingdom School of Biotechnology and Health Sciences Wuyi UniversityJiangmen 52920China School of Chemistry Cardiff UniversityMain BuildingPark PlaceCardiffCF103ATUnited Kingdom UK Catalysis Hub Research Complex at HarwellRutherford Appleton LaboratoryHarwellOxon OX110FAUnited Kingdom Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China Institute of Clean Coal Technology East China University of Science and TechnologyShanghai 200237China School of Chemical Engineering and Technology Tianjin UniversityTianjin 300072China

Excess crude glycerol derived as a by-product from biodiesel industry prompts the need to valorise glycerol to value-added *** this context,catalytic steam reforming of glycerol(SRG) was proposed as a promising and sustainable alternative for producing renewable hydrogen(H2).Herein,the development of nickel(Ni) supported on ceria-modified mesoporous γ-alumina(γ-Al2 O3) catalysts and their applications in catalytic SRG(at550-750℃ atmospheric pressure and weight hourly space velocity,WHSV,of 44,122 ml·g^-1·h^-1(STP)) is *** of the developed catalysts were characterised using many technique *** findings show that ceria modification improved Ni dispersion on γ-Al2 O3 catalyst support with highly active small Ni particles,which led to a remarkable catalytic performance with the total glycerol conversion(ca.99%),glycerol conversion into gaseous products(ca.77%) and H2 yield(ca.62%).The formation rate for H2 production(14.4 ×10^(-5)mol·s^-1·g^-1, TOF(H2)=3412 s^-1) was significantly improved with the Ni@12 Ce-Al2 O3 catalyst,representing nearly a 2-fold increase compared with that of the conventional Ni@AI2 O3 *** addition,the developed catalyst also exhibited comparatively high stability(for 12 h) and coke resistance ability.

关键词： Steam reforming of glycerol(SRG) Hydrogen(H2) Nickel(Ni)catalysts Ceria Y-Alumina(γ-Al2O3)

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Frustrated Magnetic Interactions and Quenched Spin Fluctuations in CrAs

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Chinese Physics Letters 2022年第12期39卷 89-93页

作者：秦亚媛沈瑶郝一清沃弘樑申守栋 Russell A.Ewings Yang Zhao Leland W.Harriger Jeffrey W.Lynn 赵俊 State Key Laboratory of Surface Physics and Department of Physics Fudan UniversityShanghai 200433China Shanghai Qizhi Institute Shanghai 200232China ISIS Pulsed Neutron and Muon Source STFC Rutherford Appleton LaboratoryHarwell CampusDidcotOxonOX110QXUnited Kingdom NIST Center for Neutron research National Institute of Standards and TechnologyGaithersburgMD 20899USA Department of Materials Science and Engineering University of MarylandCollege ParkMD 20742USA Institute of Nanoelectronics and Quantum Computing Fudan UniversityShanghai 200433China Shanghai research Center for Quantum Sciences Shanghai 201315China

The discovery of pressure-induced superconductivity in helimagnets(CrAs,MnP)has attracted considerable interest in understanding the relationship between complex magnetism and unconventional ***,the nature of the magnetism and magnetic interactions that drive the unusual double-helical magnetic order in these materials remains ***,we report neutron scattering measurements of magnetic excitations in CrAs single crystals at ambient *** experiments reveal well defined spin wave excitations up to about 150 meV with a pseudogap below 7 meV,which can be effectively described by the Heisenberg model with nearest neighbor exchange *** surprisingly,the spin excitations are largely quenched above the Néel temperature,in contrast to cuprates and iron pnictides where the spectral weight is mostly preserved in the paramagnetic *** results suggest that the helimagnetic order is driven by strongly frustrated exchange interactions,and that CrAs is at the verge of itinerant and correlation-induced localized states,which is therefore highly pressure-tunable and favorable for superconductivity.

关键词： excitation exchange pressure

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Characteristics of a gold-doped electrode for application in high-performance lithium-sulfur battery

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Journal of Energy Chemistry 2022年第1期31卷 116-128,I0004页

作者： Vittorio Marangon Daniele Di Lecce Dan J.L.Brett Paul R.Shearing Jusef Hassoun University of Ferrara Department of Chemical and Pharmaceutical SciencesVia Fossato di Mortara 17Ferrara44121Italy Electrochemical Innovation Lab Department of Chemical EngineeringUCLLondon WC1E 7JEUnited Kingdom The Faraday Institution Quad OneBecquerel AveHarwell CampusDidcot OX11 ORAUnited Kingdom National Interuniversity Consortium of Materials Science and Technology(INSTM) University of Ferrara Research UnitUniversity of FerraraVia Fossato di Mortara17Ferrara 44121Italy

Bulk sulfur incorporating 3 wt% gold nano-powder is investigated as possible candidate to maximize the fraction of active material in the Li-S battery *** material is prepared via simple mixing of gold with molten sulfur at 120℃,quenching at room temperature,and *** comprehensive study reports relevant electrochemical data,advanced X-ray computed tomography(CT)imaging of the positive and negative electrodes,and a thorough structural and morphological characterization of the S:Au 97:3 w/w *** cathode exhibits high rate capability within the range from C/10 to 1C,a maximum capacity above 1300 mAh gs^(-1),and capacity retention between 85%and 91%after 100 cycles at 1C and C/3 *** novel formulation enables a sulfur fraction in the composite cathode film as high as 78 wt%,an active material loading of 5.7 mg cm^(-2),and an electrolyte/sulfur(E/S)ratio of 5μL mg^(-1),which lead to a maximum areal capacity of 5.4 mAh cm^(-2).X-ray CT at the micro-and nanoscale reveals the microstructural features of the positive electrode that favor fast conversion kinetics in the *** analysis of sulfur distribution in the porous cathode displays that electrodeposition during the initial cycle may trigger an activation process in the cell leading to improved ***,the tomography study reveals the characteristics of the lithium anode and the cell separator upon a galvanostatic test prolonged over 300 cycles at a 2C rate.

关键词： Lithium-sulfur battery Sulfur loading Electrolyte/sulfur ratio Gold nanoparticles X-ray tomography

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Design and fabrication of gas cell targets for laboratory astrophysics experiments on the Orion high-power laser facility

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High Power Laser Science and Engineering 2017年第3期5卷 62-66页

作者： C.Spindloe D.Wyatt S.Astbury G.F.Swadling T.Clayson C.Stehlé J.M.Foster E.Gumbrell R.Charles C.N.Danson P.Brummitt F.Suzuki-Vidal Science and Technology Facilities Council Harwell Science and Innovation Campus Blackett Laboratory Imperial College Lawrence Livermore National Laboratory LERMA Sorbonne UniversitésUPMC Univ.Paris06Observatoire de ParisPSL Research University AWE plc

This paper describes the design and fabrication of a range of ‘gas cell' microtargets produced by the Target Fabrication Group in the Central Laser Facility(CLF) for academic access experiments on the Orion laser facility at the Atomic Weapons Establishment(AWE). The experiments were carried out by an academic consortium led by Imperial College London. The underlying target methodology was an evolution of a range of targets used for experiments on radiative shocks and involved the fabrication of a precision machined cell containing a number of apertures for interaction foils or diagnostic windows. The interior of the cell was gas-filled before laser irradiation. This paper details the assembly processes, thin film requirements and micro-machining processes needed to produce the targets. Also described is the implementation of a gas-fill system to produce targets that are filled to a pressure of 0.1–1 bar. The paper discusses the challenges that are posed by such a target.

关键词： astrophysics microtargets

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Battery state-of-charge estimation using machine learning analysis of ultrasonic signatures

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能源与人工智能(英文) 2022年第4期10卷 60-72页

作者： Elias Galiounas Tom G.Tranter Rhodri E.Owen James B.Robinson Paul R.Shearing Dan J.L.Brett Electrochemical Innovation Lab Department of Chemical EngineeringUniversity College LondonLondonWC1E 7JEUK The Faraday Institution Quad OneBecquerel AvenueHarwell CampusDidcotOX11 The Alan Turing Institute British Library96 Euston RoadLondon NW12DB

The potential of acoustic signatures to be used for State-of-Charge(SoC)estimation is demonstrated using artificial neural network regression *** approach represents a streamlined method of processing the entire acoustic waveform instead of performing manual,and often arbitrary,waveform peak *** applications where computational economy is prioritised,simple metrics of statistical significance are used to formally identify the most informative waveform *** alone can be exploited for SoC *** is further shown that signal portions representing both early and late interfacial reflections can correlate highly with the SoC and be of predictive value,challenging the more common peak selection methods which focus on the *** later echoes represent greater through-thickness coverage,and are intuitively more information-rich,their presence is not *** waveform treatment offers a more robust approach to correlating acoustic signatures to electrochemical *** is further demonstrated that transformation into the frequency domain can reduce the dimensionality of the problem significantly,while also improving the estimation *** importantly,it is shown that acoustic signatures can be used as sole model inputs to produce highly accurate SoC estimates,without any complementary voltage *** makes the method suitable for applications where redundancy and diversification of SoC estimation approaches is *** is obtained experimentally from a 210 mAh LiCoO2/graphite pouch *** estimation errors as low as 0.75%are achieved on a SoC scale of 0-100%.

关键词： Battery diagnostics Ultrasonic battery monitoring Acoustic battery inspection Mechanical-electrochemical correlation Machine learning Artificial neural networks

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