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Laser-induced plasma formation in water with up to 400 mJ double-pulse LIBS

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Plasma Science and Technology 2024年第1期26卷 93-100页

作者： Marion HeNKeL Michelle SIeMeNS Ralf MeTHLING Benjamin eMDe Jörg HeRMSDORF Steffen FRANKe Diego GONZALeZ leibniz institute for Plasma Science and Technology(INP) Felix-Hausdorff-Straße 2Greifswald 17489Germany Laser Zentrum Hannover e.v.(LZH) Hollerithallee 8Hannover 30419Germany

Double-pulse LIBS is a promising technique for deep-sea *** measurements in shallow water with up to 400 mJ each pulse were done to select laser parameters which promote optimized spectral line emission from plasma even at elevated pressures,where line broadening until loss of most of the spectral information can *** emission spectroscopy,using a Czerny-Turner spectrometer,has been applied to investigate the dependence of the emitted radiation on laser parameters and hydrostatic *** has been found,that higher laser pulse energies,especially with short pulse delay as required in high water pressure,can also have an adverse effect on the measured spectrum.

关键词： double-pulse LIBS underwater plasma formation emission spectrosocpy

Co-aromatization of methane and hexane over Pt encapsulated in ZSM-5 zeolite and the electronic effect of K promoters

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Science China Chemistry 2024年第3期67卷 1017-1027页

作者： Bei Liu Fan Wang Xiaomeng Dou Pengfei Li Hongwei Xiang Yong Yang Peng He State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China Department of Chemistry Tsinghua UniversityBeijing 100084China National energy R&D Center for Coal to Liquid Fuels Synfuels China Technology Co.Ltd.Beijing 101407China University of Chinese Academy of Sciences Beijing 101408China leibniz-institut für Katalyse e.v.an der Universitat Rostock Rostock 18059Germany

The co-aromatization of methane with higher hydrocarbons represents a promising route to valorize methane, an abundant but underexploited carbon resource. In this study, we elucidate a novel approach to enhance the catalytic co-aromatization of hexane and methane by confining Pt within zeolite catalysts and modulating its electron density. Our findings show that encapsulating Pt within MFI structure is pivotal for activating the feedstock and fostering the formation of aromatic products. Interaction between K atoms and the silanol nest forms siloxy groups which are critical for the stabilization of Pt species. Tuning the K content in PtSn@MFI catalysts adeptly alters the electronic configuration of Pt clusters. This modification is corroborated by infrared and X-ray photoelectron spectroscopy analysis, and density functional theory calculations. Remarkably, the catalyst with 0.8 wt% K exhibits an optimal Pt electron density, driving its superior efficacy in the co-aromatization reaction, converting 0.78 mol of methane for each mole of hexane processed. By employing ~(13)C isotopic labeling and solid-state NMR studies, we demonstrate the participation of methane in the adsorbed species inside the zeolite channel and its incorporation to the benzyl site of the substitute group and phenyl rings in aromatic compounds, underscoring the importance of Pt encapsulation.

关键词： Pt encapsulation MFI zeolite methane activation co-aromatization ^(13)C solid-state NMR

From non-carbon host toward carbon-free lithium-sulfur batteries

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Nano Research 2024年第3期17卷 1337-1365页

作者： Yanqi Feng Hui Liu Qiongqiong Lu School of Materials Science and engineering Shaanxi Key Laboratory of Green Preparation and Functionalization for Inorganic MaterialsShaanxi University of Science and TechnologyXi’an 710021China institute of Materials Henan Key Laboratory of Advanced Conductor MaterialsHenan Academy of SciencesZhengzhou 450046China leibniz institute for Solid State and Materials Research(IFW)Dresden e.v. Helmholtzstraβe 2001069 DresdenGermany School of Materials&e.vironment engineering Chengdu Technological UniversityChengdu 611730China

Lithium-sulfur(Li-S)batteries with advantages of high energy densities(2600 Wh·kg^(-1)/2800 Wh·L^(-1))and sulfur abundance are regarded as promising candidates for next-generation high-energy ***,the conventional carbon host used in sulfur cathodes suffers from poor chemical adsorption towards Li-polysulfides(LPS)in liquid electrolyte and sluggish redox kinetics,leading to low capacity and rate ***,carbon host used in Li metal anode with the intrinsic property of poor lithiophilicity and high Li-nucleation barrier gives rise to uncontrollable dendrite growth and further battery ***,non-carbon hosts with chemical adsorption toward LPS and catalytic activity for accelerating LPS redox conversion as well as lithiophilic property for guiding uniform Li deposition are proposed and demonstrated a high efficiency in both sulfur cathodes and Li metal *** this review,the principle and challenges of Li-S batteries are first presented,then recent work using non-carbon hosts in Li-S batteries is summarized comprehensively,and the mechanism of non-carbon host in improving sulfur utilization and stabilizing Li metal anode is discussed in ***,remaining challenges and outlook on the implementation of non-carbon host for practical carbon-free Li-S batteries are also provided.

关键词： sulfur cathode Li metal anode polysulfides adsorption catalytic effect Li dendrite carbon-free lithium-sulfur batteries

Generation and transformation ofα-oxy carbene intermediates enabled by copper-catalyzed carbonylation

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Green Carbon 2024年第1期2卷 70-80页

作者： Yang Yuan Xiao-Feng Wu Dalian National Laboratory for Clean energy Dalian Institute of Chemical PhysicsChinese Academy of Sciences116023 DalianLiaoningChina leibniz-institut für Katalyse e.v. Albert-Einstein-Straße 29a18059 RostockGermany

Since the Fischer-Tropsch reaction was discovered by Otto Roelen in 1938,transition metal-catalyzed carbo-nylation reactions come in as one of the most important methods for preparing carbonyl-containing and carbon chain-increased *** a result,the field of carbonylation research has rece.ved considerable attention over the past decades and continues to *** the continuous development of carbonylation and the in-depth study of the mechanism,more mechanistic details and variations have been revealed,which provide more possibilities for organic ***,copper catalysis has been introduced to the carbonylative functio-nalization of alkenes,thus enabling the rapid assembly of functionalized carbonyl compounds from simple starting *** this Account,we summarize the new findings in the Cu-catalyzed borocarbonylation of alkenes based on the generation and transformation ofα-oxy carbene *** believe that the results presented in this Account will further inspire the design of new carbonylation reactions.

关键词： Carbonylation Copper catalyst Carbene Carbon monoxide Domino reaction

Temperature and structure measurements of he.vy-ion-heated diamond using in situ X-ray diagnostics

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Matter and Radiation at extremes 2024年第4期9卷 80-89页

作者： J.Lutgert P.Hesselbach M.Schorner v.Bagnoud R.Belikov P.Drechsel B.Heuser O.SHumphries P.Katrik B.Lindqvist C.Qu R.Redmer D.Riley G.Schaumann S.Schumacher A.Tauschwitz D.varentsov K.Weyrich X.Yu B.Zielbauer Zs.Major P.Neumayer D.Kraus institut fur Physik Universitat RostockAlbert-Einstein-Str.2318059 RostockGermany GSI Helmholtzzentrum fur Schwerionenforschung Planckstr.164291 DarmstadtGermany institut für Angewandte Physik Goethe-Universität Frankfurt am MainMax-von-Laue-Str.160438 Frankfurt am MainGermany institut fur Geowissenschaften Goethe-Universitat Frankfurt am MainAltenhoferallee 160438 Frankfurt am MainGermany Helmholtz-Zentrum Dresden-Rossendorf Bautzner Landstr.40001328 DresdenGermany european XFeL GmbH Holzkoppel 422869 SchenefeldGermany Centre for Plasma Physics School of Mathematics and PhysicsQueen’s University BelfastUniversity RoadBelfast BT71NNUnited Kingdom institut für Kernphysik Technische Universität DarmstadtSchlossgartenstr.964289 DarmstadtGermany State Key Laboratory of Nuclear Physics and Technology Institute of Heavy Ion PhysicsPeking UniversityBeijing 100871China Helmholtz institut Jena Frobelstieg 307743 JenaGermany

We present in situ measurements of spectrally resolved X-ray scattering and X-ray diffraction from monocrystalline diamond samples heatedwith an intense pulse of he.vy *** this way,we determine the samples’heating dynamics and their microscopic and macroscopic structuralintegrity over a timespan of several *** the ratio of elastic to inelastic scattering with state-of-the-art density functionaltheory molecular dynamics simulations allows the inference of average temperatures around 1300 K,in agreement with predictions fromstopping power *** simultaneous diffraction measurements show no hints of any volumetric graphitization of the material,butdo indicate the onset of fracture in the diamond *** experiments pave the way for future studies at the Facility for Antiproton andIon Research,where a substantially increased intensity of the he.vy ion beam will be available.

关键词： heated intense structure

Palladium-catalyzed oxidative double alkoxycarbonylation of ethylene toward succinic acid derivatives

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Green Carbon 2024年第2期2卷 205-208页

作者： Zhi-Peng Bao Cunyao Li Li Yan Yunjie Ding Xiao-Feng Wu Dalian National Laboratory for Clean energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianLiaoning 116023China leibniz-institut für Katalyse e.v. Rostock 18059Germany

employing biodegradable plastics is one of the choices to solve white pollution *** succinate(PBS),as a biodegradable plastic with good stability and heat resistance,is produced by polymerization of succinic acid and butylene ***,inadequate supply of the direct upstream material succinic acid restricts the development of this *** this work,we provide a carbonylative strategy to construct succinic acid derivatives from carbon monoxide(CO),ethylene and *** reaction catalyzed by palladium catalyst under oxidative conditions.

关键词： ethylene Alcohols Palladium Carbonylation Succinic acid derivatives

Realizing methanol synthesis from CO and water via the synergistic effect of Cu^(0)/Cu^(+)over Cu/ZrO_(2) catalyst

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Journal of energy Chemistry 2024年第6期93卷 126-134,I0004页

作者： Yuan Fang Fan Wang Yang Chen Qian Lv Kun Jiang Hua Yang Huibo Zhao Peng Wang Yuyan Gan Lizhi Wu Yu Tang Xinhua Gao Li Tan institute of Molecular Catalysis and In Situ/Operando Studies Fujian Key Laboratory of Electrochemical Energy Storage MaterialsState Key Laboratory of Photocatalysis on Energy and EnvironmentCollege of ChemistryFuzhou UniversityFuzhou 350108FujianChina leibniz-institut für Katalyse e.v.an der Universität Rostock Albert-Einstein Strasse 9118059 RostockGermany Department of Chemistry Tsinghua UniversityBeijing 100084China State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical engineering College of Chemistry and Chemical EngineeringNingxia UniversityYinchuan 750021Ningxi1China

The optimizing utilization of ca rbon resources has drawn wide attention all over the world,while exploiting the high-efficiency catalytic routes remains a ***,a direct methanol synthesis route is realized from pure CO and H_(2)O over 10%Cu/t-ZrO_(2) catalyst,where the time yield of methanol is144.43 mmol mol_(Cu)^(-1)h^(-1)and the methanol selectivity in hydrocarbons is 100%,The Cu species highly dispersed in the t-ZrO_(2) support lead parts of them in the cationic *** Cu^(+)sites contribute to the dissociation of H_(2)O,providing the H*source for methanol synthesis,while the formed Cu^(0) sites promote the absorption and transfer of H*during the ***,the H_(2)O is even a better H resource than H_(2) due to its better dissociation effectivity in this catalytic *** present work offers a new approach for methanol synthesis from CO and new insight into the process of supplying H donor.

关键词： H_(2)O CO Methanol Cu-based catalysts t-ZrO_(2)

enlarged interlayer of separator coating enabling high-performance lithiumsulfur batteries

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Frontiers of Chemical Science and engineering 2024年第2期18卷 103-112页

作者： Yanqi Feng Hui Liu Xiaoting Liu Qiongqiong Lu School of Materials&e.vironment engineering Chengdu Technological UniversityChengdu 611730China School of Materials Science and engineering Shaanxi Key Laboratory of Green Preparation and Functionalization for Inorganic MaterialsShaanxi University of Science and TechnologyXi’an 710021China Green Catalysis Center and College of ChemistryZhengzhou UniversityZhengzhou 450001China institute of Materials Henan Key Laboratory of Advanced Conductor MaterialsHenan Academy of SciencesZhengzhou 450046China leibniz institute for Solid State and Materials Research(IFW) Dresden e.V.Dresden 01069Germany

Lithiumsulfur batteries have been intensively studied due to their high theoretical energy density and abundant sulfur resources. However, their commercial application is hindered by the low redox kinetics and high sulfur losses. In principle, in the design of cathodes and separators, the adsorption toward lithium-polysulfides should be enhanced and the conversion of soluble high-order lithium-polysulfides should be catalyzed. Herein, a Kv_(3)O_(8)·0.75H_(2)O separator is designed as an effective lithium-polysulfides mediator in lithiumsulfur batteries. The intercalated K+ would enlarge the interlayer spacing of vanadium oxides, preventing the collapse of the layer structure and improving the electrical/ion conductivity of the interface. More.ver, the Kv_(3)O_(8)·0.75H_(2)O modified separator possess a prior adsorption and high redox kinetics toward lithium-polysulfides due to the enhanced diffusion kinetics, which guarantees the high-rate capability and efficient utilization of sulfur. As a result, lithiumsulfur batteries exhibit a high capacity of 1362 mAh·g^(-1) and a long lifespan with a low capacity loss of 0.073% per cycle. This work may provide an alternative way to establish a functional separator to balance the adsorption and conversion of polysulfides during the redox back and forth.

关键词： lithium kinetics adsorption

Recent advances in intermediate-temperature CO_(2) capture: Materials,technologies and applications

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Journal of energy Chemistry 2024年第3期90卷 435-452,I0010页

作者： Chengbo Zhao Leiming Wang Liang Huang Nicholas M.Musyoka Tianshan Xue Jabor Rabeah Qiang Wang engineering Research Center for Water Pollution Source Control&eco-remediation College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China State Key Laboratory of efficient Production of Forest Resources Beijing Forestry UniversityBeijing 100083China China Machinery Huanyu Certification and Inspection Co. Ltd.Beijing 102609China Nottingham Ningbo China Beacons of excellence Research and Innovation institute University of Nottingham Ningbo ChinaNingbo 315100ZhejiangChina institute of Atmospheric e.vironment Chinese Research Academy of Environmental SciencesBeijing 100012China leibniz-institut für Katalyse e.v. Albert-Einstein-Str.29aRostock D-18059Germany

Carbon capture,utilization and storage(CCUS) is widely recognized as a vital strategy for mitigating the impact of human induced climate *** various CO_(2) adsorbents,intermediate-temperature solid adsorbents have garnered significant attention due to their potential applications in hydrogen utilization,specifically in the water gas shift,steam reforming and gasification *** processes are crucial for achieving carbon *** laboratory-level studies have showcased the high adsorption capacity of these materials via various synthesis and modification methods,their practical application in complex industrial e.vironments remains challenging,impeding the commercialization *** review aims to critically summarize the recent research progress made in intermediatetemperature(200-400℃) solid CO_(2) adsorbents,particularly focusing on indicators such as cyclability,gas selectivity,and formability,which play vital roles in industrial application ***,we provide an ove.view of laboratory-level advanced technologies specifically tailored for industrial ***,we highlight several industrial-ready advanced technologies that can pave the way for overcoming the challenges associated with large-scale *** insights provided by this review aim to assist researchers in identifying the most relevant research directions for industrial *** promoting advances in the application of solid adsorbents,we strive to facilitate the ultimate goal of achieving carbon neutrality.

关键词： Intermediate-temperature CO_(2) capture MgO LDHs Industrialization