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Pulsed laser interference patterning of transition-metal carbides for stable alkaline water electrolysis kinetics

carbon Energy 2024年第5期6卷 65-80页

作者： Yewon Oh Jayaraman Theerthagiri Ahreum Min cheol Joo Moon Yiseul Yu Myong Yong choi Department of chemistry(BK21 FOUr) Research Institute of Natural SciencesGyeongsang National UniversityJinjuRepublic of Korea core−Facility center for Photochemistry and Nanomaterials Gyeongsang National UniversityJinjuRepublic of Korea

We investigated the role of metal atomization and solvent decomposition into reductive species and carbon clusters in the phase formation of transition-metal carbides(TMcs;namely,co_(3)c,Fe_(3)c,Tic,and Moc)by pulsed laser ablation of co,Fe,Ti,and Mo metals in *** interaction between carbon s-p-orbitals and metal d-orbitals causes a redistribution of valence structure through charge transfer,leading to the formation of surface defects as observed by X-ray photoelectron *** defects influence the evolved TMcs,making them effective for hydrogen and oxygen evolution reactions(HEr and OEr)in an alkaline ***_(3)c with more oxygen affinity promoted coO(OH)intermediates,and the electrochemical surface oxidation to co_(3)O_(4)was captured via in situ/operando electrochemical raman probes,increasing the number of active sites for OEr *** with more d-vacancies exhibits strong hydrogen binding,promoting HEr kinetics,whereas Fe_(3)c and Tic with more defect states to trap charge carriers may hinder both OEr and HEr *** results show that the assembled membrane-less electrolyzer with co_(3)c∥co_(3)c and Moc∥Moc electrodes requires~2.01 and 1.99 V,respectively,to deliver a 10 mA cm−2 with excellent electrochemical and structural *** addition,the ascertained pulsed laser synthesis mechanism and unit-cell packing relations will open up sustainable pathways for obtaining highly stable electrocatalysts for electrolyzers.

关键词： acetone H_(2)and O_(2)evolution reactions pulsed laser ablation surface defects transition-metal carbides water electrolyzer

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Tailoring local structures of atomically dispersed copper sites for highly selective cO_(2) electroreduction

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carbon Energy 2024年第4期6卷 79-90页

作者： Kyung‐Jong Noh Byoung Joon Park Ying Wang Yejung choi Sang‐Hoon You Yong‐Tae Kim Kug‐Seung Lee Jeong Woo Han Department of chemical Engineering Pohang University of Science and Technology(POSTECH)PohangGyeongbukRepublic of Korea Department of Materials Science and Engineering Pohang University of Science and Technology(POSTECH)PohangGyeongbukRepublic of Korea Pohang Accelerator Laboratory(PAL) Beamline DivisionPohangGyeongbukRepublic of Korea

Atomically‐dispersed copper sites coordinated with nitrogen‐doped carbon(cu–N–c)can provide novel possibilities to enable highly selective and active electrochemical cO_(2) reduction ***,the construction of optimal local electronic structures for nitrogen‐coordinated cu sites(cu–N_(4))on carbon remains ***,we synthesized the cu–N–c catalysts with atomically‐dispersed edge‐hosted cu–N_(4) sites(cu–N_(4)c_(8))located in a micropore between two graphitic sheets via a facile method to control the concentration of metal ***‐hosted cu–N_(4)c_(8) catalysts outperformed the previously reported M–N–c catalysts for cO_(2)‐to‐cO conversion,achieving a maximum cO Faradaic efficiency(FEcO)of 96%,a cO current density of–8.97 mA cm^(–2) at–0.8 V versus reversible hydrogen electrode(rHE),and over FEcO of 90%from–0.6 to–1.0 V versus *** studies revealed that the micropore of the graphitic layer in edge‐hosted cu–N_(4)c_(8) sites causes the d‐orbital energy level of the cu atom to shift upward,which in return decreases the occupancy of antibonding states in the*cOOH *** research suggests new insights into tailoring the locally coordinated structure of the electrocatalyst at the atomic scale to achieve highly selective electrocatalytic reactions.

关键词： atomic local structure density functional theory electrochemical cO_(2)reduction metal nitrogen‐doped carbon single‐atom catalyst

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critical factors to inhibit water-splitting side reaction in carbon-based electrode materials for zinc metal anodes

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carbon Energy 2022年第6期4卷 1080-1092页

作者： Dong Hyuk Kang Eunji Lee Beom Sik Youn Son Ha Jong chan Hyun Juhee Yoon Dawon Jang Kyoung Sun Kim Hyungsub Kim Sang Moon Lee Sungho Lee Hyoung-Joon Jin Hyung-Kyu Lim Young Soo Yun KU-KIST Graduate School of converging Science and Technology Korea UniversitySeoulSeongbuk-guSouth Korea Division of chemical Engineering and Bioengineering Kangwon National UniversityChuncheonGangwon-doSouth Korea Department of Eco-Polymer Science and Engineering Inha UniversityIncheonMichuhol-guSouth Korea carbon composite Materials research center Institute of Advanced Composite MaterialsKorea Institute of Science and Technology(KIST)Jeollabuk-doSouth Korea Department of chemical and Biological Engineering Korea UniversitySeoulSeongbuk-guSouth Korea Neutron Science Division Korea Atomic Energy Research Institute(KAERI)DaejeonYuseong-guSouth Korea research center for Materials Analysis Korea Basic Science Institute(KBSI)DaejeonYuseong-guSouth Korea Department of Integrative Energy Engineering Korea UniversitySeoulSeongbuk-guSouth Korea

Zinc metal anodes(ZMA)have high theoretical capacities(820 mAh g−1 and 5855 mAh cm−3)and redox potential(−0.76 V *** hydrogen electrode),similar to the electrochemical voltage window of the hydrogen evolution reaction(HEr)in a mild acidic electrolyte system,facilitating aqueous zinc batteries competitive in next-generation energy storage ***,the HEr and byproduct formation effectuated by water-splitting deteriorate the electrochemical performance of ZMA,limiting their *** this study,a key factor in promoting the HEr in carbon-based electrode materials(cEMs),which can provide a larger active surface area and guide uniform zinc metal deposition,was investigated using a series of threedimensional structured templating carbon electrodes(3D-TcEs)with different local graphitic orderings,pore structures,and surface *** ultramicropores of cEMs are the determining critical factors in initiating HEr and clogging active surfaces by Zn(OH)2 byproduct formation,through a systematic comparative study based on the 3D-TcE series *** the 3D-TcEs had a proper graphitic structure with few ultramicropores,they showed highly stable cycling performances over 2000 cycles with average coulombic efficiencies of≥99%.These results suggest that a well-designed cEM can lead to high-performance ZMA in aqueous zinc batteries.

关键词： aqueous batteries carbon electrode hydrogen evolution reaction multivalent ion zinc metal anode

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Effects of nanopores and sulfur doping on hierarchically bunched carbon fibers to protect lithium metal anode

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carbon Energy 2021年第5期3卷 784-794页

作者： Ji In Jung Sunwoo Park Son Ha Se Youn cho Hyoung-Joon Jin Young Soo Yun Program in Environmental and Polymer Engineering Inha UniversityIncheonSouth Korea KU-KIST Graduate School of converging Science and Technology Korea UniversitySeoulSouth Korea carbon composite Materials research center Korea Institute of Science and TechnologyWanju-gunJeollabuk-doSouth Korea Department of Polymer Science and Engineering Inha UniversityIncheonSouth Korea Department of Integrative Energy Engineering Korea UniversitySeoulSouth Korea

Studies on three-dimensional structured carbon templates have focused on how to guide homogeneous lithium metal nucleation and growth for lithium metal anodes(LMAs).However,there is still insufficient evidence for a key factor to achieve their high electrochemical ***,the effects of nanopores and sulfur doping on carbon-based nanoporous host(cNH)electrode materials for LMAs were investigated using natural polymer-derived *** pore-filling behaviors of lithium metal in the nanopores of the cNH electrode materials were first observed by ex situ scanning electron microscopy analysis,where the protective lithium metal nucleation and growth process led to significantly high coulombic efficiency(cE)of~99.4%and stable 600 *** addition,a comparison study of cNH and sulfurdoped cNH(S-cNH)electrodes,which differ only in the presence or absence of sulfur,revealed that sulfur doping can cause lower electrochemical series resistance,higher cE value,and better cycling stability in a wide range of current densities and number of ***,S-cNH-based LMAs showed high electrochemical performance in full-cell Li-S battery tests using a sulfur copolymer cathode,where a high energy density of 1370Wh kgelectrode−1 and an excellent power density of 4120Wkgelectrode−1 were obtained.

关键词： carbon template Li-S batteries lithium metal anode lithium metal batteries nanoporous carbon sulfur doping

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Overview of emerging catalytic materials for electrochemical green ammonia synthesis and process

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carbon Energy 2023年第12期5卷 31-82页

作者： Venkata Thulasivarma chebrolu Daehee Jang Gokana Mohana rani chaeeun Lim Kijung Yong Won Bae Kim Department of chemical Engineering Pohang University of Science and Technology(POSTECH)PohangGyeongbukSouth Korea Department of Biological Sciences and Bioengineering Inha UniversityIncheonRepublic of Korea

The concept of“green-ammonia-zero-carbon emission”is an emerging research topic in the global community and many countries driving toward decarbonizing a diversity of applications dependent on fossil *** light of this,electrochemical nitrogen reduction reaction(ENrr)received great attention at ambient *** low efficiency(%)and ammonia(NH_(3))production rates are two major challenges in making a sustainable ***,hydrogen evolution reaction is another crucial factor for realizing this NH_(3)synthesis to meet the large-scale commercial ***,the(i)importance of NH_(3)as an energy carrier for the next future,(ii)discussion with ENrr theory and the fundamental mechanism,(iii)device configuration and types of electrolytic systems for NH_(3)synthesis including key metrics,(iv)then moving into rising electrocatalysts for ENrr such as single-atom catalysts(SAcs),MXenes,and metal–organic frameworks that were scientifically summarized,and(v)finally,the current technical contests and future perceptions are ***,this review aims to give insightful direction and a fresh motivation toward ENrr and the development of advanced electrocatalysts in terms of cost,efficiency,and technologically large scale for the synthesis of green NH_(3).

关键词： electrochemical ammonia synthesis hydrogen energy carrier metal-organic-frameworks MXenes single-atom-catalysts

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Passivation engineering via silica‐encapsulated quantum dots for highly sensitive photodetection

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carbon Energy 2023年第9期5卷 49-62页

作者： Ji Yun chun Byung Gi Kim Jin Young Kim Woongsik Jang Dong Hwan Wang School of Integrative Engineering Chung‐Ang UniversitySeoulRepublic of Korea

Organometal halide perovskites are promising semiconducting materials for photodetectors because of their favorable optoelectrical *** nanoscale perovskite materials such as quantum dots(QDs)show novel behavior,they have intrinsic stability *** this study,an effectively silane barrier-capped quantum dot(QD@APDEMS)is thinly applied onto a bulk perovskite photosensitive layer for use in ***@APDEMS is synthesized with a silane ligand with hydrophobic cH_(3)-terminal groups,resulting in excellent dispersibility and durability to enable effective *** introduction of the QD@APDEMS layer results in the formation of a lowdefect perovskite film with enlarged *** is attributed to the grain boundary interconnection effect via interaction between the functional groups of QD@APDEMS and uncoordinated Pb^(2+)in grain *** passivating the grain boundaries,where various trap sites are distributed,hole chargecarrier injection and shunt leakage can be ***,from the energy point of view,the deep highest occupied molecular orbital(HOMO)level of QD@APDEMS can work as a hole charge injection *** charge dynamics(generation,transfer,and recombination properties)and reduced trap density of QD@APDEMS are *** this perovskite film is used in a photodetector,the device performance(especially the detectivity)stands out among existing perovskites evaluated for energy sensing device applications.

关键词： grain boundary passivation perovskite quantum dots photodetectors photosensitive layers trap

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Aggregation-induced emission luminogens for organic light-emitting diodes with a single-component emitting layer

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聚集体(英文) 2023年第1期4卷 41-89页

作者： Jinhyo Hwang Peethani Nagaraju Min Ju cho Dong Hoon choi Department of chemistry Research Institute for Natural SciencesKorea UniversitySeongbuk-guSeoulRepublic of Korea

Organic light-emitting diodes(OLEDs)have garnered increasing attention as a promising candidate for application in next-generation displays and solid-state lighting *** doping technique commonly used to fabricate light-emitting layers(EMLs)of OLEDs disperses the emitting material in a host matrix to mitigate aggregation-induced quenching(AcQ).Alternatively,owing to their high efficiency and ease of manufacture,nondoped OLEDs have been developed as a substitute for doped *** fabricating nondoped OLEDs,it is essential to suppress the AcQ effect in the EML and efficiently utilize the generated excitons for radiative *** the discovery of aggregation-induced emission(AIE)by Tang et al.,significant work has been done to improve the stability and efficiency of nondoped OLEDs based on fluorescent AIE luminogens(AIEgens).Fluorescent AIEgens,synthesized using various molecular frameworks,such as silole,tetra/triphenylethylene,tetraphenylpyrazine,and tetraphenylbenzene,exhibit high photoluminescence quantum yields in the solid ***,many studies have reported that fluorescent AIEgen-based OLEDs have excellent external quantum efficiency and exhibit emission at various wavelengths,including deep-blue/blue/green *** the development of fluorescent AIEgens,delayed fluorescent AIEgens with efficient triplet utilization through reverse intersystem crossing and AIE properties have been adopted as ideal emitters and used in nondoped *** review systematically discusses and summarizes recent reports on the development of AIEgens for nondoped OLEDs by grouping them into fluorescent and delayed fluorescent *** purpose of this review is to provide deep insights into the design of novel AIEgens for high-performance nondoped OLEDs.

关键词： aggregation-induced emission nondoped emitting layer organic light-emitting diode

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Geometric and physical configurations of meta-atoms for advanced metasurface holography

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InfoMat 2021年第7期3卷 739-754页

作者： Joohoon Kim Younghwan Yang Trevon Badloe Inki Kim Gwanho Yoon Junsuk rho Department of Mechanical Engineering Pohang University of Science and TechnologyPohangSouth Korea Department of Manufacturing Systems and Design Engineering Seoul National University of Science and TechnologySeoulSouth Korea Department of chemical Engineering Pohang University of Science and TechnologyPohangSouth Korea

Metasurfaces consisting of subwavelength structures,so-called meta-atoms,have steadily attracted considerable attention for advanced holography due to their advantages in terms of high-resolution holographic images,large field of view,and compact device *** contrast to conventional holographic displays using bulky conventional diffractive optical elements,metasurface holography enables arbitrary complex wavefront shaping with a much smaller *** this review,we classify metasurface holography according to the meta-atom design methodologies,which can further expand hologram *** describe light-matter interactions,particularly in metasurface systems,using the relevant the Jones matrix to rigorously explain modulations of the amplitude,phase,and polarization of *** different types of metaatoms are presented,and the corresponding achievable wavefronts that form the holographic images in the far-field are also *** a simple classification will give a straightforward approach to design and further realize advanced metasurface holographic devices.

关键词： Jones calculus meta-atom metahologram metamaterial metasurface

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Phased,chromosome-scale genome assemblies of tetraploid potato reveal a complex genome,transcriptome,and predicted proteome landscape underpinning genetic diversity

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Molecular Plant 2022年第3期15卷 520-536页

作者： Genevieve Hoopes Xiaoxi Meng John P.Hamilton Sai reddy Achakkagari Fernanda de Alves Freitas Guesdes Marie E.Bolger Joseph J.coombs Danny Esselink Natalie r.Kaiser Linda Kodde Maria Kyriakidou Brian Lavrijssen Natascha van Lieshout rachel Shereda Heather K.Tuttle Brieanne Vaillancourt Joshua c.Wood Jan Mde Boer Nolan Bornowski Peter Bourke David Douches Herman Jvan Eck Dave Ellis Max J.Feldman Kyle M.Gardner Johannes c.P.Hopman Jiming Jiang Walter S.De Jong Joseph c.Kuhl richard G.Novy Stan Oome Vidyasagar Sathuvalli Ek Han Tan remco A.Ursum M.Isabel Vales Kelly Vining richard G.F.Visser Jack Vossen G.craig Yencho Noelle L.Anglin christian W.B.Bachem Jeffrey B.Endelman Laura M.Shannon Martina V.Stromvik Helen H.Tai Bjorn Usadel c.robin Buell richard Finkers Department of Plant Biology Michigan State UniversityEast LansingMI 48824USA Department of Horticultural Science University of MinnesotaSt.PaulMN 55108USA Department of Plant Science McGill UniversitySainte-Anne-de-BellevueQC H9X 3V9Canada Plant Breeding Wageningen University&ResearchPlant Breeding6708 PB Wageningenthe Netherlands IBG-4 Bioinformatics Forschungszentrum JülichWilhelm Johnen Str52428 JülichGermany Department of Plant Soiland Microbial SciencesMichigan State UniversityEast LansingMI 48824USA Bayer crop Science WoodlandCA 95695USA Averis Seeds B.V. 9640 AA Veendamthe Netherlands International Potato center 1895 Avenida La MolinaLimaPeru USDA-ArS ProsserWA 99350USA Agriculture and Agri-Food canada Fredericton research and Development centre FrederictonNB E3B 4Z7Canada School of Integrative Plant Science Cornell UniversityIthacaNY 14853-1901USA Department of Plant Sciences University of IdahoMoscowID 83844USA USDA-ArS Small Grains and Potato Germplasm ResearchAberdeenID 83210USA HZPc research B.V. Edisonweg 58501 XG Jourethe Netherlands Department of crop and Soil Science Oregon State UniversityHermistonOR 97838USA School of Biology and Ecology University of Maine5735 Hitchner Hall OronoME 04469USA Department of Horticultural Sciences Texas A&M UniversityCollege StationTX 77843-2133USA Department of Horticulture Oregon State UniversityCorvallisOR 97331USA Department of Horticultural Science North Carolina State UniversityRaleighNC 27695-7609USA Department of Horticulture University of Wisconsin-MadisonMadisonWI 53706USA Department of Horticulture Michigan State UniversityEast LansingMI 48824USA Institute for Biological Data Science Heinrich Heine UniversityDusseldorf40225 DusseldorfGermany Plant resilience Institute Michigan State UniversityEast LansingMI 48824USA Present address:GenNovation B.V. Wageningenthe Netherlands

cultivated potato is a clonally propagated autotetraploid species with a highly heterogeneous *** assemblies of six cultivars including two chromosome-scale phased genome assemblies revealed extensive allelic diversity,including altered coding and transcript sequences,preferential allele expression,and structural variation that collectively result in a highly complex transcriptome and predicted proteome,which are distributed across the homologous *** species contribute to the extensive allelic diversity in tetraploid cultivars,demonstrating ancestral introgressions predating modern breeding *** a clonally propagated autotetraploid that undergoes limited meiosis,dysfunctional and deleterious alleles are not purged in tetraploid *** a quarter of the loci bore mutations are predicted to have a high negative impact on protein function,complicating breeder’s efforts to reduce genetic *** StcDF1 locus controls maturity,and analysis of six tetraploid genomes revealed that 12 allelic variants of StcDF1 are correlated with maturity in a dosage-dependent *** of the complexity of the tetraploid potato genome with its rampant structural variation and embedded deleterious and dysfunctional alleles will be key not only to implementing precision breeding of tetraploid cultivars but also to the construction of homozygous,diploid potato germplasm containing favorable alleles to capitalize on heterosis in F1 hybrids.

关键词： potato allele diversity phased assembly polyploid pan-genome wild introgressions

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