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First-Principles Assessment of chemical Lithiation of Sulfide Electrolytes and its Impact on Their Transport, Electronic and Mechanical Properties

SSRN

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SSRN 2022年

作者： Hao, Wei Lee, Myungsuk Hwang, Gyeong S. Materials Science and Engineering Program The University of Texas at Austin AustinTX78712 United States McKetta Department of Chemical Engineering The University of Texas at Austin AustinTX78712 United States SK Innovation Korea Republic of

Sulfide-based solid electrolytes (SEs) have received considerable attention, but their practical application is hindered by the lack of chemical stability. When in contact with Li metal, sulfide SEs may undergo decomposition induced by lithiation, which could be largely responsible for the high interfacial impedance observed between them. While the underlying mechanism is still uncertain, this first-principles study examines the structural evolution of sulfide materials, Li3PS4 and Li10GeP2S12, upon lithiation and its impact on their transport, electronic and mechanical properties. Our calculations demonstrate that the lithiation reaction is thermodynamically favorable until reaching full lithiation in which PS43- and GeS44- tetrahedral anions are completely decomposed to S2-, P3- and Ge4- atomic ions. This process is also found to involve the transition formation of small P(Ge) clusters and more importantly an increase in the relative density which may cause void formation at the Li metal/SE interface. Moreover, our analyses highlight that, even when fully lithiated, the sulfide materials could retain the high Li-ion conductivity as well as the ability to block electron transport. This suggests that the chemical decomposition of sulfide SEs would not be the only factor that is responsible for the increase of interfacial impedance during electrochemical cycling. © 2022, The Authors. All rights reserved.

关键词： Solid electrolytes

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Two-Dimensional Metal-Organic Frameworks/Epoxy Composite Coatings with Superior O2/H2O Resistance for Anticorrosion Applications

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ACS applied materials & interfaces 2024年第31期16卷 41421-41434页

作者： Hao-Hsuan Hsia You-Liang Chen Yu-Ting Tai Hong-Kang Tian Chung-Wei Kung Wei-Ren Liu Department of Chemical Engineering R&D Center for Membrane Technology Research Center for Circular Economy Chung Yuan Christian University Taoyuan 32023 Taiwan. Department of Graduate Institude of Applied Science and Technology National Taiwan University of Science and Technology Taipei City 106335 Taiwan. Department of Chemical Engineering National Cheng Kung University Tainan City 70101 Taiwan. Program on Smart and Sustainable Manufacturing Academy of Innovative Semiconductor and Sustainable Manufacturing National Cheng Kung University Tainan 70101 Taiwan. Hierarchical Green-Energy Materials (Hi-GEM) Research Center National Cheng Kung University Tainan 70101 Taiwan.

Corrosion protection technology plays a crucial role in preserving infrastructure, ensuring safety and reliability, and promoting long-term sustainability. In this study, we combined experiments and various analyses to investigate the mechanism of corrosion occurring on the epoxy-based anticorrosive coating containing the additive of two-dimensional (2D) and water-stable zirconium-based metalorganic frameworks (Zr-MOFs). By using benzoic acid as the modulator for the growth of the MOF, a 2D MOF constructed from hexazirconium clusters and BTB linkers (BTB = 1,3,5-tri(4-carboxyphenyl)benzene) with coordinated benzoate (BA-ZrBTB) can be synthesized. By coating the BA-ZrBTB/epoxy composite film (BA-ZrBTB/EP) on the surface of cold-rolled steel (CRS), we found the lowest coating roughness (RMS) of BA-ZrBTB/EP is 2.83 nm with the highest water contact angle as 99.8°, which represents the hydrophobic coating surface. Notably, the corrosion rate of the BA-ZrBTB/EP coating is 2.28 × 10 mpy, which is 4 orders of magnitude lower than that of the CRS substrate. Moreover, the energy barrier for oxygen diffusion through BA-ZrBTB/EP coating is larger than that for epoxy coating (EP), indicating improved oxygen resistance for adding 2D Zr-MOFs as the additive. These results underscore the high efficiency and potential of BA-ZrBTB as a highly promising agent for corrosion prevention in various commercial applications. Furthermore, this study represents the first instance of applying 2D Zr-MOF materials in anticorrosion applications, opening up new possibilities for advanced corrosion-resistant coatings.

关键词： 2D structure Zr-based MOFs anticorrosion density functional theory epoxy hydrophobic

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Unlocking Green Potential: Enhancing Biomass Valorization Via Thermal Depolymerization With Spent Catalysts

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SSRN 2023年

作者： Damayanti, Damayanti Wulandari, Yeni Ria Marpaung, David Septian Supriyadi, Didik Yohana, Dian Tessa Saputri, Desi Riana Sanjaya, Andri Fahni, Yunita Taharuddin, Taharuddin Wu, Ho Shing Department of Chemical Engineering Institut Teknologi Sumatera Jl. Terusan Ryacudu Way Huwi Kec. Jati Agung Lampung Selatan 35365 Indonesia Department of Chemical Engineering and Materials Science Yuan Ze University 135 Yuan Tung Road Chung Li Taoyuan320315 Taiwan Study Program of Industrial Chemical Engineering Technology Lampung State Polytechnic Indonesia Department of Biosystems Engineering Institut Teknologi Sumatera Jl. Terusan Ryacudu Way Huwi Kec. Jati Agung Lampung Selatan 35365 Indonesia Institut Teknologi Sumatera Indonesia

Biomass is globally recognized as an up-and-coming environmentally friendly carbon-based energy source, Suitable catalysts for managing thermal depolymerization of biomass present an alternative method for reducing overall energy usage while maintaining the *** spent catalyst could increase bio-organics production by up to 11%,31%,6%,and 21% in rice straw,brown solid,alkaline, and dealkaline lignin pyrolysis, respectively. The amount of biochar produced in the thermal depolymerization was reduced to 18%,27%,35%,and 32% in rice straw, brown solid, alkaline, and dealkaline pyrolysis, respectively, upon utilizing the spent catalyst. These findings indicate the potential of the spent catalyst for the biomass thermal depolymerization process. © 2023, The Authors. All rights reserved.

关键词： Lignin

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Ionic Liquid-Stabilized Single-Atom Rh Catalyst Against Leaching

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CCS Chemistry 2021年第10期3卷 1814-1822页

作者： Shipeng Ding Max JHülsey Hua An Qian He Hiroyuki Asakura Min Gao Jun-ya Hasegawa Tsunehiro Tanaka Ning Yan Department of Chemical and Biomolecular Engineering National University of SingaporeSingapore 117585 Joint School of the National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207 Department of Materials Science and Engineering National University of SingaporeSingapore 117575 Department of Molecular Engineering Graduate School of EngineeringJapan and Elements Strategy Initiative for Catalysts and Batteries(ESICB)Kyoto UniversityKyoto 615-8510615-8245 Institute for Catalysis Hokkaido UniversitySapporo 001-0021

Single-atom catalysts(SACs)are promising in some reactions typically promoted by homogeneous ***,the leaching of active species from the support in liquid-phase reactions hinders their potential ***,taking the hydroformylation reaction as an example,we report ionic liquid(IL)-induced stabilization of single Rh atoms against *** the ILs examined.

关键词： single-atom catalysts electrostatic stab ilization ionic liquid leaching

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Aggregation-induced emission of copper nanoclusters

Aggregate

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Aggregate 2021年第6期2卷 28-42页

作者： Yu-e Shi Jinzhu Ma Anrui Feng Zhenguang Wang Andrey L.Rogach Key Laboratory of Chemical Biology of Hebei Province Key Laboratory of Medicinal Chemistry and Molecular DiagnosisMinistry of EducationCollege of Chemistry&Environmental ScienceHebei UniversityBaodingP.R.China Department of Materials Science and Engineering&Centre for Functional Photonics(CFP) City University of Hong KongKowloonHong KongS.A.R.P.R.China

Copper nanoclusters(Cu NCs)have recently emerged as promising luminophores,featuring ultra-small size,reasonable photostability,large Stokes shift,and long emission ***-induced emission(AIE)has been often used to further improve both the emission intensity and stability of these clusters,with plenty of potential applications in the fields of chemical sensing and *** review starts with a summary of the current understanding of emission mechanisms of Cu NCs and proceeds with the analysis of contributions from the Cu metal core and the organic *** summarize the recent research progress on the design of ligands,and the ways on how to induce aggregation of the Cu NCs through electrostatic charge neutralization,host-guest interactions,and the use of *** also discuss the current understanding of emission mechanisms of Cu NCs experiencing AIE,such as the often-cited restriction of intramolecular motion and contributions from Cu(I)molecular *** finish this review by providing concluding remarks and offering our own perspective on the active field of AIE of Cu NCs,with a hope to further promote the research on the fundamental aspects of this useful phenomenon.

关键词： aggregation-induced emission copper nanoclusters surface ligands

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Elucidating Dynamic Conductive State Changes in Amorphous Lithium Lanthanum Titanate for Resistive Switching Devices

arXiv

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arXiv 2023年

作者： Shimizu, Ryosuke Cheng, Diyi Zhu, Guomin Han, Bing Marchese, Thomas S. Burger, Randall Xu, Mingjie Pan, Xiaoqing Zhang, Minghao Meng, Ying Shirley Department of NanoEngineering University of California San Diego La Jolla CA United States Materials Science and Engineering Program University of California San Diego La Jolla CA United States Pritzker school of Molecular Engineering University of Chicago ChicagoIL60637 United States Irvine Materials Research Institute University of California Irvine IrvineCA92697 United States

Exploration of novel resistive switching materials attracts attention to replace conventional Si-based transistor and to achieve neuromorphic computing that can surpass the limit of the current Von-Neumann computing for the time of Internet of Things (IoT). materials priorly used to serve as an electrode or electrolyte in batteries have demonstrated metal-insulator transitions upon an external electrical biasing due to resulting compositional change. This property is desirable for future resistive switching devices. Amorphous lithium lanthanum titanate (a-LLTO) was originally developed as a solid-state electrolyte with relatively high lithium ionic conductivity (~10-3 S/cm) and low electronic conductivity (~10-10 S/cm) among oxide-type solid electrolytes. However, it has been suggested that electric conductivity of a-LLTO changes depending on oxygen content. In this work, the investigation of switching behavior of a-LLTO sandwiched by nickel electrodes was conducted by employing a range of voltage sweep techniques, ultimately establishing a stable and optimal operating condition within the voltage window of -3.5 V to 3.5 V. This voltage range effectively balances the desirable trait of a substantial resistance change by three orders of magnitude with the imperative avoidance of LLTO decomposition. This switching behavior is also confirmed at nanodevice of Ni/LLTO/Ni through in-situ biasing inside focused-ion beam/scanning electron microscope (FIB-SEM). Experiment and computation with different LLTO composition shows that LLTO has two distinct conductivity states due to Ti reduction. The distribution of these two states is discussed using simplified binary model, implying the conductive filament growth during low resistance state. Consequently, our study deepens understanding of LLTO electronic properties and encourages the interdisciplinary application of battery materials for resistive switching devices. © 2023, CC BY.

关键词： Electric conductivity

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Electron microscopy observations of the diversity of Ryugu organic matter and its relationship to minerals at the micro- to nano-scale

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Meteoritics and Planetary science 2024年第8期59卷 2023-2043页

作者： Stroud, Rhonda M. Barosch, Jens Bonal, Lydie Burgess, Katherine Cody, George D. De Gregorio, Bradley T. Daly, Luke Dartois, Emmanuel Dobrică, Elena Duprat, Jean Engrand, Cecile Harries, Dennis Hashiguchi, Minako Ishii, Hope Kebukawa, Yoko Kilcoyne, A. David Langenhorst, Falko Lee, Martin R. Nittler, Larry R. Quirico, Eric Okumura, Taiga Remusat, Laurent Sandford, Scott Yabuta, Hikaru Abe, Masanao Abreu, Neyda M. Bagot, Paul A. J. Beck, Pierre Bejach, Laure Bland, Phil A. Bridges, John C. Cymes, Brittany A. Dazzi, Alexandre de la Peña, Francisco Deniset-Besseau, Ariane Enju, Satomi Enokido, Yuma Frank, David R. Gray, Jennifer Haruta, Mitsutaka Hata, Satoshi Hicks, Leon Igami, Yohei Jacob, Damien Kamide, Kanami Komatsu, Mutsumi Laforet, Sylvain Leroux, Hugues Le Guillou, Corentin Martins, Zita Marinova, Maya Martinez, James Mathurin, Jérémie Matsumoto, Megumi Matsumoto, Toru Matsuno, Junya McFadzean, Samuel Michikami, Tatsuhiro Mitsukawa, Itaru Miyake, Akira Miyahara, Masaaki Miyazaki, Akiko Montagnac, Gilles Mostefaoui, Smail Nakamura, Tomoki Nakato, Aiko Naraoka, Hiroshi Nakauchi, Yusuke Nakazawa, Satoru Nishimura, Masahiro Noguchi, Takaaki Ohtaki, Kenta Ohigashi, Takuji Okada, Tatsuaki Okumura, Shota Okazaki, Ryuji Phan, Thi H. V. Rebois, Rolando Sakamoto, Kanako Saiki, Takanao Saito, Hikaru Seto, Yusuke Shigenaka, Miho Smith, William Suga, Hiroki Sun, Mingqi Tachibana, Shogo Takahashi, Yoshio Takeichi, Yasuo Takeuchi, Akihisa Takigawa, Aki Tamenori, Yusuke Tanaka, Satoshi Terui, Fuyuto Thompson, Michelle S. Tomioka, Naotaka Tsuchiyama, Akira Tsuda, Yuichi Uesugi, Kentaro Uesugi, Masayuki Usui, Tomohiro Verdier-Paoletti, Maximilien Wakabayashi, Daisuke Watanabe, Sei-ichiro Yada, Toru Yamashita, Shohei Yasutake, Masahiro Yogata, Kasumi Yoshikawa, Makoto Yurimoto, Hisayoshi Zanetta, Pierre-M. Zega, Thomas Zolensky, Michael E. School of Earth and Space Exploration Arizona State University Materials Science and Technology Division US Naval Research Laboratory Earth and Planets Laboratory Carnegie Institution for Science Institut de Planétologie et d'Astrophysique Université Grenoble Alpes School of Geographical and Earth Sciences University of Glasgow Australian Centre for Microscopy and Microanalysis University of Sydney Department of Materials University of Oxford Institut des Sciences Moléculaires d'Orsay Université Paris-Saclay Centre National de la Recherche Scientifique Hawai‘i Institute of Geophysics and Planetology the University of Hawai‘i at Mānoa Institut de Mineralogie Physique des Materiaux et Cosmochimie Museum National d'Histoire Naturelle Centre National de la Recherche Scientifique UMR 7590 Sorbonne Université Laboratoire de Physique des 2 Infinis Irène Joliot-Curie Centre National de la Recherche Scientifique Université Paris-Saclay Luxembourg Institute of Science and Technology European Space Resources Innovation Centre Graduate School of Environmental Studies Nagoya University Department of Chemistry and Life Science Yokohama National University Institute of Geoscience Friedrich Schiller University Jena Department of Earth and Planetary Science The University of Tokyo NASA Ames Research Center Department of Earth and Planetary Systems Science Hiroshima University Institute of Space and Astronautical Science Japan Aerospace Exploration Agency The Graduate University for Advanced Studies SOKENDAI Langley Research Center NASA School of Earth and Planetary Sciences Curtin University School of Physics and Astronomy University of Leicester Institut Chimie Physique Centre National de la Recherche Scientifique Université Paris-Saclay Université de Lille CNRS INRAE Centrale Lille Université Artois FR 2638-IMEC-Institut Michel-Eugène Chevreul Department of Mathematics Physics and Earth Science Ehime University Department of Earth Science Tohoku University Materials Characterization Lab Th

Transmission electron microscopy analyses of Hayabusa2 samples show that Ryugu organic matter exhibits a range of morphologies, elemental compositions, and carbon functional chemistries consistent with those of carbonaceous chondrites that have experienced low-temperature aqueous alteration. Both nanoglobules and diffuse organic matter are abundant. Non-globular organic particles are also present, and including some that contain nanodiamond clusters. Diffuse organic matter is finely distributed in and around phyllosilicates, forms coatings on other minerals, and is also preserved in vesicles in secondary minerals such as carbonate and pyrrhotite. The average elemental compositions determined by energy-dispersive spectroscopy of extracted, demineralized insoluble organic matter samples A0107 and C0106 are C₁₀₀N₃O₉S₁ and C₁₀₀N₃O₇S₁, respectively, with the difference in O/C slightly outside the difference in the standard error of the mean. The functional chemistry of the nanoglobules varies from mostly aromatic C=C to mixtures of aromatic C=C, ketone C=O, aliphatic (CH_n), and carboxyl (COOH) groups. Diffuse organic matter associated with phyllosilicates has variable aromatic C, ketone and carboxyl groups, and some localized aliphatics, but is dominated by molecular carbonate (CO₃) absorption, comparable to prior observations of clay-bound organic matter in CI meteorites. © 2024 The Authors. Meteoritics & Planetary science published by Wiley Periodicals LLC on behalf of The Meteoritical Society.

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Zwitterion-Bearing Silica Sol for Enhancing Antifouling Performance and Mechanical Strength of Transparent Pdms Coatings

SSRN

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SSRN 2024年

作者： Tan, Jinyan Esteves, A. Catarina C. Yang, Jinlong Zhou, Shuxue Department of Materials Science State Key Laboratory of Molecular Engineering of Polymers Advanced Coatings Research Center Ministry of Education of China Fudan University Shanghai200438 China Laboratory of Physical Chemistry Department of Chemical Engineering and Chemistry Eindhoven University of Technology Eindhoven5600 MB Netherlands Eindhoven University of Technology Eindhoven5600 MB Netherlands International Research Center for Marine Biosciences Ministry of Science and Technology Shanghai Ocean University Shanghai201306 China

The simultaneous improvement of mechanical strength and inhibition of slime attachment for polydimethylsiloxane(PDMS)-based fouling-release coatings remains as a great challenge. In this work, a zwitterionic precursor (N-methoxyacylethyl)-3-aminopropyltriethoxysilane (MAPS) was co-hydrolyzed with tetraethoxysilane (TEOS) to afford zwitterion-bearing silica sols (h-MAPS). The h-MAPS was then simply blended with hydroxyl-terminated PDMS (PDMS-OH, 3060 cSt and 20000 cSt) to fabricate zwitterion-containing PDMS coatings. The pre-hydrolysis process, including hydrolysis time and TEOS content, is critical to the transparency of the coatings. High optical transparency in the range of 88.1-91.4% at 550 nm could be reached using appropriate h-MAPS. Both PDMS-OH (3060 cSt)- and PDMS-OH (20000 cSt)-based coatings presented excellent resistance to slime attachment in real marine environment at relatively high h-MAPS content. An improvement in anti-protein adsorption and anti-bacteria properties was achieved for the coatings based on PDMS-OH (3060 cSt) attributed to the presence of more zwitterions at its surface. Addition of h-MAPS could increase the elastic modulus and tensile strength of PDMS coatings, particularly with high efficiency for the later one. More importantly, although the tensile strength of zwitterion-containing PDMS coatings at high h-MPAS content could be up to 15 MPa, its pseudobarnacle removal strength was lower than 0.4 MPa even after seawater immersion, indicating it retained a good fouling-release performance. As a whole, zwitterion-bearing silica sols can not only provide a new approach for introduction of zwitterions into PDMS coatings, but also efficiently solve the multiple drawbacks of PDMS-based fouling-release coatings, simultaneously. © 2024, The Authors. All rights reserved.

关键词： Coatings

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Grain boundary complexion modification for interface stability in garnet based solid-state Li batteries

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Journal of Power Sources 2024年 602卷

作者： Wang, Chih-Chieh Hsu, Wei-Chun Chang, Chia-Yu Ihrig, Martin Thuy Tran, Ngoc Thanh Lin, Shih-kang Windmüller, Anna Tsai, Chih-Long Eichel, Rüdiger-A. Chiu, Kuo-Feng Department of Materials and Optoelectronic Science National Sun Yat-sen University Kaohsiung80424 Taiwan Institute of Energy and Climate Research Forschungszentrum Jülich GmbH Jülich52425 Germany Department of Chemical Engineering National Taiwan University of Science and Technology Taipei City106 Taiwan Research Center National Cheng Kung University Tainan70101 Taiwan Department of Materials Science and Engineering National Cheng Kung University Tainan70101 Taiwan Program on Smart and Sustainable Manufacturing Academy of Innovative Semiconductor and Sustainable Manufacturing National Cheng Kung University Tainan70101 Taiwan Program on Semiconductor Packaging and Testing Academy of Innovative Semiconductor and Sustainable Manufacturing National Cheng Kung University Tainan70101 Taiwan Core Facility Center National Cheng Kung University Tainan70101 Taiwan Department of Materials Science and Engineering Feng Chia University Taichung407 Taiwan

The garnet type solid-state electrolyte (SSE) encounters challenges related to poor interfacial contact with Li metal and dendrite penetration problem. This study addresses these issues by manipulating the surface property of garnet-based LLZTO (Li6.5La3Zr1.6Ta0.4O12) SSE. The manipulation is achieved by varying thickness of Al2O3 atomic layer deposition (ALD), followed by sintering. Research results show that the relative density, ionic conductivity, and hardness of LLZTO are improved while electronic conductivity is reduced due to the formation of multiple complexions at grain boundary (GB). The SSE pellets also demonstrate improved wettability with Li metal, leading to stable galvanostatic Li plating/stripping cycling with low polarization, which allows for batter battery performance than pristine one. The concept of modifying SSE through the grain boundary complexion modification by thin ALD coating for enhancing the dendrite tolerance with better electrochemical properties of SSE may open a new direction for solid state battery research. © 2024 Elsevier B.V.

关键词： Grain boundaries

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Study on Ag(I) Loaded ZIF-8 and Ag(I) Ion Release in Artificial Seawater

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materials 2023年第5期16卷 2040页

作者： Tsai, Shang-Tien Tang, Wei-Cheng Wei, Yeu-Kuen Wu, Kevin C.-W. Program of Green Materials and Precision Devices National Taiwan University Taipei10617 Taiwan Material and Chemical Research Laboratories Industrial Technology Research Institute Hsinchu30011 Taiwan Department of Chemical Engineering National Taiwan University Taipei10617 Taiwan Institute of Biomedical Engineering & Nanomedicine National Health Research Institutes 35 Keyan Road Miaoli35053 Taiwan Department of Chemical Engineering and Materials Science Yuan Ze University Taoyuan32003 Taiwan Yonsei Frontier Lab Yonsei University 50 Yonsei-ro Seoul03722 Korea Republic of

From a porous structure perspective, the one-stage de novo synthesis method and impregnation method were applied to synthesize Ag(I) ion-containing ZIF-8 samples. With the de novo synthesis method, Ag(I) ions could be located inside micropores or adsorbed on the external surface of the ZIF-8 by selecting AgNO3 in water or Ag2CO3 in ammonia solution as precursors, respectively. The ZIF-8 confining Ag(I) ion exhibited a much lower constant releasing rate than the Ag(I) ion adsorbed on the ZIF-8 surface in artificial seawater. As such, strong diffusion resistance in association with the confinement effect is contributed by ZIF-8’s micropore. On the other hand, the release of Ag(I) ions adsorbed on the external surface was diffusion limited. Therefore, the releasing rate would reach a maximum not increasing with Ag(I) loading in the ZIF-8 sample. © 2023 by the authors.

关键词： Ions

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