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Investigation of Li-ion transport in Li7P3S11 and solid-state lithium batteries

Journal of Energy Chemistry 2019年第11期28卷 1-7页

作者： Chuang Yu swapna ganapathy Ernst R.H.van Eck Lambert van Eijck Niek de Klerk Erik M.Kelder Marnix Wagemaker Department of Radiation Science and Technology Delft University of TechnologyMekelweg 152629JB Delftthe Netherlands Institute for Molecules and Materials Radboud University NijmegenHeyendaalseweg 1356525 AJ Nijmegenthe Netherlands

The high Li-ion conductivity of the Li7P3S11 sulfide-based solid electrolyte makes it a promising candidate for all-solid-state lithium batteries. The Li-ion transport over electrode-electrolyte and electrolyteelectrolyte interfaces, vital for the performance of solid-state batteries, is investigated by impedance spectroscopy and solid-state NMR experiments. An all-solid-state Li-ion battery is assembled with the Li7P3S11 electrolyte, nano-Li2S cathode and Li-In foil anode, showing a relatively large initial discharge capacity of 1139.5 m Ah/g at a current density of 0.064 m A/cm^ 2 retaining 850.0 m Ah/g after 30 cycles. Electrochemical impedance spectroscopy suggests that the decrease in capacity over cycling is due to the increased interfacial resistance between the electrode and the electrolyte. 1D exchange ^7Li NMR quantifies the interfacial Li-ion transport between the uncycled electrode and the electrolyte, resulting in a diffusion coefficient of 1.70(3) ×10^-14cm^2/s at 333 K and an energy barrier of 0.132 e V for the Li-ion transport between Li2S cathode and Li7P3S11 electrolyte. This indicates that the barrier for Li-ion transport over the electrode-electrolyte interface is small. However, the small diffusion coefficient for Li-ion diffusion between the Li2S and the Li7P3S11 suggests that these contact interfaces between electrode and electrolyte are relatively scarce, challenging the performance of these solid-state batteries.

关键词： Li7P3S11 Li-ion transport Spin-lattice NMR Exchange NMR Solid-state battery

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An integrated approach to the key parameters in methanol‐to‐olefins reaction catalyzed by MFI/MEL zeolite materials

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Chinese Journal of Catalysis 2022年第7期43卷 1879-1893页

作者： Chuncheng Liu Evgeny A.Uslamin Sophie H.van Vreeswijk Irina Yarulina swapna ganapathy Bert M.Weckhuysen Freek Kapteijn Evgeny A.Pidko Inorganic Systems Engineering Department of Chemical EngineeringDelft University of TechnologyVan der Maasweg 92629 HZ Delftthe Netherlands BASF SE Process Research and Chemical EngineeringLudwigshafen 67056Germany Inorganic Chemistry and Catalysis Debye Institute for Nanomaterials ScienceUtrecht UniversityUniversiteitsweg 993854 CG Utrechtthe Netherlands Catalysis Engineering Department of Chemical EngineeringDelft University of TechnologyVan der Maasweg 92629 HZ Delftthe Netherlands

Identification of the catalyst characteristics correlating with the key performance parameters including selectivity and stability is key to the rational catalyst design. Herein we focused on the identification of property-performance relationships in the methanol-to-olefin(MTO) process by studying in detail the catalytic behaviour of MFI, MEL and their respective intergrowth zeolites. The detailed material characterization reveals that both the high production of propylene and butylenes and the large Me OH conversion capacity correlate with the enrichment of lattice Al sites in the channels of the pentasil structure as identified by 27 Al MAS NMR and 3-methylpentane cracking results. The lack of correlation between MTO performance and other catalyst characteristics, such as crystal size, presence of external Brønsted acid sites and Al pairing suggests their less pronounced role in defining the propylene selectivity. Our analysis reveals that catalyst deactivation is rather complex and is strongly affected by the enrichment of lattice Al in the intersections, the overall Al-content, and crystal size. The intergrowth of MFI and MEL phases accelerates the catalyst deactivation rate.

关键词： Structure‐performance relationship Zeolite catalysis Methanol‐to‐olefin conversion Al‐distribution Acidity Intergrowth MFI/MEL Pentasil

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