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 electrolyteelectro...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.展开更多
A novel protocol for the synthesis of perylene diimides(PDIs),by reacting perylene dianhydride(PDA)with aliphatic amines is reported.Full conversions were obtained at temperatures between 20 and 60℃,using DBU as the ...A novel protocol for the synthesis of perylene diimides(PDIs),by reacting perylene dianhydride(PDA)with aliphatic amines is reported.Full conversions were obtained at temperatures between 20 and 60℃,using DBU as the base in DMF or DMSO.A“green”synthesis of PDIs,that runs at higher temperatures,was developed using K_(2)CO_(3) in DMSO.展开更多
The properties of nanoparticles are often different from those of larger grains of the same solid material because of their very large specific surface area. This enables many novel applications, but properties such a...The properties of nanoparticles are often different from those of larger grains of the same solid material because of their very large specific surface area. This enables many novel applications, but properties such as agglomeration can also hinder their potential use. By creating nanostructured particles one can take optimum benefit from the desired properties while minimizing the adverse effects. We aim at developing high-precision routes for scalable production of nanostructured particles. Two gas-phase synthesis routes are explored. The first one - covering nanoparticles with a continuous layer - is carried out using atomic layer deposition in a fluidized bed. Through fluidization, the full surface area of the nanoparticles becomes available. With this process, particles can be coated with an ultra-thin film of constant and well-tunable thickness. For the second route - attaching nanoparticles to larger particles - a novel approach using electrostatic forces is demonstrated. The micron-sized particles are charged with one polarity using tribocharging. Using electrospraying, a spray of charged nanoparticles with opposite polarity is generated. Their charge prevents agglomeration, while it enhances efficient deposition at the surface of the host particle. While the proposed processes offer good potential for scale-up, further work is needed to realize large-scale processes.展开更多
基金funding from the European Research Council under the European Union’s Seventh Framework Programme (FP/2007-2013)/ERC Grant Agreement no.[307161] of M.W.
文摘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.
基金This work was in part funded by The Netherlands Organization for Scientific Research(NWO)by the Materials for Sustainability project SPEAR under Grant No.739.017.012.
文摘A novel protocol for the synthesis of perylene diimides(PDIs),by reacting perylene dianhydride(PDA)with aliphatic amines is reported.Full conversions were obtained at temperatures between 20 and 60℃,using DBU as the base in DMF or DMSO.A“green”synthesis of PDIs,that runs at higher temperatures,was developed using K_(2)CO_(3) in DMSO.
文摘The properties of nanoparticles are often different from those of larger grains of the same solid material because of their very large specific surface area. This enables many novel applications, but properties such as agglomeration can also hinder their potential use. By creating nanostructured particles one can take optimum benefit from the desired properties while minimizing the adverse effects. We aim at developing high-precision routes for scalable production of nanostructured particles. Two gas-phase synthesis routes are explored. The first one - covering nanoparticles with a continuous layer - is carried out using atomic layer deposition in a fluidized bed. Through fluidization, the full surface area of the nanoparticles becomes available. With this process, particles can be coated with an ultra-thin film of constant and well-tunable thickness. For the second route - attaching nanoparticles to larger particles - a novel approach using electrostatic forces is demonstrated. The micron-sized particles are charged with one polarity using tribocharging. Using electrospraying, a spray of charged nanoparticles with opposite polarity is generated. Their charge prevents agglomeration, while it enhances efficient deposition at the surface of the host particle. While the proposed processes offer good potential for scale-up, further work is needed to realize large-scale processes.