Gas-sieving zeolitic membranes fabricated by condensation of precursor nanosheets.

The synthesis of molecular-sieving zeolitic membranes by the assembly of building blocks, avoiding the hydrothermal treatment, is highly desired to improve reproducibility and scalability. Here we report exfoliation of the sodalite precursor RUB-15 into crystalline 0.8-nm-thick nanosheets, that host hydrogen-sieving six-membered rings (6-MRs) of SiO4 tetrahedra. Thin films, fabricated by the filtration of a suspension of exfoliated nanosheets, possess two transport pathways: 6-MR apertures and intersheet gaps. The latter were found to dominate the gas transport and yielded a molecular cutoff of 3.6 Å with a H2/N2 selectivity above 20. The gaps were successfully removed by the condensation of the terminal silanol groups of RUB-15 to yield H2/CO2 selectivities up to 100. The high selectivity was exclusively from the transport across 6-MR, which was confirmed by a good agreement between the experimentally determined apparent activation energy of H2 and that computed by ab initio calculations. The scalable fabrication and the attractive sieving performance at 250-300 °C make these membranes promising for precombustion carbon capture.

Ultra-high throughput manufacturing method for composite solid-state electrolytes.

The transition from liquid organic electrolytes to solid-state electrolytes promises safer and more energy-dense lithium ion batteries. Although this technology has been demonstrated, the question of how to manufacture solid-state batteries at the cost and scales needed to be competitive remains. Here we propose and demonstrate curtain coating as a method for manufacturing composite solid-state electrolytes in roll-to-roll processes at web-speeds of over 80 m/min. The method is compatible with existing lithium-ion battery electrode manufacturing lines and is able to produce uniform electrolyte films with thicknesses below 15 micrometers.

Colloidal Phase-Change Materials: Synthesis of Monodisperse GeTe Nanoparticles and Quantification of Their Size-Dependent Crystallization.

Phase-change memory materials refer to a class of materials that can exist in amorphous and crystalline phases with distinctly different electrical or optical properties, as well as exhibit outstanding crystallization kinetics and optimal phase transition temperatures. This paper focuses on the potential of colloids as phase-change memory materials. We report a novel synthesis for amorphous GeTe nanoparticles based on an amide-promoted approach that enables accurate size control of GeTe nanoparticles between 4 and 9 nm, narrow size distributions down to 9-10%, and synthesis upscaling to reach multigram chemical yields per batch. We then quantify the crystallization phase transition for GeTe nanoparticles, employing high-temperature X-ray diffraction, differential scanning calorimetry, and transmission electron microscopy. We show that GeTe nanoparticles crystallize at higher temperatures than the bulk GeTe material and that crystallization temperature increases with decreasing size. We can explain this size-dependence using the entropy of crystallization model and classical nucleation theory. The size-dependences quantified here highlight possible benefits of nanoparticles for phase-change memory applications.

Quantification and modeling of mechanical degradation in lithium-ion batteries based on nanoscale imaging.

Capacity fade in lithium-ion battery electrodes can result from a degradation mechanism in which the carbon black-binder network detaches from the active material. Here we present two approaches to visualize and quantify this detachment and use the experimental results to develop and validate a model that considers how the active particle size, the viscoelastic parameters of the composite electrode, the adhesion between the active particle and the carbon black-binder domain, and the solid electrolyte interphase growth rate impact detachment and capacity fade. Using carbon-silicon composite electrodes as a model system, we demonstrate X-ray nano-tomography and backscatter scanning electron microscopy with sufficient resolution and contrast to segment the pore space, active particles, and carbon black-binder domain and quantify delamination as a function of cycle number. The validated model is further used to discuss how detachment and capacity fade in high-capacity materials can be minimized through materials engineering.