Capture and storage of the long-lived ⁸⁵Kr is an efficient approach to mitigate the emission of volatile radionuclides from the spent nuclear fuel reprocessing facilities. However, it is challenging to separate krypton (Kr) from xenon (Xe) because of the chemical inertness and similar physical properties. Herein we prepared high-silica CHA zeolite membranes with ultra-high selectivity and irradiation stability for Kr/Xe separation. The suitable aperture size and rigid framework endures the membrane a strong size-exclusion effect. The ultrahigh selectivity of 51–152 together with the Kr permeance of 0.7–1.3×10⁻⁸ mol m⁻² s⁻¹ Pa⁻¹ of high-silica CHA zeolite membranes far surpass the state-of-the-art polymeric membranes. The membrane is among the most stable polycrystalline membranes for separation of humid Kr/Xe mixtures. Together with the excellent irradiation stability, high-silica CHA zeolite membranes pave the way to separate radioactive Kr from Xe for a notable reduction of the volatile nuclear waste storage volume.

A sound knowledge of fundamental mechanical properties of water ice is of crucial importance to address a wide range of applications in earth science, engineering, as well as ice sculpture and winter sports, such as ice skating, ice fishing, ice climbing, bobsleighs, and so on. Here, we report large-scale molecular dynamics (MD) simulations of mechanical properties of bi- and poly-crystalline hexagonal ice (I_h) under mechanical loads. Results show that bicrystals, upon tension, exhibit either brittle or ductile fracture, depending on the microstructure of grain boundaries (GBs), whereas they show ductile fracture by amorphization and crystallographic slips emitted from GBs under compression. Under shearing, the strength of bicrystals exhibits a characteristic plateau or sawtooth behavior drawn out the initial elastic strains. Nanograined polycrystals are destabilized by strain-induced amorphization and collective GB sliding. Their mechanical responses depend on the grain size. Both tensile and compressive strengths decrease as grain size decreases, showing inverse Hall-Petch weakening behavior. Large fraction of amorphous water structure in polycrystals with small grain size is mainly responsible for the inverse Hall-Petch softening. Dislocation nucleation and propagation are also identified in nanograined ice, which is in good agreement with experimental measurements. Beyond the elastic strain, a combination of GB sliding, grain rotation, amorphization and recrystallization, phase transformation, and dislocation nucleation dominate the plastic deformation in both bicrystals and polycrystals.

A sound knowledge of thermodynamic properties of sII hydrates is of great importance to understand the stability of sII gas hydrates in petroleum pipelines and in natural settings. Here, we report direct molecular dynamics (MD) simulations of the thermal expansion coefficient, the compressibility, and the specific heat capacity of C₃H₈, or tetrahydrofuran (THF), in mixtures of CH₄ or CO₂, in sII hydrates under a wide, relevant range of pressure and temperature conditions. The simulations were started with guest molecules positioned at the cage center of the hydrate. Annealing simulations were additionally performed for hydrates with THF. For the isobaric thermal expansion coefficient, an effective correction method was used to modify the lattice parameters, and the corrected lattice parameters were subsequently used to obtain thermal expansion coefficients in good agreement with experimental measurements. The simulations indicated that the isothermal expansion coefficient and the specific heat capacity of C₃H₈-pure hydrates were comparable but slightly larger than those of THF-pure hydrates, which could form Bjerrum defects. The considerable variation in the compressibility between the two appeared to be due to crystallographic defects. However, when a second guest molecule occupied the small cages of the THF hydrate, the deviation was smaller, because the subtle guest-guest interactions can offset an unfavorable configuration of unstable THF hydrates, caused by local defects in free energy. Unlike the methane molecule, the carbon dioxide molecule, when filling the small cage, can increase the expansion coefficient and compressibility as well as decrease the heat capacity of the binary hydrate, similar to the case of sI hydrates. The calculated bulk modulus for C₃H₈-pure and binary hydrates with CH₄ or CO₂ molecule varied between 8.7 and 10.6 GPa at 287.15K between 10 and 100 MPa. The results for the specific heat capacities varied from 3155 to 3750.0 J kg^-1 K^-1 for C₃H₈-pure and binary hydrates with CH₄ or CO₂ at 287.15K. These results are the first of this kind reported so far. The simulations show that the thermodynamic properties of hydrates largely depend on the enclathrated compounds. This provides a much-needed atomistic characterization of the sII hydrate properties and gives an essential input for large-scale discoveries of hydrates and processing as a potential energy source.