Structure-Selection Dynamics of Cobalt Nanoparticles from Solution Synthesis and Their Impact on the Oxygen Evolution Reaction.

Resolving the three-dimensional structure of transition metal oxide nanoparticles (TMO-NPs), upon self-restructuring from solution, is crucial for tuning their structure-functionality. Yet, this remains challenging as this process entails complex structure fluctuations, which are difficult to track experimentally and, hence, hinder the knowledge-driven optimization of TMO-NPs. Herein, we combine high-energy synchrotron X-ray absorption and X-ray total scattering experiments with atomistic multiscale simulations to investigate the self-restructuring of self-assembled Co-NPs from solution under dark or photocatalytic water oxidation conditions at distinct reaction times and atomic length-scales.

Ultrafast Sintering of Dense LiLaZrO Membranes for Li Metal All-Solid-State Batteries.

Ultrafast sintering (UFS) is a compelling approach for fabricating LiLaZrO (LLZO) solid-state electrolytes (SSEs), paving the way for advancing and commercializing Li-garnet solid-state batteries. Although this method is commonly applied to the sintering of LLZO ceramics, its use for producing dense, phase-pure LLZO SSEs has thus far been primarily limited to millimeter-thick pellets, which are unsuitable for commercial solid-state batteries. This study presents ultrafast sintering as a highly effective approach for fabricating self-standing, dense, 45 µm-thick LLZO membranes.

Dimethyl carbonate synthesis from CO and methanol over CeO: elucidating the surface intermediates and oxygen vacancy-assisted reaction mechanism.

Surface intermediate species and oxygen vacancy-assisted mechanism over CeO catalyst in the direct dimethyl carbonate (DMC) synthesis from carbon dioxide and methanol are suggested by means of transient spectroscopic methodologies in conjunction with multivariate spectral analysis. How the two reactants, CO and methanol, interact with the CeO surface and how they form decisive surface intermediates leading to DMC are unraveled by DFT-based molecular dynamics simulation by precise statistical sampling of various configurations of surface states and intermediates. The atomistic simulations and uncovered stability of different intermediate states perfectly explain the unique DMC formation profile experimentally observed upon transient operations, strongly supporting the proposed oxygen vacancy-assisted reaction mechanism.