Chemical conversion based on crystal facet effect of transition metal oxide and construction methods for sharp-faced nanocrystals

The in-depth researches have found that the nanocrystal facet of transition metal oxide (TMO) greatly affects its heterogeneous catalytic performance, as well as the property of photocatalysis, gas sensing, electrochemical...

On the Role of Solvent in the Formation of Vacancies on Ibuprofen Crystal Facets

Surface defects play a crucial role in the process of crystal growth, as the incorporation of growth units generally takes place on under-coordinated sites on the growing crystal facet. In this work, we use molecular dynamics simulations to obtain information on the role of the solvent in the roughening of three morphologically-relevant crystal faces of form I of racemic ibuprofen. To this aim, we devise a computational strategy based on combining independent Well Tempered Metadynamics with Mean Force Integration. This approach enables us to evaluate the energetic cost associated with the formation of a surface vacancy for a set of ten solvents, covering a range of polarities and hydrogen-bonding ability. We find that both the mechanism of defect formation on these facets and the work associated with the process are indeed markedly solvent-dependent. The methodology developed in this work has been designed with the aim of capturing solvent effects at the atomistic scale while maintaining the computational efficiency necessary for implementation in high-throughput computational screenings of crystallization solvents.

High-Index Faceted Nanocrystals as Highly Efficient Bifunctional Electrocatalysts for High-Performance Lithium–Sulfur Batteries

Precisely regulating of the surface structure of crystalline materials to improve their catalytic activity for lithium polysulfides is urgently needed for high-performance lithium–sulfur (Li–S) batteries. Herein, high-index faceted iron oxide (Fe2O3) nanocrystals anchored on reduced graphene oxide are developed as highly efficient bifunctional electrocatalysts, effectively improving the electrochemical performance of Li–S batteries. The theoretical and experimental results all indicate that high-index Fe2O3 crystal facets with abundant unsaturated coordinated Fe sites not only have strong adsorption capacity to anchor polysulfides but also have high catalytic activity to facilitate the redox transformation of polysulfides and reduce the decomposition energy barrier of Li2S. The Li–S batteries with these bifunctional electrocatalysts exhibit high initial capacity of 1521 mAh g−1 at 0.1 C and excellent cycling performance with a low capacity fading of 0.025% per cycle during 1600 cycles at 2 C. Even with a high sulfur loading of 9.41 mg cm−2, a remarkable areal capacity of 7.61 mAh cm−2 was maintained after 85 cycles. This work provides a new strategy to improve the catalytic activity of nanocrystals through the crystal facet engineering, deepening the comprehending of facet-dependent activity of catalysts in Li–S chemistry, affording a novel perspective for the design of advanced sulfur electrodes.