Enabling Logistics Automation in Nanofactory: Cobalt Phosphide Embedded Metal-Organic Frameworks for Efficient Electrocatalytic Nitrate Reduction to Ammonia.

Electrocatalytic nitrate reduction reaction (NitRR) in neutral condition offers a promising strategy for green ammonia synthesis and wastewater treatment, the rational design of electrocatalysts is the cornerstone. Inspired by modern factory design where both machines and logistics matter for manufacturing, it is reported that cobalt phosphide (CoP) nanoparticles embedded in zinc-based zeolite imidazole frameworks (Zn-ZIF) function as a nanofactory with high performance. By selective phosphorization of ZnCo bimetallic zeolite imidazole framework (ZnCo-ZIF), the generated CoP nanoparticles act as "machines" (active sites) for molecular manufacturing (NO to NH conversion).

Group-VIII transition metal boride as promising hydrogen evolution reaction catalysts.

Searching for alternative catalysts for hydrogen evolution reaction (HER) under acidic conditions has been a major challenge in chemistry. Herein, we demonstrate that it is now feasible to identify unprecedented transition metal boride phases that are both stable and active for HER via stochastic global potential energy surface scanning. We show that B alloying alters the most stable crystal phase from face-centered (fcc) to hexagonal close packing (hcp) for both Pd and Rh.

Engineering Carbon Nanotube Fiber for Real-Time Quantification of Ascorbic Acid Levels in a Live Rat Model of Alzheimer's Disease.

Ascorbic acid (AA) levels are closely correlated with physiological and pathological events in brain diseases, but the mechanism remains unclear, mainly due to the difficulty of accurately analyzing AA levels in live brain. In this study, by engineering tunable defects and oxygen-containing species in carbon nanotubes, a novel aligned carbon nanotube fiber was developed as an accurate microsensor for the ratiometric detection of AA levels in live rat brains with Alzheimer's disease (AD). AA oxidation is greatly facilitated on the fiber surface at a low potential, leading to high sensitivity as well as high selectivity against potential sources of interference in the brain.

Subnano Pt Particles from a First-Principles Stochastic Surface Walking Global Search.

Subnano transition metal particles have wide applications in chemistry. For the complexity of their potential energy surface, it has long been a great challenge for both theory and experiment to determine the structure of subnano clusters and thus predict their physiochemical properties. Here we explore the structure configurations for 35 subnano PtN (N = 12-46) clusters using a first-principles Stochastic Surface Walking (SSW) global search.

Restructuring and Hydrogen Evolution on Pt Nanoparticle.

The restructuring of nanoparticles at the condition is a common but complex phenomenon in nanoscience. Here, we present the first systematic survey on the structure dynamics and its catalytic consequence for hydrogen evolution reaction (HER) on Pt nanoparticles, as represented by a magic number Pt octahedron (∼1 nm size). Using a first principles calculation based global structure search method, we stepwise follow the significant nanoparticle restructuring under HER conditions as driven by thermodynamics to expose {100} facets, and reveal the consequent large activity enhancement due to the marked increase of the concentration of the active site, being identified to be apex atoms.

Confined platinum nanoparticle in carbon nanotube: structure and oxidation.

A supported nanoparticle is dynamic in reaction conditions, but how this dynamic behavior is influenced by the support remains elusive. Using the stochastic surface walking global optimization method, herein, we report the structure, thermodynamics and catalytic properties of Pt nanoparticles inside and outside a carbon nanotube (CNT). We reveal that confined metal nanoparticles are, surprisingly, structurally more flexible at low temperatures but less likely to melt at high temperatures.

Quasi-planar aromatic B36 and B36(-) clusters: all-boron analogues of coronene.

Flat boron has recently emerged as a fascinating concept in cluster science. Here we present computational evidence for the quasi-planar all-boron aromatic B36 (C6v, (1)A1) and B36(-) (C2v, (2)A1) clusters, established as the global-minimum structures on the basis of Stochastic Surface Walking (SSW) searches. The energetics for low-lying isomeric structures are evaluated using the validated density-functional method at the PBE0/6-311+G* level.

Observation of an all-boron fullerene.

After the discovery of fullerene-C60, it took almost two decades for the possibility of boron-based fullerene structures to be considered. So far, there has been no experimental evidence for these nanostructures, in spite of the progress made in theoretical investigations of their structure and bonding. Here we report the observation, by photoelectron spectroscopy, of an all-boron fullerene-like cage cluster at B40(-) with an extremely low electron-binding energy.

Optimum nanoparticles for electrocatalytic oxygen reduction: the size, shape and new design.

The electrocatalytic oxygen reduction reaction (ORR) on nanoparticles has attracted much attention in recent years for its significance in fuel cell applications. Here by combining density functional theory (DFT) calculations with the periodic continuum solvation model based on modified-Poisson-Boltzmann (CM-MPB) electrostatics, we analyzed the ORR activity on a set of differently sized Pt nanoparticles in order to identify the optimum particles for a better designed catalyst. We show that Pt nanoparticles of ∼2 nm size have the highest ORR mass activity, which is attributed to the variation of the effective reaction sites on the exposed {111} facet at the electrochemical conditions.

Periodic mesoporous organosilicas with controlled pore symmetries for peptides enrichment.

Periodic mesoporous organosilicas (PMOs) with controlled structures have been synthesized by using cetyltrimethylammonium bromide (CTAB) and sodium perfluorooctanoate (PFONa) as co-templates, 1,2-bis (triethoxysilyl)ethane (BTEE) as an organosilica precursor. By increasing the weight ratio of PFONa/CTAB, a structure transformation from a cubic (Pm-3n) to a two-dimensional hexagonal (p6m) mesostructure and then to multilamellar vesicles can be observed. The cubic and hexagonal samples have similar particle size (200-750 nm), pore size (2.