Molecular Engineering to Tune the Ligand Environment of Atomically Dispersed Nickel for Efficient Alcohol Electrochemical Oxidation

Atomically dispersed metals maximize the number of catalytic sites and enhance their activity. However, their challenging synthesis and characterization strongly complicates their optimization. Here, the aim is to demonstrate that tuning the electronic environment of atomically dispersed metal catalysts through the modification of their edge coordination is an effective strategy to maximize their performance. This article focuses on optimizing nickel-based electrocatalysts toward alcohol electrooxidation in alkaline solution. A new organic framework with atomically dispersed nickel is first developed. The coordination environment of nickel within this framework is modified through the addition of carbonyl (CO) groups. The authors then demonstrate that such nickel-based organic frameworks, combined with carbon nanotubes, exhibit outstanding catalytic activity and durability toward the oxidation of methanol (CH₃OH), ethanol (CH₃CH₂OH), and benzyl alcohol (C₆H₅CH₂OH); the smaller molecule exhibits higher catalytic performance. These outstanding electrocatalytic activities for alcohol electrooxidation are attributed to the presence of the carbonyl group in the ligand chemical environment, which enhances the adsorption for alcohol, as revealed by density functional theory calculations. The work not only introduces a new atomically dispersed Ni-based catalyst, but also demonstrates a new strategy for designing and engineering high-performance catalysts through the tuning of their chemical environment.     

Designing a benchmark for the performance evaluation of agent-based simulation applications on HPC

The Journal of Supercomputing - Agent-based modeling and simulation (ABMS) is a class of computational models for simulating the actions and interactions of autonomous agents with the goal of...     

Enacting archetypes in movies: grounding the unconscious mind in emotion-driven media

Abstract

The concept of emotion-driven media integrates affective computing into developing new types of digital media by including the human spectator as an essential part of the whole system. Enactive media, as a landmark in this direction, provides a theoretical basis that is rooted in the enactivist approach in cognitive science. Based on this thesis, it is required to establish a practical procedure for developing the media content through integrating psychological approaches. We demonstrate a systematic approach for developing the content for emotion-driven media. The theory of archetypes, one of the psychoanalytical approaches, was applied for editing movie clips as the media content, and coupled the content with emotional responses by using experimental psychological methodologies. The results showed that it is promising to utilise archetypal movie clips as the content of emotion-driven media and archetypal symbolism can be a useful resource for developing the content of media systems.     

Functional mimicry of a discontinuous antigenic site by a designed synthetic peptide

Functional reproduction of the discontinuous antigenic site D of foot-and-mouth disease virus (FMDV) has been achieved by means of synthetic peptide constructions that integrate each of the three protein loops that define the antigenic site into a single molecule. The site D mimics were designed on the basis of the X-ray structure of FMDV type C-S8c1 with the aid of molecular dynamics, so that the five residues assumed to be involved in antigenic recognition are located on the same face of the molecule, exposed to solvent and defining a set of native-like distances and angles. The designed site D mimics are disulfide-linked heterodimers that consist of a larger unit containing VP2(71-84), followed by a polyproline module and by VP3(52-62), and a smaller unit corresponding to VP1(188-194) (VP=viral protein). Guinea pig antisera to the peptides recognized the viral particle and competed with site D-specific monoclonal antibodies, while inoculation with a simple (not covalently joined to one another) admixture of the three VP1-VP3 sequences yielded no detectable virus-specific serum conversion. Similar results have been reproduced in two bovines. Antisera to the peptides also moderately neutralize FMDV in cell cultures and partially protect guinea pigs against challenge with the virus. These results demonstrate functional mimicry of the discontinuous site D by the peptides, which are therefore obvious candidates for a multicomponent, peptide-based vaccine against FMDV.     

New insights into the heating mechanisms and self-regulating abilities of manganite perovskite nanoparticles suitable for magnetic fluid hyperthermia

The heating and self-regulating abilities of La(1-x)Sr(x)MnO(3+Δ) ferromagnetic nanoparticles for magnetic fluid hyperthermia are studied. The samples, synthesized by the Glycine Nitrate Process, present non-agglomerated particles but are partially constituted by polycrystalline nanoparticles, displaying average crystallite diameters ranging from 21 to 31 nm. The strontium content of these nanoparticles, between 0.14 and 0.39, is associated with non-stoichiometry effects in the materials, and both govern their Curie temperatures (T(C)), which range between 13 and 86 °C, respectively. Heating experiments carried out on samples suspended in an aqueous agarose gel and with different alternating magnetic fields derive unexpected maximum temperatures that cannot be explained on the basis of static magnetization data. The measurement of the thermal dependence of the specific absorption rate (SAR) of nanopowders by adiabatic magnetothermia reveals the existence of a dissipation peak just below T(C), which is assigned to a Hopkinson peak. This thermal dependence of SAR, together with a simple thermal model that considers a linear approximation for the heat power losses, is crucial to clarify the behavior observed in heating experiments and also to discuss the possibilities of the samples as self-regulating hyperthermia mediators. This analysis emphasizes that, for the correct design of a self-regulating system, the heat power losses determined by the surrounding conditions must be taken into account as well as the heating capacity of the magnetic nanoparticles.     

In Vitro and In Vivo Interrogation of Bio-sprayed Cells

Bio-sprays can directly form pre-organized cell-bearing structures for applications ranging from engineering functional tissues to the forming of cultures, most useful for modeling disease, to the discovery and development of drugs. Bio-electrosprays and aerodynamically assisted bio-jets, are leading approaches that have been demonstrated as having far-reaching ramifications for regenerative biology and medicine.