A mobile robotic chemist.

Technologies such as batteries, biomaterials and heterogeneous catalysts have functions that are defined by mixtures of molecular and mesoscale components. As yet, this multi-length-scale complexity cannot be fully captured by atomistic simulations, and the design of such materials from first principles is still rare1-5. Likewise, experimental complexity scales exponentially with the number of variables, restricting most searches to narrow areas of materials space. Robots can assist in experimental searches6-14 but their widespread adoption in materials research is challenging because of the diversity of sample types, operations, instruments and measurements required. Here we use a mobile robot to search for improved photocatalysts for hydrogen production from water15. The robot operated autonomously over eight days, performing 688 experiments within a ten-variable experimental space, driven by a batched Bayesian search algorithm16-18. This autonomous search identified photocatalyst mixtures that were six times more active than the initial formulations, selecting beneficial components and deselecting negative ones. Our strategy uses a dexterous19,20 free-roaming robot21-24, automating the researcher rather than the instruments. This modular approach could be deployed in conventional laboratories for a range of research problems beyond photocatalysis.

Development of Biphasic Formulations for Use in Electrowetting-Based Liquid Lenses with a High Refractive Index Difference.

Commercial electrowetting-based liquid lenses are optical devices containing two immiscible liquids as an optical medium. The first phase is a droplet of a high refractive index oil phase placed in a ring-shaped chassis. The second phase is electrically conductive and has a similar density over a wide temperature range. Droplet curvature and refractive index difference of two liquids determine the optical strength of the lens. Liquid lenses take advantage of the electrowetting effect, which induces a change of the interface's curvature by applying a voltage, thereby providing a variable focal that is useful in autofocus applications. The first generation of lens modules were highly reliable, but the optical strength and application scope was limited by a low refractive index difference between the oil and conductive phase. Described herein is an effort to increase the refractive index difference between both phases, while maintaining other critical application characteristics of the liquids, including a low freezing point, viscosity, phase miscibility, and turbidity after thermal shock. An important challenge was the requirement that both phases have to have matching densities and hence had to be optimized simultaneously. Using high throughput experimentation in conjunction with statistical design of experiments (DOE), we have developed a series of empirical models to predict multiple physicochemical properties of both phases and derived ideal locations within the formulation space. This approach enabled the development of reliable liquid lenses with a previously unavailable refractive index difference of Δ nD of ≥0.290, which enabled true optical zooming capability.

Characterization of surfactant complex mixtures using Raman spectroscopy and signal extraction methods: Application to laundry detergent deformulation.

This paper presents the analysis of surfactants in complex mixtures using Raman spectroscopy combined with signal extraction (SE) methods. Surfactants are the most important component in laundry detergents. Both their identification and quantification are required for quality control and regulation purposes. Several synthetic mixtures of four surfactants contained in an Ecolabel laundry detergent were prepared and analyzed by Raman spectroscopy. SE methods, Independent Component Analysis and Multivariate Curve Resolution, were then applied to spectral data for surfactant identification and quantification. The influence of several pre-processing treatments (normalization, baseline correction, scatter correction and smoothing) on SE performances were evaluated by experimental design. By using optimal pre-processing strategy, SE methods allowed satisfactorily both identifying and quantifying the four surfactants. When applied to the pre-processed Raman spectrum of the Ecolabel laundry detergent sample, SE models remained robust enough to predict the surfactant concentrations with sufficient precision for deformulation purpose. Comparatively, a supervised modeling technique (PLS regression) was very efficient to quantify the four surfactants in synthetic mixtures but appeared less effective than SE methods when applied to the Raman spectrum of the detergent sample. PLS seemed too sensitive to the other components contained in the laundry detergent while SE methods were more robust. The results obtained demonstrated the interest of SE methods in the context of deformulation.

A new species of the archaic primate Zanycteris from the late Paleocene of western Colorado and the phylogenetic position of the family Picrodontidae.

A new species of an archaic primate (Pleisadapiformes) is described based on a maxilla containing the first and second upper molars from the Fort Union Formation, Atwell Gulch Member in northwestern Colorado. The preserved teeth show the unusual dental characteristics of members of the rare and poorly documented Picrodontidae family, including an elongated centrocrista and wide occlusal surface. The new species is placed within the genus Zanycteris (represented by a single specimen from southern Colorado). This placement is based on similarities in regard to the parastyle, curvilinear centrocrista, and wider anterior stylar shelf on the upper molars. However, the new species differs from the only known species of Zanycteris in exhibiting an upper first molar that is 30% larger in area, while retaining a similarly sized upper second molar. Phylogenetic analysis supports the separation of the Picrodontidae family from the Paromomyidae, while still recognizing picrodontids position within Pleisadapiformes. The unusual dental features of the upper molars likely functioned in life as an enhanced shearing surface between the centrocrista and cristid obliqua crests for a specialized diet of fruit. A similar arrangement is found in the living bat Ariteus (Jamaican fig-eating bat), which feeds on fleshy fruit. The new species showcases the rapid diversification of archaic primates shortly after the extinction of the dinosaurs during the Paleocene, and the unusual dental anatomy of picrodontids to exploit new dietary specializations.

Rearrangement of beta-amino alcohols and application to the synthesis of biologically active compounds.

Beta-amino alcohols derived from natural amino acids have been used extensively as a powerful source of chirality. Transformation of the hydroxy group of these beta-amino alcohols into a good leaving group, by using trifluoroacetic anhydride, led to rearranged beta-amino alcohols in good yields and with high enantiomeric excesses. This rearrangement has allowed the transformation of substituted prolinols to substituted 3-hydroxypiperidines and linear beta-amino alcohols, issued from natural amino acids, to rearranged beta-amino alcohols.