Rational design of a (S)-selective-transaminase for asymmetric synthesis of (1S)-1-(1,1′-biphenyl-2-yl)ethanamine

Amine transaminases offer an environmentally sustainable synthesis route for the production of pure chiral amines. However, their catalytic efficiency toward bulky ketone substrates is greatly limited by steric hindrance and therefore presents a great challenge for industrial synthetic applications. We hereby report an example of rational transaminase enzyme design to help alleviate these challenges. Starting from the Vibrio fluvialis amine transaminase that has no detectable catalytic activity toward the bulky aromatic ketone 2-acetylbiphenyl, we employed a rational design strategy combining in silico and in vitro studies to engineer the transaminase enzyme with a minimal number of mutations, achieving an high catalytic activity and high enantioselectivity. We found that, by introducing two mutations W57G/R415A, detectable enzyme activity was achieved. The rationally designed variant, W57F/R88H/V153S/K163F/I259M/R415A/V422A, showed an improvement in reaction rate by more than 1716-fold toward the bulky ketone under study, producing the corresponding enantiomeric pure (S)-amine (enantiomeric excess (ee) value of >99%)

The signature of competition in ecomorphological traits across the avian radiation

Competition for shared resources represents a fundamental driver of biological diversity. However, the tempo and mode of phenotypic evolution in deep-time has been predominantly investigated using trait evolutionary models which assume that lineages evolve independently from each other. Consequently, the role of species interactions in driving macroevolutionary dynamics remains poorly understood. Here, we quantify the prevalence for signatures of competition between related species in the evolution of ecomorphological traits across the bird radiation. We find that mechanistic trait models accounting for the effect of species interactions on phenotypic divergence provide the best fit for the data on at least one trait axis in 27 out of 59 clades ranging between 21 and 195 species. Where it occurs, the signature of competition generally coincides with positive species diversity-dependence, driven by the accumulation of lineages with similar ecologies, and we find scarce evidence for trait-dependent or negative diversity-dependent phenotypic evolution. Overall, our results suggest that the footprint of interspecific competition is often eroded in long-term patterns of phenotypic diversification, and that other selection pressures may predominantly shape ecomorphological diversity among extant species at macroevolutionary scales

The signature of competition in ecomorphological traits across the avian radiation

Competition for shared resources represents a fundamental driver of biological diversity. However, the tempo and mode of phenotypic evolution in deep-time has been predominantly investigated using trait evolutionary models which assume that lineages evolve independently from each other. Consequently, the role of species interactions in driving macroevolutionary dynamics remains poorly understood. Here, we quantify the prevalence for signatures of competition between related species in the evolution of ecomorphological traits across the bird radiation. We find that mechanistic trait models accounting for the effect of species interactions on phenotypic divergence provide the best fit for the data on at least one trait axis in 27 out of 59 clades ranging between 21 and 195 species. Where it occurs, the signature of competition generally coincides with positive species diversity-dependence, driven by the accumulation of lineages with similar ecologies, and we find scarce evidence for trait-dependent or negative diversity-dependent phenotypic evolution. Overall, our results suggest that the footprint of interspecific competition is often eroded in long-term patterns of phenotypic diversification, and that other selection pressures may predominantly shape ecomorphological diversity among extant species at macroevolutionary scales

Isolation and Characterisation of a Halotolerant ω-Transaminase from a Triassic Period Salt Mine and Its Application to Biocatalysis

Abstract Chiral amines are valuable intermediates for the pharmaceutical industry, with up to 40% of current pharmaceuticals containing an amine functionality. However, their syntheses by conventional chemical methods often suffer from a number of key drawbacks. Transaminases (TAms) are pyridoxal phosphate (PLP) dependent enzymes capable of transferring an amine group to a prochiral ketone, offering a green and economically viable alternative to chiral amine production. Despite some high profile successes, TAms suffer from limited substrate scope and the ability to function under challenging conditions often required in reaction processes. Mining of untapped, extremophilic environments represents a viable approach in the search for novel enzymes. We report the cloning and expression of an (S)-selective ?-TAm from a Halomonas sp. (Ad2-TAm), isolated from an extreme hypersaline environment formed during the Triassic period (circa 220 mya). Ad2-TAm exhibits an ability to convert a range of structurally diverse aldehyde and ketone substrates, with no decrease in conversion up to 1.5?M (8.8%) NaCl. The enzyme is also tolerant to the presence of organic cosolvents up to 30% and accepts a range of amino donors. These characteristics make Ad2-TAm a promising candidate for industrial applications, whilst also highlighting the value of extreme environments as a source of novel enzymes for the pharmaceutical industry as a whole

Relations between soil hydraulic properties and burn severity

Wildfire can affect soil hydraulic properties, often resulting in reduced infiltration. The magnitude of change in infiltration varies depending on the burn severity. Quantitative approaches to link burn severity with changes in infiltration are lacking. This study uses controlled laboratory measurements to determine relations between a remotely sensed burn severity metric (dNBR, change in normalised burn ratio) and soil hydraulic properties (SHPs). SHPs were measured on soil cores collected from an area burned by the 2013 Black Forest fire in Colorado, USA. Six sites with the same soil type were selected across a range of burn severities, and 10 random soil cores were collected from each site within a 30-m diameter circle. Cumulative infiltration measurements were made in the laboratory using a tension infiltrometer to determine field-saturated hydraulic conductivity, Kfs, and sorptivity, S. These measurements were correlated with dNBR for values ranging from 124 (low severity) to 886 (high severity). SHPs were related to dNBR by inverse functions for specific conditions of water repellency (at the time of sampling) and soil texture. Both functions had a threshold value for dNBR between 124 and 420, where Kfs and S were unchanged and equal to values for soil unaffected by fire. For dNBRs >~420, the Kfs was an exponentially decreasing function of dNBR and S was a linearly decreasing function of dNBR. These initial quantitative empirical relations provide a first step to link SHPs to burn severity, and can be used in quantitative infiltration models to predict post-wildfire infiltration and resulting runoff