The challenge of prebiotic chemistry is to
trace the syntheses of life’s key building blocks
from a handful of primordial substrates. Here we
report a forward-synthesis algorithm that
generates a full network of prebiotic chemical
reactions accessible from these substrates under
generally accepted conditions. This network
contains both reported and previously unidentified
routes to biotic targets, as well as plausible
syntheses of abiotic molecules. It also exhibits
three forms of nontrivial chemical emergence, as
the molecules within the network can act as
catalysts of downstream reaction types; form
functional chemical systems, including
self-regenerating cycles; and produce surfactants
relevant to primitive forms of biological
compartmentalization. To support these claims,
computer-predicted, prebiotic syntheses of several
biotic molecules as well as a multistep,
self-regenerative cycle of iminodiacetic acid were
validated by experiment.
Materials exhibiting excitation-wavelength-dependent photoluminescence, PL, are useful in a range of biomedical and optoelectronic applications. This paper describes a nanoparticulate material whose PL is tunable across the entire visible range and is achieved without adjusting particle size, any postsynthetic doping, or surface modification. A straightforward thermal decomposition of rhenium (VII) oxide precursor yields nanoparticles that comprise Re atoms at different oxidation states. Studies of time-resolved emission spectra and DFT calculations both indicate that tunable PL of such mixed-valence particles originates from the presence of multiple emissive states that become "active" at different excitation wavelengths. In addition, the nanoparticles exhibit photocatalytic activity that, under visible-light irradiation, is superior to that of TiO nanomaterials.
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