Deaminative chlorination of aminoheterocycles

Selective modification of heteroatom-containing aromatic structures is in high demand as it permits rapid evaluation of molecular complexity in advanced intermediates. Inspired by the selectivity of deaminases in nature, herein we present a simple methodology that enables the NH2 groups in aminoheterocycles to be conceived as masked modification handles. With the aid of a simple pyrylium reagent and a cheap chloride source, C(sp2)‒NH2 can be converted into C(sp2)‒Cl bonds. The method is characterized by its wide functional group tolerance and substrate scope, allowing the modification of >20 different classes of heteroaromatic motifs (five- and six-membered heterocycles), bearing numerous sensitive motifs. The facile conversion of NH2 into Cl in a late-stage fashion enables practitioners to apply Sandmeyer- and Vilsmeier-type transforms without the burden of explosive and unsafe diazonium salts, stoichiometric transition metals or highly oxidizing and unselective chlorinating agents.

Controlled Oxygenation of Multiple Contiguous C–H Bonds via Electrophotocatalysis

Chemical reactions that directly convert carbon-hydrogen (C–H) bonds to carbon-oxygen (C–O) bonds provide a powerful means to rapidly synthesize valuable organic compounds. However, achieving multiple C–H bond oxygenation reactions at the same time is challenging, particularly because of the risk of overoxidation. Here, we report the selective oxygenation of two or three contiguous C–H bonds, enabling the conversion of simple alkylarenes to diols, triols, or their corresponding acetates. The reactions are achieved using electrophotocatalysis—a process that utilizes both light and electricity to activate a single catalyst—to promote the oxidation reactions. The rapid increase in molecular complexity achieved by these multiple oxygenations enables the synthesis of some compounds of pharmaceutical interest by dramatically shorter sequences than previously achieved.

The Detection of a Hot Molecular Core in the Extreme Outer Galaxy

Interstellar chemistry in low-metallicity environments is crucial to understand chemical processes in the past metal-poor universe. Recent studies of interstellar molecules in nearby low-metallicity galaxies have suggested that metallicity has a significant effect on the chemistry of star-forming cores. Here we report the first detection of a hot molecular core in the extreme outer Galaxy, which is an excellent laboratory to study star formation and the interstellar medium in a Galactic low-metallicity environment. The target star-forming region, WB 89–789, is located at a galactocentric distance of 19 kpc. Our Atacama Large Millimeter/submillimeter Array observations in 241–246, 256–261, 337–341, and 349–353 GHz have detected a variety of carbon-, oxygen-, nitrogen-, sulfur-, and silicon-bearing species, including complex organic molecules (COMs) containing up to nine atoms, toward a warm (>100 K) and compact (<0.03 pc) region associated with a protostar (∼8 × 103 L ☉). Deuterated species such as HDO, HDCO, D2CO, and CH2DOH are also detected. A comparison of fractional abundances of COMs relative to CH3OH between the outer Galactic hot core and an inner Galactic counterpart shows a remarkable similarity. On the other hand, the molecular abundances in the present source do not resemble those of low-metallicity hot cores in the Large Magellanic Cloud. The results suggest that great molecular complexity exists even in the primordial environment of the extreme outer Galaxy. The detection of another embedded protostar associated with high-velocity SiO outflows is also reported.

Application of Nanomaterials to Ensure Quality and Nutritional Safety of Food

Nanomaterials (NMs) are emerging novel tools for preserving quality, enhancing shelf life, and ensuring food safety. Owing to the distinctive physicochemical characters, engineered NMs under varying sizes and dimensions have great potentials for application in the manufacturing, packaging, processing, and safety of quality agrifood. The promise of various kinds of novel NMs that are useful for food industries has opened a possibility of a new revolution in agroprocessing industries in both the emerging and advanced nations. The rapid advancement of nanoscience has provided a great impact on material science that has allowed researchers to understand every aspect of molecular complexity and its functions in life sciences. The reduced size of NMs that increase the surface area is useful in the specific target of different organs, and biodegradable nanospheres are helpful in the transport of bioactive molecules across the cellular barriers. However, nanotechnology creates a great revolution in several sections including agriculture and food industry and also reduces environmental pollution, while the toxicity of some NMs in the food industry poses a great concern to researchers for their greater application. However, most of the developed countries have regulatory control acts but developing countries do not have them yet. Therefore, for the safe use of NMs and also to minimize the health and environmental risks in both the developed and developing countries, it is indispensable to recognize the toxicity-constructed, toxicodynamic, and toxicokinetic features of NMs, which should carefully be emphasized at the home and industrial levels. The current study highlights the updates of the NMs to safeguard the quality and nutritional safety of foods at home and also at the industrial level.

Adaptive ratchets and the evolution of molecular complexity

Biological systems have evolved to amazingly complex states, yet we do not understand in general how evolution operates to generate increasing genetic and functional complexity. Molecular recognition sites are short genome segments or peptides binding a cognate recognition target of sufficient sequence similarity. Such sites are simple, ubiquitous modules of sequence information, cellular function, and evolution. Here we show that recognition sites, if coupled to a time-dependent target, can rapidly evolve to complex states with larger code length and smaller coding density than sites recognising a static target. The underlying fitness model contains selection for recognition, which depends on the sequence similarity between site and target, and a uniform cost per unit of code length. Site sequences are shown to evolve in a specific adaptive ratchet, which produces selection of different strength for code extensions and compressions. Ratchet evolution increases the adaptive width of evolved sites, accelerating the adaptation to moving targets and facilitating refinement and innovation of recognition functions. We apply these results to the recognition of fast-evolving antigens by the human immune system. Our analysis shows how molecular complexity can evolve as a collateral to selection for function in a dynamic environment.