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Recent synthetic efforts aimed at reconstructing the beginning of life on our planet point at the plausibility of scenarios fueled by extraterrestrial energy sources. In the current work we show that beyond nucleobases the sugar components of the first informational polymers can be synthesized in this way. We demonstrate that a laser-induced high-energy chemistry combined with TiO2 catalysis readily produces a mixture of pentoses, among them ribose, arabinose and xylose. This chemistry might be highly relevant to the Late Heavy Bombardment period of Earth's history about 4-3.85 billion years ago. In addition, we present an in-depth theoretical analysis of the most challenging step of the reaction pathway, i.e., the TiO2-catalyzed dimerization of formaldehyde leading to glycolaldehyde.
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http://dx.doi.org/10.1038/srep23199 | DOI Listing |
Nanomaterials (Basel)
December 2017
Department of Chemistry, University of Crete, Voutes, 71003 Iraklion, Greece.
A simple method for the synthesis of formate esters and formamides is presented based on the Au/TiO₂-catalyzed aerobic oxidative coupling between alcohols or amines and formaldehyde. The suitable form of formaldehyde is paraformaldehyde, as cyclic trimeric 1,3,5-trioxane is inactive. The reaction proceeds via the formation of an intermediate hemiacetal or hemiaminal, respectively, followed by the Au nanoparticle-catalyzed aerobic oxidation of the intermediate.
View Article and Find Full Text PDFEnviron Sci Technol
August 2016
Department of Chemistry, ‡Department of Soil and Crop Sciences and §Department of Civil and Environmental Engineering, Colorado State University, Fort Collins, Colorado 80523, United States.
1,4-dioxane is an emerging groundwater contaminant with significant regulatory implications. Because it is resistant to traditional groundwater treatments, remediation of 1,4-dioxane is often limited to costly ex situ UV-based advanced oxidation. By varying applied voltage, electrical conductivity, seepage velocity, and influent contaminant concentration in flow-through reactors, we show that electrochemical oxidation is a viable technology for in situ and ex situ treatment of 1,4-dioxane under a wide range of environmental conditions.
View Article and Find Full Text PDFSci Rep
March 2016
Institute of Biophysics, Academy of Sciences of the Czech Republic, Královopolská 135, CZ-612 65 Brno, Czech Republic.
Recent synthetic efforts aimed at reconstructing the beginning of life on our planet point at the plausibility of scenarios fueled by extraterrestrial energy sources. In the current work we show that beyond nucleobases the sugar components of the first informational polymers can be synthesized in this way. We demonstrate that a laser-induced high-energy chemistry combined with TiO2 catalysis readily produces a mixture of pentoses, among them ribose, arabinose and xylose.
View Article and Find Full Text PDFChemosphere
January 2016
Department of Earth and Environmental Sciences and Research Institute of Natural Science (RINS), Gyeongsang National University, Jinju 660-701, Republic of Korea. Electronic address:
A photo-oxidation process using UV-LEDs and TiO2 was studied for removal of cyanide contained in mine wastewater and leachates. This study focused on monitoring of a TiO2-catalyzed LED photo-oxidation process, particularly emphasizing the effects of TiO2 form and light source on the efficiency of cyanide removal. The generation of hydroxyl radicals was also examined during the process to evaluate the mechanism of the photo-catalytic process.
View Article and Find Full Text PDF