Metal-catalyst-free gas-phase synthesis of long-chain hydrocarbons.

Autor: Martínez L; ESISNA group. Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC), c/ Sor Juana Inés de la Cruz 3, 28049, Madrid, Spain., Merino P; ESISNA group. Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC), c/ Sor Juana Inés de la Cruz 3, 28049, Madrid, Spain.; Instituto de Física Fundamental (IFF-CSIC), c/ Serrano 123, 28006, Madrid, Spain., Santoro G; ESISNA group. Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC), c/ Sor Juana Inés de la Cruz 3, 28049, Madrid, Spain., Martínez JI; ESISNA group. Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC), c/ Sor Juana Inés de la Cruz 3, 28049, Madrid, Spain., Katsanoulis S; Institute for Mechanical Systems, ETH Zurich, Leonhardstrasse 21, 8092, Zurich, Switzerland., Ault J; School of Engineering, Brown University, Providence, RI, 02912, USA., Mayoral Á; Instituto de Nanociencia y Materiales de Aragon (INMA), Spanish National Research Council (CSIC), University of Zaragoza, 50009, Zaragoza, Spain.; Laboratorio de Microscopias Avanzadas (LMA), University of Zaragoza, 50009, Zaragoza, Spain.; Center for High-Resolution Electron Microscopy (CћEM), School of Physical Science and Technology, ShanghaiTech University, 393 Middle Huaxia Road, Pudong, Shanghai, 201210, China., Vázquez L; ESISNA group. Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC), c/ Sor Juana Inés de la Cruz 3, 28049, Madrid, Spain., Accolla M; ESISNA group. Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC), c/ Sor Juana Inés de la Cruz 3, 28049, Madrid, Spain.; Catania Astrophysical Observatory (INAF), Via Santa Sofia, 78, 95123, Catania, Italy., Dazzi A; Institute of Chemical Physics, Université Paris-Saclay, 91400, Orsay, France., Mathurin J; Institute of Chemical Physics, Université Paris-Saclay, 91400, Orsay, France., Borondics F; Synchrotron Soleil, L'Orme des Merisiers, Saint-Aubin - BP 48, 91192, Gif-sur-Yvette, France., Blázquez-Blázquez E; Instituto de Ciencia y Tecnología de Polímeros, ICTP-CSIC, c/ Juan de la Cierva 3, 28006, Madrid, Spain., Shauloff N; Department of Chemistry, Ben Gurion University of the Negev, Beer Sheva, 84105, Israel., Lebrón-Aguilar R; Instituto de Química-Física Rocasolano (IQFR-CSIC), c/ Serrano 119, 28006, Madrid, Spain., Quintanilla-López JE; Instituto de Química-Física Rocasolano (IQFR-CSIC), c/ Serrano 119, 28006, Madrid, Spain., Jelinek R; Department of Chemistry, Ben Gurion University of the Negev, Beer Sheva, 84105, Israel., Cernicharo J; Instituto de Física Fundamental (IFF-CSIC), c/ Serrano 123, 28006, Madrid, Spain., Stone HA; Department of Mechanical and Aerospace Engineering, Princeton University, Princeton, NJ, 08544, USA., de la Peña O'Shea VA; Photoactivated Processes Unit IMDEA Energía, Av. Ramón de la Sagra, 3 28935, Móstoles, Spain., de Andres PL; ESISNA group. Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC), c/ Sor Juana Inés de la Cruz 3, 28049, Madrid, Spain. pedro.deandres@csic.es., Haller G; Institute for Mechanical Systems, ETH Zurich, Leonhardstrasse 21, 8092, Zurich, Switzerland. georgehaller@ethz.ch., Ellis GJ; Instituto de Ciencia y Tecnología de Polímeros, ICTP-CSIC, c/ Juan de la Cierva 3, 28006, Madrid, Spain. gary@ictp.csic.es., Martín-Gago JA; ESISNA group. Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC), c/ Sor Juana Inés de la Cruz 3, 28049, Madrid, Spain. gago@icmm.csic.es.; Institute of Physics of the CAS, Cukrovarnicka 10, Prague, Czech Republic. gago@icmm.csic.es.
Jazyk: angličtina
Zdroj: Nature communications [Nat Commun] 2021 Oct 12; Vol. 12 (1), pp. 5937. Date of Electronic Publication: 2021 Oct 12.
DOI: 10.1038/s41467-021-26184-0
Abstrakt: Development of sustainable processes for hydrocarbons synthesis is a fundamental challenge in chemistry since these are of unquestionable importance for the production of many essential synthetic chemicals, materials and carbon-based fuels. Current industrial processes rely on non-abundant metal catalysts, temperatures of hundreds of Celsius and pressures of tens of bars. We propose an alternative gas phase process under mild reaction conditions using only atomic carbon, molecular hydrogen and an inert carrier gas. We demonstrate that the presence of CH 2 and H radicals leads to efficient C-C chain growth, producing micron-length fibres of unbranched alkanes with an average length distribution between C 23 -C 33 . Ab-initio calculations uncover a thermodynamically favourable methylene coupling process on the surface of carbonaceous nanoparticles, which is kinematically facilitated by a trap-and-release mechanism of the reactants and nanoparticles that is confirmed by a steady incompressible flow simulation. This work could lead to future alternative sustainable synthetic routes to critical alkane-based chemicals or fuels.
(© 2021. The Author(s).)
Databáze: MEDLINE
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