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

Autor: Alexandre Dazzi, Mario Accolla, José A. Martín-Gago, Jesús Eduardo Quintanilla-López, Jesse T. Ault, Lidia Martínez, Stergios Katsanoulis, Gonzalo Santoro, Luis Vázquez, Jérémie Mathurin, Nitzan Shauloff, Pablo Merino, Alvaro Mayoral, Enrique Blázquez-Blázquez, Víctor A. de la Peña O’Shea, Raz Jelinek, Pedro L. de Andrés, José I. Martínez, George Haller, Ferenc Borondics, Gary Ellis, José Cernicharo, Rosa Lebrón-Aguilar, Howard A. Stone
Přispěvatelé: European Research Council, Ministerio de Economía y Competitividad (España), Comunidad de Madrid, Ministerio de Ciencia e Innovación (España), Gobierno de Aragón, National Natural Science Foundation of China, ShanghaiTech University, German Research Foundation, Martínez, Lidia [0000-0002-9370-2962], Merino, Pablo [0000-0002-0267-4020], Santoro, Gonzalo [0000-0003-4751-2209], Martínez, José I. [0000-0002-2086-8603], Katsanoulis, Stergios [0000-0002-1186-5937], Mayoral, Álvaro [0000-0002-5229-2717], Vázquez, Luis [0000-0001-6220-2810], Accolla, Mario [0000-0002-9509-5967], Borondics, Ferenc [0000-0001-9975-4301], Blázquez-Blázquez, Enrique [0000-0003-2488-5635], Lebrón-Aguilar, Rosa [0000-0001-6103-6814], Quintanilla-López, Jesús Eduardo [0000-0003-1863-7408], Jelinek, Raz [0000-0002-0336-1384], Cernicharo, José [0000-0002-3518-2524], Stone, Howard A. [0000-0002-9670-0639], Peña O'Shea, Víctor A. de la [0000-0001-5762-4787], de Andrés Rodríguez, Pedro Luis [0000-0002-9012-2890], Haller, George [0000-0003-1260-877X], Ellis, Gary James [0000-0003-4851-6092], Martín-Gago, José A. [0000-0003-2663-491X], Martínez, Lidia, Merino, Pablo, Santoro, Gonzalo, Martínez, José I., Katsanoulis, Stergios, Mayoral, Álvaro, Vázquez, Luis, Accolla, Mario, Borondics, Ferenc, Blázquez-Blázquez, Enrique, Lebrón-Aguilar, Rosa, Quintanilla-López, Jesús Eduardo, Jelinek, Raz, Cernicharo, José, Stone, Howard A., Peña O'Shea, Víctor A. de la, de Andrés Rodríguez, Pedro Luis, Haller, George, Ellis, Gary James, Martín-Gago, José A., Instituto de Ciencia de Materiales de Madrid (ICMM), Consejo Superior de Investigaciones Científicas [Madrid] (CSIC), Max-Planck-Institut für Festkörperforschung, Max-Planck-Gesellschaft, Instituto de Física Fundamental [Madrid] (IFF), Institut des Biomolécules Max Mousseron [Pôle Chimie Balard] (IBMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), ETH Zurich, School of Engineering (Brown Engineering), Brown University, ShanghaiTech University [Shanghai], University of Zaragoza - Universidad de Zaragoza [Zaragoza], Institut de Chimie Physique (ICP), Institut de Chimie du CNRS (INC)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Instituto de Ciencia y Tecnologia de Polimeros (ICTP-CSIC), Ben-Gurion University of the Negev (BGU), Instituto de Química Física Rocasolano (IQFR), Department of Mechanical and Aerospace Engineering [Princeton] (MAE), Princeton University, Photoactivated Processes Unit IMDEA Energía, European Project: 610256,EC:FP7:ERC,ERC-2013-SyG,NANOCOSMOS(2014)
Rok vydání: 2021
Předmět:
Zdroj: Digital.CSIC. Repositorio Institucional del CSIC
instname
Zaguán. Repositorio Digital de la Universidad de Zaragoza
Nature Communications
Nature Communications, 2021, 12, pp.5937. ⟨10.1038/s41467-021-26184-0⟩
Nature Communications, Vol 12, Iss 1, Pp 1-8 (2021)
ISSN: 2041-1723
Popis: 8 pags, 4 figs. -- The online version contains supplementary material available at https://doi.org/10.1038/s41467-021-26184-0
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 CH2 and H radicals leads to efficient C-C chain growth, producing micron-length fibres of unbranched alkanes with an average length distribution between C23-C33. 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.
We thank Jose Criado for the artwork schematics of the system, in figures 4 and S1; Funding: We thank the European Research Council for funding support under Synergy grant ERC-2013-SyG, G.A. 610256 (NANOCOSMOS). Also, we acknowledge partial support from the Spanish MINECO through grants PID2020-113142RB-C21, PID2019106315RB-I00, and PID2019-106315RB-I00, EU ERC CoG HyMAP 648319, and from the regional government through project S2018-NMT-4367 (FotoArt-CM). AM acknowledges to the Spanish Ministry of Science (RYC2018-024561-I), to the Regional Government of Aragon (DGA E13_20R), to the National Natural Science Foundation of China (NFSC-21850410448, NSFC-21835002), and to the The Centre for Highresolution Electron Microscopy (ChEM), supported by SPST of ShanghaiTech University under contract No. EM02161943. S.K. and G.H. acknowledge funding from the Turbulent Superstructures Program of the German National Science Foundation (DFG)
Databáze: OpenAIRE
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