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

Lidia Martínez, Pablo Merino, Gonzalo Santoro, José I. Martínez, Stergios Katsanoulis, Jesse Ault, Álvaro Mayoral, Luis Vázquez, Mario Accolla, Alexandre Dazzi, Jeremie Mathurin, Ferenc Borondics, Enrique Blázquez-Blázquez, Nitzan Shauloff, Rosa Lebrón-Aguilar, Jesús E. Quintanilla-López, Raz Jelinek, José Cernicharo, Howard A. Stone, Victor A. Peña O’Shea, Pedro L. Andres (), George Haller (), Gary J. Ellis () and José A. Martín-Gago ()
Additional contact information
Lidia Martínez: ESISNA group. Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC)
Pablo Merino: ESISNA group. Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC)
Gonzalo Santoro: ESISNA group. Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC)
José I. Martínez: ESISNA group. Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC)
Stergios Katsanoulis: ETH Zurich
Jesse Ault: Brown University
Álvaro Mayoral: University of Zaragoza
Luis Vázquez: ESISNA group. Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC)
Mario Accolla: ESISNA group. Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC)
Alexandre Dazzi: Université Paris-Saclay
Jeremie Mathurin: Université Paris-Saclay
Ferenc Borondics: Synchrotron Soleil, L’Orme des Merisiers, Saint-Aubin - BP 48
Enrique Blázquez-Blázquez: Instituto de Ciencia y Tecnología de Polímeros, ICTP-CSIC
Nitzan Shauloff: Ben Gurion University of the Negev
Rosa Lebrón-Aguilar: Instituto de Química-Física Rocasolano (IQFR-CSIC)
Jesús E. Quintanilla-López: Instituto de Química-Física Rocasolano (IQFR-CSIC)
Raz Jelinek: Ben Gurion University of the Negev
José Cernicharo: Instituto de Física Fundamental (IFF-CSIC)
Howard A. Stone: Princeton University
Victor A. Peña O’Shea: Photoactivated Processes Unit IMDEA Energía, Av. Ramón de la Sagra
Pedro L. Andres: ESISNA group. Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC)
George Haller: ETH Zurich
Gary J. Ellis: Instituto de Ciencia y Tecnología de Polímeros, ICTP-CSIC
José A. Martín-Gago: ESISNA group. Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC)

Nature Communications, 2021, vol. 12, issue 1, 1-8

Abstract: Abstract 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.

Date: 2021
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DOI: 10.1038/s41467-021-26184-0

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