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. de la Peña O’SheaPedro L. de Andres, George Haller, Gary J. Ellis, José A. Martín-Gago

Research output: Contribution to journalArticlepeer-review

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.

Original languageAmerican English
Article number5937
JournalNature Communications
Volume12
Issue number1
DOIs
StatePublished - 1 Dec 2021

All Science Journal Classification (ASJC) codes

  • General Chemistry
  • General Biochemistry,Genetics and Molecular Biology
  • General Physics and Astronomy

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