The mechanism of hydrogen donation by bio-acids over metal supported on nitrogen-doped carbon nanotubes

Jiajun Zhang, Xiaolei Zhang, Amin Osatiashtiani, Kai Hong Luo, Dekui Shen, Jun Li, Anthony Bridgwater

Research output: Contribution to journalArticle

Abstract

Biomass-derived carboxylic acids (e.g. acetic acid AcOH and formic acid FA) are a green and low-cost hydrogen source to replace hazardous H2 gas in in-situ hydrogenation processes. To date, bio-acids dehydrogenation has been mainly conducted using noble metal catalysts which would negatively impact the process economy, thus development of efficient non-noble metal catalysts for this purpose is highly desirable. In this study, the performance of transition metals supported on nitrogen doped carbon nanotubes was thoroughly evaluated by computational modelling based on Density Functional Theory (DFT). Results revealed that, out of the 10 selected transition metal candidates, molybdenum (Mo) was most active for binding AcOH and a combination of Mo and nitrogen doping significantly enhanced binding to the carboxylic acid molecules compared to pristine carbon nanotubes (CNTs). The newly designed Mo/N-CNT catalysts considerably facilitated the bio-acids decomposition compared to the non-catalytic scenarios by lowering energy barriers. FA distinctly outperformed AcOH in hydrogen donation over Mo/N-CNT catalysts, through its spontaneous cleavage leading to facile hydrogen donation.
Original languageEnglish
Article number111289
Number of pages11
JournalMolecular Catalysis
Early online date4 Nov 2020
DOIs
Publication statusE-pub ahead of print - 4 Nov 2020

Keywords

  • acetic acid
  • formic acid
  • carbon nanotubes
  • molybdenum
  • biomass

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