Lewis Acid Strength of Interfacial Metal Sites Drives CH3OH Selectivity and Formation Rates on Cu-Based CO2 Hydrogenation Catalysts

Gina Noh, Erwin Lam, Daniel T. Bregante, Jordan Meyet, Petr Šot, David W. Flaherty, Christophe Copéret

Research output: Contribution to journalArticlepeer-review

Abstract

CH3OH formation rates in CO2 hydrogenation on Cu-based catalysts sensitively depend on the nature of the support and the presence of promoters. In this context, Cu nanoparticles supported on tailored supports (highly dispersed M on SiO2; M=Ti, Zr, Hf, Nb, Ta) were prepared via surface organometallic chemistry, and their catalytic performance was systematically investigated for CO2 hydrogenation to CH3OH. The presence of Lewis acid sites enhances CH3OH formation rate, likely originating from stabilization of formate and methoxy surface intermediates at the periphery of Cu nanoparticles, as evidenced by metrics of Lewis acid strength and detection of surface intermediates. The stabilization of surface intermediates depends on the strength of Lewis acid M sites, described by pyridine adsorption enthalpies and 13C chemical shifts of -OCH3 coordinated to M; these chemical shifts are demonstrated here to be a molecular descriptor for Lewis acid strength and reactivity in CO2 hydrogenation.

Original languageEnglish (US)
Pages (from-to)9650-9659
Number of pages10
JournalAngewandte Chemie - International Edition
Volume60
Issue number17
DOIs
StatePublished - Apr 19 2021

Keywords

  • CHOH synthesis
  • CO hydrogenation
  • Lewis acids
  • heterogeneous catalysis
  • surface organometallic chemistry

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

Fingerprint Dive into the research topics of 'Lewis Acid Strength of Interfacial Metal Sites Drives CH<sub>3</sub>OH Selectivity and Formation Rates on Cu-Based CO<sub>2</sub> Hydrogenation Catalysts'. Together they form a unique fingerprint.

Cite this