Synergistic ultraviolet and visible light photo-activation enables intensified low-temperature methanol synthesis over copper/zinc oxide/alumina

DOI: 10.1038/s41467-020-15445-z

Authors: Bingqiao Xie (UNSW Australia) , Roong Jien Wong (RMIT University; UK Catalysis Hub, Research Complex at Harwell) , Tze Hao Tan (UNSW Australia) , Michael Higham (UK Catalysis Hub, Research Complex at Harwell; Cardiff University) , Emma K. Gibson (UK Catalysis Hub, Research Complex at Harwell; University of Glasgow) , Donato Decarolis (UK Catalysis Hub, Research Complex at Harwell; Cardiff University) , June Callison (UK Catalysis Hub; Cardiff University) , Kondo-Francois Aguey-Zinsou (UNSW Australia) , Michael Bowker (UK Catalysis Hub, Research Complex at Harwell; University of Cardiff) , C. Richard A. Catlow (UK Catalysis Hub, Research Complex at Harwell; Cardiff University; University College London) , Jason Scott (UNSW Australia) , Rose Amal (UNSW Australia)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Nature Communications , VOL 11

State: Published (Approved)
Published: March 2020
Diamond Proposal Number(s): 19850

Abstract: Although photoexcitation has been employed to unlock the low-temperature equilibrium regimes of thermal catalysis, mechanism underlining potential interplay between electron excitations and surface chemical processes remains elusive. Here, we report an associative zinc oxide band-gap excitation and copper plasmonic excitation that can cooperatively promote methanol-production at the copper-zinc oxide interfacial perimeter of copper/zinc oxide/alumina (CZA) catalyst. Conversely, selective excitation of individual components only leads to the promotion of carbon monoxide production. Accompanied by the variation in surface copper oxidation state and local electronic structure of zinc, electrons originating from the zinc oxide excitation and copper plasmonic excitation serve to activate surface adsorbates, catalysing key elementary processes (namely formate conversion and hydrogen molecule activation), thus providing one explanation for the observed photothermal activity. These observations give valuable insights into the key elementary processes occurring on the surface of the CZA catalyst under light-heat dual activation.

Journal Keywords: Catalytic mechanisms; Electron transfer; Heterogeneous catalysis; Photocatalysis

Diamond Keywords: Photocatalysis

Subject Areas: Chemistry, Environment, Materials


Instruments: B18-Core EXAFS

Added On: 14/04/2020 13:42

Documents:
s41467-020-15445-z.pdf

Discipline Tags:

Earth Sciences & Environment Climate Change Physical Chemistry Catalysis Energy Materials Chemistry Materials Science

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS) Extended X-ray Absorption Fine Structure (EXAFS)