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The critical role of βPdZn alloy in Pd/ZnO catalysts for the hydrogenation of carbon dioxide to methanol

DOI: 10.1021/acscatal.2c00552 DOI Help

Authors: Michael Bowker (Cardiff Catalysis Institute, Cardiff University) , Naomi Lawes (Cardiff Catalysis Institute, Cardiff University) , Isla Gow (Cardiff Catalysis Institute, Cardiff University) , James Hayward (Cardiff Catalysis Institute, Cardiff University) , Jonathan Ruiz Esquius (Cardiff Catalysis Institute, Cardiff University) , Nia Richards (Cardiff Catalysis Institute, Cardiff University) , Louise R. Smith (Cardiff Catalysis Institute, Cardiff University) , Thomas J. A. Slater (Cardiff Catalysis Institute, Cardiff University; Diamond Light Source) , Thomas E. Davies (Cardiff Catalysis Institute, Cardiff University) , Nicholas F. Dummer (Cardiff Catalysis Institute, Cardiff University) , Lara Kabalan (Cardiff Catalysis Institute, Cardiff University) , Andrew Logsdail (Cardiff Catalysis Institute, Cardiff University) , Richard C. Catlow (Cardiff Catalysis Institute, Cardiff University) , Stuart Taylor (Cardiff Catalysis Institute, Cardiff University) , Graham J Hutchings (Cardiff Catalysis Institute, Cardiff University)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Acs Catalysis , VOL 4 , PAGES 5371 - 5379

State: Published (Approved)
Published: April 2022
Diamond Proposal Number(s): 27530

Open Access Open Access

Abstract: The rise in atmospheric CO2 concentration and the concomitant rise in global surface temperature have prompted massive research effort in designing catalytic routes to utilize CO2 as a feedstock. Prime among these is the hydrogenation of CO2 to make methanol, which is a key commodity chemical intermediate, a hydrogen storage molecule, and a possible future fuel for transport sectors that cannot be electrified. Pd/ZnO has been identified as an effective candidate as a catalyst for this reaction, yet there has been no attempt to gain a fundamental understanding of how this catalyst works and more importantly to establish specific design criteria for CO2 hydrogenation catalysts. Here, we show that Pd/ZnO catalysts have the same metal particle composition, irrespective of the different synthesis procedures and types of ZnO used here. We demonstrate that all of these Pd/ZnO catalysts exhibit the same activity trend. In all cases, the β-PdZn 1:1 alloy is produced and dictates the catalysis. This conclusion is further supported by the relationship between conversion and selectivity and their small variation with ZnO surface area in the range 6–80 m2g–1. Without alloying with Zn, Pd is a reverse water-gas shift catalyst and when supported on alumina and silica is much less active for CO2 conversion to methanol than on ZnO. Our approach is applicable to the discovery and design of improved catalysts for CO2 hydrogenation and will aid future catalyst discovery.

Journal Keywords: methanol synthesis; PdZn alloy; catalysis; carbon dioxide hydrogenation; Pd catalyst; PdZn catalyst; zinc oxide support

Subject Areas: Chemistry, Environment

Diamond Offline Facilities: Electron Physical Sciences Imaging Centre (ePSIC)
Instruments: E01-JEM ARM 200CF

Added On: 21/04/2022 14:40

Documents:
acscatal.2c00552.pdf

Discipline Tags:

Earth Sciences & Environment Climate Change Physical Chemistry Catalysis Chemistry

Technical Tags:

Microscopy Electron Microscopy (EM) Scanning Transmission Electron Microscopy (STEM)