The Critical Role of βPdZn Alloy in Pd/ZnO Catalysts for the Hydrogenation of Carbon Dioxide to Methanol.

Autor: Bowker M; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, United Kingdom.; Catalyst Hub, RCAH, Rutherford Appleton Lab, Harwell, Oxford, Didcot OX11 0QX, United Kingdom.; Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, United Kingdom., Lawes N; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, United Kingdom.; Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, United Kingdom., Gow I; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, United Kingdom.; Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, United Kingdom., Hayward J; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, United Kingdom., Esquius JR; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, United Kingdom.; now at: Clean Energy Cluster, International Iberian Nanotechnology Laboratory (INL), Av. Mestre José Veiga, 4715-330 Braga, Portugal., Richards N; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, United Kingdom., Smith LR; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, United Kingdom.; Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, United Kingdom., Slater TJA; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, United Kingdom.; Electron Physical Sciences Imaging Centre, Diamond Light Source Ltd., Oxfordshire OX11 0DE, United Kingdom., Davies TE; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, United Kingdom., Dummer NF; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, United Kingdom.; Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, United Kingdom., Kabalan L; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, United Kingdom., Logsdail A; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, United Kingdom., Catlow RC; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, United Kingdom.; Catalyst Hub, RCAH, Rutherford Appleton Lab, Harwell, Oxford, Didcot OX11 0QX, United Kingdom.; Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, United Kingdom., Taylor S; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, United Kingdom.; Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, United Kingdom., Hutchings GJ; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, United Kingdom.; Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, United Kingdom.
Jazyk: angličtina
Zdroj: ACS catalysis [ACS Catal] 2022 May 06; Vol. 12 (9), pp. 5371-5379. Date of Electronic Publication: 2022 Apr 20.
DOI: 10.1021/acscatal.2c00552
Abstrakt: The rise in atmospheric CO 2 concentration and the concomitant rise in global surface temperature have prompted massive research effort in designing catalytic routes to utilize CO 2 as a feedstock. Prime among these is the hydrogenation of CO 2 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 CO 2 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 m 2 g -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 CO 2 conversion to methanol than on ZnO. Our approach is applicable to the discovery and design of improved catalysts for CO 2 hydrogenation and will aid future catalyst discovery.
Competing Interests: The authors declare no competing financial interest.
(© 2022 The Authors. Published by American Chemical Society.)
Databáze: MEDLINE
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