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Heterogeneous catalysis is at the heart of almost every chemical transformation to manufacture the products and materials that surround us in our daily lives. For a sustainable future we need better catalysts that lower the required energy to make those transformations happen. The development of computational methods such as density functional theory (DFT) over the past decades enables the accelerated design of new and improved catalysts.

Our group has many years of experience in the theory and simulation of chemical processes at surfaces, particularly those of relevance to heterogeneous catalysis. Currently, one focus of our research efforts is a special class of materials, so-called single atom alloys (SAAs). This promising new class of catalysts consists of noble coinage metal surfaces in which more reactive transition metals are atomically dispersed. These SAAs display exciting properties, which deviate from classical transition metal and alloy catalysts. We are interested in both fundamental surface properties, adsorbate binding, as well as modelling reactions and kinetic properties. This research effort, which has benefited from a close collaboration with groups at University College London and Tuft University has recently been recognized with the 2022 Faraday Division Horizon Prize of the Royal Society of Chemistry.

Since the successful predictions of new catalysts and their properties is strongly dependent on the accuracy of the computational method, another focus in our group is the development of efficient protocols to generate benchmark data to compare the workhorse DFT results with.

References:

[1] Observation and Characterization of Dicarbonyls on a RhCu Single-Atom Alloy. Y. Wang, J. Schumann,* E. E. Happel, V. Cinar, E. C. H. Sykes, M. Stamatakis, A. Michaelides, and R. T. Hannagan*, J.Phys.Chem. Lett. 2022, https://doi.org/10.1021/acs.jpclett.2c01596

[2] Tuning the Product Selectivity of Single-Atom Alloys by Active Site Modification. RT Hannagan, Y Wang, R Réocreux, J Schumann, M Stamatakis, ... Surf. Science 2022, 717, 121990.

[3] Periodic Trends in Adsorption Energies around Single-Atom Alloy Active Sites. J Schumann, Y Bao, RT Hannagan, ECH Sykes, M Stamatakis, A Michaelides J. Phys. Chem. Lett. 2021, 12 (41), 10060-10067.

[4] First-principles design of a single-atom–alloy propane dehydrogenation catalyst RT Hannagan, G Giannakakis, R Réocreux, J Schumann, J Finzel, ... Science 2021, 372 (6549), 1444-1447.

[5] Elucidating the Stability and Reactivity of Surface Intermediates on Single-Atom Alloy Catalysts. MT Darby, R Réocreux, ECH Sykes, A Michaelides, M Stamatakis ACS Catalysis (2018) 8, 5038

[6] Lonely Atoms with Special Gifts. Matthew T. Darby, Michail Stamatakis, Angelos Michaelides, and E. Charles. H. Sykes* J. Phys. Chem. Lett. 

[7] Carbon Monoxide Poisoning Resistance and Structural Stability of Single Atom Alloys. MT Darby, ECH Sykes, A Michaelides, M Stamatakis. Topics in catalysis  (2018)  61, 428

[8] Pt/Cu single-atom alloys as coke-resistant catalysts for efficient C-H activation. MD Marcinkowski, MT Darby, J Liu, JM Wimble, FR Lucci, S Lee, A Michaelides, M Flytzani-Stephanopoulos, M Stamatakis, ECH Sykes. Nat Chem (2018) 10, 325

[9] Controlling Hydrogen Activation, Spillover, and Desorption with Pd-Au Single-Atom Alloys. FR Lucci, MT Darby, MFG Mattera, CJ Ivimey, AJ Therrien, A Michaelides, M Stamatakis, ECH Sykes J Phys Chem Lett  (2016)  7, 480

Related Publications 

Stick or Spill? Scaling Relationships for the Binding Energies of Adsorbates on Single-Atom Alloy Catalysts.
R Réocreux, ECH Sykes, A Michaelides, M Stamatakis – The Journal of Physical Chemistry Letters (2022) 13, 7314
Observation and Characterization of Dicarbonyls on a RhCu Single-Atom Alloy
Y Wang, J Schumann, EE Happel, V Çınar, ECH Sykes, M Stamatakis, A Michaelides, RT Hannagan – J Phys Chem Lett (2022) 13, 6316
Periodic Trends in Adsorption Energies around Single-Atom Alloy Active Sites.
J Schumann, Y Bao, RT Hannagan, ECH Sykes, M Stamatakis, A Michaelides – The Journal of Physical Chemistry Letters (2021) 12, 10060