Parallelized Screening of Characterized and DFT-Modeled Bimetallic Colloidal Cocatalysts for Photocatalytic Hydrogen Evolution

• Published in: ACS catalysis 2020-04, Vol.10 (7), p.4244-4252
• Main Authors: Lopato, Eric M, Eikey, Emily A, Simon, Zoe C, Back, Seoin, Tran, Kevin, Lewis, Jacqueline, Kowalewski, Jakub F, Yazdi, Sadegh, Kitchin, John R, Ulissi, Zachary W, Millstone, Jill E, Bernhard, Stefan
• Format: Article
• Language: English
• Subjects: 08 HYDROGEN; Chemistry
• ISSN: 2155-5435; 2155-5435
• DOI: 10.1021/acscatal.9b05404

Using a newly designed and developed parallelized photoreactor and colorimetric detection method, a large sampling of bimetallic cocatalysts (Pd/Sn, Pd/Mo, Pd/Ru, Pd/Pb, Pd/Ni, Ni/Sn, Mo/Sn, and Pt/Sn) for photocatalytic water reduction have been tested. Of these cocatalysts, the combination of palladium and tin showed the highest synergistic behavior and peak hydrogen gas production at a low relative fraction of palladium. The resulting palladium/tin bimetallic cocatalysts were characterized, and specifically, and scanning transmission electron microscopy energy-dispersive X-ray spectroscopy indicated that palladium and tin elements reside within the same particle. The experimental catalytic activity for the palladium/tin mixture was compared to density functional theory-derived energy values associated with the adsorption of hydrogen onto a surface. This comparison demonstrated that the typical peak found in electrochemical Sabatier volcano plots at ΔG H* = ∼0 eV were replicated in the experimental photocatalytic system with a peak activity observed at ΔGH* = −0.036 eV. Computational confirmation of the results expressed here demonstrates the efficacy of colorimetric detection of hydrogen in parallel and presents a model for increasingly rapid catalyst screening.