Surface-Controlled TiO<sub>2</sub> Nanocrystals with Catalytically Active Single-Site Co Incorporation for the Oxygen Evolution Reaction
Chang Liu, Soonho Kwon, Perrin Godbold, Grayson Johnson, Sooyeon Hwang, Cheng‐Jun Sun, Hua Zhou, William A. Goddard, Sen Zhang
Abstract
High Resolution Image Download MS PowerPoint Slide The design of advanced electrocatalysts is often hindered by uncertainties in identifying and controlling the active surfaces and catalytic centers within heterogeneous materials. Here we present the synthesis of single-site Co catalysts, substitutionally doped into surface-controlled TiO 2 anatase nanocrystals, aimed at enhancing the oxygen evolution reaction (OER). Grand canonical quantum mechanics calculations reveal that the kinetics of the OER, following an adsorbate evolution mechanism, is markedly influenced by the coordination environment of Co. The simulations suggest significantly higher turnover frequencies when Co is doped into the (001) surface of TiO 2 compared to the (101) surface. Consistent with the computational findings, experimental results show that Co-doped TiO 2 (Co-TiO 2 ) nanoplates with selectively exposed {001} surfaces exhibit enhanced current densities and turnover frequencies compared to Co-TiO 2 nanobipyramids with {101} surfaces. This study highlights the synergy between theoretical calculations and precision synthesis in the development of more effective catalysts.